One-step electrodeposition prepared MoS2 composed Ni3S2 /Ni(OH)2 nanosheets as high efficient and stable metal sulfide catalyst for hydrogen precipitation in alkaline solutions

One-step electrodeposition prepared MoS2 composed Ni3S2 /Ni(OH)2 nanosheets as high efficient and stable metal sulfide catalyst for hydrogen precipitation in alkaline solutions | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Research Article One-step electrodeposition prepared MoS 2 composed Ni 3 S 2 /Ni(OH) 2 nanosheets as high efficient and stable metal sulfide catalyst for hydrogen precipitation in alkaline solutions Shunming Li, Pengyu Hu, Jingzong Qu, Jie Zhou, Zibo Wang, Yanan Wang, and 2 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-6288116/v1 This work is licensed under a CC BY 4.0 License Status: Under Review Version 1 posted 11 You are reading this latest preprint version Abstract Preparing a cheap efficient water-resolved hydrogen electrocatalyst and used it in alkaline media is important path for hydrogen conversion and storage. Herein, a MoS 2 /Ni 3 S 2 /Ni(OH) 2 on nickle form nanoflower composited electrocatalyst were synthesized via a simple one-step electrodeposition method by using a nickel foam (NF) as the based material. The obtained MoS 2 nanoflower via this simple one-step electrodeposition method has controllable strength, uniform growth and easy operated by tuning the electrodeposition coefficient and controlling the electrodeposition time. Meanwhile, the common factor leads to poor HER performance, like incomplete exposure of the active site caused by the incontrollable formation of MoS 2 blocks, was successfully avoided. The electrodeposited MoS 2 nanoflowers and Ni 3 S 2 played an important role for reducing potential during hydrogen precipitation by synergistic effects. This synergy between the two effective catalyst promotes electron transport abilities and exposes more active-sites, leading to an enhanced HER performance. In the alkaline solution of 1.0m NaOH, the graded MoS 2 /Ni 3 S 2 /Ni(OH) 2 @NF-5min electrode shows a respectively overpotential of 48 mV at 10 mA cm -2 and 175 mV at 100mA cm -2 , whilst high conductivity and good stability with the current maintained efficient for 72 hours under current density of 10mA cm -2 after 5000 cycles. Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Figure 6 Figure 7 Introduction Environmental and energy crisis has been a hot issue in today's society, finding and developing sustainable and clean energy technologies to replace traditional fossil fuels is very important. [ 1 , 2 ] In the past few decades, alternative energy have started to replace some of the traditional fossil fuels. However, caused by the distribution and geographical imitations, some renewable energy sources, like solar and geothermal, are astricted in large-scale applications. [ 3 , 4 ] Hydrogen stands out as a recognized extensive renewable energy source caused by high energy density with clean outcomes and widely gainable characteristics. [ 5 , 6 ] Among various low-cost methods for the preparation of high-purity hydrogen products, electrochemical hydrolysis is the most widely efficient adopted methods.[ 7 , 8 ] However, the hydrogen precipitation reaction (HER) involves two important half-reactions in electrochemical hydrolysis that are kinetically slow and require highly active electrocatalysts to accelerate the reaction. Noble metals can effectively lower the energy barrier and alters its kinetics, but expensive and scarcity noble catalysts also limited the hydrolysis techniques for large-scale production. [ 9 , 10 ] Therefore, the innovation and production of low-cost stable electrocatalysts remains as a important task for hydrolysis research. [ 11 – 16 ]In recent years, various materials, including transition metal alloys [ 17 – 21 ] and transition metal disulfides [ 22 – 28 ], have been broadly researched as possible substitutes for HER electrocatalysts. Compared to metal oxides, metal sulfide shows unique advantages like shallow valence bands, exhibiting strong quantum size effects with widely range chemical compositions, and some excellent optical response. Moreover, metal sulfides show significant enhancements in composite conductivity, surface morphology, and durability, which are more favorable for efficient energy conversion and storage applications. MoS 2 has received much attention because of its tunable band gap width as well as its unique two-dimensional layered structure and tunable electron transport. However, MoS 2 does not exhibit excellent HER[ 29 – 41 ] performance due to the incomplete exposure of the commonly prepared bulk MoS 2 active sites and the low electron conductivity.[ 42 – 54 ] Therefore, in this study, we designed a one-step electrodeposition method to generate three-dimensional MoS 2 nanoflowers on Ni 3 S 2 , which can largely expose the active edge sites of MoS 2 and shorten the electron transfer distance, as well as exhibit the HER properties of MoS 2 .[ 55 – 60 ] In particular, the obtained MoS 2 /Ni 3 S 2 /Ni(OH) 2 @NF-5min electrocatalysts has respectively low overpotentials of 48 mV at 10 mA cm − 2 and 175 mV at 100 mA cm − 2 , and exhibits great conductivity and durability in 1.0 M NaOH solutions, which shows an excellent application prospect for hydrogen production. Experimental section Preparation of Ni (OH) 2 and Ni 3 S 2 /Ni (OH) 2 Before preparation, Nickel foam (donated as NF，surface density 280 gm -2 , 0.5 mm, Kunshan Desco Electronics Co.) of 2.5 cm × 3.5 cm size were sonicated for 10 mins in acetone solution to remove dirt. After that, a acetone-treated NF was cleaned using ethanol and deionized water (DI). Then, the cleaned NF was immersed to remove oxides in 3 M HCl solution for 15 minutes, followed by a 10-minute wash using ethanol and deionized water and 12 hours vacuum dried at 60 °C. The Ni(OH) 2 loaded on nickel foam was prepared by one-step hydrothermal methods [61]. 1 m mol Nickel nitrate hexahydrate (Ni(NO 3 ) 2 -6H 2 O, AR 99%) and 6 mol ammonium fluoride (H 4 FN, AR 98%), and 12 mol urea (CO(NH 2 ) 2 , AR 99%) were dissolved in 40 mL of deionized water in turn and stirred for 30 min until the mixture was clear and transparent. The aqueous solution was transferred to a 50 mL vol stainless steel autoclave and the treated NF was added into the autoclave and sealed in a muffle furnace for 12 hours hydrothermal at 120 °C. Then the NF nanosheets with Ni(OH) 2 (Ni(OH) 2 @NF) were repeatedly rinsed and overnight dried at 60 °C. The Ni 3 S 2 /Ni(OH) 2 loaded on NF was prepared by hydrothermal combined with low-temperature vulcanization process [61]. 40 mL of 0.05 mol/L aqueous Na 2 S-9H 2 O solution was configured, and the solution was stirred until it was clear and transparent, and then the aqueous solution was transferred to a 50 mL stainless steel autoclave, and Ni(OH) 2 @NF was placed. The precursor was sealed into autoclave and placed in a muffle furnace at 100°C for 12 hours. The prepared material was rinsed repeatedly to obtain nanoflower-likes nanosheets with Ni 3 S 2 /Ni(OH) 2 (Ni 3 S 2 /Ni (OH) 2 @NF). The obtained samples were then dried at 60 °C for 10 hours to obtain Ni 3 S 2 /Ni(OH) 2 (Ni 3 S 2 /Ni(OH) 2 @NF composits. Electrodeposition of MoS 2 on nano-flowered Ni 3 S 2 /Ni (OH) 2 MoS 2 nanoflowers were electrodeposited [62] in a three-electrode system by using a CH660E workstation to generate nanoflower-like MoS 2 by constant potential electrodeposition on Ni 3 S 2 /Ni(OH) 2 /NF precursors. The deposition electrolyte contains 10 mM sodium molybdate dihydrate (Na 2 MoO 4 -2H 2 O, AR 99%), 20 mM sodium citrate dihydrate (Na 3 C 6 H 5 O 7 -2H 2 O, AR 99%) sodium citrate (Na 3 C 6 H 5 O 7 -2H 2 O, AR 99%) and 0.75 M thiourea (CH 4 N 2 S, AR 99%) were configured into a 50 mL electrolyte solution. All the chemicals were purchased from Aladdin Biochemical Technology company. The electrodeposition of MoS 2 in the three-electrode system , the Ni 3 S 2 /Ni(OH) 2 /NF precursors were used as working electrodes with the 2 × 2 cm 2 area and deposited at a constant potential of -1.0 V at room temperature. In order to optimize the electrodes for electrodeposition, the electrodeposition time was controlled for 1min, 3min, 5min, 7min, respectively, and the obtained materials were labeled as MoS 2 /Ni 3 S 2 /Ni(OH) 2 @NF-1min, 3min, 5 min, 7 min, and then the obtained electrodes were washed by ethanol and deionized water for three times, followed by 12 hours vacuum drying at 60 °C. According to the best electrochemical performance of different electrodeposition times, 5 min deposition samples has the best performance with a loading mass of 0.061 mg cm -2 . Characterizations The morphology information of samples was analyzed by a scanning electron microscopy (SEM) at an accelerating voltage of 15 kV. Powder X-ray diffraction (XRD) data were recorded on a Rigaku TTRIII-18KW diffractometer using Cu Kα radiation (λ = 1.5418 Å) in the range of 10 to 90° at 40 kV and 30 mA current. Characterization of the chemical composition and oxidation state of the sample surface was performed with X-ray photoelectron spectroscopy (XPS) testing with an Al Kα source. The surface charge was corrected by spectroscopically referencing the C 1s peak of the C-C