Synergistic Integration of Electronic Structure Modulating and Hierarchical Mass Transport Channels in Wood-Derived Electrocatalysts for Efficient Oxygen Evolution

Synergistic Integration of Electronic Structure Modulating and Hierarchical Mass Transport Channels in Wood-Derived Electrocatalysts for Efficient Oxygen Evolution | Authorea try { document.documentElement.classList.add('js'); } catch (e) { } var _gaq = _gaq || []; _gaq.push(['_setAccount', 'G-8VDV14Y67G']); _gaq.push(['_trackPageview']); (function() { var ga = document.createElement('script'); ga.type = 'text/javascript'; ga.async = true; ga.src = ('https:' == document.location.protocol ? 'https://ssl' : 'http://www') + '.google-analytics.com/ga.js'; var s = document.getElementsByTagName('script')[0]; s.parentNode.insertBefore(ga, s); })(); Skip to main content Preprints Collections Wiley Open Research IET Open Research Ecological Society of Japan All Collections About About Authorea FAQs Contact Us Quick Search anywhere Search for preprint articles, keywords, etc. Search Search ADVANCED SEARCH SCROLL Energy & Environmental Materials This is a preprint and has not been peer reviewed. Data may be preliminary. 27 December 2025 V1 Latest version Share on Synergistic Integration of Electronic Structure Modulating and Hierarchical Mass Transport Channels in Wood-Derived Electrocatalysts for Efficient Oxygen Evolution Authors : zihan zhang , Weizhe Yuan , Sha Chen , Cheng Zhou , Xinmin Zhang , Xiaowei Wang , Han Xu 0000-0002-3211-7081 [email protected] , Yan Qing , and Yiqiang Wu Authors Info & Affiliations https://doi.org/10.22541/au.176686758.88061981/v1 Published ENERGY & ENVIRONMENTAL MATERIALS Version of record Peer review timeline 239 views 103 downloads Contents Abstract Information & Authors Metrics & Citations View Options References Figures Tables Media Share Abstract Modulating the electronic structure of catalysts is widely recognized as an effective strategy to enhance electrocatalytic performance. This study synthesized a nanosheet array composed of Cr-Co2P confined within a P, N co-doped carbon matrix (Cr-Co2P@PNC) through a facile synchronous carbonization-phosphorization method, then anchored it onto a P-doped carbonized wood framework (PCW) to construct a composite catalyst. Benefiting from the synergistic coupling between the Cr-Co2P@PNC nanosheet array architecture and the wood-derived carbon matrix, the Cr-Co2P@PNC/PCW demonstrates remarkable catalytic activity and long-term durability for the oxygen evolution reaction (OER), achieving an overpotential of 283 mV at 50 mA cm-2 with stable operation exceeding 100 hours. Experimental characterization and theoretical calculations confirm that the coupling of wood-derived interconnected hierarchical porous structures with the nanosheet array facilitates extensive contact between active sites and electrolyte, enhancing mass transport during reactions. Cr doping modulates the electronic structure, alleviating strong adsorption at Co sites and reducing the energy barrier of the OER rate-determining step. The P, N co-doped carbon matrix promotes electron transfer and optimizes reaction kinetics. This work demonstrates an optimization strategy for OER composite catalysts while providing new perspectives for exploring renewable wood-derived catalyst designs. Article category: (Research Article) Subcategory: (Nanomaterials) Synergistic Integration of Electronic Structure Modulating and Hierarchical Mass Transport Channels in Wood-Derived Electrocatalysts for Efficient Oxygen Evolution Zihan Zhang, Weizhe Yuan, Sha Chen*, Cheng Zhou, Xinmin Zhang, Xiaowei Wang, Han Xu*, Yan Qing*, and Yiqiang Wu Z. Zhang, W. Yuan, Prof. S. Chen, C. Zhou, Prof. X. Zhang, X. Wang, Prof. H. Xu, Prof. Y. Qing, and Prof. Y. Wu School of Materials and Energy, Central South University of Forestry and Technology, Changsha 410004, P. R. China. Prof. H. Xu, Prof. Y. Qing, and Prof. Y. Wu State Key Laboratory of Utilization of Woody Oil Resource, Central South University of Forestry and Technology, Changsha 410004, P. R. China. E-mail: [email protected] E-mail: [email protected] E-mail: [email protected] Keywords: electrocatalyst, wood, hierarchical porous structure, electronic modulation, oxygen evolution reaction Modulating the electronic structure of catalysts is widely recognized as an effective strategy to enhance electrocatalytic performance. This study synthesized a nanosheet array composed of Cr-Co 2 P confined within a P, N co-doped carbon matrix (Cr-Co 2 P@PNC) through a facile synchronous carbonization-phosphorization method, then anchored it onto a P-doped carbonized wood framework (PCW) to construct a composite catalyst. Benefiting from the synergistic coupling between the