轴向磷配位修饰Co-N4活性中心促进双通道H2O2光合成

doi:10.1016/S1872-2067(25)64735-8

摘要/Abstract

摘要：

太阳能驱动的过氧化氢(H₂O₂)光合成为其绿色经济合成提供了重要途径. 单原子催化剂(SACs)因具有快速的电荷转移动力学、能够为O₂提供Pauling构型吸附活性位点以及可调的电子结构等优势, 在H₂O₂光合成方面展现出良好潜力. 其中, 钴单原子催化剂(Co-SACs)凭借其适中的d带中心而展现出最优的*OOH吸附能, 在电催化O₂还原反应(ORR)合成H₂O₂方面展现出优异的催化活性与选择性. 然而, 受限于光生载流子定向富集位点与反应物吸附位点不匹配、水氧化反应(WOR)动力学缓慢且选择性低导致的严重载流子复合, Co-SACs在光催化H₂O₂合成领域催化活性与选择性仍欠佳.

针对该问题, 本文通过磷化策略调控了高结晶氮化碳(g-C₃N₄)纳米棒(CCN)侧边缘负载的Co-N4活性位点的配位环境, 成功构筑了具有独特配位结构的Co单原子活性中心, 即一个Co原子与四个平面N原子和一个轴向P原子配位(记作Co-N₄P₁). X射线吸收谱、X射线光电子能谱和密度泛函理论(DFT)计算结果共同揭示了Co单原子的精确配位结构. 旋转环盘电流测试、活性物种电子顺磁共振测试和捕获实验、原位漫反射红外傅里叶变换光谱以及同位素标定结果共同表明, Co-N₄P₁通过高活性与选择性的2e^--ORR与2e^--WOR路径实现H₂O₂光合成. DFT计算结果表明, 其高活性与选择性源于轴向P配体对Co-N₄P₁中作为ORR活性位点的中心Co原子和作为WOR活性位点的平面配位N原子的精准电子结构调控. 具体而言, 轴向P配体诱导Co-N₄P₁的导带(CB)底附近形成由Co 3d轨道占据的中隙态, 从而促进了光生电子在中心Co活性位点的定向富集. 得益于此, ORR活性位点从倾向于4e^--ORR路径的末端-NH₂位点转移到具有Pauling吸附构型且倾向于2e^--ORR路径的Co位点, 从而提高了2e^--ORR路径选择性. 此外, 轴向P配体的引入还促进了Co 3d轨道的d带中心上移, 优化了Co位点对*OOH中间体的吸附, 使其吸附能更接近活性火山图的顶点, 从而在保证2e^--ORR路径选择性的同时提高了催化活性. 同时, 轴向P配体的引入促进了N 2p轨道的p带中心下移, 减弱了N位点对*OH中间体的吸附, 有效提高了2e^--WOR路径光合成H₂O₂的选择性. 光催化性能测试表明, Co-N₄P₁表现出了优异的H₂O₂光合成效率(295.6 µmol g^-1 h^-1)和太阳能-化学能转化效率(0.32%), 其光合成效率分别是Co-N₄ (19.2 µmol g^-1 h^-1)和CCN(27.6 µmol g^-1 h^-1)的15倍和11倍.

综上, 本文揭示了电子结构调控对促进Co-SACs高效合成H₂O₂的关键作用, 为优化H₂O₂光合成路径和提高合成效率提供了新思路.

关键词: 高结晶氮化碳, 配位工程, Co-N₄P₁单原子活性位点, 电子结构调控, H₂O₂光合成

Abstract:

Single-atom catalysts are promising for H₂O₂photosynthesis from O₂ and H₂O, but their efficiency is still limited by the ill-defined electronic structure. In this study, Co single-atoms with unique four planar N-coordination and one axial P-coordination (Co-N₄P₁) are decorated on the lateral edges of nanorod-like crystalline g-C₃N₄(CCN) photocatalysts. Significantly, the electronic structures of central Co as active sites for O₂ reduction reaction (ORR) and planar N-coordinator as active sites for H₂O oxidation reaction (WOR) in Co-N₄P₁can be well regulated by the synergetic effects of introducing axial P-coordinator, in contrast to the decorated Co single-atoms with only four planar N-coordination (Co-N₄). Specifically, directional photoelectron accumulation at central Co active sites, induced by an introduced midgap level in Co-N₄P₁, mediates the ORR active sites from 4e^--ORR-selective terminal -NH₂ sites to 2e^--ORR-selective Co sites, moreover, an elevated d-band center of Co 3d orbital strengthens ORR intermediate *OOH adsorption, thus jointly facilitating a highly selective and active 2e^--ORR pathway to H₂O₂ photosynthesis. Simultaneously, a downshifted p-band center of N 2p orbital in Co-N₄P₁ weakens WOR intermediate *OH adsorption, thus enabling a preferable 2e^--WOR pathway toward H₂O₂ photosynthesis. Subsequently, Co-N₄P₁ exhibits exceptional H₂O₂photosynthesis efficiency, reaching 295.6 μmol g^-1 h^-1 with a remarkable solar-to-chemical conversion efficiency of 0.32 %, which is 15 times that of Co-N₄ (19.2 μmol g^-1 h^-1) and 10 times higher than CCN (27.6 μmol g^-1 h^-1). This electronic structure modulation on single-atom catalysts offers a promising strategy for boosting the activity and selectivity of H₂O₂ photosynthesis.