bond with a binding energy of 284.8 eV. Transmission electron microscopy (TEM) analysis was performed on a J Tecnai G2 F30 S-TWIN operating at an accelerating voltage of 300 kV, and energy dispersive X-ray spectroscopy (EDS) was performed for elemental analysis and distribution. Electrochemical measurements All electrochemical tests were performed in a three-electrode system in 1.0 M KOH using a CHI660E electrochemical workstation ( Chenhua Co., Ltd., Shanghai, China) to evaluate the hydrolysis performance of the prepared materials. The prepared electrocatalyst HER activity was evaluated using linear scanning voltammetry (LSV) at a scan rate of 5 mv s -1 with 90% iR compensation to obtain a polarization curve. a reversible hydrogen electrode (RHE) was convert followed equation: E(RHE) = E (Hg/HgO) + 0.095 × PH + 0.098 and to recorrected 90% iR compensation. EIS (electrochemical impedance spectra) were measured at overpotential with an AC amplitude of 10 mV from100 kHz to 0.01 Hz. The obtained from cyclic voltmeter-ammeter curves (CV) at different scan rates, from the double layer capacitance (C dl ),was used to estimate the electrochemically active surface. Stability testing of the catalysts was characterized by LSV after continuous CV cycling and by the timed current method (I-t). Results and Discussion Figure 1 schematically illustrated the procedure of MoS 2 /Ni 3 S 2 / Ni(OH) 2 @NF catalysts via a combined electrodeposition and hydrothermal reaction. The electrodeposition of MoS 2 was controlled by electrodeposition time to regulate the number and thickness of the generated nanoflowers, aiming to exhibit highest activity sites. Whereas, the intermediate produced Ni 3 S 2 /Ni(OH) 2 on nickel foam was processed by co-precipitation and sulfidation treatment. Ni 2+ reacted with water ions in Ni(OH) 2 to generate interlaced nanosheets, while the Ni 3 S 2 was treated with Na 2 S solution sulfidation, and sulfur ions reacted with Ni 2+ on surface of Ni(OH) 2 @NF to reconstructed a lamellar structure. Finally, the Ni 3 S 2 / Ni(OH) 2 @NF catalysts were electrodeposited under different time for obtaining MoS 2 /Ni 3 S 2 /Ni(OH) 2 @NF catalysts. Scanning electron microscopy (SEM, company )was applied to understand the morphologies of Ni(OH) 2 @NF, Ni 3 S 2 /Ni(OH) 2 @NF and MoS 2 /Ni 3 S 2 /Ni(OH) 2 @NF catalysts. The morphology of Ni(OH) 2 @NF (as shown in Figure. 2a, b) indicated that the prepared Ni(OH) 2 grown uniformly on the NF andNi(OH) 2 appears as regular uniform flakes (Fig. 2b) and the nanosheet array was aligned and grows vertically and interconnected to a regular network structure. It is noteworthy that the obtained Ni(OH) 2 nanosheets had uniform and smooth surfaces, and extended volume ratio to enhanced the electroactive area. From Figure. 2 c and d, the morphology of the Ni 3 S 2 /Ni(OH) 2 @NF nanosheets synthesized after sulfidation didnot change significantly, but the smooth surface of the Ni(OH) 2 sheets was coarse by sulfidation reaction to produced Ni 3 S 2 . We investigated the influence of different electrodeposition times on the surface morphology of MoS 2 /Ni 3 S 2 /Ni(OH) 2 @NF catalysts. It was found that the MoS 2 attached to Ni 3 S 2 /Ni(OH) 2 @NF with electrodeposition time of 5 min, as shown in Figure 3 a, b and c, which exhibited a flowers-like composed lamellar structures with a complete morphology, uniform and clear structure. In contrast, the MoS 2 generated at 7 min of electrodeposition was covered with a thin layer of frost-like while maintaining the original nanoflower morphology ( as shown in Fig. 3d, e and f). It can be seen that the the fraction of deposited MoS 2 was increased on nanosheets edge with the increase of electrodeposition time, like 7 mins deposition time. After studied its HER performance, the best HER performance was exhibited at the controlled electrodeposition time of 5 min, which the MoS 2 /Ni 3 S 2 /Ni(OH) 2 @NF catalyst formed with a clear structure, fast electron transport and higher exposed active sites. It also indicated the suitable amount of deposited MoS 2 highly affected its electrocatalytically abilities. In Figure 4, the XRD patterns illustrated the chemical composition of the prepared catalytic materials. From the diffraction peaks corresponding to Ni (PDF#87-0712) and Ni 3 S 2 (PDF#73-0698), it can be seen that the diffraction peaks were 44.49°, 51.84°, and 76.38° point to the {111}, {200}, and {220} faces of Ni, respectively. And the diffraction peaks at 21.81°, 30.88°, 38.38°, 50.25° and 55.49° are assigned to the {010}, {110}, {111}, {120} and {211} faces of Ni 3 S 2 . It indicated the presence of Ni 3 S 2 and other objects. But the peaks of MoS 2 were not observed, which indicated that the MoS 2 crystallinity of the sample material synthesized by electrodeposition was limited and the MoS 2 content considered from electrodeposition was not superscalar. Thus, the presence and function of doped MoS 2 should be determine by another methods, like TEM and XPS characterization. To further understand the morphological structure, HR-TEM was used. The TEM was measured using pieces peeled off from the deposited film (Figure 4b), and the high magnification TEM was measured under further magnification (Figure 4c). The lattice stripe is 0.2363 nm corresponding to [111] plane of Ni 3 S 2 was measured from Figure. 4c. and a lattice stripe of 0.6112 nm corresponding to the [002] plane of MoS 2 . The HAADF-STEM elemental mapping images (as shown in Figure 4d ) shows the Mo, Ni and S elements were separately and uniformly distributed on the surface of samples. XPS was used to study its constituent elements and their corresponding chemical valence states of the MoS 2 /Ni 3 S 2 /Ni(OH) 2 @NF catalyst, as the total spectrum in Figure 5a. Figure 5b shows the characteristic peaks of Ni 2P for MoS 2 /Ni 3 S 2 /Ni(OH) 2 , where the two spin-orbit double peaks at 872.9 eV and 855.2 eV correspond to Ni 2p 1/2 and Ni 2 p 3/2 ,(格式) confirming the formation of Ni 3 S 2 . Between two Ni 2P peaks, the spin-orbit splitting energy is 17.7 eV indicated that the appearance of /Ni(OH) 2 [63], and there were two satellites at 879.1 eV and 861.8 eV.[64, 65] In the S 2p spectrum in Figure 5c, the peak at binding energy 161.3 eV corresponds to S 2p 1/2 and the peak out of binding energy 162.8 eV corresponds to S 2p 3/2 , proving the presence of S 2- . Notably, the peak at binding energy 168.1 eV was assigned to the satellite peak [ref]. In the core spectrum of the Mo 3d spectrum in Figure 5d, the Mo 3d spectrum was infit indicated that there had two spin-orbit double peaks centered at binding energies 234.9 eV and 231.7 eV, consistent with the Mo 4+ 3d 3/2 and Mo 4+ 3d 5/2 states, respectively, indicating there was a tetravalent state of Mo formation. In addition, the peak out of the binding energy is 226.1 eV indicated that the formation of Mo 6+ 3d 3/2 state was present. The HER activity of MoS 2 /Ni 3 S 2 /Ni (OH) 2 @NF electrocatalysts was evaluated in a standard three-electrode system in saturated 1 M KOH electrolyte solution at 5 mv s -1 scan rate. To explore the effects of MoS 2 in HER reaction, comparison samples were prepared and tested, such as bare Ni 3 S 2 /Ni (OH) 2 and Ni 3 S 2 /Ni (OH) 2 with electrodeposited MoS 2 by different deposition time.. Figure 6a compared the linear scanning voltammetry (LSV) curves of Pt/C, NF, Ni 3 S 2 /Ni(OH) 2 , and electrodeposited MoS 2 /Ni 3 S 2 /Ni(OH) 2 @NF electrocatalysts. The MoS 2 /Ni 3 S 2 /Ni(OH) 2 @NF electrode had a lower overpotential than Ni 3 S 2 /Ni(OH) 2 and NF electrode, and closed to Pt electrode. The HER activity was significantly increased when MoS 2 was deposited on the Ni 3 S 2 /Ni(OH) 2 electrode (Fig. 6a), indicating that the nano-flower modified Ni 3 S 2 /Ni(OH) 2 electrode formed by electrodeposition of MoS 2 was more favorable in LSV test, which caused by its more exposing active sites and better charge transfer ability in electrolyte interface and internal transmission. The electrodes with different deposition times test results shows that the electrode with 5 min deposition time exhibited a optimal low overpotential of 48 mV overpotential at a fixed current density of 10 mA cm -2 in Figure. 6a, which approximated to commercial Pt/C. But the 7 min deposition sample had a higher overpotential, which might affected by more attached MoS 2 fractions blocked their active sites and adverse to their worser HER performance. For understanding its HER dynamics, we analyzed its Tafel plots, j 0 and electrochemical impedance (EIS) curves. As shown in Figure 6b, the fitted linear Tafel slopes used for commercial Pt/C (10 w t%), Ni(OH) 2 @NF, Ni 3 S 2 /Ni(OH) 2 , MoS 2 /Ni 3 S 2 /Ni(OH) 2 @NF-1min, 3min, 5min, and 7min samples corresponded to 45.5 mV dec -1 , 131.2 mV dec -1 , 118.6 mV dec -1 , 107.2 mV dec -1 , 97.4 mV dec -1 , 108.6 mV dec -1 . The Ni 3 S 2 /Ni(OH) 2 @NF electrocatalyst Tafel slopes via MoS 2 electrodeposition indicated that the hydrogen precipitation proceeded obeyed Volmer-Heyrovsky mechanism and rate-limited the electrochemical desorption process. The electrocatalysts deposited in MoS 2 for 5 min had a Tafel slope at 97.4 mV dec -1 , demonstrating it had a high catalytic efficiency and approached to commercial Pt/C. We plotted the overpotentials for current densities of 10 and 100 mA cm -2 and show them in Figure. 