Cr-Co 2 P@PNC nanosheet array architecture and the wood-derived carbon matrix, the Cr-Co 2 P@PNC/PCW demonstrates remarkable catalytic activity and long-term durability for the oxygen evolution reaction (OER), achieving an overpotential of 283 mV at 50 mA cm -2 with stable operation exceeding 100 hours. Experimental characterization and theoretical calculations confirm that the coupling of wood-derived interconnected hierarchical porous structures with the nanosheet array facilitates extensive contact between active sites and electrolyte, enhancing mass transport during reactions. Cr doping modulates the electronic structure, alleviating strong adsorption at Co sites and reducing the energy barrier of the OER rate-determining step. The P, N co-doped carbon matrix promotes electron transfer and optimizes reaction kinetics. This work demonstrates an optimization strategy for OER composite catalysts while providing new perspectives for exploring renewable wood-derived catalyst designs. 1. Introduction To address the escalating energy crisis precipitated by rapid fossil fuel depletion, the strategic development of sustainable green energy alternatives derived from earth has become an unavoidable imperative. Hydrogen (H 2 ), as a promising energy vector, has garnered significant attention in recent years. [1, 2] Among emerging technologies, electrochemical water splitting for H 2 production stands as an ideal approach for renewable energy conversion and storage. However, due to the inherent sluggish kinetics of the oxygen evolution reaction (OER) at the anode, the efficacy of this method is critically contingent upon the availability of highly efficient catalysts. [3-5] Currently, noble metal-based catalysts containing iridium (Ir), and ruthenium (Ru) are recognized as state-of-the-art materials, yet their high costs and scarcity pose substantial challenges for the commercial application of electrochemical water splitting. Consequently, the development of cost-effective and high-performance catalysts with long-term operational stability is an urgent prerequisite. [6] Transition metal phosphides (TMPs) have emerged as promising candidates in recent years, owing to their structural tunability, elemental abundance, and distinctive electrochemical properties. [7, 8] However, the inherent limitations of pristine TMPs, particularly their low electrical conductivity, suboptimal catalytic activity, and inadequate environmental stability, lead to performance disparities when benchmarked against conventional noble metal-based catalysts. To address these challenges, rational modulation strategies to enhance the intrinsic activity of TMPs have become a critical research priority. [9-11] Among these, exogenous element doping represents a highly effective optimization approach. The introduction of dopants with varying electronegativities enables precise modulation of both electronic and geometric structures in TMPs, this atomic-level engineering not only fine-tunes existing active sites but also induces synergistic effects, thereby significantly boosting catalytic efficacy and operational durability. [12-14] Moreover, while most reported catalysts including TMPs have been predominantly synthesized in powder form to date, their performance evaluation involves both cumbersome testing procedures and the frequent addition of polymer binders. This inevitably leads to the loss of active sites and obstruction of mass transport processes. [15] Recent research has identified the direct growth of active components on three-dimensional hierarchically porous conductive substrates as a highly attractive method for improving electrocatalytic performance. To date, numerous conductive substrates, such as metal foams, carbon cloth, carbon paper, and graphene, have been utilized for integrated electrode catalysts. [16-18] Nevertheless, high costs, significant environmental toxicity, and structural limitations of these substrates reduce the cost-effectiveness and efficiency of integrated electrode catalysts, hindering their large-scale application. In conclusion, the rational design and integration of simple, cost-effective, and environmentally benign substrates with high-performance TMPs catalysts represent a scientifically pathway toward achieving a sustainable hydrogen economy. Wood, as an abundant green renewable resource, exhibits unique physicochemical properties and hierarchical architecture. [19] Functioning as a natural polymeric material, its cell walls contain abundant hydroxyl groups that provide sufficient coupling sites for in situ growth of active species through chemical bonding. Furthermore, wood’s porous structure with low tortuosity and interconnected hierarchical channels enables efficient mass