在BiVO4光阳极上构建局域电场以促进水氧化过程中的质子转移

doi:10.1016/S1872-2067(25)64665-1

催化学报 ›› 2025, Vol. 72: 176-186.DOI: 10.1016/S1872-2067(25)64665-1

在BiVO₄光阳极上构建局域电场以促进水氧化过程中的质子转移

关志星^a^,¹, 张颖^a^,¹, 冯芳芳^a, 李朝辉^a, 刘艳莉^a, 吴梓峰^a, 郑兴兴^a, 扶雄辉^a, 张渊明^a, 廖文彬^a, 陈嘉璐^a, 刘宏光^a^,^b^,^*(), 朱毅^a^,^c^,^*(), 魏永革^d^,^*()

^a暨南大学化学与材料学院, 广东广州 511443
^b五邑大学应用物理与材料学院, 广东江门 529020
^c暨南大学广东省功能配位超分子材料及应用重点实验室, 广东广州 510632
^d清华大学化学系, 有机光电子与分子工程教育部重点实验室, 北京 100084

收稿日期:2024-12-17 接受日期:2025-02-24 出版日期:2025-05-18 发布日期:2025-05-20
通讯作者: *电子信箱: hongguang_liu@jnu.edu.cn (刘宏光),tzhury@jnu.edu.cn (朱毅),yonggewei@mail.tsinghua.edu.cn (魏永革).
作者简介:¹共同第一作者.
基金资助:
广东省自然科学基金(2021A1515010390);中央高校基本科研业务费(21621401);广东省功能配位超分子材料及应用重点实验室开放基金(2020B121201005);有色金属及材料加工新技术教育部重点实验室/广西光电材料与器件重点实验室开放基金(20KF-5)

Boost proton transfer in water oxidation by constructing local electric fields on BiVO₄ photoanodes

Zhixing Guan^a^,¹, Ying Zhang^a^,¹, Fangfang Feng^a, Zhaohui Li^a, Yanli Liu^a, Zifeng Wu^a, Xingxing Zheng^a, Xionghui Fu^a, Yuanming Zhang^a, Wenbin Liao^a, Jialu Chen^a, Hongguang Liu^a^,^b^,^*(), Yi Zhu^a^,^c^,^*(), Yongge Wei^d^,^*()

^aCollege of Chemistry and Materials Science, Jinan University, Guangzhou 511443, Guangdong, China
^bSchool of Applied Physics and Materials, Wuyi University, Jiangmen 529020, Guangdong, China
^cGuangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and Applications, Jinan University, Guangzhou 510632, Guangdong, China
^dKey Laboratory of Organic Optoelectronics and Molecular Engineering of Ministry of Education Department of Chemistry, Tsinghua University, Beijing 100084, China

Received:2024-12-17 Accepted:2025-02-24 Online:2025-05-18 Published:2025-05-20
Contact: *E-mail: hongguang_liu@jnu.edu.cn (H. Liu), tzhury@jnu.edu.cn (Y. Zhu), yonggewei@mail.tsinghua.edu.cn (Y. Wei).
About author:¹ Contributed equally to this work.
Supported by:
Natural Science Foundation of Guangdong Province(2021A1515010390);Fundamental Research Funds for the Central Universities(21621401);Open Fund of Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and Applications(2020B121201005);Open Fund of Key Laboratory of New Processing Technology for Nonferrous Metal & Materials, Ministry of Education/Guangxi Key Laboratory of Optical and Electronic Materials and Devices(20KF-5)

摘要/Abstract

摘要：

太阳能驱动的光电化学(PEC)分解水技术, 是一种将太阳能直接转化为化学能的有效途径, 在解决能源危机方面具有极大的潜力. 在PEC系统中, 光阳极/电解质界面处发生析氧反应(OER), 其性能直接影响整个系统的光电转换效率. 钒酸铋(BiVO₄)作为一种理想的PEC分解水光阳极材料, 因其具有可见光吸收的窄带隙(2.4 eV)、低成本和无毒性而备受关注. 在标准AM 1.5G模拟光照射下, BiVO₄的理论光电流密度最大可达7.5 mA cm^-2, 太阳能到氢气的转换效率接近9.2%. 然而, 由于OER是一个极其复杂的涉及四个电子和四个质子的质子耦合电子转移过程, 质子转移速率是影响PEC性能的关键因素. BiVO₄水氧化反应中质子转移速率慢, 导致BiVO₄的PEC性能受到了极大的限制.