6c. MoS 2 /Ni 3 S 2 /Ni(OH) 2 @NF-5min electrodes required overpotentials at 48 mV and 175 mV, which obviously better than other catalysts but slightly lower than Pt/C. To further understand the differ of their HER kinetics, a electrochemical impedance spectroscopy (donated as EIS, as shown in Figure. 6d) was performed in 1.0 M NaOH solution in frequency from 0.01 to 100 kHz, and got their Nyquist plots. Among them, the MoS 2 /Ni 3 S 2 /Ni(OH) 2 @NF-5min catalyst had the smallest R ct among several catalyst materials with 3.8 Ω. These advantages were attributed to the introduced 3D MoS 2 enhanced the conductivity and promoted interface and catalyst internal charge transfer abilities. The other binary materials commonly got larger R ct , which may hinder the hydrogen precipitation to some extent. The comparison by EIS plots reveals that the reflection of MoS 2 clearly reduced the composite resistances and promoted the HER kinetic process. To further evaluate the hydrolysis abilities of MoS 2 /Ni 3 S 2 /Ni(OH) 2 @NF composites, we tested its bilayer capacitance (C dl ) and electrochemical active area (ECSA) via a cyclic voltmeter-ammeter scanning. As shown in Figure. 6e, the MoS 2 /Ni3S 2 /Ni(OH) 2 @NF catalysts showed larger C dl than Ni 3 S 2 /Ni(OH )2 @NF, Ni(OH) 2 @NF and NF with C dl of 52.23 mF cm -2 , 44.81 mF cm -2 , 41.83 mF cm -2 and 23.14 mF cm -2 , respectively. With Figure 7 illustrating, the ECSA obtained at different sweep CV curves of 0.04-0.16, it can be visualized that the electrochemically active area of MoS 2 /Ni 3 S 2 /Ni(OH) 2 @NF is larger, which confirms that the suitable introduction of MoS 2 extended more electrochemically active area. In addition, the stability of the electrocatalyst, we performed a stability test as shown in Figure 6f. After a 5000 CV cycling at a constant current density of 10 mA cm -2 for 72 hour, there is invisible current decay, which indicated that the composites synthesized by electrodeposited MoS 2 on Ni 3 S 2 /Ni(OH) 2 @NF has an outstanding stability. After the stability tests we performed XPS spectroscopy tests and SEM test for further determined its structural stability. The SEM results shows that the morphology change is inviable, as its valance states of Mo, S, Ni didnot alter from its XPS results in Figure, which illustrate that there were bare deconstructed after stability electrochemical tests and proves this Ni 3 S 2 /Ni(OH) 2 @NF nanoflowers have excellent electrocatalytical ability and stability. Conclusion In this work, we prepared a cheap efficient MoS 2 /Ni 3 S 2 /Ni(OH) 2 @NF catalyst via an one-step electrodepositing MoS 2 infractions on 3D nanoflower-like Ni 3 S 2 /Ni(OH) 2 @NF-based electrode. This catalyst exhibited low overpotentials of 48 at 10 mA cm -2 and 175 mV at 10 and 100 mA cm -2 current densities, as well as the long-stability of 72 hours current without decay after 5000 CV cycles at constant current density at 10 mA cm -2 . The electrodeposited MoS 2 nanoflowers and Ni 3 S 2 reduces overpotential for hydrogen precipitation process and synergically improves their electron transport abilities and exposes more active-sites, leading to an enhanced HER performance. Its excellent performance in HER and the simple and low-cost preparation procedure might provide a novel catalyst and new synthesis strategies for the sustainable hydrogen energy development. Abbreviations HER : Hydrogen Evolution Reaction NF : Nickel Foam LSV : Linear Scanning Voltammetry XRD : X-ray Diffraction XPS : X-ray Photoelectron Spectroscopy SEM : Scanning Electron Microscopy TEM : Transmission Electron Microscopy EDS : Energy Dispersive X-ray Spectroscopy EIS : Electrochemical Impedance Spectroscopy CV : Cyclic Voltammetry C~dl~ : Double Layer Capacitance ECSA : Electrochemically Active Surface Area RHE : Reversible Hydrogen Electrode R~ct~ : Charge Transfer Resistance NaOH : Sodium Hydroxide KOH : Potassium Hydroxide DI : Deionized AR : Analytical Reagent Declarations Ethical Approval and Consent to Participate : This study was approved by the relevant ethics committee, and all participants provided informed consent. Consent for Publication : All authors have read and approved the final manuscript for publication. Competing Interests : The authors declare that they have no known competing financial interests or personal relationships that could have influenced the work reported in this paper. This manuscript has not been published elsewhere. Author Contributions: Shunming Li : Performed experiments, analyzed data, and drafted the manuscript. Pengyu Hu : Conducted material characterization. Jingzong Qu : Contributed to manuscript drafting. Jie Zhou : Assisted in data analysis. Zibo Wang & Yanan Wang : Reviewed and revised the manuscript. Anran Chen : Supervised the experiments. Tao Sun : Oversaw the project, provided guidance, and administered the study. Funding: This work was supported by School of Materials and Energy, Yunnan University, Kunming. Data Availability: All data generated in this study are original and available upon reasonable request. Acknowledgments: I would like to express my deepest gratitude to my family for their unwavering support, encouragement, and patience throughout this research journey. Their love and understanding have been my greatest motivation. I am also sincerely thankful to my advisors and professors for their invaluable guidance, insightful feedback, and continuous encouragement. Additionally, I extend my appreciation to my colleagues and classmates for their stimulating discussions, technical assistance, and moral support, which greatly contributed to the completion of this work. Without their help, this achievement would not have been possible. Finally, I acknowledge all those who, directly or indirectly, supported me in this endeavor. References T.F. Li, G. Luo, K.H. Liu, X. Li, D.M. Sun, L. Xu, Y.F. Li, Y.W. Tang, Encapsulation of Ni3Fe Nanoparticles in N-Doped Carbon Nanotube-Grafted Carbon Nanofibers as High-Efficiency Hydrogen Evolution Electrocatalysts, Adv. Funct. Mater., 28 (2018) 9. 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Zhao, Controlled synthesis of Ni(OH)(2)/Ni3S2 hybrid nanosheet arrays as highly active and stable electrocatalysts for water splitting, Journal of Materials Chemistry A, 6 (2018) 6938-6946. B.S. Soram, J.Y. Dai, I.S. Thangjam, N.H. Kim, J.H. Lee, One-step electrodeposited MoS2@Ni-mesh electrode for flexible and transparent asymmetric solid-state supercapacitors, Journal of Materials Chemistry A, 8 (2020) 24040-24052. L. Zhang, I.S. Amiinu, X. Ren, Z. Liu, G. Du, A.M. Asiri, B. Zheng, X. Sun, Surface Modification of a NiS2 Nanoarray with Ni(OH)(2) toward Superior Water Reduction Electrocatalysis in Alkaline Media, Inorganic Chemistry, 56 (2017) 13651-13654. L. Lv, Z. Li, K.-H. Xue, Y. Ruan, X. Ao, H. Wan, X. Miao, B. Zhang, J. Jiang, C. Wang, K. Ostrikov, Tailoring the electrocatalytic activity of bimetallic nickel-iron diselenide hollow nanochains for water oxidation, Nano Energy, 47 (2018) 275-284. C. Wang, P. Zhang, J. Lei, W. Dong, J. Wang, Integrated 3D [email protected] Nanowire Network with Synergistic Cooperation as Highly Efficient Electrocatalysts for Hydrogen Evolution Reaction in Alkaline Medium, Electrochimica Acta, 246 (2017) 712-719. F. Yu, F. Li, B. Zhang, H. Li, L. Sun, Efficient Electrocatalytic Water Oxidation by a Copper Oxide Thin Film in Borate Buffer, Acs Catalysis, 5 (2015) 627-630. Additional Declarations No competing interests reported. Supplementary Files GraphicalAbstract.docx Cite Share Download PDF Status: Under Review Version 1 posted Editorial decision: Revision requested 03 Apr, 2025 Reviews received at journal 03 Apr, 2025 Reviews received at journal 03 Apr, 2025 Reviewers agreed at journal 02 Apr, 2025 Reviews received at journal 01 Apr, 2025 Reviewers agreed at journal 30 Mar, 2025 Reviewers agreed at journal 28 Mar, 2025 Reviewers invited by journal 28 Mar, 2025 Editor assigned by journal 28 Mar, 2025 Submission checks completed at journal 28 Mar, 2025 First submitted to journal 23 Mar, 2025 You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. As a division of Research Square Company, we’re committed to making research communication faster, fairer, and more useful. 