Liquid metal dispersed single-atom catalyst with high-temperature stability

Liquid metal dispersed single-atom catalyst with high-temperature stability | 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 Article Liquid metal dispersed single-atom catalyst with high-temperature stability Lei Fu, Ziyue Zeng, Chenyang Wang1, Mingjun Sun, Dong Liu, Donghong Zhang, and 9 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-7086103/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 13 Mar, 2026 Read the published version in Nature Communications → Version 1 posted You are reading this latest preprint version Abstract Single-atom catalysts (SACs) enable greener and more economically sustainable chemical production by significantly improving thermocatalysis efficiency and selectivity through maximized atom utilization and highly homogeneous metal coordination environments. Unfortunately, single-atom catalysts (SACs) are fundamentally constrained by the stability owing to the severe aggregation of single atoms especially under the high-temperature thermocatalysis operations, which compromises the overall catalytic performance. Here, we report a strategy to realize the highly thermal-stable SACs resistance to sintering at harsh conditions through harnessing the inherently metal affinity and fluidity of liquid metal. A stable liquid metal-active metal interaction is formed, profiting from the superior metal affinity of liquid metal. Combined with the fluidity of liquid metal, active metal atoms can move but remain confined to the liquid metal as the metallic single-atom state at high temperatures. This catalyst exhibits outstanding thermal durability for ethane dehydrogenation, sustaining stable operation for over 100 h at 650 o C with an impressive ethylene selectivity of 98%. The strategy of constructing stable metal-metal interactions by utilizing the inherently metal affinity and dynamic fluidity of liquid metal will pave a practical way for the design of highly thermal-stable SACs. Physical sciences/Chemistry/Catalysis Physical sciences/Materials science/Materials for energy and catalysis Figures Figure 1 Figure 2 Figure 3 Figure 4 Introduction Industrial thermocatalysis holds great promise for improving the efficiency and sustainability of thermochemical processes and producing value-added chemicals in the modern chemical industry 1–3 . Single-atom catalysts (SACs) have garnered extensive attention for the development of highly efficient, sustainable, cost-effective catalysts in thermocatalysis fields due to their maximized atom utilization and highly homogeneous metal coordination environment 4–8 . However, constructing highly thermally durable SACs is a significant challenge in industrial applications. This is owing to the inherently ultra-high surface energy of single atoms, and the high temperature (> 300 o C) provides enough energy to overcome the diffusion barrier of single atoms, leading to the migration of single atoms and severe agglomeration 9 . In the current paradigm, it is prevalent to stabilize SACs by modulating supports (such as carbon-based supports 10 and metal oxides characterized by defection 11–14 and so on) that tune interactions between metal atoms and supports. However, the presence of a strong bonding interaction between the supports and the single atoms may result in the compromise of the unique coordination structure of the single atoms, thereby diminishing the catalytic activity and even deactivation 15,16 . In terms of the strategy of using porous supports to spatially confine single atoms (such as molecular sieves, and metal-organic frameworks) 17,18 , surmounting the substantial surface energy of the single atoms is still difficult, which will lead to inevitable aggregation of single atoms at elevated temperatures 19,20 . Hence, designing an optimal support that balances metal-support interaction for realizing highly efficient thermal-stable SACs remains a formidable obstacle. Inspired by the rule of thumb “like dissolves like”, it is promising to take advantage of unique metal-metal interaction to efficiently disperse active metals to acquire stable single atoms with inherently high metal activity by using the liquid metal as the dispersion. Herein, we achieve the highly efficient dispersion of single atoms with unprecedented thermal stability by utilizing the inherent fluidity and metal affinity of liquid metal. As a demonstration, gallium (Ga) capable of an ideal liquid environment was employed to spontaneously disperse active metal platinum (Pt). Exceptionally thermal-stable Pt single atoms dispersed by Ga that survived at 650°C were realized. In this system, profiting from the superior metal affinity of Ga with Pt, Pt–Pt bonds are broken at elevated temperatures, and subsequently the mobile Pt atoms are captured by Ga to form stable Pt–Ga interaction, accomplishing the highly efficient dispersion of Pt single atoms. The fluidity of liquid metal and the stable Pt–Ga interaction ensures that the Pt atoms can remain dynamically scattered to the whole liquid metal dispersion system. Additionally, liquid metal dispersed single atoms can self-update onto the catalysis interface continuously, promoting catalytic reactions at the interface. Hence, these liquid metal dispersed SACs manifested remarkable thermal durability for ethane dehydrogenation (EDH), sustaining stable operation for over 100 hours at 650 o C with ethylene selectivity of 98%. This elucidates the promising potential of this approach in realizing highly thermal-stable SACs. Results The design of thermal-stable liquid metal dispersed SACs With increasing temperature, the surface energy of single atoms will dramatically rise, and the migration of single atoms will be accelerated, leading to severe aggregation and sintering 9,21 . In essence, the competition of aggregation reflected the competitive bonding between single atom/single atom and single atom/support. Establishing highly-efficiency as well as stable metal-support interaction is crucial for blocking the aggregation and sintering of single atoms at high temperatures. In this work, we make the realization of thermal-stable SACs by utilizing liquid metal to disperse and stabilize active metals (Fig. 1 a). The abundance of metallic bonds in the liquid metal makes it an ideal medium for effectively dispersing active metals with similar metallic bonds and the active metals can keep the highly active metallic state. At elevated temperatures, enough energy was provided to break metallic bonds in the active metals. Furthermore, the fluidity of liquid metals boosts the spontaneous random movement of heterogeneous atoms, which drives the disordered dispersion of active atoms in liquid metals at elevated temperatures, similar to Brownian motion. These dynamically migrating single atoms can be subsequently combined with liquid metal profiting from its good metallic affinity and form stable interaction between liquid metal and active metal. In light of this, equipped with the naturally metallic affinity and fluidity of liquid metal, the highly thermal-stable SACs can be realized. The preparation of liquid metal dispersed SACs is by dissolving Pt nanoparticles into liquid Ga at elevated temperatures. The mechanism illustrating the programmable formation process of the liquid metal dispersed SACs is summarized in Fig. 1 a. Firstly, the Pt powders were sprinkled evenly over the liquid metal. As the temperature gradually increases, the solubility of the active metal in the dispersion is further increased, and the active metal can efficiently disperse in the liquid metal within its limited solubility. The Pt − Pt bonds in the original Pt metal nanoparticles are broken and tend to bind tightly to Ga atoms and form a thermodynamically stable configuration with Ga atoms benefiting from the good affinity between Ga and Pt under high temperatures. Thereby the stable Pt − Ga interaction curtails the sintering of Pt single atoms and maintains the stability of SACs. Moreover, according to the Arrhenius Eq. 2 2 , the thermal motion of atoms would be intensified by high temperature, promoting the rapid diffusion between Pt and Ga atoms and the continuous renewal of Pt single atoms exposed on the catalytic surface (Fig. 1 b). In