Wang Ziming, Yue Xiaoyang, Liao Yulong, Xiang Quanjun
Yangtze Delta Region Institute (Huzhou), University of Electronic Science and Technology of China, Huzhou, 313001, P. R. China.
State Key Laboratory of Electronic Thin Film and Integrated Devices, School of Electronic Science and Engineering, University of Electronic Science and Technology of China, Chengdu, 610054, P. R. China.
ChemSusChem. 2025 Feb 16;18(4):e202401810. doi: 10.1002/cssc.202401810. Epub 2024 Nov 7.
The photoelectrochemical (PEC) dual-electron pathway for water oxidation to produce hydrogen peroxide (HO) shows promising prospects. However, the dominance of the four-electron pathway leading to O evolution competes with this reaction, severely limiting the efficiency of HO production. Here, we report a InO passivator-coated BiVO (BVO) photoanode, which effectively enhances the selectivity and yield of HO production via PEC water oxidation. Based on XPS spectra and DFT calculations, a heterojunction is formed between InO and BVO, promoting the effective separation of interface and surface charges. More importantly, Mott-Schottky analysis and open-circuit potential measurements demonstrate that the InO passivation layer on the BVO photoanode shifts the hole quasi-Fermi level towards the anodic direction, enhancing the oxidation level of holes. Additionally, the widening of the depletion layer and the flattening of the band bending on the InO-coated BVO photoanode favor the generation of HO while suppressing the competitive O evolution reaction. In addition, the coating of InO can also inhibit the decomposition of HO and improve the stability of the photoanode. This work provides new perspectives on regulating PEC two/four-electron transfer for selective HO production via water oxidation.
用于水氧化生成过氧化氢(HO)的光电化学(PEC)双电子途径显示出广阔的前景。然而,导致氧气析出的四电子途径占主导地位,与该反应相互竞争,严重限制了HO的生产效率。在此,我们报道了一种涂覆有InO钝化剂的BiVO(BVO)光阳极,它通过PEC水氧化有效地提高了HO生产的选择性和产率。基于XPS光谱和DFT计算,InO和BVO之间形成了异质结,促进了界面和表面电荷的有效分离。更重要的是,Mott-Schottky分析和开路电位测量表明,BVO光阳极上的InO钝化层将空穴准费米能级向阳极方向移动,提高了空穴的氧化水平。此外,涂覆InO的BVO光阳极上耗尽层的加宽和能带弯曲的变平有利于HO的生成,同时抑制竞争性的析氧反应。此外,InO涂层还可以抑制HO的分解,提高光阳极的稳定性。这项工作为通过水氧化调节PEC双/四电子转移以选择性生产HO提供了新的视角。