transport of ions, water, and gases, making it an ideal substrate for establishing gas-solid-liquid triple-phase interfaces in electrocatalytic systems. [20-22] Inspired by this efficient synergistic transport network, we developed a facile strategy involving Cr-incorporated ZIF-L precursors. Through a facile synchronous carbonization-phosphorization process, we confined Cr-Co 2 P nanosheets within a P, N co-doped carbon matrix (Cr-Co 2 P@PNC) while anchoring them onto the porous framework of P-doped carbonized wood (PCW). The Cr dopant modulates the local electronic structure of active sites, optimizing adsorption energies of reaction intermediates. The carbon-coated architecture enhances electron transport, thereby facilitating the OER process. Remarkably, Cr-Co 2 P@PNC/PCW demonstrates exceptional OER performance, achieving a low overpotential of 283 mV at 50 mA cm -2 with negligible activity decay during 100 hours continuous operation. This study innovatively integrates doping engineering with porous architecture of natural wood, establishing a novel strategy for designing cost-effective, high-performance OER electrocatalysts. 2. Results and Discussion 2.1. Materials Characterization The fabrication process of Cr-Co 2 P@PNC/PCW is illustrated in Figure 1 . Initially, poplar wood was sectioned along the growth direction of natural wood into slices followed by cleaning and drying. Scanning electron microscopy (SEM) image reveal abundant aligned low-tortuosity open channels in natural wood ( Figure 2a ), where hydroxyl-rich cellulose ribbons provided substantial coordination sites, creating favorable environments for active species immobilization. [23] Cr-ZIF-L nanosheets were then uniformly anchored within wood vessels via room-temperature impregnation to obtain Cr-ZIF-L/NW precursors. Relative to ZIF-L/NW, Cr doping induced no morphological alterations (Figure S1, Supporting Information). X-ray diffraction (XRD) characterizations of Cr-ZIF-L/NW revealed two broad characteristic peaks at 15.6° and 22.6° corresponding to cellulose I crystalline structure, while no discernible diffraction peaks assignable to any zeolitic imidazolate framework phases were detected (Figure S2a, Supporting Information), attributable to the weak crystallographic signals of the loading material being obscured by the robust signal of the substrate material. For further characterization, the powder collected from the wood slice substrate was re-analyzed by XRD, which showed that the powder sample closely matched the simulated pattern and structure of ZIF-L(Co) reported in the literature (Figure S2b, Supporting Information), [24] suggesting the successful synthesis of the precursor. Finally, Cr-Co 2 P@PNC/PCW composite electrocatalysts were obtained through synchronous carbonization-phosphorization. The pyrolytic derivatives of Cr-ZIF-L preserved ordered nanosheet array architectures, with observed increased surface roughness and reduced nanosheet thickness (Figure 2b, c). These ultrathin nanosheet arrays exposed abundant active sites to accelerate electron transfer, thereby enhancing OER catalytic performance. Notably, natural wood lumens inherently possess interconnected vessel pits that serve as microchannels to facilitate electrolyte infiltration and diffusion. Observation of pit regions in Cr-Co 2 P@PNC/PCW lumens reveals that nanosheet arrays are orderly arranged around the pits without causing blockage, demonstrating that Cr-Co 2 P@PNC/PCW effectively maintains these advantageous transport structures (Figure S3a, b, Supporting Information). The contact angle of Cr-Co 2 P@PNC/PCW (29.04°) significantly lower than those of PCW (90.36°) and NW (96.16°), indicating the construction of nanosheet arrays substantially enhanced hydrophilicity to increase electrolyte accessibility (Figure S4, Supporting Information). Transmission electron microscopy (TEM) images reveal that the nanosheets in Cr-Co 2 P@PNC/PCW are primarily composed of carbon-coated nanoparticles with diameters of approximately 30 nm (Figure S5, Supporting Information), which enhances the accessibility of the reaction surface and thereby optimizes the reaction kinetics of OER. [25] Clear lattice stripe can be observed in the high-resolution TEM (HRTEM) image, which can be directed to the (112) planes of Co 2 P (Figure 2d, e). The measured interplanar spacing of 0.231 nm exhibited a 0.09 nm increase compared to standard (112) planes, confirming lattice expansion due to Cr doping. [26, 27] Selected-area electron diffraction (SAED) patterns additionally identified (402) planes of Co 2 P (Figure 2f). STEM imaging with corresponding EDS mapping verified homogeneous distribution of Co, P, N, and Cr throughout the nanosheet architecture (Figure 