contrast, when single atoms are anchored to solid supports, their co-migration with the supports becomes kinetically constrained. Once the metal-support interactions become insufficient to compensate for the inherently high surface energy of single atoms, these atoms tend to detach from the solid supports and aggregate. This process is exothermic, where minimization of total surface energy governs particle growth 23 . Meanwhile, some single atoms may embed into the lattice of supports, becoming buried when the interaction between the support and metal atoms is too strong. These processes lead to the loss of active sites, reducing the stability of SACs and consequently affecting their activity and selectivity (Fig. 1 c). Thermal stability of active metal atoms monodispersed in liquid Ga Ab initio molecular dynamics (AIMD) simulations were employed to elucidate the atomic-scale dispersed state of active metal in liquid metal (computational details are provided in the supplementary information). Using Pt 10 as a model of Pt cluster, we investigated the structural evolution of both clustered and dispersed Pt 10 in liquid Ga during 10 ps simulations at 923 K (Fig. 2 a, b and Supplementary Mov. 1, 2). The calculated total energy versus time curves for the Ga 90 Pt 10 system containing clustered Pt 10 and dispersed Pt 10 (Fig. 2 c) reveal that the dispersed Pt 10 generally exhibits lower total energy compared to the aggregated Pt 10 clusters within the simulated 10 ps. The results indicate that the remarkable atomic diffusion of liquid Ga metal at high temperature promotes the migration of heterogeneous active metal atoms, thereby stabilizing their dispersed atomic state in liquid Ga. The relatively high Pt concentration in the Ga 90 Pt 10 system leads to intermittent formation of Pt 2 dimer, as evidenced by the time-dependent curve of the shortest Pt–Pt distance (Supplementary Fig. 1). To further elucidate the actual existence state of Pt atoms in liquid Ga, we performed AIMD simulations of the Ga 98 Pt 2 system (a Pt 2 dimer embedded in Ga 98 ) at 923 K. The 10 ps NVT ensemble simulations (Fig. 2 d) display that the Pt-Pt interatomic distance progressively increases from 4.18 Å to 11.63 Å, significantly exceeding the Pt–Pt bond length of 2.65 ~ 2.79 Å 25 . This unequivocally confirms that Pt atoms preferentially exist as monatomic species in the liquid Ga (Supplementary Fig. 2 and Mov. 3, 4). Further statistical analysis of the coordination environment of Pt atoms in the Ga 98 Pt 2 system shows that the dominant coordination numbers for individual Pt atoms are 8 or 9 (Supplementary Fig. 3 and Fig. 2 e), implying that monodispersed Pt atoms migrate within liquid Ga in the form of clusters such as Ga₈Pt or Ga₉Pt (Supplementary Fig. 4). To fundamentally understand the thermodynamic preference for Pt mono-dispersion in liquid Ga, we systematically evaluated the binding interactions through potential energy curve calculations of three representative diatomic systems: Ga₂, GaPt, and Pt₂ (Fig. 2 f). The calculated bond dissociation energies show a clear ranking: E (Pt–Pt) (107.9 kcal/mol) > E (Ga–Pt) (74.9 kcal/mol) > E (Ga–Ga) (32.5 kcal/mol). Crucially, the formation of two Ga–Pt bonds (149.8 kcal/mol) is energetically favored over either maintaining a Pt–Pt bond (107.9 kcal/mol) or the combined Pt–Pt and Ga–Ga bonding (140.4 kcal/mol). This energetic advantage, coupled with the inherently weaker Ga–Ga interactions in liquid Ga compared to isolated Ga₂ molecules 26 and the good affinity between Ga and Pt 27 , enables Ga atoms to disrupt Pt–Pt bonds to form stable Pt–Ga–Pt bridging units. Meanwhile, we calculated the formation energies of Pt₂Ga, (Ga₆Pt)₂Ga, and (Ga₇Pt)₂Ga molecules, which were determined to be 101.1, 46.2, and 57.9 kcal/mol, respectively (Supplementary Fig. 5 and Fig. 2 g). Additionally, we roughly estimated the energy barriers of Ga atom insertion into the Pt–Pt bond to be 58.2, 13.4, and 40.2 kcal/mol by performing rigid scans of the Pt–Ga–Pt angle (Supplementary Fig. 6 and Fig. 2 g). These results clearly demonstrate that, both thermodynamically and kinetically, Ga atoms in liquid Ga at 923 K can readily disrupt Pt–Pt bonds, thereby promoting the mono-dispersion of Pt atoms. The stable Ga 8 Pt and similar clusters that are formed profited from the favorable affinity between Ga and Pt inhibit the aggregation and sintering of Pt during thermal motion, laying the foundation for synthesizing the highly thermal-stable SACs. Characterization of liquid catalyst To further validate that liquid metal can act as the dispersion for single atoms, we synthesized a Ga-dispersed Pt single-atom catalyst (Pt@Ga) following the strategy described above. The detailed structure of the catalyst was characterized by transmission electron microscopy (TEM) and energy dispersive spectrometry (EDS). The Pt species in the liquid metal existed in a monodisperse distribution without the obvious occurrence of aggregated Pt (Fig. 3 a). The bright-field image of Pt@Ga liquid catalyst maintains an almost invariant brightness across the whole particle and the corresponding selected area electron diffraction (SAED) data shows no diffraction spots of Pt in the amorphous ring, revealing the lack of long-range order structure in the Ga–Pt catalyst (Supplementary Figs. 7 and 3b). Furthermore, the X-ray photoelectron spectroscopy (XPS) spectrum was employed to reveal the chemical composition and electronic structure of the liquid metal dispersed SAC. Prior to the execution of XPS measurements, the sample underwent etching with argon ions to eliminate the natural oxide layer and surface contaminants. Then, the XPS measurements indicate that the as-synthesized catalyst contains approximately 0.2 at% Pt and 99.8 at% Ga (Fig. 3 c, d). Ga 2 p peaks appear at 1116.73 eV and 1116.59 eV, which are consistent with the reported binding energies of metallic Ga (Ga 0 2 p 3/2 =1116.70 eV). Meanwhile, due to the higher electronegativity of Pt (2.28) than that of Ga (1.81) 28 , the Pt in the Pt@Ga system served as the electron acceptor, and the Pt 4 f 7/2 and 4 f 5/2 peaks in Pt@Ga exhibit positive shift (1.0 eV) than those in pure Pt metal. It is a consensus that metallic Pt 0 species occupy a preeminent role as the active sites for many catalytic processes 29–31 . Consequently, the single-atom dispersion of Pt in liquid metal won’t sacrifice the activity of catalysts. This approach guarantees a proficient and robust distribution of single atoms, thereby preserving their unparalleled catalytic activity. Furthermore, the absence of the obvious aggregation of Pt atoms in the Pt@Ga was further identified by X-ray diffraction (XRD) tests, where no signal of Pt (PDF#04-0802) is observed (Supplementary Fig. 8). The XRD results supported our idea that the Pt species constantly migrated in liquid metal, probably resulting in the dispersion of Pt in single-atom. To mitigate the potential inaccuracies arising from the insensitivity of XRD to small Pt clusters, the pair distribution function (PDF) analysis was conducted to delve into the interatomic structure of the Pt@Ga liquid catalyst (Supplementary Fig. 9). The absence of Pt–Pt bonds indicates that Pt is distributed nearly at the atomic level within the liquid Ga without the formation of Pt clusters. These observations suggest that liquid metal can achieve the efficiently uniform dispersion of highly active single atoms at elevated temperatures. To further verify the exact dispersion state of Pt in Pt@Ga catalyst, X-ray absorption spectroscopy (XAS) measurements were conducted. According to the X-ray absorption near-edge structure (XANES) spectrum presented in Fig. 3 e, the adsorption edge energy of Pt in Pt@Ga is lower than that of the Pt reference foil at room temperature, revealing an average valence lower than Pt 0 . The negative charge results from the higher electronegativity of Pt than Ga, which is consistent with the results of XPS. The electron transfer from Ga to Pt favors stable metal-support interaction between Ga and Pt. Correspondingly, the k 3 -weighted R -space Fourier transformed spectra of the extended X-ray absorption fine structure spectra (EXAFS) show the prominent peak at 2.14 Å for Pt@Ga SAC, distinguished from that of the Pt–O (1.62 Å) bonds