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Also discoverable on Platform About Our Team In Review Editorial Policies Advisory Board Help Center Resources Author Services Accessibility API Access RSS feed Manage Cookie Preferences © Research Square 2026 | ISSN 2693-5015 (online) Privacy Policy Terms of Service Do Not Sell My Personal Information {"props":{"pageProps":{"initialData":{"identity":"rs-6288116","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Research Article","associatedPublications":[],"authors":[{"id":437944566,"identity":"a7c40f5a-1ff2-46ff-b846-4871ee81e20e","order_by":0,"name":"Shunming Li","email":"","orcid":"","institution":"Yunnan University","correspondingAuthor":false,"prefix":"","firstName":"Shunming","middleName":"","lastName":"Li","suffix":""},{"id":437944568,"identity":"5bca6ee7-fb73-48bf-925a-31e16c76de5b","order_by":1,"name":"Pengyu Hu","email":"","orcid":"","institution":"Yunnan 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Wang","email":"","orcid":"","institution":"Yunnan University","correspondingAuthor":false,"prefix":"","firstName":"Yanan","middleName":"","lastName":"Wang","suffix":""},{"id":437944573,"identity":"65914333-5d84-40fb-afd6-e4b4a33b4b25","order_by":6,"name":"Tao Sun","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAAzklEQVRIiWNgGAWjYPACGzk2+cMHDnz4QYRaHgiVZswvwZZ4cGYP8VoOJ86cwWN8mIONCC327IcPf+bdkWZscLvnw2GgCfL8YgcI2MKTlibNe8ZGzuDO2Q2HCywYDGfOTiDksBwzZt42oC0HcjccnsHDkGBwm5AW/jfGn3nbDiduOJDz4DAPGzFaJHIMpEFaZs7IYSBSy41naZJzgQ7j5zlmAAxkCcJ+Ye9PPvzhbRswKtmbH3/48MNGnl+agBZ0IEGa8lEwCkbBKBgF2AEAZ0xFXEaQM/UAAAAASUVORK5CYII=","orcid":"","institution":"Yunnan University","correspondingAuthor":true,"prefix":"","firstName":"Tao","middleName":"","lastName":"Sun","suffix":""},{"id":437944574,"identity":"5e524e77-f3f4-4188-86dc-df16290fe693","order_by":7,"name":"Anran Chen","email":"","orcid":"","institution":"Yunnan University","correspondingAuthor":false,"prefix":"","firstName":"Anran","middleName":"","lastName":"Chen","suffix":""}],"badges":[],"createdAt":"2025-03-23 12:08:22","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-6288116/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-6288116/v1","draftVersion":[],"editorialEvents":[],"editorialNote":"","failedWorkflow":false,"files":[{"id":80813202,"identity":"1523d481-69ab-4407-965a-3031871c3b33","added_by":"auto","created_at":"2025-04-17 10:39:50","extension":"png","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":103140,"visible":true,"origin":"","legend":"\u003cp\u003eSchematic diagram of MoS\u003csub\u003e2\u003c/sub\u003e/Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/ Ni (OH)\u003csub\u003e2\u003c/sub\u003e@NF preparation\u003c/p\u003e","description":"","filename":"floatimage1.png","url":"https://assets-eu.researchsquare.com/files/rs-6288116/v1/c836fc5fd40e5f2fef11efc9.png"},{"id":80815087,"identity":"620977e8-eb0d-4cb3-b51c-e343d6bd86b3","added_by":"auto","created_at":"2025-04-17 10:55:50","extension":"png","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":513371,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eSEM images of Ni(OH)2@NF (a, b) and Ni3S2/Ni(OH)2@NF (c, d)\u003c/strong\u003e\u003c/p\u003e","description":"","filename":"floatimage2.png","url":"https://assets-eu.researchsquare.com/files/rs-6288116/v1/374cf9cf8972c8ab03c8ae77.png"},{"id":80814306,"identity":"4addafbc-73da-4b2d-8ffb-78e0db269172","added_by":"auto","created_at":"2025-04-17 10:47:50","extension":"png","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":354769,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eSEM images of MoS2/Ni3S2/Ni(OH)2@NF-5min (a, b, c) and MoS2/Ni3S2/Ni(OH)2@NF-7min (d, e, f)\u003c/strong\u003e\u003c/p\u003e","description":"","filename":"floatimage3.png","url":"https://assets-eu.researchsquare.com/files/rs-6288116/v1/8b228bb74007414aaba9d9ea.png"},{"id":80814309,"identity":"b99bd34e-9b8c-4be9-bbd3-3a40b42362b9","added_by":"auto","created_at":"2025-04-17 10:47:50","extension":"png","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":371537,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003e(a) XRD images of MoS2/Ni3S2/Ni(OH)2@NF. (b) TEM image. (c) HRTEM image. (d) Corresponding EDS element mapping.\u003c/strong\u003e\u003c/p\u003e","description":"","filename":"floatimage4.png","url":"https://assets-eu.researchsquare.com/files/rs-6288116/v1/33b2ae0e0e899b877450bd79.png"},{"id":80815090,"identity":"e7532012-ded9-4a4a-af53-1177554cce74","added_by":"auto","created_at":"2025-04-17 10:55:50","extension":"png","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":209784,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eMoS2/Ni3S2/Ni(OH)2@NF-5min XPS spectra of (a) total spectrum, (b) Ni 2P, (c) S 2p and (d) Mo 3d peaks. (The binding energy of each elements were corrected using the C 1s peak at 284.8 eV.)\u003c/strong\u003e\u003c/p\u003e","description":"","filename":"floatimage5.png","url":"https://assets-eu.researchsquare.com/files/rs-6288116/v1/8b71f5c7b67579e0abd07879.png"},{"id":80813220,"identity":"db0e40b0-45df-4dc2-82d5-3451c79eae68","added_by":"auto","created_at":"2025-04-17 10:39:50","extension":"png","order_by":6,"title":"Figure 6","display":"","copyAsset":false,"role":"figure","size":239237,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003e(a) Pt/C, Ni (OH)2/NF, Ni3S2/ Ni (OH)2/NF, MoS2/ Ni3S2/ Ni(OH)2/NF-1min, LSV curves for MoS2/ Ni3S2/ Ni (OH)2/NF-3min, MoS2/ Ni3S2/ Ni(OH)2/NF-5min, MoS2/ Ni3S2/ Ni(OH)2/NF-7min, (b) Tafel slope, (c) corresponding overpotentials at 10 and 100 cm-2, and(d) impedance, （e）electrochemical double layer capacitance. (f) HER stability .\u003c/strong\u003e\u003c/p\u003e","description":"","filename":"floatimage6.png","url":"https://assets-eu.researchsquare.com/files/rs-6288116/v1/9585016c52390306a6adccc0.png"},{"id":80813207,"identity":"bf230d1e-8e7f-4d34-b02b-fa9f47337d98","added_by":"auto","created_at":"2025-04-17 10:39:50","extension":"png","order_by":7,"title":"Figure 7","display":"","copyAsset":false,"role":"figure","size":314291,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eECSA obtained from different sweep speed CV curves\u003c/strong\u003e\u003c/p\u003e","description":"","filename":"floatimage7.png","url":"https://assets-eu.researchsquare.com/files/rs-6288116/v1/64b83f8d47d8938c3e477fb2.png"},{"id":80815733,"identity":"62822275-3a9a-4e3b-81ee-c4d65ad133cd","added_by":"auto","created_at":"2025-04-17 11:03:50","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":3171324,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-6288116/v1/4f7dac94-ca35-43d5-af80-ec0108772ddc.pdf"},{"id":80814313,"identity":"b872110a-0df9-41f7-b2ab-0281a115d79b","added_by":"auto","created_at":"2025-04-17 10:47:50","extension":"docx","order_by":3,"title":"","display":"","copyAsset":false,"role":"supplement","size":256661,"visible":true,"origin":"","legend":"","description":"","filename":"GraphicalAbstract.docx","url":"https://assets-eu.researchsquare.com/files/rs-6288116/v1/ab0ef9d2df6a12e1ab43e53a.docx"}],"financialInterests":"No competing interests reported.","formattedTitle":"\u003cp\u003eOne-step electrodeposition prepared MoS\u003csub\u003e2\u003c/sub\u003e composed Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e /Ni(OH)\u003csub\u003e2\u003c/sub\u003e nanosheets as high efficient and stable metal sulfide catalyst for hydrogen precipitation in alkaline solutions\u003c/p\u003e","fulltext":[{"header":"Introduction","content":"\u003cp\u003eEnvironmental and energy crisis has been a hot issue in today's society, finding and developing sustainable and clean energy technologies to replace traditional fossil fuels is very important. [\u003cspan citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e, \u003cspan citationid=\"CR2\" class=\"CitationRef\"\u003e2\u003c/span\u003e] In the past few decades, alternative energy have started to replace some of the traditional fossil fuels. However, caused by the distribution and geographical imitations, some renewable energy sources, like solar and geothermal, are astricted in large-scale applications. [\u003cspan citationid=\"CR3\" class=\"CitationRef\"\u003e3\u003c/span\u003e, \u003cspan citationid=\"CR4\" class=\"CitationRef\"\u003e4\u003c/span\u003e] Hydrogen stands out as a recognized extensive renewable energy source caused by high energy density with clean outcomes and widely gainable characteristics. [\u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e]\u003c/p\u003e \u003cp\u003eAmong various low-cost methods for the preparation of high-purity hydrogen products, electrochemical hydrolysis is the most widely efficient adopted methods.[\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e] However, the hydrogen precipitation reaction (HER) involves two important half-reactions in electrochemical hydrolysis that are kinetically slow and require highly active electrocatalysts to accelerate the reaction. Noble metals can effectively lower the energy barrier and alters its kinetics, but expensive and scarcity noble catalysts also limited the hydrolysis techniques for large-scale production. [\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e, \u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e] Therefore, the innovation and production of low-cost stable electrocatalysts remains as a important task for hydrolysis research. [\u003cspan additionalcitationids=\"CR12 CR13 CR14 CR15\" citationid=\"CR11\" class=\"CitationRef\"\u003e11\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR16\" class=\"CitationRef\"\u003e16\u003c/span\u003e]In recent years, various materials, including transition metal alloys [\u003cspan additionalcitationids=\"CR18 CR19 CR20\" citationid=\"CR17\" class=\"CitationRef\"\u003e17\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR21\" class=\"CitationRef\"\u003e21\u003c/span\u003e] and transition metal disulfides [\u003cspan additionalcitationids=\"CR23 CR24 CR25 CR26 CR27\" citationid=\"CR22\" class=\"CitationRef\"\u003e22\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR28\" class=\"CitationRef\"\u003e28\u003c/span\u003e], have been broadly researched as possible substitutes for HER electrocatalysts. Compared to metal oxides, metal sulfide shows unique advantages like shallow valence bands, exhibiting strong quantum size effects with widely range chemical compositions, and some excellent optical response. Moreover, metal sulfides show significant enhancements in composite conductivity, surface morphology, and durability, which are more favorable for efficient energy conversion and storage applications.