2g). ICP-OES quantification yielded a Cr: Co molar ratio of 1:12.6 (Table S1), closely matching the precursor feeding ratio (1:10), conclusively confirming successful incorporation of Cr elements. In the XRD pattern of Cr-Co 2 P@PNC/PCW, the broad diffraction peak between 10° and 40° originates from the PCW substrate, while the peaks at 40.7°, 43.3°, and 52.0° are ascribed to the (112), (211), and (020) planes of Co 2 P (JCPDS No. 04-007-1524). Compared to undoped Co 2 P@PNC/PCW, no additional Cr-containing phases were detected, indicating the absence of new crystalline phases post Cr doping ( Figure 3a ). To validate the role of the P, N co-doped carbon encapsulation, Cr-Co 2 P/PCW without this coating was synthesized using Cr-doped Co layered double hydroxide precursors (Cr-Co LDH), with corresponding XRD patterns and SEM images provided in the supporting information (Figure S6a–c, Supporting Information). Raman spectra exhibited D band (1339 cm -1 ) and G band (1601 cm -1 ) peaks (Figure 3b), where the intensity ratio (I D /I G ) serves as a critical indicator for carbon defect density and graphitization degree. [28] Compared with PCW, Cr-Co 2 P@PNC/PCW displayed the higher I D /I G ratio, indicating that Cr-Co 2 P@PNC/PCW has a carbon structure rich in defects, which is conducive to improving catalytic activity. Nitrogen (N 2 ) adsorption-desorption isotherms revealed the mesoporous nature of Cr-Co 2 P@PNC/PCW, showing Type IV isotherms with evident hysteresis loops (Figure 3c). Moreover, the Brunauer-Emmet-Teller (BET) surface area of Cr-Co 2 P@PNC/PCW reached 308.2 m 2 g -1 , significantly surpassing that of PCW (81.1 m 2 g -1 ). The chemical composition and valence states of surface elements were further investigated using X-ray photoelectron spectroscopy (XPS). The XPS spectrum of Cr-Co 2 P@PNC/PCW clearly shows the presence of C, O, Co, Cr, N and P elements (Figure S7a, Supporting Information). In the high-resolution Co 2p spectrum, the peaks at 797.86 and 781.76 eV along with two shake-up satellite peaks (802.72 and 786.28 eV) can be fitted to Co 2p 1/2 and Co 2p 3/2 , while the peaks at 793.69 and 778.83 eV correspond to the Co-P bonds (Figure 3d). It is notable that compared with Co 2 P@PNC/PCW, the Co-P bonds in Cr-Co 2 P@PNC/PCW exhibit a negative shift of 0.29 eV, indicating that Cr doping induces electronic synergy reconstruction and charge density redistribution. [29-31] In the high-resolution Cr 2p spectrum, the peak at 587.08 eV corresponds to Cr 2p 1/2 , and the peaks at 580.48 and 577.48 eV can be assigned to Cr 2p 3/2 , where the binding energy at 580.48 eV and 577.48 eV can be attributed to Cr 3+ and Cr 0 , respectively. (Figure 3e). [29, 32] Furthermore, no signals corresponding to Cr-P bonds are detected, confirming that Cr is introduced through doping. The high-resolution P 2p spectrum can be deconvoluted into five peaks at 135.53, 133.54, 131.92, 130.54 and 129.64 eV, which are respectively assigned to P=O bonds, P-O bonds, C-P bonds, and the characteristic P 2p 1/2 and P 2p 3/2 peaks of metal phosphides (Figure S7b, Supporting Information). [33, 34] Among these, the P=O and P-O bonds should originate from oxygen adsorbed on the sample surface. Besides, the C-P bonds confirm that P elements have been doped into the carbon matrix, which can optimize the electronic structure of the carbon material and regulate its surface polarity, effectively enhancing the electronic coupling effect between the loaded substances and the substrate, thereby improving catalytic activity. In the high-resolution C 1s spectrum, the peaks at 288.95, 287.00, 286.11 and 284.80 eV originate from O-C=O bonds, C-N bonds, C-P bonds and C=C bonds, respectively. [33, 35, 36] The emergent C-N bond coupled with the reappearance of the C-P bond further verifies the formation of P, N co-doped carbon matrix (Figure S7c, Supporting Information). The high-resolution N 1s spectrum reveals that the nitrogen originating from the five-membered aromatic rings in the ZIF precursor persists in the carbon matrix after pyrolysis, which predominantly exists in the forms of oxidized N, graphite N, and pyridinic N (Figure S7d, Supporting Information). [37, 38] Additionally, the relevant XPS spectra of Co 2 P@PNC/PCW are presented in the supporting information (Figure S8, Supporting Information). The valence state and coordination structure of the catalyst were analyzed through X-ray absorption near edge structure (XANES) and extended X-ray absorption fine structure (EXAFS). As shown in Figure 3f, the position of the pre-edge absorption peak indicates that the Co valence state in Cr-Co 2 P@PNC/PCW is intermediate between Co foil and Co 2 P@PNC/PCW, suggesting increased electron density at Co sites after