for PtO 2 and the Pt–Pt bonds (2.24 Å) for Pt foil (Fig. 3 f). All these results intuitively indicate that the Pt exists in the single-atom state in liquid metal. Ethane dehydrogenation performance of liquid metal dispersed SACs Based on the computational results, the liquid metal dispersed SACs theoretically feature excellent thermal stability at high temperatures. As a proof of concept, the thermal stability was validated by the ethane dehydrogenation (EDH) experiment. As shown in Fig. 4 a, when exposed to ethane, Pt single atoms exposed on the surface capture ethane molecules and synergistically activate C–H bonds, leading to selective ethane dehydrogenation to ethylene. Meanwhile, the fluidic characteristic of liquid metal dispersed SACs at operated conditions enables continuous replenishment of catalytically active Pt atoms onto the surface. And stable interaction between Pt − Ga effectively blocks the aggregation of Pt atoms during the constant migration. Benefiting from the advantages mentioned above, these adaptive surface active sites maintain long-term activity and thermal stability. To circumvent the issue of inadequate interaction between the liquid metal dispersed SACs and the reaction gas, the porous support is utilized to amplify the gas mass transfer rate. So, we coupled liquid metal supported SACs with porous MFI zeolite (ZSM-5) by the physical approach of ultrasonication to increase the contact surface area between the liquid metal support SACs and gas reactants. As demonstrated in Supplementary Fig. 10, EDS mappings revealed well-distributing of Ga, Si, and Al, indicating the liquid metal is uniformly loaded in the ZSM-5 zeolite framework. Upon heating, Pt will be spontaneously dispersed in Ga homogeneously, achieving the preparation of a zeolite-dispersed liquid metal supported SACs (Pt@Ga/ZSM-5). Further, we performed in situ XRD to explore the dispersing process of Pt (Supplementary Fig. 11). The diffraction peak observed at 43–47 o originates from the carbon in situ reactor (Supplementary Fig. 12). Initially, the characteristic peaks of Pt can be apparently observed located at 39.76 o and 46.24 o . With the temperature increasing, the characteristic peaks of Pt were gradually weakened and disappeared subsequently, proving the dispersion of Pt particles. The catalytic performance was evaluated in non-oxidative EDH at 923 K in a fixed-bed quartz U-tube reactor under atmosphere pressure with feed gas of 12.5 vol% C 2 H 6 in Ar. The commercial aluminosilicate ZSM-5 exhibited ethane conversion at 10.7% and ethylene selectivity at 84.3% under the given conditions (Fig. 4 b, c). The poor selectivity originates from the absence of active metal sites with high ethylene selectivity, resulting in inefficient dehydrogenation and dominant side reactions. The reactive gas adsorbs specifically onto the acidic sites of the molecular sieve during its passage, leading to the production of coke. Accumulated coke deactivates the catalyst by both filling the micropores and blocking the active sites 32 . Therefore, the pure ZSM-5 suffers from poor catalyst performances. Interestingly, the liquid metal dispersed SAC was highly active with ethane conversion at 17.8% and ethylene selectivity at 98.5%, outperforming the counterparts. The performance of the liquid metal dispersed SAC in the durability test was presented in Fig. 4 d. It exhibits sustainable conversion and selectivity in the continuous reaction for 100 h, where the constant ethane conversion of ~ 18% is obtained without attenuation. And liquid metal dispersed SAC exhibits a steady ethene productivity of around 14.3 g g Pt −1 h − 1 during the 100 h EDH test. The catalyst displays no deactivation trend during the testing period, indicating a reasonable expectation of more perdurable stability. Notably, the XANES spectrum and R -space of liquid metal dispersed SAC after 100 h ethane dehydrogenation at Pt L 3 -edge is similar to that of pristine liquid single-atom catalyst (Fig. 4 e, f and Fig. 3 e, f), demonstrating exceptional structural integrity under prolonged thermal catalysis. The catalytic performance and structural characterization together confirmed the superior thermal stability of liquid metal dispersed SAC in extremely high temperatures, which remarkably outperforms the traditional solid support loaded SACs. The excellent stability, selectivity, and conversion indicate the potential importance of liquid metal dispersed SAC for the reaction limited in harsh conditions in the future. Conclusions We succeeded in achieving the highly thermal-stable SACs by harnessing the inherent fluidity and metal affinity of liquid metal to form stable metal-metal interaction at high temperatures. In this system, the Pt–Pt bond in the active metal is broken at elevated temperatures and then Pt atoms are captured by liquid metal to form a highly stable Pt–Ga interaction, which enables Pt atoms to constantly remain uniformly dynamically decentralized to liquid metal. Crucially, the Pt atoms can maintain a highly-stable dispersed state during ethane dehydrogenation at 650 o C for 100 h, while the catalyst maintains an impressive selectivity of 98%. Our strategy provides accessible guidance for acquiring highly thermal-stable SACs by using liquid metal as the dispersion. Declarations Competing interests The authors declare no competing interests. Author contributions L.F. conceived the research concept. L.F., and M.Q.Z. supervised the research. Z.Y.Z. and C.Y.W. carried out the main experiments, collected and analyzed the data. F.D. supervised the theoretical calculations, and M.J.S. performed the computational simulations. M.Y.D., X.T., D.L. and D.H.L contributed to the catalytic performance evaluation. S.Y.H. contributed to sample preparation and data analysis. Z.J.L. and Y.S.M. processed the XAFS results. Y.L.Z. performed transmission electron microscopy characterizations. L.L. contributed to the in situ XRD characterizations. L.F., M.Q.Z., Z.Y.Z., C.Y.W., and M.J.S. cowrote the manuscript. All the authors contributed to data analysis and scientific discussion. Acknowledgements The research was supported by the Natural Science Foundation of China (22025303), the Fundamental Research Funds for the Central Universities (2042025kf0007), and the Postdoctoral Fellowship Program of CPFS (GZB20240567). We thank the Center for Electron Microscopy at Wuhan University for their substantial supports of TEM work. We thank the Core Facility of Wuhan University for the measurement of inductively coupled plasma-atomic emission spectrometry, XPS, TEM, and the Core Research Facilities of the College of Chemistry and Molecular Sciences at Wuhan University for the XRD and PDF characterizations. We also thank the BL11B beamline of the Shanghai Synchrotron Radiation Facility for the XAFS characterization. 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Supplementary Files SupplementaryInformation.docx Supplementary Information SupplementaryMovie1thestructuralevolutionofPt10clustersinliquidGa.mp4 Supplementary Movie 1-the structural evolution of Pt10 clusters in liquid Ga SupplementaryMovie2thestructuralevolutionofdispersedPt10inliquidGa.mp4 Supplementary Movie 2-the structural evolution of dispersed Pt10 in liquid Ga SupplementaryMovie3theNPTMDsimulationtfortheGa98Pt2system.mp4 Supplementary Movie 3-the NPT MD simulationt for the Ga98Pt2 system SupplementaryMovie4theNVTMDsimulationtfortheGa98Pt2system.mp4 Supplementary Movie 4-the NVT MD simulationt for the Ga98Pt2 system Cite Share Download PDF Status: Published Journal Publication published 13 Mar, 2026 Read the published version in Nature Communications → Version 1 posted 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. 