BiVO4 光阳极动态阴离子交换促进水氧化过氧化氢的产生,ACS Catalysis

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BiVO4 光阳极动态阴离子交换促进水氧化过氧化氢的产生
ACS Catalysis ( IF 11.3 ) Pub Date : 2023-11-02 , DOI: 10.1021/acscatal.3c03380
Shipeng Wan _{1,

2} , Jie Jin ₂ , Chaoran Dong ₁ , Yuan Lu ₂ , Qin Zhong ₁ , Kan Zhang ₁ , Jong Hyeok Park ₂

Affiliation

_{通过HCO 3}^-或CO ₃^-介质进行光电化学（PEC）水氧化H ₂ O ₂生产已引起了广泛的研究兴趣，但其活性低且不稳定。在此，我们报告了一种阴离子交换策略，使用磷酸盐 (PO ₄^3– ) 修饰的 BiVO ₄ (PBVO) 光阳极来增强半导体电解质 (SE) 界面亥姆霍兹层的HCO ₃^{-氧化动力学，以获得优异的 H}₂ O ₂生产。结果，与优化的PBVO光阳极相比，平均PEC H ₂ O ₂法拉第效率（FE）达到82.6%，最佳FE为92.1%，生产率为66.5 μmol h ^–1。此外，实现了全细胞结构下稳定的PEC水分解为H ₂和H ₂ O _{2 ，连续照射6 h后H}₂ O ₂积累浓度为2.34 × 10 ^–3 M。优异的PEC性能归因于PBVO光阳极表面的PO ₄^3–在水氧化过程中与HCO ₃^–交换形成CO ₃^–吸附的BiVO ₄光阳极，动力学上促进了电荷转移SE 接口。同时，在内亥姆霍兹层中PO ₄³和 HCO ³_交换过程中形成的^H₂ PO _{4可以稳定 H}₂ O ₂。这项工作为理解 SE 界面亥姆霍兹层中的 PEC 氧化过程提供了新的见解。

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Promoting Water Oxidative Hydrogen Peroxide Production by Dynamic Anion Exchange on BiVO4 Photoanodes

Photoelectrochemical (PEC) water oxidative H₂O₂ production through HCO₃^– or CO₃^– medium has been attracting great research interest, yet it suffers from low activity and instability. Herein, we report an anion exchange strategy using a phosphate (PO₄^3–) modified BiVO₄ (PBVO) photoanode to enhance the HCO₃^– oxidation kinetics at the Helmholtz layer of the semiconductor-electrolyte (S-E) interface for superior H₂O₂ production. As a result, an average PEC H₂O₂ Faradaic efficiency (FE) of 82.6% was achieved over the optimized PBVO photoanode with the best FE of 92.1% and a production rate of 66.5 μmol h^–1. Moreover, the stable PEC water splitting to H₂ and H₂O₂ from full-cell configuration is realized, with a H₂O₂ accumulation concentration of 2.34 × 10^–3 M after 6 h consecutive irradiation. The excellent PEC performance can be ascribed to the fact that PO₄^3–on the surface of the PBVO photoanode exchanges with HCO₃^– to form the CO₃^– adsorbed BiVO₄ photoanode during the process of water oxidation, kinetically promoting charge transfer at the S-E interface. Simultaneously, H₂PO₄^– that is formed during the exchange of PO₄^3– and HCO₃^– in the inner Helmholtz layer can stabilize H₂O₂. This work provides a new insight for understanding PEC oxidation processes in the Helmholtz layer of the S-E interface.

更新日期：2023-11-02

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