Cr doping, which aligns with XPS results. [39, 40] Fourier transform EXAFS (FT-XAFAS) of the Co K-edge in Cr-Co 2 P@PNC/PCW reveals distinct peaks at 1.50 Å and 2.11 Å, corresponding to Co-P bonds and Co-Co/Cr bonds, respectively. Compared to Co 2 P@PNC/PCW, Cr-Co 2 P@PNC/PCW exhibits a slightly shorter Co-P bond length with the emergence of Co-Co and Co-Cr bonds, likely due to lattice expansion induced by Cr doping that reduces atomic spacing in Cr-Co 2 P@PNC/PCW (Figure 3g and S9, Supporting Information). [41] High-resolution wavelet transforms (WT) EXAFS plots in k-space further confirm the Co coordination configuration (Figure 3h and 3i). These results demonstrate that Cr doping optimizes the electronic structure and coordination environment of Cr-Co 2 P@PNC/PCW by modulating the Co valence state and atomic spacing. 2.2 Electrochemical performance The electrocatalytic OER performance of the Cr-Co 2 P@PNC/PCW self-supporting electrode was evaluated using a standard three-electrode system in 1.0 M KOH, with investigation of the effects of different catalyst components and structures on performance. As shown in Figure 4a and 4b , Cr-Co 2 P@PNC/PCW exhibits overpotentials of only 283 mV and 301 mV to achieve current densities of 50 mA cm -2 and 100 mA cm -2 , outperforming Co 2 P@PNC/PCW (346 mV and 372 mV), Cr-Co 2 P/PCW (365 mV and 407 mV), and RuO 2 /PCW (463 mV and 582 mV). Compared with Co 2 P@PNC/PCW (80.0 mV dec -1 ), Co 2 P/PCW (103.0 mV dec -1 ), and RuO 2 /PCW (195.1 mV dec -1 ), Cr-Co 2 P@PNC/PCW shows a lower Tafel slope of 68.6 mV dec -1 (Figure 4c), indicating that the P, N co-doped carbon matrix and nanosheet array construction can significantly enhance OER activity and optimize catalytic reaction kinetics. A series of composite catalysts (Cr-Co 2 P@PNC/PCW-x) were prepared by adjusting Cr doping content. LSV curves and Tafel slopes demonstrate that the catalyst with 20% Cr content (Cr-Co 2 P@PNC/PCW) exhibits optimal performance (Figure S10a and S10b, Supporting Information). Furthermore, to investigate the effect of Cr doping on intrinsic catalytic activity, the turnover frequency (TOF) was calculated. At an overpotential of 100 mV, Cr-Co 2 P@PNC/PCW shows a TOF value of 0.012 s -1 , higher than 0.006 s -1 for Co 2 P@PNC/PCW (Figure S11, Supporting Information), suggesting that appropriate Cr doping effectively enhances intrinsic activity and improves electrocatalytic performance, while excessive Cr doping may reduce catalytic activity due to insufficient exposure of active sites. [42] To verify the influence of substrate structure on catalytic performance, Cr-Co 2 P@PNC/CC and Cr-Co 2 P@PNC/CP catalysts were prepared by replacing the PCW substrate with carbon cloth and carbon paper. Cr-Co 2 P@PNC/PCW demonstrates lower overpotentials at the current densities of 50 mA cm -2 and 100 mA cm -2 compared to these counterparts (Figure S12, Supporting Information), proving that the wood-derived hierarchical porous structure and interconnected microchannels can effectively enhance OER catalytic performance. Electrochemical impedance spectroscopy (EIS) analysis (Figure 4d and S13, Supporting Information) shows that Cr-Co 2 P@PNC/PCW has the smallest charge transfer resistance (R ct ), which indicates higher conductivity and faster charge transfer rates. Additionally, the electrochemical active surface area (ECSA) was evaluated through double-layer capacitance (C dl ) measurements using cyclic voltammetry (CV) curves. As shown in Figure 4e and S14, the C dl value of Cr-Co 2 P@PNC/PCW (303.6 mF cm -2 ) is significantly larger than those of Co 2 P@PNC/PCW (264.4 mF cm -2 ), Cr-Co 2 P/PCW (133.2 mF cm -2 ) and PCW (40.6 mF cm -2 ), suggesting that Cr-Co 2 P@PNC/PCW with larger ECSA can expose more active sites. The normalized current density determined by ESCA (J ESCA ) further confirms the intrinsic catalytic activity. After normalization, Cr-Co 2 P@PNC/PCW still exhibits the highest J ESCA within the reaction interval (Figure 4f), which conclusively demonstrates its superior intrinsic catalytic activity. [43] Compared with many recently reported non-noble metal electrocatalysts, the Cr-Co 2 P@PNC/PCW self-supporting electrode also demonstrates more outstanding OER catalytic performance (Figure 4g and Table S2). In addition to catalytic activity, stability serves as another crucial criterion for evaluating the potential application prospects of electrocatalysts. As shown in Figure 4h, Cr-Co 2 P@PNC/PCW demonstrates only a 4.5% potential increase rate after 100 hours of continuous operation at 50 mA cm -2 , confirming its exceptional durability. Furthermore, we analyzed the structural and compositional evolution of Cr-Co 2 P@PNC/PCW after the stability test. Post-OER