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University","correspondingAuthor":false,"prefix":"","firstName":"Donghong","middleName":"","lastName":"Zhang","suffix":""},{"id":487345336,"identity":"1a0e03fd-485f-445d-b9a8-4d8bbfb9a151","order_by":6,"name":"Shiyi He","email":"","orcid":"","institution":"Wuhan University","correspondingAuthor":false,"prefix":"","firstName":"Shiyi","middleName":"","lastName":"He","suffix":""},{"id":487345337,"identity":"5aa7618b-6f21-4f7c-8ff4-0336c8eb9ece","order_by":7,"name":"Zijia Liang","email":"","orcid":"","institution":"Wuhan University","correspondingAuthor":false,"prefix":"","firstName":"Zijia","middleName":"","lastName":"Liang","suffix":""},{"id":487345338,"identity":"483749ee-c308-40ab-8a0a-523fd75fc782","order_by":8,"name":"Yushen Ma","email":"","orcid":"","institution":"Wuhan University","correspondingAuthor":false,"prefix":"","firstName":"Yushen","middleName":"","lastName":"Ma","suffix":""},{"id":487345339,"identity":"65393756-1a81-4240-8fef-b8b830191146","order_by":9,"name":"Yile Zhang","email":"","orcid":"","institution":"Wuhan University","correspondingAuthor":false,"prefix":"","firstName":"Yile","middleName":"","lastName":"Zhang","suffix":""},{"id":487345340,"identity":"0b31781f-5992-42fe-877e-418bb512e837","order_by":10,"name":"Ling Li","email":"","orcid":"","institution":"Wuhan University","correspondingAuthor":false,"prefix":"","firstName":"Ling","middleName":"","lastName":"Li","suffix":""},{"id":487345341,"identity":"3b4b7dca-140d-49ac-93f3-b38da0985c70","order_by":11,"name":"Xin Tian","email":"","orcid":"","institution":"Wuhan University","correspondingAuthor":false,"prefix":"","firstName":"Xin","middleName":"","lastName":"Tian","suffix":""},{"id":487345342,"identity":"60fc243f-7649-4583-92f8-5dc543cfd271","order_by":12,"name":"Mengqi Zeng","email":"","orcid":"https://orcid.org/0000-0002-1442-052X","institution":"Wuhan University","correspondingAuthor":false,"prefix":"","firstName":"Mengqi","middleName":"","lastName":"Zeng","suffix":""},{"id":487345343,"identity":"cc5af9ed-d4c9-4590-a18b-2edb5de4c59e","order_by":13,"name":"Mingyue Ding","email":"","orcid":"https://orcid.org/0000-0001-8769-4153","institution":"Wuhan University","correspondingAuthor":false,"prefix":"","firstName":"Mingyue","middleName":"","lastName":"Ding","suffix":""},{"id":487345344,"identity":"d164a040-c543-45b4-b544-44a3ff678f68","order_by":14,"name":"Feng Ding","email":"","orcid":"","institution":"Suzhou Laboratory","correspondingAuthor":false,"prefix":"","firstName":"Feng","middleName":"","lastName":"Ding","suffix":""}],"badges":[],"createdAt":"2025-07-09 16:45:11","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-7086103/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-7086103/v1","draftVersion":[],"editorialEvents":[{"content":"https://doi.org/10.1038/s41467-026-70476-2","type":"published","date":"2026-03-13T04:00:00+00:00"}],"editorialNote":"","failedWorkflow":false,"files":[{"id":87174240,"identity":"fd3d255b-cd1f-42ae-a255-766d606ca02a","added_by":"auto","created_at":"2025-07-21 08:16:21","extension":"jpeg","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":1093083,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eThe design of thermal-stable liquid metal dispersed SACs. a\u003c/strong\u003e The schematic diagram for the synthesis of liquid metal dispersed SACs. \u003cstrong\u003eb\u003c/strong\u003e,\u003cstrong\u003e c\u003c/strong\u003e The migration of active single atoms in liquid metal (\u003cstrong\u003eb\u003c/strong\u003e) and on traditional solid support (\u003cstrong\u003ec\u003c/strong\u003e).\u003c/p\u003e","description":"","filename":"floatimage1.jpeg","url":"https://assets-eu.researchsquare.com/files/rs-7086103/v1/2650e79f8bb418efd7adbbe4.jpeg"},{"id":87175366,"identity":"12c4ba63-fcb6-4dc5-9564-a3f3dbec6619","added_by":"auto","created_at":"2025-07-21 08:32:21","extension":"jpeg","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":1258819,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eTheoretical calculations of heterogeneous active metal atoms monodispersed in liquid Ga. a\u003c/strong\u003e,\u003cstrong\u003e b\u003c/strong\u003e The extracted 0 ps, 5 ps, and 10 ps snapshots from AIMD trajectories of both clustered (\u003cstrong\u003ea\u003c/strong\u003e) and dispersed (\u003cstrong\u003eb\u003c/strong\u003e) Pt\u003csub\u003e10\u003c/sub\u003e in liquid Ga. \u003cstrong\u003ec\u003c/strong\u003e Total energy versus time curves for the Ga\u003csub\u003e90\u003c/sub\u003ePt\u003csub\u003e10\u003c/sub\u003e system containing clustered Pt\u003csub\u003e10\u003c/sub\u003e and dispersed Pt\u003csub\u003e10\u003c/sub\u003e. \u003cstrong\u003ed\u003c/strong\u003e Time evolution of Pt–Pt interatomic distance in the Ga\u003csub\u003e98\u003c/sub\u003ePt\u003csub\u003e2\u003c/sub\u003e system under NVT ensemble simulation. \u003cstrong\u003ee\u003c/strong\u003e Statistical distribution of Pt coordination numbers in Ga\u003csub\u003e98\u003c/sub\u003ePt\u003csub\u003e2\u003c/sub\u003e from AIMD simulations.\u003cstrong\u003e f \u003c/strong\u003eThe calculated potential energy curves of three diatomic systems: Ga\u003csub\u003e2\u003c/sub\u003e, GaPt, and Pt\u003csub\u003e2\u003c/sub\u003e. \u003cstrong\u003eg\u003c/strong\u003e The formation energies and energy barriers associated with Ga atom insertion into Pt–Pt bonds in Pt\u003csub\u003e2\u003c/sub\u003eGa, (Ga\u003csub\u003e6\u003c/sub\u003ePt)\u003csub\u003e2\u003c/sub\u003eGa, and (Ga\u003csub\u003e7\u003c/sub\u003ePt)\u003csub\u003e2\u003c/sub\u003eGa molecular systems (the rough estimation suggests that the reaction can overcome an energy barrier of 67 kcal/mol at 923 K\u003csup\u003e24\u003c/sup\u003e).\u003c/p\u003e","description":"","filename":"floatimage2.jpeg","url":"https://assets-eu.researchsquare.com/files/rs-7086103/v1/30e97867459e5641c43ec2da.jpeg"},{"id":87174247,"identity":"ba600fcd-e3ac-4e6c-b14b-78c77788a93a","added_by":"auto","created_at":"2025-07-21 08:16:21","extension":"jpeg","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":571898,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eCharacterization of liquid catalyst.\u003c/strong\u003e \u003cstrong\u003ea\u003c/strong\u003e TEM images and EDS elements mapping of the liquid catalyst. \u003cstrong\u003eb\u003c/strong\u003e SAED pattern of the liquid catalyst,\u003cstrong\u003e c\u003c/strong\u003e,\u003cstrong\u003e d \u003c/strong\u003eXPS spectra of Ga 2p (c) and Pt 4f (d) in liquid catalyst. \u003cstrong\u003ee\u003c/strong\u003e Normalized XANES spectra at the Pt \u003cem\u003eL\u003c/em\u003e\u003csub\u003e3\u003c/sub\u003e-edge. \u003cstrong\u003ef\u003c/strong\u003e FT Pt \u003cem\u003eL\u003c/em\u003e\u003csub\u003e3\u003c/sub\u003e-edge EXAFS spectra in R space of liquid catalyst with phase correction.\u003c/p\u003e","description":"","filename":"floatimage3.jpeg","url":"https://assets-eu.researchsquare.com/files/rs-7086103/v1/08f568c56120460d51712067.jpeg"},{"id":87174975,"identity":"05944368-e19a-4330-a4dd-b836fdeb2230","added_by":"auto","created_at":"2025-07-21 08:24:21","extension":"jpeg","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":1020280,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eEthane dehydrogenation performance of liquid metal dispersed SACs.\u003c/strong\u003e \u003cstrong\u003ea\u003c/strong\u003e Schematic showing the structure evolution of adaptive surface active sites in liquid metal dispersed SAC when exposed to ethane atmosphere. \u003cstrong\u003eb\u003c/strong\u003e,\u003cstrong\u003e c\u003c/strong\u003e Catalytic performances at 650 °C. \u003cstrong\u003ed\u003c/strong\u003e Long-term stability test. \u003cstrong\u003ee\u003c/strong\u003e XANES spectra of the liquid metal dispersed SAC after 100 h ethane dehydrogenation taken at Pt \u003cem\u003eL\u003c/em\u003e\u003csub\u003e3\u003c/sub\u003e edge. \u003cstrong\u003ef\u003c/strong\u003e \u003cem\u003ek\u003c/em\u003e\u003csub\u003e3\u003c/sub\u003e-weighted FFT spectra in \u003cem\u003eR\u003c/em\u003e-space at Pt \u003cem\u003eL\u003c/em\u003e\u003csub\u003e3\u003c/sub\u003e edge.