本文针对BiVO₄水氧化反应中质子转移速率慢的问题, 提出了一种通过在BiVO₄光阳极表面引入羧基配体构建局域电场来加速质子转移的新方法. 以乙酸、乙二酸和丙三酸作为配体, 通过溶剂热法将其修饰在BiVO₄表面, 制备出C₂H₄O₂-BiVO₄, C₂H₂O₄-BiVO₄和C₆H₈O₆-BiVO₄. 通过X射线多晶衍射、X射线光电子能谱(XPS)、扫描电镜、透射电镜和傅里叶变换红外光谱等表征, 证明C_xH_xO_x-BiVO₄光阳极成功制备. 将制备的C_xH_xO_x-BiVO₄光阳极应用于PEC分解水实验中; 结果表明, 与BiVO₄相比, C_xH_xO_x-BiVO₄光阳极在AM 1.5G光照下显示出更快的质子转移速率和更优异的PEC水氧化性能. 其中, C₆H₈O₆-BiVO₄的光电流密度最大, 是BiVO₄的3.5倍, 在1.23 V_RHE下达到3.50 mA cm^-2, 起始电位也从0.70 V_RHE负移至0.38 V_RHE. 法拉第效率达97%, 证实了光电流的增强是来源于水氧化反应. XPS揭示了从BiVO₄到有机羧酸配体的显著电荷转移现象, 证明了局域电场的生成. 通过动力学同位素效应(KIE)和密度泛函理论计算, 证明了局域电场的存在能够加快质子转移, 且局域电场越强, KIE值越低, 质子转移越快, 热力学过电势越低. 与BiVO₄光阳极相比, C_xH_xO_x-BiVO₄的KIE值显著降低, 且质子转移速率的顺序为C₆H₈O₆-BiVO₄ > C₂H₂O₄-BiVO₄ > C₂H₄O₂-BiVO₄, 这与其PEC水氧化性能的顺序是一致的. 这是因为C₆H₈O₆吸电子能力最强, 产生的局域电场最强, KIE值最低, 质子转移最快, 过电势最低, 光电流最强. 另外, 对OER机理的分析研究表明, 随着质子转移速率增加, 质子耦合电子转移机制(PCET)转变为热力学上更有利的电子转移机制(ET). BiVO₄的KIE值高达1.8 (> 1.5), 质子转移速率慢, 质子转移对整个OER过程影响大, 此时OER机制以PCET为主, OER速率慢. 随着C₂H₄O₂, C₂H₂O₄和C₆H₈O₆的引入, KIE值逐步降低, C₆H₈O₆-BiVO₄的KIE值仅为1.0 (< 1.5), 质子转移不再是OER速率的决速步骤, 此时OER机制以ET为主, OER速率加快. 因此, 通过在BiVO₄表面修饰有机羧酸配体构建局域电场, 可以加速质子的转移, 有效促进OER从PCET机制向ET机制转变, 提升BiVO₄光阳极的水氧化性能.

综上所述, 本研究提出了一种通过在光阳极表面修饰有机羧酸配体构建局域电场来加速质子转移进而增强OER效率的策略, 为提高光电催化分解水的性能提供了新的思路.

关键词: 质子转移, BiVO₄, 析氧反应, 局域电场, 光阳极

Abstract:

The slow-proton-fast-electron process severely limits the catalytic efficiency of oxygen evolution reaction. A method is proposed to accelerate proton transfer by building up local electric fields. Modifying acetic, ethanedioic and propanetricarboxylic (C₆H₈O₆) ligands on BiVO₄ surface results in a potential difference between BiVO₄ and ligands that generates a local electric field which serves as a driving force for proton transfer. Among the ligands, carrying the strongest electron-withdrawing ability, the modification of C₆H₈O₆ forms the strongest local electric field and leads to the fastest proton transfer and the smallest thermodynamic overpotential. C₆H₈O₆-BiVO₄ exhibits 3.5 times photocurrent density as high as that of pure BiVO₄, which is 3.50 mA cm^-2 at 1.23 V_RHE. The onset potential of C₆H₈O₆-BiVO₄ shifts negatively from 0.70 to 0.38 V_RHE. The mechanism for OER transitions from thermodynamically high energy proton-coupled electron transfer to thermodynamically low energy electron transfer as proton transfer is accelerated.