characterization reveals that Cr-Co 2 P@PNC/PCW maintains its original nanosheet array morphology (Figure S15, Supporting Information), indicating superior structural stability. XRD patterns show weakened diffraction peaks for Cr-Co 2 P@PNC/PCW after OER testing (Figure S16a, Supporting Information). In the high-resolution Co 2p spectrum, the characteristic signals of Co-P bonds disappear, while new peaks corresponding to Co 3+ emerge at 795.99 eV and 780.70 eV (Figure S16b, Supporting Information). These changes can be attributed to surface reconstruction and the transformation of phosphides into (oxy)hydroxide. [29, 44, 45] Concurrently, the Cr 2p spectrum exhibits tangible negative shifts in Cr 2p 1/2 and Cr 2p 3/2 binding energies due to hydroxide formation (Figure S16c, Supporting Information). [46] Consistent with the Co 2p spectrum, no Co-P bond signals are observed in the P 2p spectrum (Figure S16d, Supporting Information). These results collectively demonstrate the formation of metal (oxy)hydroxide through surface reconstruction during the OER process. 2.3. Electrocatalytic Mechanism To further elucidate the electronic modulation effect of Cr doping in the OER process, we investigated the catalytic mechanism of Cr-Co 2 P@PNC/PCW through DFT calculations and experimental studies. Theoretical models for Cr-Co 2 P@PNC and Co 2 P@PNC were established, with detailed computational procedures and structural configurations provided in the Supporting Information (Figure S17-S20, Supporting Information). The density of states (DOS) analysis for Cr-Co 2 P@PNC (Figure 5a) reveals predominant Co contributions near the Fermi level, confirming Co as the primary active site for OER. Projected partial density of states (PDOS) analysis of Co 3d orbitals demonstrates that Cr doping shifts the d-band center of Co farther from the Fermi level (Figure 5b), indicating higher antibonding state occupancy and weakened adsorption of intermediates. [47, 48] This electronic structure modulation optimizes the binding capability between active sites and reaction intermediates, facilitating subsequent reaction steps. Gibbs free energy calculations for each reaction stage identified the rate determining step (RDS) as the transformation from O* to OOH* intermediates (Figure 5c). The Cr-Co 2 P@PNC exhibits a significantly reduced RDS energy barrier (1.72 eV) compared to Co 2 P@PNC (1.98 eV), demonstrating that Cr doping lower’s reaction barriers through electron-regulated reconstruction, thereby enhancing OER activity. Operando Bode plots revealed the charge transfer dynamics during OER (Figure 5d, e). With increasing potential, Cr-Co 2 P@PNC/PCW showed a rapid decrease in the low-frequency peak region which corresponds to charge transfer at the catalyst-electrolyte interface, while Co 2 P@PNC/PCW exhibited a significantly slower decay rate. This clear contrast indicates that Cr-Co 2 P@PNC/PCW achieves faster intermediates conversion and enhanced OER activity. [25, 49, 50] Comparative analysis of charge transfer resistance for both catalysts during OER is summarized in Figure 5f and S21. Within the 1.4-1.5 V potential window, R ct values for Cr-Co 2 P@PNC/PCW and Co 2 P@PNC/PCW decrease sharply, indicating the occurrence of structural reorganization. Above 1.5 V, R ct approaches zero for both catalysts, confirming active OER progression. Notably, Cr-Co 2 P@PNC/PCW consistently exhibits lower R ct across the entire potential range, evidencing its superior intrinsic activity. [51] The charge density difference analysis illustrates charge transfer from Co sites to the adsorbed *OOH intermediate, where yellow and cyan regions respectively represent electron accumulation region and depletion region (Figure 5g, h). Compared with the undoped catalyst, Cr-Co 2 P@PNC/PCW exhibits weaker electron transfer, which is attributed to Cr doping modifying the electronic structure of Co sites, enabling electron gain at Co to optimize *OOH trapping capability, thereby further clarifying the intrinsic mechanism of enhanced activity in Cr-Co 2 P@PNC/PCW. [52, 53] Additionally, the charge density difference between Cr-Co 2 P and the P, N-co-doped carbon matrix was calculated (Figure S22, Supporting Information). The results indicate electron transfer between them, which promotes the OER process. [54] The mechanism of OER enhancement by Cr-Co 2 P@PNC/PCW is summarized in Figure 5i, these theoretical findings reveal that Cr doping modifies the electronic structure of Co active sites, fine-tuning their binding capability with reaction intermediates to accelerate the *O to *OOH transformation, thereby achieving superior OER performance. Figure 1. Schematic illustration of the synthesis of Cr-Co 2 P@PNC/PCW. Figure 2. Morphology