\u003c/p\u003e","description":"","filename":"floatimage4.jpeg","url":"https://assets-eu.researchsquare.com/files/rs-7086103/v1/fa79c6ed5ff783a3cdf52200.jpeg"},{"id":108171055,"identity":"022610a3-d6f4-42bd-bf8b-1e91eb28456e","added_by":"auto","created_at":"2026-04-30 07:05:37","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":4249225,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-7086103/v1/36dfba01-46e9-41b9-95be-b9b587d6999d.pdf"},{"id":87174973,"identity":"09e1cdb4-84ce-4956-8a4a-d644e07c29ac","added_by":"auto","created_at":"2025-07-21 08:24:21","extension":"docx","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":3170077,"visible":true,"origin":"","legend":"Supplementary Information","description":"","filename":"SupplementaryInformation.docx","url":"https://assets-eu.researchsquare.com/files/rs-7086103/v1/ada2eb2eb36b062e0ca6e3e8.docx"},{"id":87174255,"identity":"77683fe9-1226-4f18-abb7-2bef5842eadd","added_by":"auto","created_at":"2025-07-21 08:16:22","extension":"mp4","order_by":2,"title":"","display":"","copyAsset":false,"role":"supplement","size":30041784,"visible":true,"origin":"","legend":"Supplementary Movie 1-the structural evolution of Pt10 clusters in liquid Ga","description":"","filename":"SupplementaryMovie1thestructuralevolutionofPt10clustersinliquidGa.mp4","url":"https://assets-eu.researchsquare.com/files/rs-7086103/v1/878121d70e2dcfebe9e6f18f.mp4"},{"id":87174977,"identity":"af10b37e-541a-4c22-8fc7-51c4ab20cf80","added_by":"auto","created_at":"2025-07-21 08:24:22","extension":"mp4","order_by":3,"title":"","display":"","copyAsset":false,"role":"supplement","size":30483117,"visible":true,"origin":"","legend":"Supplementary Movie 2-the structural evolution of dispersed Pt10 in liquid Ga","description":"","filename":"SupplementaryMovie2thestructuralevolutionofdispersedPt10inliquidGa.mp4","url":"https://assets-eu.researchsquare.com/files/rs-7086103/v1/cc61e112526072139366b5c0.mp4"},{"id":87174263,"identity":"c6e93f70-3587-4b76-b5b0-c424ecdb4dc2","added_by":"auto","created_at":"2025-07-21 08:16:22","extension":"mp4","order_by":4,"title":"","display":"","copyAsset":false,"role":"supplement","size":29505863,"visible":true,"origin":"","legend":"Supplementary Movie 3-the NPT MD simulationt for the Ga98Pt2 system","description":"","filename":"SupplementaryMovie3theNPTMDsimulationtfortheGa98Pt2system.mp4","url":"https://assets-eu.researchsquare.com/files/rs-7086103/v1/ddd2a6b1297d6e02b9d0a53c.mp4"},{"id":87174262,"identity":"c6ae5f8f-6d51-450e-b297-49258c846aee","added_by":"auto","created_at":"2025-07-21 08:16:22","extension":"mp4","order_by":5,"title":"","display":"","copyAsset":false,"role":"supplement","size":30346087,"visible":true,"origin":"","legend":"Supplementary Movie 4-the NVT MD simulationt for the Ga98Pt2 system","description":"","filename":"SupplementaryMovie4theNVTMDsimulationtfortheGa98Pt2system.mp4","url":"https://assets-eu.researchsquare.com/files/rs-7086103/v1/e3d0be7822adeae33b2380b6.mp4"}],"financialInterests":"There is \u003cb\u003eNO\u003c/b\u003e Competing Interest.","formattedTitle":"Liquid metal dispersed single-atom catalyst with high-temperature stability","fulltext":[{"header":"Introduction","content":"\u003cp\u003eIndustrial thermocatalysis holds great promise for improving the efficiency and sustainability of thermochemical processes and producing value-added chemicals in the modern chemical industry\u003csup\u003e1\u0026ndash;3\u003c/sup\u003e. Single-atom catalysts (SACs) have garnered extensive attention for the development of highly efficient, sustainable, cost-effective catalysts in thermocatalysis fields due to their maximized atom utilization and highly homogeneous metal coordination environment\u003csup\u003e4\u0026ndash;8\u003c/sup\u003e. However, constructing highly thermally durable SACs is a significant challenge in industrial applications. This is owing to the inherently ultra-high surface energy of single atoms, and the high temperature (\u0026gt;\u0026thinsp;300 \u003csup\u003eo\u003c/sup\u003eC) provides enough energy to overcome the diffusion barrier of single atoms, leading to the migration of single atoms and severe agglomeration\u003csup\u003e9\u003c/sup\u003e. In the current paradigm, it is prevalent to stabilize SACs by modulating supports (such as carbon-based supports\u003csup\u003e10\u003c/sup\u003e and metal oxides characterized by defection\u003csup\u003e11\u0026ndash;14\u003c/sup\u003e and so on) that tune interactions between metal atoms and supports. However, the presence of a strong bonding interaction between the supports and the single atoms may result in the compromise of the unique coordination structure of the single atoms, thereby diminishing the catalytic activity and even deactivation\u003csup\u003e15,16\u003c/sup\u003e. In terms of the strategy of using porous supports to spatially confine single atoms (such as molecular sieves, and metal-organic frameworks)\u003csup\u003e17,18\u003c/sup\u003e, surmounting the substantial surface energy of the single atoms is still difficult, which will lead to inevitable aggregation of single atoms at elevated temperatures\u003csup\u003e19,20\u003c/sup\u003e. Hence, designing an optimal support that balances metal-support interaction for realizing highly efficient thermal-stable SACs remains a formidable obstacle.\u003c/p\u003e\u003cp\u003eInspired by the rule of thumb \u0026ldquo;like dissolves like\u0026rdquo;, it is promising to take advantage of unique metal-metal interaction to efficiently disperse active metals to acquire stable single atoms with inherently high metal activity by using the liquid metal as the dispersion. Herein, we achieve the highly efficient dispersion of single atoms with unprecedented thermal stability by utilizing the inherent fluidity and metal affinity of liquid metal. As a demonstration, gallium (Ga) capable of an ideal liquid environment was employed to spontaneously disperse active metal platinum (Pt). Exceptionally thermal-stable Pt single atoms dispersed by Ga that survived at 650\u0026deg;C were realized. In this system, profiting from the superior metal affinity of Ga with Pt, Pt\u0026ndash;Pt bonds are broken at elevated temperatures, and subsequently the mobile Pt atoms are captured by Ga to form stable Pt\u0026ndash;Ga interaction, accomplishing the highly efficient dispersion of Pt single atoms. The fluidity of liquid metal and the stable Pt\u0026ndash;Ga interaction ensures that the Pt atoms can remain dynamically scattered to the whole liquid metal dispersion system. Additionally, liquid metal dispersed single atoms can self-update onto the catalysis interface continuously, promoting catalytic reactions at the interface. Hence, these liquid metal dispersed SACs manifested remarkable thermal durability for ethane dehydrogenation (EDH), sustaining stable operation for over 100 hours at 650 \u003csup\u003eo\u003c/sup\u003eC with ethylene selectivity of 98%. This elucidates the promising potential of this approach in realizing highly thermal-stable SACs.\u003c/p\u003e"},{"header":"Results","content":"\u003cp\u003e\u003cb\u003eThe design of thermal-stable liquid metal dispersed SACs\u003c/b\u003e\u003c/p\u003e\u003cp\u003eWith increasing temperature, the surface energy of single atoms will dramatically rise, and the migration of single atoms will be accelerated, leading to severe aggregation and sintering\u003csup\u003e9,21\u003c/sup\u003e. In essence, the competition of aggregation reflected the competitive bonding between single atom/single atom and single atom/support. Establishing highly-efficiency as well as stable metal-support interaction is crucial for blocking the aggregation and sintering of single atoms at high temperatures. In this work, we make the realization of thermal-stable SACs by utilizing liquid metal to disperse and stabilize active metals (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ea). The abundance of metallic bonds in the liquid metal makes it an ideal medium for effectively dispersing active metals with similar metallic bonds and the active metals can keep the highly active metallic state. At elevated temperatures, enough energy was provided to break metallic bonds in the active metals. Furthermore, the fluidity of liquid metals boosts the spontaneous random movement of heterogeneous atoms, which drives the disordered dispersion of active atoms in liquid metals at elevated temperatures, similar to Brownian motion. These dynamically migrating single atoms can be subsequently combined with liquid metal profiting from its good metallic affinity and form stable interaction between liquid metal and active metal. In light of this, equipped with the naturally metallic affinity and fluidity of liquid metal, the highly thermal-stable SACs can be realized.