Key words: Proton transfer, BiVO₄, Oxygen evolution reaction, Local electric field, Photoanodes

关志星, 张颖, 冯芳芳, 李朝辉, 刘艳莉, 吴梓峰, 郑兴兴, 扶雄辉, 张渊明, 廖文彬, 陈嘉璐, 刘宏光, 朱毅, 魏永革. 在BiVO₄光阳极上构建局域电场以促进水氧化过程中的质子转移[J]. 催化学报, 2025, 72: 176-186.

Zhixing Guan, Ying Zhang, Fangfang Feng, Zhaohui Li, Yanli Liu, Zifeng Wu, Xingxing Zheng, Xionghui Fu, Yuanming Zhang, Wenbin Liao, Jialu Chen, Hongguang Liu, Yi Zhu, Yongge Wei. Boost proton transfer in water oxidation by constructing local electric fields on BiVO₄ photoanodes[J]. Chinese Journal of Catalysis, 2025, 72: 176-186.

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图/表 6

Fig. 1. (a) Formation of CXHXOX-BiVO4 photoanodes. (b,c) SEM images of pristine BiVO4 photoanodes and C2H4O2-BiVO4 photoanodes. (d) TEM images of C2H4O2-BiVO4 photoanodes. (e) HRTEM image of C2H4O2-BiVO4 photoanodes. XRD pattern (f) and FT-IR spectra (g) of BiVO4 and CXHXOX-BiVO4 photoanodes. (h-l) the corresponding EDS elemental mapping images of C2H4O2-BiVO4 photoanode for Bi, V, C, and O, respectively.

Fig. 2. (a) Photocurrent-potential (J-V) curves. (b) Transient photocurrents. (c) Applied bias photon-to-current efficiencies (ABPEs) under a Xenon lamp at 100 mW/cm2 in a 0.1 mol/L phosphate buffer (pH 7.0). (d) Incident photon-to-current efficiencies (IPCEs) under a two-electrode system in a 0.1 mol/L phosphate buffer solution and the applied bias voltage is 1.23 VRHE. (e) Electrochemical impedance spectra (EIS) measured at 1.23 VRHE. (f) UV/Vis diffuse spectra. Inset: Tauc plots of BiVO4 and CxHxOx-BiVO4. (g) the efficiency of light absorption (ηabs). (h) Charge separation efficiency (ηsep). (i) Surface carrier transfer (ηox) of pristine BiVO4 and CxHxOx-BiVO4 photoanodes.

Fig. 3. (a,c,e) J-V curves of BiVO4 and CxHxOx-BiVO4 photoanodes in 0.1 mol/L phosphate H2O and D2O solutions, respectively. (b,d,f) The KIE values of BiVO4 and CxHxOx-BiVO4 calculated from the photocurrent density ratio in H2O and D2O solutions (KIE = JH2O/JD2O). Raman spectra of C2H4O2-BiVO4 after and before PEC (g), C2H2O4-BiVO4 after and before PEC (h), and C6H8O6-BiVO4 after and before PEC (i).

Fig. 4. (a) Mott-Schottky plots of BiVO4 and CXHXOX-BiVO4 photoanodes measured in a 0.1 mol/L phosphate buffer (pH = 7.0) in the dark. Bi 4f (b), V 2p (c), and O 1s (d) XPS spectra for bare BiVO4 and CXHXOX-BiVO4 photoanodes, respectively.

Fig. 5. Charge density difference analyses on BiVO4 (a), C2H4O2-BiVO4 (b), C2H2O4-BiVO4 (c), C6H8O6-BiVO4 (d), gray and blue colors represent charge depletion and accumulation, respectively. The isosurface value is set as 0.02 e/bohr3. (e) DFT-optimized structures and adsorption energies of H2O at the surfaces of BiVO4 and C6H8O6-BiVO4. (f) Gibbs free energy profiles of OER for BiVO4, C2H4O2-BiVO4, C2H2O4-BiVO4 and C6H8O6-BiVO4.

Scheme 1. Electron-proton transfer pathways during interfacial hole transfer for oxidation of BiVO4 (a), C2H4O2-BiVO4 (b), C2H2O4-BiVO4 (c), and C6H8O6-BiVO4 (d).

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在BiVO₄光阳极上构建局域电场以促进水氧化过程中的质子转移

Boost proton transfer in water oxidation by constructing local electric fields on BiVO₄ photoanodes

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