\u003c/p\u003e \u003cp\u003eMoS\u003csub\u003e2\u003c/sub\u003e has received much attention because of its tunable band gap width as well as its unique two-dimensional layered structure and tunable electron transport. However, MoS\u003csub\u003e2\u003c/sub\u003e does not exhibit excellent HER[\u003cspan additionalcitationids=\"CR30 CR31 CR32 CR33 CR34 CR35 CR36 CR37 CR38 CR39 CR40\" citationid=\"CR29\" class=\"CitationRef\"\u003e29\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR41\" class=\"CitationRef\"\u003e41\u003c/span\u003e] performance due to the incomplete exposure of the commonly prepared bulk MoS\u003csub\u003e2\u003c/sub\u003e active sites and the low electron conductivity.[\u003cspan additionalcitationids=\"CR43 CR44 CR45 CR46 CR47 CR48 CR49 CR50 CR51 CR52 CR53\" citationid=\"CR42\" class=\"CitationRef\"\u003e42\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR54\" class=\"CitationRef\"\u003e54\u003c/span\u003e] Therefore, in this study, we designed a one-step electrodeposition method to generate three-dimensional MoS\u003csub\u003e2\u003c/sub\u003e nanoflowers on Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e, which can largely expose the active edge sites of MoS\u003csub\u003e2\u003c/sub\u003e and shorten the electron transfer distance, as well as exhibit the HER properties of MoS\u003csub\u003e2\u003c/sub\u003e.[\u003cspan additionalcitationids=\"CR56 CR57 CR58 CR59\" citationid=\"CR55\" class=\"CitationRef\"\u003e55\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR60\" class=\"CitationRef\"\u003e60\u003c/span\u003e] In particular, the obtained MoS\u003csub\u003e2\u003c/sub\u003e/Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF-5min electrocatalysts has respectively low overpotentials of 48 mV at 10 mA cm\u003csup\u003e\u0026minus;\u0026thinsp;2\u003c/sup\u003e and 175 mV at 100 mA cm\u003csup\u003e\u0026minus;\u0026thinsp;2\u003c/sup\u003e, and exhibits great conductivity and durability in 1.0 M NaOH solutions, which shows an excellent application prospect for hydrogen production.\u003c/p\u003e"},{"header":"Experimental section","content":"\u003cp\u003e\u003cstrong\u003ePreparation of Ni (OH)\u003csub\u003e2\u003c/sub\u003e and Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni (OH)\u003csub\u003e2\u003c/sub\u003e\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eBefore preparation, Nickel foam (donated as NF，surface density 280 gm\u003csup\u003e-2\u003c/sup\u003e, 0.5 mm, Kunshan Desco Electronics Co.) of 2.5 cm \u0026times; 3.5 cm size were sonicated for 10 mins in acetone solution to remove dirt. After that, a acetone-treated NF was cleaned using ethanol and deionized water (DI). Then, the cleaned NF was immersed to remove oxides in 3 M HCl solution for 15 minutes, followed by a 10-minute wash using ethanol and deionized water and 12 hours vacuum dried at 60 \u0026deg;C. The Ni(OH)\u003csub\u003e2\u003c/sub\u003e loaded on nickel foam was prepared by one-step hydrothermal methods [61]. 1 m mol Nickel nitrate hexahydrate (Ni(NO\u003csub\u003e3\u003c/sub\u003e)\u003csub\u003e2\u003c/sub\u003e-6H\u003csub\u003e2\u003c/sub\u003eO, AR 99%) and 6 mol ammonium fluoride (H\u003csub\u003e4\u003c/sub\u003eFN, AR 98%), and 12 mol urea (CO(NH\u003csub\u003e2\u003c/sub\u003e)\u003csub\u003e2\u003c/sub\u003e, AR 99%) were dissolved in 40 mL of deionized water in turn and stirred for 30 min until the mixture was clear and transparent. The aqueous solution was transferred to a 50 mL vol stainless steel autoclave and the treated NF was added into the autoclave and sealed in a muffle furnace for 12 hours hydrothermal at 120 \u0026deg;C. Then the NF nanosheets with Ni(OH)\u003csub\u003e2\u003c/sub\u003e (Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF) were repeatedly rinsed and overnight dried at 60 \u0026deg;C. The Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e loaded on NF was prepared by hydrothermal combined with low-temperature vulcanization process [61]. 40 mL of 0.05 mol/L aqueous Na\u003csub\u003e2\u003c/sub\u003eS-9H\u003csub\u003e2\u003c/sub\u003eO solution was configured, and the solution was stirred until it was clear and transparent, and then the aqueous solution was transferred to a 50 mL stainless steel autoclave, and Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF was placed. The precursor was sealed into autoclave and placed in a muffle furnace at 100\u0026deg;C for 12 hours. The prepared material was rinsed repeatedly to obtain nanoflower-likes nanosheets with Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e(Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni (OH)\u003csub\u003e2\u003c/sub\u003e@NF). The obtained samples were then dried at 60 \u0026deg;C for 10 hours to obtain Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e (Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF composits.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eElectrodeposition of MoS\u003csub\u003e2\u0026nbsp;\u003c/sub\u003eon nano-flowered Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni (OH)\u003csub\u003e2\u003c/sub\u003e\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eMoS\u003csub\u003e2\u003c/sub\u003e nanoflowers were electrodeposited\u0026nbsp;[62]\u0026nbsp;in a three-electrode system by using a CH660E workstation to generate nanoflower-like MoS\u003csub\u003e2\u003c/sub\u003e by constant potential electrodeposition on Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e/NF precursors. The deposition electrolyte contains 10 mM sodium molybdate dihydrate (Na\u003csub\u003e2\u003c/sub\u003eMoO\u003csub\u003e4\u003c/sub\u003e-2H\u003csub\u003e2\u003c/sub\u003eO, AR 99%), 20 mM sodium citrate dihydrate (Na\u003csub\u003e3\u003c/sub\u003eC\u003csub\u003e6\u003c/sub\u003eH\u003csub\u003e5\u003c/sub\u003eO\u003csub\u003e7\u003c/sub\u003e-2H\u003csub\u003e2\u003c/sub\u003eO, AR 99%) sodium citrate (Na\u003csub\u003e3\u003c/sub\u003eC\u003csub\u003e6\u003c/sub\u003eH\u003csub\u003e5\u003c/sub\u003eO\u003csub\u003e7\u003c/sub\u003e-2H\u003csub\u003e2\u003c/sub\u003eO, AR 99%) and 0.75 M thiourea (CH\u003csub\u003e4\u003c/sub\u003eN\u003csub\u003e2\u003c/sub\u003eS, AR 99%) were configured into a 50 mL electrolyte solution. All the chemicals were purchased from Aladdin Biochemical Technology company. The electrodeposition of MoS\u003csub\u003e2\u003c/sub\u003e in the three-electrode system , the Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e/NF precursors were used as working electrodes with the 2 \u0026times; 2 cm\u003csup\u003e2\u0026nbsp;\u003c/sup\u003earea and deposited at a constant potential of -1.0 V at room temperature. In order to optimize the electrodes for electrodeposition, the electrodeposition time was controlled for 1min, 3min, 5min, 7min, respectively, and the obtained materials were labeled as MoS\u003csub\u003e2\u003c/sub\u003e/Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF-1min, 3min, 5 min, 7 min, and then the obtained electrodes were washed by ethanol and deionized water for three times, followed by 12 hours vacuum drying at 60 \u0026deg;C. According to the best electrochemical performance of different electrodeposition times, 5 min deposition samples has the best performance with a loading mass of 0.061 mg cm\u003csup\u003e-2\u003c/sup\u003e .\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eCharacterizations\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe morphology information of samples was analyzed by a scanning electron microscopy (SEM) at an accelerating voltage of 15 kV. Powder X-ray diffraction (XRD) data were recorded on a Rigaku TTRIII-18KW diffractometer using Cu K\u0026alpha; radiation (\u0026lambda; = 1.5418 \u0026Aring;) in the range of 10 to 90\u0026deg; at 40 kV and 30 mA current. Characterization of the chemical composition and oxidation state of the sample surface was performed with X-ray photoelectron spectroscopy (XPS) testing with an Al K\u0026alpha; source. The surface charge was corrected by spectroscopically referencing the C 1s peak of the C-C bond with a binding energy of 284.8 eV. Transmission electron microscopy (TEM) analysis was performed on a J Tecnai G2 F30 S-TWIN operating at an accelerating voltage of 300 kV, and energy dispersive X-ray spectroscopy (EDS) was performed for elemental analysis and distribution.