characterization. (a) SEM image of tangential section of natural wood. (b-c) SEM images of the tangential section of Cr-Co 2 P@PNC/PCW. (d-e) HRTEM images of Cr-Co 2 P@PNC/PCW alongside the corresponding fast Flourier transform pattern from the designated area in (e). (f) SAED pattern of the Cr-Co 2 P@PNC/PCW. (g) HAADF-STEM image and corresponding STEM-EDS elemental mappings of Cr-Co 2 P@PNC/PCW. Figure 3. (a) XRD patterns of Cr-Co 2 P@PNC/PCW, Co 2 P@PNC/PCW and CW. (b) Raman spectra for Cr-Co 2 P@PNC/PCW and PCW. (c) N 2 adsorption-desorption isotherm curves for Cr-Co 2 P@PNC/PCW and PCW. (d) XPS spectra of Co 2p for Cr-Co 2 P@PNC/PCW and Co 2 P@PNC/PCW. (e) XPS spectra of Cr 2p for Cr-Co 2 P@PNC/PCW. (f) Co K-edge X-ray absorption near edge structure (XANES) spectra of Cr-Co 2 P@PNC/PCW, Co 2 P@PNC/PCW and Co foil. (g) FT-EXAFS spectra of Cr-Co 2 P@PNC/PCW, Co 2 P@PNC/PCW and Co foil. WT-EXAFS spectra of (h) Cr-Co 2 P@PNC/PCW and (i) Co 2 P@PNC/PCW. Figure 4. Electrocatalytic OER performance. (a) LSV curves of the different catalysts. (b) Corresponding overpotential histograms at 50 and 100 mA·cm −2 . (c) Corresponding Tafel slopes. (d) Nyquist plots of catalysts for OER in 1.0 M KOH. (e) Double-layer capacitances of catalysts for OER. (f) Normalized LSV curves by ECSA of Cr-Co 2 P@PNC/PCW, Co 2 P@PNC/PCW and Cr-Co 2 P/PCW . (g) Performance comparison with recent studies. (h) Long-term stability of the Cr-Co 2 P@PNC/PCW at 50 mA·cm −2 in 1.0 M KOH. Figure 5. DFT calculations and OER mechanism analysis. (a) Calculated DOS for Cr-Co 2 P@PNC/PCW. (b) PDOS of Co on Cr-Co 2 P@PNC/PCW and Co 2 P@PNC/PCW. (c) Free energy diagrams of OER on Cr-Co 2 P@PNC/PCW and Co 2 P@PNC/PCW. Operando Bode phase angle plots for (d) Cr-Co 2 P@PNC/PCW and (e) Co 2 P@PNC/PCW. (f) The fitting R ct values of Cr-Co 2 P@PNC/PCW and Co 2 P@PNC/PCW at different applied potentials. Charge density differences of *OOH on Co atoms for (g) Cr-Co 2 P@PNC/PCW and (h) Co 2 P@PNC/PCW. (i) Schematic illustration of the OER mechanisms for the Cr-Co 2 P@PNC/PCW electrocatalyst. 3. Conclusion In summary, we developed a straightforward method to anchor Cr-Co 2 P@PNC nanosheet arrays on a PCW framework. Benefiting from the structural effects and electronic modulation arising from the cross-linked hierarchical porous structure of the wood-derived framework and the nanosheet arrays confined in the P, N co-doped carbon matrix, the catalyst exhibits superior catalytic activity (283 mV at 50 mA cm -2 ) and long-term durability (at 50 mA cm -2 for 100 h with only 4.8% decay rate). Experimental profiles and DFT calculations confirm that Cr doping induces electronic reconstruction to optimize intermediate adsorption, while the P, N co-doped carbon matrix facilitates electron transfer to enhance reaction kinetics. Therefore, the enhanced OER activity can be attributed to the synergistic effects of Cr doping, P, N co-doped carbon encapsulation, and the wood-derived carbon architecture. This study provides a rational and feasible approach for designing efficient water electrolysis catalysts and opens possibilities for next-generation energy conversion systems leveraging renewable biomass-based matrices. 4. Experimental Section Chemicals and Materials : Since every reagent was of analytical grade and used without further purification. The study’s natural poplar wood came from Chenzhou in the region of Hunan. Shanghai Titan Technology Co., Ltd. (Adamas-beta®) supplied Cobalt (Ⅱ) nitrate hexahydrate (Co(NO 3 ) 2 ·6H 2 O), Chromic (Ⅲ) nitrate nonahydrate (Cr(NO 3 ) 2 ·9H 2 O), potassium hydroxide (KOH), urea (CO(NH 2 ) 2 ), and 2-Methylimidazole (> 99%). Ethanol (AR) and hydrochloric acid (HCl, A. R.) were purchased from Beijing Chemical Works. Deionized water (DIW) was used to prepare all solutions. Commercial Ruthenium oxide (IV) (RuO 2 ) purchased from Aladdin (Shanghai, China). Pretreatment of Natural Wood (NW) : Natural poplar wood (NW) was cut into 2.5 cm × 1 cm × 0.2 cm slices along the growth direction. The slices were repeatedly polished with 320-grit sandpaper, then ultrasonically cleaned in anhydrous ethanol and deionized water. Subsequently, the slices were immersed in 1.0 M HCl solution under stirring for 1 h to remove impurities, followed by ultrasonic ethanol rinsing. Finally, the slices were dried at 60 °C for 12 h. Synthesis of Cr-ZIF-L/NW, Cr-ZIF-L/NW-x, and ZIF-L/NW : First, 0.2 mmol Cr(NO 3 ) 3 ·9H 2 O was dissolved in 10 mL deionized water. Pretreated wood slices were immersed in this solution and ultrasonicated for 10 min. Separately, 2 mmol Co(NO 3 ) 2 ·6H 2 O and 32 mmol 2-methylimidazole were dissolved in 30 mL and 40 mL deionized water, respectively. The Co(NO 3 ) 2 ·6H 2 O solution and Cr(NO 3 ) 3 ·9H 2 O