Key words: Crystalline carbon nitride, Coordination engineering, Single atom Co-N₄P₁ active sites, Modulating electronic structure, Overall H₂O₂ photosynthesis

梁诗诺, 李冯俊, 黄菲, 王心俣, 刘升卫. 轴向磷配位修饰Co-N₄活性中心促进双通道H₂O₂光合成[J]. 催化学报, 2025, 76: 81-95.

Shinuo Liang, Fengjun Li, Fei Huang, Xinyu Wang, Shengwei Liu. Modulating electronic structure of g-C₃N₄ hosted Co-N₄ active sites by axial phosphorus coordination for efficient overall H₂O₂ photosynthesis from oxygen and water[J]. Chinese Journal of Catalysis, 2025, 76: 81-95.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(25)64735-8

https://www.cjcatal.com/CN/Y2025/V76/I9/81

图/表 12

Scheme 1. Schematic of the Co-N4P1 catalyst.

Fig. 1. SEM image of sample CCN (a), Co-N4 (b) and Co-N4P1 (c). TEM (d), HRTEM (e) and AC-HAADF-STEM (f) images of Co-N4P1. (g) HRTEM image of CCN. HAADF-STEM image (h) and the corresponding EDS elemental mappings (i-l) of the typical sample Co-N4P1.

Fig. 2. XPS and XAFS characterizations. XPS spectra of Co 2p (a) and P 2p (b). Normalized Co K-edge XANES spectra (c) and k2-weighted Co K-edge FT-EXAFS spectra (d) at R space of Co-N4, Co-N4P1 and reference samples. The k2-weighted Co K-edge EXAFS fitting curve of Co-N4 (e) and Co-N4P1 (f) at R space. (g-j) WT-EXAFS spectra of Co foil, Co-N4, CoPc, Co-N4P1.

Fig. 3. DFT optimized structure and the corresponding formation energy of the Co-N4 (a) and Co-N4P1 (b) catalysts (model (1)).

Fig. 4. PDOS plots of Co-N4 (a) and Co-N4P1 (b) obtained by DFT calculations; and corresponding LUMO and HOMO orbitals of Co-N4 (c) and Co-N4P1 (d). UV-vis diffuse reflectance spectra (e) and the illustrated band structures (f) of samples CCN and Co-N4 and Co-N4P1.

Fig. 5. The steady-state PL spectra (a), time-resolved PL spectra (b), transient photocurrent responses (c), Nyquist plots of EIS curves (d), electrochemical O2 reduction (e) and H2O oxidation (f) curves of samples CCN, Co-N4 and Co-N4P1.

Fig. 6. (a) H2O2 photosynthesis performance on CCN, Co-N4 and Co-N4P1 samples. Experimental conditions: photocatalyst (0.25 g L-1, 40 mL) under full spectrum irradiation (λ ?≥ 320?nm, 200 mW cm-2), 1?atm O2 with pure water (pH = 7) and T = 298 K. (b) The corresponding fitted formation rate constants (Kf) and decomposition rate constants (Kd). (c) Cycling stability of the Co-N4P1 catalyst. (d) AQE of Co-N4P1 as a function of wavelength. (e) H2O2 photosynthesis performance in an oxygen-free environment on CCN, Co-N4 and Co-N4P1 samples. (f) Activity comparison of Co-N4P1 with reported state-of-the-art photocatalysts under visible-light (λ? ≥ 420?nm), 1?atm O2, pure water (pH = 7) and T?=?298?K.

Fig. 7. (a) Influence of CH3OH (h+ scavenger) for the H2O2 photosynthesis on CCN, Co-N4 and Co-N4P1. (b) ESR spectra of superoxide radicals (•O2-). (c) The Koutecky-Levich plots obtained by RDE measurements at −2.0 V (vs. Ag/AgCl). (d) Influence of AgNO3 (e- scavenger) for the H2O2 generation on CCN, Co-N4 and Co-N4P1. (e) ESR spectra of hydroxyl radicals (•OH). (f) H218O isotope experiment to explore the H2O2 evolution through WOR pathway for Co-N4P1.

Fig. 8. In situ DRIFTS spectra under H2O and O2 of Co-N4 (a) and Co-N4P1 (b).

Fig. 9. The adsorption of O2 (a) and H2O (b) at different sites for Co-N4 and Co-N4P1.

Fig. 10. (a) Comparison of ∆G*OOH for the 2e?-ORR in catalytic activity volcanoes plot on Co-N4 and Co-N4P1 and other transition metal (Mn, Fe, Ni, Cu) single atom catalysts [28]. (b) Calculated free energy diagrams for WOR on Co-N4 and Co-N4P1. PDOS for Co 3d (c) and N 2p (d). COHP analyses of the Co-O bonds (e) and N-O bonds (f). (g) Schematic diagram about the optimize *OOH and *OH intermediate adsorption.

Scheme 2. Schematic illustration of reaction pathways toward H2O2 photosynthesis at the spatially separated ORR and WOR centers over Co-N4P1.

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轴向磷配位修饰Co-N₄活性中心促进双通道H₂O₂光合成

Modulating electronic structure of g-C₃N₄ hosted Co-N₄ active sites by axial phosphorus coordination for efficient overall H₂O₂ photosynthesis from oxygen and water

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