\u003cstrong\u003e\u0026nbsp;\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eElectrochemical measurements\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eAll electrochemical tests were performed in a three-electrode system in 1.0 M KOH using a CHI660E electrochemical workstation ( Chenhua Co., Ltd., Shanghai, China) to evaluate the hydrolysis performance of the prepared materials. The prepared electrocatalyst HER activity was evaluated using linear scanning voltammetry (LSV) at a scan rate of 5 mv s\u003csup\u003e-1\u003c/sup\u003e with 90% iR compensation to obtain a polarization curve. a reversible hydrogen electrode (RHE) was convert followed equation: E(RHE) = E (Hg/HgO) + 0.095 \u0026times; PH + 0.098 and to recorrected 90% iR compensation. \u0026nbsp;EIS (electrochemical impedance spectra) were measured at overpotential with an AC amplitude of 10 mV from100 kHz to 0.01 Hz. The obtained from cyclic voltmeter-ammeter curves (CV) at different scan rates, from the double layer capacitance (C\u003csub\u003edl\u003c/sub\u003e),was used to estimate the electrochemically active surface. Stability testing of the catalysts was characterized by LSV after continuous CV cycling and by the timed current method (I-t).\u003c/p\u003e"},{"header":"Results and Discussion","content":"\u003cp\u003eFigure 1 schematically illustrated the procedure of MoS\u003csub\u003e2\u003c/sub\u003e/Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/ Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF catalysts via a combined electrodeposition and hydrothermal reaction. The electrodeposition of MoS\u003csub\u003e2\u003c/sub\u003e was controlled by electrodeposition time to regulate the number and thickness of the generated nanoflowers, aiming to exhibit highest activity sites. Whereas, the intermediate produced Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e on nickel foam was processed by co-precipitation and sulfidation treatment. Ni\u003csup\u003e2+\u003c/sup\u003e reacted with water ions in Ni(OH)\u003csub\u003e2\u003c/sub\u003e to generate interlaced nanosheets, while the Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e was treated with Na\u003csub\u003e2\u003c/sub\u003eS solution sulfidation, and sulfur ions reacted with Ni\u003csup\u003e2+\u003c/sup\u003e on surface of Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF to reconstructed a lamellar structure. Finally, the Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/ Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF catalysts were electrodeposited under different time for obtaining MoS\u003csub\u003e2\u003c/sub\u003e/Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF catalysts.\u003c/p\u003e\n\u003cp\u003eScanning electron microscopy (SEM, company )was applied to understand the morphologies of Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF, Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF and MoS\u003csub\u003e2\u003c/sub\u003e/Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF catalysts. The morphology of Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF (as shown in Figure. 2a, b) indicated that the prepared Ni(OH)\u003csub\u003e2\u003c/sub\u003e grown uniformly on the NF andNi(OH)\u003csub\u003e2\u003c/sub\u003e appears as regular uniform flakes (Fig. 2b) and the nanosheet array was aligned and grows vertically and interconnected to a regular network structure. It is noteworthy that the obtained Ni(OH)\u003csub\u003e2\u003c/sub\u003e nanosheets had uniform and smooth surfaces, and extended volume ratio to enhanced the electroactive area. From Figure. 2 c and d, the morphology of the Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF nanosheets synthesized after sulfidation didnot change significantly, but the smooth surface of the Ni(OH)\u003csub\u003e2\u0026nbsp;\u003c/sub\u003esheets was coarse by sulfidation reaction to produced Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e.\u003c/p\u003e\n\u003cp\u003eWe investigated the influence of different electrodeposition times on the surface morphology of MoS\u003csub\u003e2\u003c/sub\u003e/Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF catalysts. It was found that the MoS\u003csub\u003e2\u003c/sub\u003e attached to Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF with electrodeposition time of 5 min, as shown in Figure 3 a, b and c, which exhibited a flowers-like composed lamellar structures with a complete morphology, uniform and clear structure. In contrast, the MoS\u003csub\u003e2\u003c/sub\u003e generated at 7 min of electrodeposition was covered with a thin layer of frost-like while maintaining the original nanoflower morphology ( as shown in Fig. 3d, e and f). It can be seen that the the fraction of deposited MoS\u003csub\u003e2\u003c/sub\u003e was increased on nanosheets edge with the increase of electrodeposition time, like 7 mins deposition time. After studied its HER performance, the best HER performance was exhibited at the controlled electrodeposition time of 5 min, which the MoS\u003csub\u003e2\u003c/sub\u003e/Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF catalyst formed with a clear structure, fast electron transport and higher exposed active sites. It also indicated the suitable amount of deposited MoS\u003csub\u003e2\u003c/sub\u003e highly affected its electrocatalytically abilities.\u0026nbsp;\u003c/p\u003e\n\u003cp\u003eIn Figure 4, the XRD patterns illustrated the chemical composition of the prepared catalytic materials. From the diffraction peaks corresponding to Ni (PDF#87-0712) and Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e (PDF#73-0698), it can be seen that the diffraction peaks were 44.49\u0026deg;, 51.84\u0026deg;, and 76.38\u0026deg; point to the {111}, {200}, and {220} faces of Ni, respectively. And the diffraction peaks at 21.81\u0026deg;, 30.88\u0026deg;, 38.38\u0026deg;, 50.25\u0026deg; and 55.49\u0026deg; are assigned to the {010}, {110}, {111}, {120} and {211} faces of Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e. It indicated the presence of Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e and other objects. But the peaks of MoS\u003csub\u003e2\u003c/sub\u003e were not observed, which indicated that the MoS\u003csub\u003e2\u003c/sub\u003e crystallinity of the sample material synthesized by electrodeposition was limited and the MoS\u003csub\u003e2\u003c/sub\u003e content considered from electrodeposition was not superscalar. Thus, the presence and function of doped MoS\u003csub\u003e2\u0026nbsp;\u003c/sub\u003eshould be determine by another methods, like TEM and XPS characterization. To further understand the morphological structure, HR-TEM was used. The TEM was measured using pieces peeled off from the deposited film (Figure 4b), and the high magnification TEM was measured under further magnification (Figure 4c). The lattice stripe is 0.2363 nm corresponding to [111] plane of Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e was measured from Figure. 4c. and a lattice stripe of 0.6112 nm corresponding to the [002] plane of MoS\u003csub\u003e2\u003c/sub\u003e. The HAADF-STEM elemental mapping images (as shown in Figure 4d ) shows the Mo, Ni and S elements were separately and uniformly distributed on the surface of samples.\u003c/p\u003e\n\u003cp\u003eXPS was used to study its constituent elements and their corresponding chemical valence states of the MoS\u003csub\u003e2\u003c/sub\u003e/Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF catalyst, as the total spectrum in Figure 5a. Figure 5b shows the characteristic peaks of Ni 2P for MoS\u003csub\u003e2\u003c/sub\u003e/Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e, where the two spin-orbit double peaks at 872.9 eV and 855.2 eV correspond to Ni 2p\u003csub\u003e1/2\u003c/sub\u003e and Ni 2 p\u003csub\u003e3/2\u003c/sub\u003e,(格式) confirming the formation of Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e. Between two Ni 2P peaks, the spin-orbit splitting energy is 17.7 eV indicated that the appearance of /Ni(OH)\u003csub\u003e2\u003c/sub\u003e[63], and there were two satellites at 879.1 eV and 861.8 eV.[64, 65] In the S 2p spectrum \u0026nbsp;in Figure 5c, the peak at binding energy 161.3 eV corresponds to S 2p\u003csub\u003e1/2\u0026nbsp;\u003c/sub\u003eand the peak out of binding energy 162.8 eV corresponds to S 2p\u003csub\u003e3/2\u003c/sub\u003e, proving the presence of S\u003csup\u003e2-\u003c/sup\u003e. Notably, the peak at binding energy 168.1 eV was assigned to the satellite peak [ref]. In the core spectrum of the Mo 3d spectrum in Figure 5d, the Mo 3d spectrum was infit indicated that there had two spin-orbit double peaks centered at binding energies 234.9 eV and 231.7 eV, consistent with the Mo\u003csup\u003e4+\u003c/sup\u003e 3d\u003csub\u003e3/2\u003c/sub\u003e and Mo\u003csup\u003e4+\u003c/sup\u003e 3d\u003csub\u003e5/2\u003c/sub\u003e states, respectively, indicating there was a tetravalent state of Mo formation. In addition, the peak out of the binding energy is 226.1 eV indicated that the formation of Mo\u003csup\u003e6+\u003c/sup\u003e 3d\u003csub\u003e3/2\u003c/sub\u003e state was present.