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003eThe preparation of liquid metal dispersed SACs is by dissolving Pt nanoparticles into liquid Ga at elevated temperatures. The mechanism illustrating the programmable formation process of the liquid metal dispersed SACs is summarized in Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ea. Firstly, the Pt powders were sprinkled evenly over the liquid metal. As the temperature gradually increases, the solubility of the active metal in the dispersion is further increased, and the active metal can efficiently disperse in the liquid metal within its limited solubility. The Pt\u0026thinsp;\u0026minus;\u0026thinsp;Pt bonds in the original Pt metal nanoparticles are broken and tend to bind tightly to Ga atoms and form a thermodynamically stable configuration with Ga atoms benefiting from the good affinity between Ga and Pt under high temperatures. Thereby the stable Pt\u0026thinsp;\u0026minus;\u0026thinsp;Ga interaction curtails the sintering of Pt single atoms and maintains the stability of SACs. Moreover, according to the Arrhenius Eq.\u0026nbsp;2\u003csup\u003e2\u003c/sup\u003e, the thermal motion of atoms would be intensified by high temperature, promoting the rapid diffusion between Pt and Ga atoms and the continuous renewal of Pt single atoms exposed on the catalytic surface (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003eb). In contrast, when single atoms are anchored to solid supports, their co-migration with the supports becomes kinetically constrained. Once the metal-support interactions become insufficient to compensate for the inherently high surface energy of single atoms, these atoms tend to detach from the solid supports and aggregate. This process is exothermic, where minimization of total surface energy governs particle growth\u003csup\u003e23\u003c/sup\u003e. Meanwhile, some single atoms may embed into the lattice of supports, becoming buried when the interaction between the support and metal atoms is too strong. These processes lead to the loss of active sites, reducing the stability of SACs and consequently affecting their activity and selectivity (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ec).\u003c/p\u003e\u003cp\u003e\u003cb\u003eThermal stability of active metal atoms monodispersed in liquid Ga\u003c/b\u003e\u003c/p\u003e\u003cp\u003eAb initio molecular dynamics (AIMD) simulations were employed to elucidate the atomic-scale dispersed state of active metal in liquid metal (computational details are provided in the supplementary information). Using Pt\u003csub\u003e10\u003c/sub\u003e as a model of Pt cluster, we investigated the structural evolution of both clustered and dispersed Pt\u003csub\u003e10\u003c/sub\u003e in liquid Ga during 10 ps simulations at 923 K (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ea, b and Supplementary Mov. 1, 2). The calculated total energy versus time curves for the Ga\u003csub\u003e90\u003c/sub\u003ePt\u003csub\u003e10\u003c/sub\u003e system containing clustered Pt\u003csub\u003e10\u003c/sub\u003e and dispersed Pt\u003csub\u003e10\u003c/sub\u003e (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ec) reveal that the dispersed Pt\u003csub\u003e10\u003c/sub\u003e generally exhibits lower total energy compared to the aggregated Pt\u003csub\u003e10\u003c/sub\u003e clusters within the simulated 10 ps. The results indicate that the remarkable atomic diffusion of liquid Ga metal at high temperature promotes the migration of heterogeneous active metal atoms, thereby stabilizing their dispersed atomic state in liquid Ga.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003eThe relatively high Pt concentration in the Ga\u003csub\u003e90\u003c/sub\u003ePt\u003csub\u003e10\u003c/sub\u003e system leads to intermittent formation of Pt\u003csub\u003e2\u003c/sub\u003e dimer, as evidenced by the time-dependent curve of the shortest Pt\u0026ndash;Pt distance (Supplementary Fig.\u0026nbsp;1). To further elucidate the actual existence state of Pt atoms in liquid Ga, we performed AIMD simulations of the Ga\u003csub\u003e98\u003c/sub\u003ePt\u003csub\u003e2\u003c/sub\u003e system (a Pt\u003csub\u003e2\u003c/sub\u003e dimer embedded in Ga\u003csub\u003e98\u003c/sub\u003e) at 923 K. The 10 ps NVT ensemble simulations (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ed) display that the Pt-Pt interatomic distance progressively increases from 4.18 \u0026Aring; to 11.63 \u0026Aring;, significantly exceeding the Pt\u0026ndash;Pt bond length of 2.65\u0026thinsp;~\u0026thinsp;2.79 \u0026Aring;\u003csup\u003e25\u003c/sup\u003e. This unequivocally confirms that Pt atoms preferentially exist as monatomic species in the liquid Ga (Supplementary Fig.\u0026nbsp;2 and Mov. 3, 4). Further statistical analysis of the coordination environment of Pt atoms in the Ga\u003csub\u003e98\u003c/sub\u003ePt\u003csub\u003e2\u003c/sub\u003e system shows that the dominant coordination numbers for individual Pt atoms are 8 or 9 (Supplementary Fig.\u0026nbsp;3 and Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ee), implying that monodispersed Pt atoms migrate within liquid Ga in the form of clusters such as Ga₈Pt or Ga₉Pt (Supplementary Fig.\u0026nbsp;4).\u003c/p\u003e\u003cp\u003eTo fundamentally understand the thermodynamic preference for Pt mono-dispersion in liquid Ga, we systematically evaluated the binding interactions through potential energy curve calculations of three representative diatomic systems: Ga₂, GaPt, and Pt₂ (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ef). The calculated bond dissociation energies show a clear ranking: \u003cem\u003eE\u003c/em\u003e(Pt\u0026ndash;Pt) (107.9 kcal/mol)\u0026thinsp;\u0026gt;\u0026thinsp;\u003cem\u003eE\u003c/em\u003e(Ga\u0026ndash;Pt) (74.9 kcal/mol)\u0026thinsp;\u0026gt;\u0026thinsp;\u003cem\u003eE\u003c/em\u003e(Ga\u0026ndash;Ga) (32.5 kcal/mol). Crucially, the formation of two Ga\u0026ndash;Pt bonds (149.8 kcal/mol) is energetically favored over either maintaining a Pt\u0026ndash;Pt bond (107.9 kcal/mol) or the combined Pt\u0026ndash;Pt and Ga\u0026ndash;Ga bonding (140.4 kcal/mol). This energetic advantage, coupled with the inherently weaker Ga\u0026ndash;Ga interactions in liquid Ga compared to isolated Ga₂ molecules\u003csup\u003e26\u003c/sup\u003e and the good affinity between Ga and Pt\u003csup\u003e27\u003c/sup\u003e, enables Ga atoms to disrupt Pt\u0026ndash;Pt bonds to form stable Pt\u0026ndash;Ga\u0026ndash;Pt bridging units. Meanwhile, we calculated the formation energies of Pt₂Ga, (Ga₆Pt)₂Ga, and (Ga₇Pt)₂Ga molecules, which were determined to be 101.1, 46.2, and 57.9 kcal/mol, respectively (Supplementary Fig.\u0026nbsp;5 and Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eg). Additionally, we roughly estimated the energy barriers of Ga atom insertion into the Pt\u0026ndash;Pt bond to be 58.2, 13.4, and 40.2 kcal/mol by performing rigid scans of the Pt\u0026ndash;Ga\u0026ndash;Pt angle (Supplementary Fig.\u0026nbsp;6 and Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eg). These results clearly demonstrate that, both thermodynamically and kinetically, Ga atoms in liquid Ga at 923 K can readily disrupt Pt\u0026ndash;Pt bonds, thereby promoting the mono-dispersion of Pt atoms. The stable Ga\u003csub\u003e8\u003c/sub\u003ePt and similar clusters that are formed profited from the favorable affinity between Ga and Pt inhibit the aggregation and sintering of Pt during thermal motion, laying the foundation for synthesizing the highly thermal-stable SACs.\u003c/p\u003e\u003cp\u003e\u003cb\u003eCharacterization of liquid catalyst\u003c/b\u003e\u003c/p\u003e\u003cp\u003eTo further validate that liquid metal can act as the dispersion for single atoms, we synthesized a Ga-dispersed Pt single-atom catalyst (Pt@Ga) following the strategy described above. The detailed structure of the catalyst was characterized by transmission electron microscopy (TEM) and energy dispersive spectrometry (EDS). The Pt species in the liquid metal existed in a monodisperse distribution without the obvious occurrence of aggregated Pt (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ea). The bright-field image of Pt@Ga liquid catalyst maintains an almost invariant brightness across the whole particle and the corresponding selected area electron diffraction (SAED) data shows no diffraction spots of Pt in the amorphous ring, revealing the lack of long-range order structure in the Ga\u0026ndash;Pt catalyst (Supplementary Figs.