solution containing wood slices were simultaneously added to the 2-methylimidazole solution under stirring for 10 min. After static aging at room temperature for 3 h, the obtained Cr-ZIF-L/NW was rinsed with deionized water and methanol, then vacuum-dried at 60 ℃. For comparison, samples with varying Cr/Co molar ratios (0.1, 0.3, 0.4 mmol Cr(NO 3 ) 3 ·9H 2 O or without Cr addition) were prepared and designated as Cr-ZIF-L/NW-0.1, Cr-ZIF-L/NW-0.3, Cr-ZIF-L/NW-0.4, and ZIF-L/NW. Synthesis of Cr-Co 2 P@PNC/PCW, Cr-Co 2 P@PNC/PCW-x and Co 2 P@PNC/PCW : Cr-ZIF-L/NW and 1.0 g of NaH 2 PO 2 ·H 2 O were placed in two separate ceramic boats, with the NaH 2 PO 2 ·H 2 O containing boat positioned upstream in the tube furnace. Under a nitrogen atmosphere, the temperature was raised to 300 ℃ at a heating rate of 2 ℃ min -1 and held for 2 h, then further increased to 500 ℃ and held for 2 h, and finally raised to 800 ℃ and held for 4 h. Cr-Co 2 P@PNC/PCW-x and Cr-Co 2 P@PNC/PCW were prepared using the same procedure, with Cr-ZIF-L/NW-x and ZIF-L/NW replacing Cr-ZIF-L/NW as precursors, respectively. Synthesis of Cr-Co 2 P/PCW, PCW, Cr-Co 2 P@PNC/CC and Cr-Co 2 P@PNC/CP : Cr-Co 2 P/PCW and PCW was prepared by identical synchronous carbonization-phosphorization protocol as implemented for Cr-Co 2 P@PNC/PCW. The precursor of Cr-Co 2 P/PCW was substituted from Cr-ZIF-L/NW to Cr-Co LDH/NW, in which the Cr-Co LDH arrays were prepared according to previously reported synthesis methods for layered double hydroxides. Specifically, 1.2 mmol Cr(NO 3 ) 3 ·9H 2 O, 6 mmol Co(NO 3 ) 2 ·6H 2 O, and 12 mmol urea were dissolved in 15 mL anhydrous ethanol and thoroughly mixed. The mixture along with the wood slices was then transferred into a 30 mL lining. The autoclave was placed in an oven and maintained at 120 ℃ for 8 h. After cooling to room temperature, the obtained Cr-Co LDH/NW was repeatedly washed with deionized water and anhydrous ethanol, followed by vacuum drying at 60 ℃. For Cr-Co 2 P@PNC/CC and Cr-Co 2 P@PNC/CP, the substrate material was replaced with carbon cloth (CC) and carbon paper (CP), respectively, while maintaining equivalent synthetic procedures to those described above. Detailed characterizations, electrochemical measurements, and DFT computational methods are provided in the Supporting Information. Acknowledgements This work was supported by National Natural Science Foundation of China (No. 32571967, 32271792), Yuelushan Laboratory Breeding Project (No. YLS-2025-ZY04072), and the Scientific Research Project of Hunan Provincial Education Department (No. 23B0276). The authors also thank Shiyanjia Lab (www.shiyanjia. com) for the support of SEM, TEM and XPS tests. Conflicts of Interest There are no conflicts to declare. Supporting Information Supporting Information is available from the Wiley Online Library or from the author. 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Collection Energy & Environmental Materials Keywords electrocatalyst electronic modulation hierarchical porous structure oxygen evolution reaction wood Authors Affiliations zihan zhang Central South University of Forestry and Technology View all articles by this author Weizhe Yuan Central South University of Forestry and Technology View all articles by this author Sha Chen Central South University of Forestry and Technology View all articles by this author Cheng Zhou Central South University of Forestry and Technology View all articles by this author Xinmin Zhang Central South University of Forestry and Technology View all articles by this author Xiaowei Wang Central South University of Forestry and Technology View all articles by this author Han Xu 0000-0002-3211-7081 [email protected] Central South University of Forestry and Technology View all articles by this author Yan Qing Central South University of Forestry and Technology View all articles by this author Yiqiang Wu Central South University of Forestry and Technology View all articles by this author Metrics & Citations Metrics Article Usage 239 views 103 downloads .FvxKWukQNSOunydq8rnd { width: 100px; } Citations Download citation zihan zhang, Weizhe Yuan, Sha Chen, et al. Synergistic Integration of Electronic Structure Modulating and Hierarchical Mass Transport Channels in Wood-Derived Electrocatalysts for Efficient Oxygen Evolution. Authorea . 27 December 2025. DOI: https://doi.org/10.22541/au.176686758.88061981/v1 If you have the appropriate software installed, you can download article citation data to the citation manager of your choice. Simply select your manager software from the list below and click Download. For more information or tips please see 'Downloading to a citation manager' in the Help menu . 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