\u003c/p\u003e\n\u003cp\u003eThe HER activity of MoS\u003csub\u003e2\u003c/sub\u003e/Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni (OH)\u003csub\u003e2\u003c/sub\u003e@NF electrocatalysts was evaluated in a standard three-electrode system in saturated 1 M KOH electrolyte solution at 5 mv s\u003csup\u003e-1\u003c/sup\u003e scan rate. To explore the effects of MoS\u003csub\u003e2\u003c/sub\u003e in HER reaction, comparison samples were prepared and tested, such as bare Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni (OH)\u003csub\u003e2\u003c/sub\u003e and Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni (OH)\u003csub\u003e2\u003c/sub\u003e with electrodeposited MoS\u003csub\u003e2\u003c/sub\u003e by different deposition time.. Figure 6a compared the linear scanning voltammetry (LSV) curves of Pt/C, NF, Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e, and electrodeposited MoS\u003csub\u003e2\u003c/sub\u003e/Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF electrocatalysts. The MoS\u003csub\u003e2\u003c/sub\u003e/Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF electrode had a lower overpotential than Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e and NF electrode, and closed to Pt electrode. The HER activity was significantly increased when MoS\u003csub\u003e2\u0026nbsp;\u003c/sub\u003ewas deposited on the Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e electrode (Fig. 6a), indicating that the nano-flower modified Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e electrode formed by electrodeposition of MoS\u003csub\u003e2\u003c/sub\u003e was more favorable in LSV test, which caused by its more exposing active sites and better charge transfer ability in electrolyte interface and internal transmission. The electrodes with different deposition times test results shows that the electrode with 5 min deposition time exhibited a optimal low overpotential of 48 mV overpotential at a fixed current density of 10 mA cm\u003csup\u003e-2\u0026nbsp;\u003c/sup\u003ein Figure. 6a, which approximated to commercial Pt/C. But the 7 min deposition sample had a higher overpotential, which might affected by more attached MoS\u003csub\u003e2\u003c/sub\u003e fractions blocked their active sites and adverse to their worser HER performance.\u003c/p\u003e\n\u003cp\u003eFor understanding its HER dynamics, we analyzed its Tafel plots, j\u003csub\u003e0\u003c/sub\u003e and electrochemical impedance (EIS) curves. As shown in Figure 6b, the fitted linear Tafel slopes used for commercial Pt/C (10 w t%), Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF, Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e, MoS\u003csub\u003e2\u003c/sub\u003e/Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF-1min, 3min, 5min, and 7min samples corresponded to 45.5 mV dec\u003csup\u003e-1\u003c/sup\u003e, 131.2 mV dec\u003csup\u003e-1\u003c/sup\u003e, 118.6 mV dec\u003csup\u003e-1\u003c/sup\u003e, 107.2 mV dec\u003csup\u003e-1\u003c/sup\u003e, 97.4 mV dec\u003csup\u003e-1\u003c/sup\u003e, 108.6 mV dec\u003csup\u003e-1\u003c/sup\u003e. The Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF electrocatalyst Tafel slopes via MoS\u003csub\u003e2\u003c/sub\u003e electrodeposition indicated that the hydrogen precipitation proceeded obeyed Volmer-Heyrovsky mechanism and rate-limited the electrochemical desorption process. The electrocatalysts deposited in MoS\u003csub\u003e2\u003c/sub\u003e for 5 min had a Tafel slope at 97.4 mV dec\u003csup\u003e-1\u003c/sup\u003e, demonstrating it had a high catalytic efficiency and approached to commercial Pt/C. We plotted the overpotentials for current densities of 10 and 100 mA cm\u003csup\u003e-2\u003c/sup\u003e and show them in Figure. 6c. MoS\u003csub\u003e2\u003c/sub\u003e/Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF-5min electrodes required overpotentials at 48 mV and 175 mV, which obviously better than other catalysts but slightly lower than Pt/C. To further understand the differ of their HER kinetics, a electrochemical impedance spectroscopy (donated as EIS, as shown in Figure. 6d) was performed in 1.0 M NaOH solution in frequency from 0.01 to 100 kHz, and got their Nyquist plots. Among them, the MoS\u003csub\u003e2\u003c/sub\u003e/Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF-5min catalyst had the smallest R\u003csub\u003ect\u003c/sub\u003e among several catalyst materials with 3.8 \u0026Omega;. These advantages were attributed to the introduced 3D MoS\u003csub\u003e2\u003c/sub\u003e enhanced the conductivity and promoted interface and catalyst internal charge transfer abilities. The other binary materials commonly got larger R\u003csub\u003ect\u003c/sub\u003e, which may hinder the hydrogen precipitation to some extent. The comparison by EIS plots reveals that the reflection of MoS\u003csub\u003e2\u003c/sub\u003e clearly reduced the composite resistances and promoted the HER kinetic process.\u003c/p\u003e\n\u003cp\u003eTo further evaluate the hydrolysis abilities of MoS\u003csub\u003e2\u003c/sub\u003e/Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF composites, we tested its bilayer capacitance (C\u003csub\u003edl\u003c/sub\u003e) and electrochemical active area (ECSA) via a cyclic voltmeter-ammeter scanning. As shown in Figure. 6e, the MoS\u003csub\u003e2\u003c/sub\u003e/Ni3S\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF catalysts showed larger C\u003csub\u003edl\u003c/sub\u003e than Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH\u003csub\u003e)2\u003c/sub\u003e@NF, Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF and NF with C\u003csub\u003edl\u003c/sub\u003e of 52.23 mF cm\u003csup\u003e-2\u003c/sup\u003e, 44.81 mF cm\u003csup\u003e-2\u003c/sup\u003e, 41.83 mF cm\u003csup\u003e-2\u003c/sup\u003e and 23.14 mF cm\u003csup\u003e-2\u003c/sup\u003e, respectively. With Figure 7 illustrating, the ECSA obtained at different sweep CV curves of 0.04-0.16, it can be visualized that the electrochemically active area of MoS\u003csub\u003e2\u003c/sub\u003e/Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF is larger, which confirms that the suitable introduction of MoS\u003csub\u003e2\u003c/sub\u003e extended more electrochemically active area.\u003c/p\u003e\n\u003cp\u003eIn addition, the stability of the electrocatalyst, we performed a stability test as shown in Figure 6f. After a 5000 CV cycling at a constant current density of 10 mA cm\u003csup\u003e-2\u003c/sup\u003e for 72 hour, there is invisible current decay, which indicated that the composites synthesized by electrodeposited MoS\u003csub\u003e2\u003c/sub\u003e on Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF has an outstanding stability. After the stability tests we performed XPS spectroscopy tests and SEM test for further determined its structural stability. The SEM results shows that the morphology change is inviable, as its valance states of Mo, S, Ni didnot alter from its XPS results in Figure, which illustrate that there were bare deconstructed after stability electrochemical tests and proves this Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF nanoflowers have excellent electrocatalytical ability and stability.\u003c/p\u003e"},{"header":"Conclusion","content":"\u003cp\u003eIn this work, we prepared a cheap efficient MoS\u003csub\u003e2\u003c/sub\u003e/Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF catalyst via an one-step electrodepositing MoS\u003csub\u003e2\u003c/sub\u003e infractions on 3D nanoflower-like Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF-based electrode. This catalyst exhibited low overpotentials of 48 at 10 mA cm\u003csup\u003e-2\u003c/sup\u003eand 175 mV at 10 and 100 mA cm\u003csup\u003e-2\u003c/sup\u003e current densities, as well as the long-stability of 72 hours current without decay after 5000 CV cycles at constant current density at 10 mA cm\u003csup\u003e-2\u003c/sup\u003e. The electrodeposited MoS\u003csub\u003e2\u003c/sub\u003e nanoflowers and Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e reduces overpotential for hydrogen precipitation process and synergically improves their electron transport abilities and exposes more active-sites, leading to an enhanced HER performance. Its excellent performance in HER and the simple and low-cost preparation procedure might provide a novel catalyst and new synthesis strategies for the sustainable hydrogen energy development.\u003c/p\u003e\n"},{"header":"Abbreviations","content":"\u003cp\u003e\u003cstrong\u003eHER\u003c/strong\u003e: Hydrogen Evolution Reaction\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eNF\u003c/strong\u003e: Nickel Foam\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eLSV\u003c/strong\u003e: Linear Scanning Voltammetry\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eXRD\u003c/strong\u003e: X-ray Diffraction\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eXPS\u003c/strong\u003e: X-ray Photoelectron Spectroscopy\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eSEM\u003c/strong\u003e: Scanning Electron Microscopy\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eTEM\u003c/strong\u003e: Transmission Electron Microscopy\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eEDS\u003c/strong\u003e: Energy Dispersive X-ray Spectroscopy\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eEIS\u003c/strong\u003e: Electrochemical Impedance Spectroscopy\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eCV\u003c/strong\u003e: Cyclic Voltammetry\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eC~dl~\u003c/strong\u003e: Double Layer Capacitance\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eECSA\u003c/strong\u003e: Electrochemically Active Surface Area\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eRHE\u003c/strong\u003e: Reversible Hydrogen Electrode\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eR~ct~\u003c/strong\u003e: Charge Transfer Resistance\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eNaOH\u003c/strong\u003e: Sodium Hydroxide\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eKOH\u003c/strong\u003e: Potassium Hydroxide\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eDI\u003c/strong\u003e: Deionized\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eAR\u003c/strong\u003e: Analytical Reagent\u003c/p\u003e\n"},{"header":"Declarations","content":"\u003cp\u003e\u003cstrong\u003eEthical Approval and Consent to Participate\u003c/strong\u003e: This study was approved by the relevant ethics committee, and all participants provided informed consent.