\u0026nbsp;7 and 3b). Furthermore, the X-ray photoelectron spectroscopy (XPS) spectrum was employed to reveal the chemical composition and electronic structure of the liquid metal dispersed SAC. Prior to the execution of XPS measurements, the sample underwent etching with argon ions to eliminate the natural oxide layer and surface contaminants. Then, the XPS measurements indicate that the as-synthesized catalyst contains approximately 0.2 at% Pt and 99.8 at% Ga (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ec, d). Ga 2\u003cem\u003ep\u003c/em\u003e peaks appear at 1116.73 eV and 1116.59 eV, which are consistent with the reported binding energies of metallic Ga (Ga\u003csup\u003e0\u003c/sup\u003e 2\u003cem\u003ep\u003c/em\u003e\u003csub\u003e3/2\u003c/sub\u003e=1116.70 eV). Meanwhile, due to the higher electronegativity of Pt (2.28) than that of Ga (1.81)\u003csup\u003e28\u003c/sup\u003e, the Pt in the Pt@Ga system served as the electron acceptor, and the Pt 4\u003cem\u003ef\u003c/em\u003e\u003csub\u003e7/2\u003c/sub\u003e and 4\u003cem\u003ef\u003c/em\u003e\u003csub\u003e5/2\u003c/sub\u003e peaks in Pt@Ga exhibit positive shift (1.0 eV) than those in pure Pt metal. It is a consensus that metallic Pt\u003csup\u003e0\u003c/sup\u003e species occupy a preeminent role as the active sites for many catalytic processes\u003csup\u003e29\u0026ndash;31\u003c/sup\u003e. Consequently, the single-atom dispersion of Pt in liquid metal won\u0026rsquo;t sacrifice the activity of catalysts. This approach guarantees a proficient and robust distribution of single atoms, thereby preserving their unparalleled catalytic activity. Furthermore, the absence of the obvious aggregation of Pt atoms in the Pt@Ga was further identified by X-ray diffraction (XRD) tests, where no signal of Pt (PDF#04-0802) is observed (Supplementary Fig.\u0026nbsp;8). The XRD results supported our idea that the Pt species constantly migrated in liquid metal, probably resulting in the dispersion of Pt in single-atom. To mitigate the potential inaccuracies arising from the insensitivity of XRD to small Pt clusters, the pair distribution function (PDF) analysis was conducted to delve into the interatomic structure of the Pt@Ga liquid catalyst (Supplementary Fig.\u0026nbsp;9). The absence of Pt\u0026ndash;Pt bonds indicates that Pt is distributed nearly at the atomic level within the liquid Ga without the formation of Pt clusters. These observations suggest that liquid metal can achieve the efficiently uniform dispersion of highly active single atoms at elevated temperatures.\u003c/p\u003e\u003cp\u003eTo further verify the exact dispersion state of Pt in Pt@Ga catalyst, X-ray absorption spectroscopy (XAS) measurements were conducted. According to the X-ray absorption near-edge structure (XANES) spectrum presented in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ee, the adsorption edge energy of Pt in Pt@Ga is lower than that of the Pt reference foil at room temperature, revealing an average valence lower than Pt\u003csup\u003e0\u003c/sup\u003e. The negative charge results from the higher electronegativity of Pt than Ga, which is consistent with the results of XPS. The electron transfer from Ga to Pt favors stable metal-support interaction between Ga and Pt. Correspondingly, the \u003cem\u003ek\u003c/em\u003e\u003csub\u003e3\u003c/sub\u003e-weighted \u003cem\u003eR\u003c/em\u003e-space Fourier transformed spectra of the extended X-ray absorption fine structure spectra (EXAFS) show the prominent peak at 2.14 \u0026Aring; for Pt@Ga SAC, distinguished from that of the Pt\u0026ndash;O (1.62 \u0026Aring;) bonds for PtO\u003csub\u003e2\u003c/sub\u003e and the Pt\u0026ndash;Pt bonds (2.24 \u0026Aring;) for Pt foil (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ef). All these results intuitively indicate that the Pt exists in the single-atom state in liquid metal.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003e\u003cb\u003eEthane dehydrogenation performance of liquid metal dispersed SACs\u003c/b\u003e\u003c/p\u003e\u003cp\u003eBased on the computational results, the liquid metal dispersed SACs theoretically feature excellent thermal stability at high temperatures. As a proof of concept, the thermal stability was validated by the ethane dehydrogenation (EDH) experiment. As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ea, when exposed to ethane, Pt single atoms exposed on the surface capture ethane molecules and synergistically activate C\u0026ndash;H bonds, leading to selective ethane dehydrogenation to ethylene. Meanwhile, the fluidic characteristic of liquid metal dispersed SACs at operated conditions enables continuous replenishment of catalytically active Pt atoms onto the surface. And stable interaction between Pt\u0026thinsp;\u0026minus;\u0026thinsp;Ga effectively blocks the aggregation of Pt atoms during the constant migration. Benefiting from the advantages mentioned above, these adaptive surface active sites maintain long-term activity and thermal stability.\u003c/p\u003e\u003cp\u003eTo circumvent the issue of inadequate interaction between the liquid metal dispersed SACs and the reaction gas, the porous support is utilized to amplify the gas mass transfer rate. So, we coupled liquid metal supported SACs with porous MFI zeolite (ZSM-5) by the physical approach of ultrasonication to increase the contact surface area between the liquid metal support SACs and gas reactants. As demonstrated in Supplementary Fig.\u0026nbsp;10, EDS mappings revealed well-distributing of Ga, Si, and Al, indicating the liquid metal is uniformly loaded in the ZSM-5 zeolite framework. Upon heating, Pt will be spontaneously dispersed in Ga homogeneously, achieving the preparation of a zeolite-dispersed liquid metal supported SACs (Pt@Ga/ZSM-5). Further, we performed \u003cem\u003ein situ\u003c/em\u003e XRD to explore the dispersing process of Pt (Supplementary Fig.\u0026nbsp;11). The diffraction peak observed at 43\u0026ndash;47\u003csup\u003eo\u003c/sup\u003e originates from the carbon \u003cem\u003ein situ\u003c/em\u003e reactor (Supplementary Fig.\u0026nbsp;12). Initially, the characteristic peaks of Pt can be apparently observed located at 39.76\u003csup\u003eo\u003c/sup\u003e and 46.24\u003csup\u003eo\u003c/sup\u003e. With the temperature increasing, the characteristic peaks of Pt were gradually weakened and disappeared subsequently, proving the dispersion of Pt particles.\u003c/p\u003e\u003cp\u003eThe catalytic performance was evaluated in non-oxidative EDH at 923 K in a fixed-bed quartz U-tube reactor under atmosphere pressure with feed gas of 12.5 vol% C\u003csub\u003e2\u003c/sub\u003eH\u003csub\u003e6\u003c/sub\u003e in Ar. The commercial aluminosilicate ZSM-5 exhibited ethane conversion at 10.7% and ethylene selectivity at 84.3% under the given conditions (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eb, c). The poor selectivity originates from the absence of active metal sites with high ethylene selectivity, resulting in inefficient dehydrogenation and dominant side reactions. The reactive gas adsorbs specifically onto the acidic sites of the molecular sieve during its passage, leading to the production of coke. Accumulated coke deactivates the catalyst by both filling the micropores and blocking the active sites\u003csup\u003e32\u003c/sup\u003e. Therefore, the pure ZSM-5 suffers from poor catalyst performances. Interestingly, the liquid metal dispersed SAC was highly active with ethane conversion at 17.8% and ethylene selectivity at 98.5%, outperforming the counterparts. The performance of the liquid metal dispersed SAC in the durability test was presented in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ed. It exhibits sustainable conversion and selectivity in the continuous reaction for 100 h, where the constant ethane conversion of ~\u0026thinsp;18% is obtained without attenuation. And liquid metal dispersed SAC exhibits a steady ethene productivity of around 14.3 g g\u003csub\u003ePt\u003c/sub\u003e\u003csup\u003e\u0026minus;1\u003c/sup\u003e h\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e during the 100 h EDH test. The catalyst displays no deactivation trend during the testing period, indicating a reasonable expectation of more perdurable stability. Notably, the XANES spectrum and \u003cem\u003eR\u003c/em\u003e-space of liquid metal dispersed SAC after 100 h ethane dehydrogenation at Pt \u003cem\u003eL\u003c/em\u003e\u003csub\u003e3\u003c/sub\u003e-edge is similar to that of pristine liquid single-atom catalyst (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ee, f and Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ee, f), demonstrating exceptional structural integrity under prolonged thermal catalysis. The catalytic performance and structural characterization together confirmed the superior thermal stability of liquid metal dispersed SAC in extremely high temperatures, which remarkably outperforms the traditional solid support loaded SACs. The excellent stability, selectivity, and conversion indicate the potential importance of liquid metal dispersed SAC for the reaction limited in harsh conditions in the future.