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eConsent for Publication\u003c/strong\u003e: All authors have read and approved the final manuscript for publication.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eCompeting Interests\u003c/strong\u003e: The authors declare that they have no known competing financial interests or personal relationships that could have influenced the work reported in this paper. This manuscript has not been published elsewhere.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eAuthor Contributions:\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eShunming Li\u003c/strong\u003e: Performed experiments, analyzed data, and drafted the manuscript.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003ePengyu Hu\u003c/strong\u003e: Conducted material characterization.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eJingzong Qu\u003c/strong\u003e: Contributed to manuscript drafting.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eJie Zhou\u003c/strong\u003e: Assisted in data analysis.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eZibo Wang \u0026amp; Yanan Wang\u003c/strong\u003e: Reviewed and revised the manuscript.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eAnran Chen\u003c/strong\u003e: Supervised the experiments.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eTao Sun\u003c/strong\u003e: Oversaw the project, provided guidance, and administered the study.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eFunding:\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThis work was supported by\u0026nbsp;School of Materials and Energy, Yunnan University, Kunming.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eData Availability:\u0026nbsp;\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eAll data generated in this study are original and available upon reasonable request.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eAcknowledgments:\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003e\u0026nbsp;I would like to express my deepest gratitude to my family for their unwavering support, encouragement, and patience throughout this research journey. Their love and understanding have been my greatest motivation. I am also sincerely thankful to my advisors and professors for their invaluable guidance, insightful feedback, and continuous encouragement. Additionally, I extend my appreciation to my colleagues and classmates for their stimulating discussions, technical assistance, and moral support, which greatly contributed to the completion of this work. Without their help, this achievement would not have been possible. Finally, I acknowledge all those who, directly or indirectly, supported me in this endeavor.\u003c/p\u003e\n"},{"header":"References","content":"\u003col\u003e\n\u003cli\u003eT.F. Li, G. Luo, K.H. Liu, X. Li, D.M. Sun, L. Xu, Y.F. Li, Y.W. Tang, Encapsulation of Ni3Fe Nanoparticles in N-Doped Carbon Nanotube-Grafted Carbon Nanofibers as High-Efficiency Hydrogen Evolution Electrocatalysts, Adv. Funct. Mater., 28 (2018) 9.\u003c/li\u003e\n\u003cli\u003eZ.W. Seh, J. Kibsgaard, C.F. Dickens, I. Chorkendorff, J.K. 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Sun, Efficient Electrocatalytic Water Oxidation by a Copper Oxide Thin Film in Borate Buffer, Acs Catalysis, 5 (2015) 627-630.\u003c/li\u003e\n\u003c/ol\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":false,"hideJournal":false,"highlight":"","institution":"","isAcceptedByJournal":true,"isAuthorSuppliedPdf":false,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"catalysis-letters","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"","sideBox":"Learn more about [Catalysis Letters](https://link.springer.com/journal/10562)","snPcode":"10562","submissionUrl":"https://submission.springernature.com/new-submission/10562/3","title":"Catalysis Letters","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"stoa","reportingPortfolio":"Springer Hybrid","inReviewEnabled":true,"inReviewRevisionsEnabled":false},"keywords":"","lastPublishedDoi":"10.21203/rs.3.rs-6288116/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-6288116/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003ePreparing a cheap efficient water-resolved hydrogen electrocatalyst and used it in alkaline media is important path for hydrogen conversion and storage. Herein, a MoS\u003csub\u003e2\u003c/sub\u003e/Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e on nickle form nanoflower composited electrocatalyst were synthesized via a simple one-step electrodeposition method by using a nickel foam (NF) as the based material. The obtained MoS\u003csub\u003e2 \u003c/sub\u003enanoflower via this simple one-step electrodeposition method has controllable strength, uniform growth and easy operated by tuning the electrodeposition coefficient and controlling the electrodeposition time. Meanwhile, the common factor leads to poor HER performance, like incomplete exposure of the active site caused by the incontrollable formation of MoS\u003csub\u003e2\u003c/sub\u003e blocks, was successfully avoided. The electrodeposited MoS\u003csub\u003e2\u003c/sub\u003e nanoflowers and Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e played an important role for reducing potential during hydrogen precipitation by synergistic effects. This synergy between the two effective catalyst promotes electron transport abilities and exposes more active-sites, leading to an enhanced HER performance. In the alkaline solution of 1.0m NaOH, the graded MoS\u003csub\u003e2\u003c/sub\u003e/Ni\u003csub\u003e3\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Ni(OH)\u003csub\u003e2\u003c/sub\u003e@NF-5min electrode shows a respectively overpotential of 48 mV at 10 mA cm\u003csup\u003e-2\u003c/sup\u003eand 175 mV at 100mA cm\u003csup\u003e-2\u003c/sup\u003e, whilst high conductivity and good stability with the current maintained efficient for 72 hours under current density of 10mA cm\u003csup\u003e-2 \u003c/sup\u003eafter 5000 cycles.\u003c/p\u003e","manuscriptTitle":"One-step electrodeposition prepared MoS2 composed Ni3S2 /Ni(OH)2 nanosheets as high efficient and stable metal sulfide catalyst for hydrogen precipitation in alkaline solutions","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2025-04-17 10:39:45","doi":"10.21203/rs.3.rs-6288116/v1","editorialEvents":[{"type":"communityComments","content":0},{"type":"decision","content":"Revision requested","date":"2025-04-03T12:18:59+00:00","index":"","fulltext":""},{"type":"editorInvitedReview","content":"","date":"2025-04-03T07:37:41+00:00","index":"hide","fulltext":""},{"type":"editorInvitedReview","content":"","date":"2025-04-03T06:37:43+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"30654795130375902101316246132700217844","date":"2025-04-03T00:24:14+00:00","index":"hide","fulltext":""},{"type":"editorInvitedReview","content":"","date":"2025-04-02T02:27:00+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"273788619244600014687964034199453943264","date":"2025-03-31T01:14:33+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"175225567672764711802221168988486330418","date":"2025-03-28T20:12:07+00:00","index":"hide","fulltext":""},{"type":"reviewersInvited","content":"","date":"2025-03-28T13:43:01+00:00","index":"","fulltext":""},{"type":"editorAssigned","content":"","date":"2025-03-28T04:10:04+00:00","index":"","fulltext":""},{"type":"checksComplete","content":"","date":"2025-03-28T04:08:01+00:00","index":"","fulltext":""},{"type":"submitted","content":"Catalysis Letters","date":"2025-03-23T12:01:20+00:00","index":"","fulltext":""}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"catalysis-letters","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"","sideBox":"Learn more about [Catalysis Letters](https://link.springer.com/journal/10562)","snPcode":"10562","submissionUrl":"https://submission.springernature.com/new-submission/10562/3","title":"Catalysis Letters","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"stoa","reportingPortfolio":"Springer Hybrid","inReviewEnabled":true,"inReviewRevisionsEnabled":false}}],"origin":"","ownerIdentity":"c56e08c7-41ee-4ae8-9e21-7aab2faf9a57","owner":[],"postedDate":"April 17th, 2025","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"under-review","subjectAreas":[],"tags":[],"updatedAt":"2025-05-23T14:38:40+00:00","versionOfRecord":[],"versionCreatedAt":"2025-04-17 10:39:45","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-6288116","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-6288116","identity":"rs-6288116","version":["v1"]},"buildId":"XKTyCvWXoU3ODBz1xrDgd","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}