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e"},{"header":"Conclusions","content":"\u003cp\u003eWe succeeded in achieving the highly thermal-stable SACs by harnessing the inherent fluidity and metal affinity of liquid metal to form stable metal-metal interaction at high temperatures. In this system, the Pt\u0026ndash;Pt bond in the active metal is broken at elevated temperatures and then Pt atoms are captured by liquid metal to form a highly stable Pt\u0026ndash;Ga interaction, which enables Pt atoms to constantly remain uniformly dynamically decentralized to liquid metal. Crucially, the Pt atoms can maintain a highly-stable dispersed state during ethane dehydrogenation at 650 \u003csup\u003eo\u003c/sup\u003eC for 100 h, while the catalyst maintains an impressive selectivity of 98%. Our strategy provides accessible guidance for acquiring highly thermal-stable SACs by using liquid metal as the dispersion.\u003c/p\u003e"},{"header":"Declarations","content":"\u003ch2\u003eCompeting interests\u003c/h2\u003e\n\u003cp\u003eThe authors declare no competing interests.\u003c/p\u003e\n\u003ch2\u003eAuthor contributions\u003c/h2\u003e\n\u003cp\u003eL.F. conceived the research concept. L.F., and M.Q.Z. supervised the research. Z.Y.Z. and C.Y.W. carried out the main experiments, collected and analyzed the data. F.D. supervised the theoretical calculations, and M.J.S. performed the computational simulations. M.Y.D., X.T., D.L. and D.H.L contributed to the catalytic performance evaluation. S.Y.H. contributed to sample preparation and data analysis. Z.J.L. and Y.S.M. processed the XAFS results. Y.L.Z. performed transmission electron microscopy characterizations. L.L. contributed to the in situ XRD characterizations. L.F., M.Q.Z., Z.Y.Z., C.Y.W., and M.J.S. cowrote the manuscript. All the authors contributed to data analysis and scientific discussion.\u003c/p\u003e\n\u003ch2\u003eAcknowledgements\u003c/h2\u003e\n\u003cp\u003eThe research was supported by the Natural Science Foundation of China (22025303), the Fundamental Research Funds for the Central Universities (2042025kf0007), and the Postdoctoral Fellowship Program of CPFS (GZB20240567). We thank the Center for Electron Microscopy at Wuhan University for their substantial supports of TEM work. We thank the Core Facility of Wuhan University for the measurement of inductively coupled plasma-atomic emission spectrometry, XPS, TEM, and the Core Research Facilities of the College of Chemistry and Molecular Sciences at Wuhan University for the XRD and PDF characterizations. We also thank the BL11B beamline of the Shanghai Synchrotron Radiation Facility for the XAFS characterization.\u003c/p\u003e\n\u003ch2\u003eData availability\u003c/h2\u003e\n\u003cp\u003eThe data that support the findings of this study are available from the corresponding authors on reasonable request.\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\n\u003cli\u003ePeng, M.\u003cem\u003e et al.\u003c/em\u003e Thermal catalytic reforming for hydrogen production with zero CO\u003csub\u003e2\u003c/sub\u003e emission. \u003cem\u003eScience\u003c/em\u003e \u003cstrong\u003e387\u003c/strong\u003e, 769\u0026minus;775 (2025).\u003c/li\u003e\n\u003cli\u003eWang, Y., Zhang, Y., Wang, X., Liu, Y. \u0026amp; Wu, Z. Photothermal direct methane conversion to formaldehyde at the gas-solid interface under ambient pressure. \u003cem\u003eNat. 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Rev.\u003c/em\u003e \u003cstrong\u003e113\u003c/strong\u003e, 109248 (2019).\u003c/li\u003e\n\u003c/ol\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":true,"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":"nature-portfolio","isNatureJournal":true,"hasQc":false,"allowDirectSubmit":false,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"","title":"Nature Portfolio","twitterHandle":"","acdcEnabled":false,"dfaEnabled":false,"editorialSystem":"ejp","reportingPortfolio":"","inReviewEnabled":true,"inReviewRevisionsEnabled":false},"keywords":"","lastPublishedDoi":"10.21203/rs.3.rs-7086103/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-7086103/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eSingle-atom catalysts (SACs) enable greener and more economically sustainable chemical production by significantly improving thermocatalysis efficiency and selectivity through maximized atom utilization and highly homogeneous metal coordination environments. Unfortunately, single-atom catalysts (SACs) are fundamentally constrained by the stability owing to the severe aggregation of single atoms especially under the high-temperature thermocatalysis operations, which compromises the overall catalytic performance. Here, we report a strategy to realize the highly thermal-stable SACs resistance to sintering at harsh conditions through harnessing the inherently metal affinity and fluidity of liquid metal. A stable liquid metal-active metal interaction is formed, profiting from the superior metal affinity of liquid metal. Combined with the fluidity of liquid metal, active metal atoms can move but remain confined to the liquid metal as the metallic single-atom state at high temperatures. This catalyst exhibits outstanding thermal durability for ethane dehydrogenation, sustaining stable operation for over 100 h at 650 \u003csup\u003eo\u003c/sup\u003eC with an impressive ethylene selectivity of 98%. The strategy of constructing stable metal-metal interactions by utilizing the inherently metal affinity and dynamic fluidity of liquid metal will pave a practical way for the design of highly thermal-stable SACs.\u003c/p\u003e","manuscriptTitle":"Liquid metal dispersed single-atom catalyst with high-temperature stability","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2025-07-21 08:16:16","doi":"10.21203/rs.3.rs-7086103/v1","editorialEvents":[],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"nature-communications","isNatureJournal":true,"hasQc":false,"allowDirectSubmit":false,"externalIdentity":"NCOMMS","sideBox":"Learn more about [Nature Communications](http://www.nature.com/ncomms/)","snPcode":"","submissionUrl":"https://mts-ncomms.nature.com/","title":"Nature Communications","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"ejp","reportingPortfolio":"Nature Communications","inReviewEnabled":true,"inReviewRevisionsEnabled":false}}],"origin":"","ownerIdentity":"762c7b33-7c07-4d0e-816e-a96e1f82fe2c","owner":[],"postedDate":"July 21st, 2025","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"published-in-journal","subjectAreas":[{"id":51740888,"name":"Physical sciences/Chemistry/Catalysis"},{"id":51740889,"name":"Physical sciences/Materials science/Materials for energy and catalysis"}],"tags":[],"updatedAt":"2026-04-30T07:05:31+00:00","versionOfRecord":{"articleIdentity":"rs-7086103","link":"https://doi.org/10.1038/s41467-026-70476-2","journal":{"identity":"nature-communications","isVorOnly":false,"title":"Nature Communications"},"publishedOn":"2026-03-13 04:00:00","publishedOnDateReadable":"March 13th, 2026"},"versionCreatedAt":"2025-07-21 08:16:16","video":"","vorDoi":"10.1038/s41467-026-70476-2","vorDoiUrl":"https://doi.org/10.1038/s41467-026-70476-2","workflowStages":[]},"version":"v1","identity":"rs-7086103","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-7086103","identity":"rs-7086103","version":["v1"]},"buildId":"XKTyCvWXoU3ODBz1xrDgd","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}