硫化钴装饰BiVO4光阳极提升其光电化学水分解性能

doi:10.1016/S1872-2067(21)63845-7

催化学报 ›› 2022, Vol. 43 ›› Issue (2): 433-441.DOI: 10.1016/S1872-2067(21)63845-7

硫化钴装饰BiVO₄光阳极提升其光电化学水分解性能

周志明^a, 陈金金^a^,^b, 王擎龙^a, 蒋兴星^a, 申燕^a^,^*()

^a华中科技大学武汉光电国家实验室, 湖北武汉 430074
^b华中科技大学洁净与可再生能源中国-欧盟研究所, 湖北武汉 430074

收稿日期:2021-03-26 接受日期:2021-03-26 出版日期:2022-02-18 发布日期:2021-05-24
通讯作者: 申燕
基金资助:
国家重点研究发展计划(2018YFB1502900);国家自然科学基金(21975088);国家自然科学基金重大国际项目(51961165106)

Enhanced photoelectrochemical water splitting using a cobalt-sulfide-decorated BiVO₄ photoanode

Zhiming Zhou^a, Jinjin Chen^a^,^b, Qinlong Wang^a, Xingxing Jiang^a, Yan Shen^a^,^*()

^aWuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology, Wuhan 430074, Hubei, China
^bChina-EU Institute for Clean and Renewable Energy, Huazhong University of Science and Technology, Wuhan 430074, Hubei, China

Received:2021-03-26 Accepted:2021-03-26 Online:2022-02-18 Published:2021-05-24
Contact: Yan Shen
Supported by:
This work was supported by the National Key Research and Development Program of China(2018YFB1502900);the National Natural Science Foundation of China(21975088);the National Natural Science Foundation of China Major International (Regional) Joint Research Project(51961165106)

摘要/Abstract

摘要：

太阳能驱动的光电化学(PEC)水分解可以有效地将太阳能转化为化学能, 作为解决环境排放和能源危机最具前景的途径之一, 已经引起了科学界的广泛关注. PEC水分解系统由两个半反应组成: 在光阳极上的析氧反应(OER)和光阴极上的析氢反应(HER). PEC系统的太阳能转化效率主要由光阳极/电解质界面的OER过程所决定, 这是一个非常复杂且涉及质子偶联的多步四电子转移过程. 钒酸铋(BiVO₄)是应用于PEC水分解的典型且具有实际应用前景的光阳极材料之一. 然而, 由于不良的表面电荷转移、电荷在光阳极/电解质结面处的表面复合以及缓慢的OER动力学等因素, 导致BiVO₄的PEC性能受到严重限制.
本文开发了一种新颖有效的解决方案, 以低成本、高电导率和具有快速电荷转移能力的硫化钴装饰来提升BiVO₄光阳极的PEC活性, X射线多晶衍射(XRD)、X射线光电子能谱(XPS)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)等表征, 研究结果表明CoS成功装饰于BiVO₄表面. 采用紫外-可见吸收光谱(UV-Vis DRS)研究了BiVO₄和复合光阳极CoS/BiVO₄的光学性质, 结果表明, 与纯的BiVO₄相比, CoS/BiVO₄光阳极在可见光范围内光吸收能力有所增强.
将制备的BiVO₄和CoS/BiVO₄光阳极应用于PEC分解水实验中, 结果表明, 相对于1.23 V可逆氢电极, 在光照下, CoS/BiVO₄光阳极的光电流密度显著提升, 可高达3.2 mA cm ^-2, 是纯BiVO₄的2.5倍以上. 与纯BiVO₄相比, CoS/BiVO₄光阳极的起始氧化电位显示出负向偏移0.2 V, 表明析氧过电势得到有效减小. 入射光子转换效率(IPCE)测试结果表明, CoS/BiVO₄光阳极的入射光子转换效率在500 nm之前的可见光范围内得到明显提升, 其中, CoS/BiVO₄的IPCE值在380 nm处达到最大. 此外, 由于CoS的装饰作用, CoS/BiVO₄光阳极的电荷注入效率和电荷分离效率均得到较大的提升, 分别达到75.8% (相较于纯BiVO₄光阳极的36.7%)和79.8%(相较于纯BiVO₄光阳极的66.8%). 电化学阻抗谱(EIS)测试结果表明, 通过CoS的装饰, CoS/BiVO₄光阳极的界面电荷转移电阻得到有效降低, 证明其界面电荷转移动力学得到有效提升. 光致发光光谱测试结果表明, CoS的装饰显著提高了BiVO₄的光生电子-空穴对的分离效率, 进一步证明BiVO₄表面的CoS装饰在其PEC分解水中起着非常积极的作用. 本文为通过表面修饰设计应用于PEC水分解的有效的光阳极提供了新思路.

关键词: 光电化学水分解, 钒酸铋, 硫化钴, 电荷分离和传输, 光阳极

Abstract:

Solar-driven water splitting is considered as a promising method to mitigate the energy crisis and various environmental issues. Bismuth vanadate (BiVO₄) is photoanode material with tremendous potential for photoelectrochemical (PEC) water splitting. However, its PEC performance is severely hindered owing to poor surface charge transfer, surface recombination at the photoanode/electrolyte junction, and sluggish oxygen evolution reaction (OER) kinetics. In this regard, a novel solution was developed in this study to address these issues by decorating the surface of BiVO₄ with cobalt sulfide, whose attractive features such as low cost, high conductivity, and rapid charge-transfer ability assisted in improving the PEC activity of the BiVO₄ photoanode. The fabricated photoanode exhibited a significantly enhanced photocurrent density of 3.2 mA cm ^-2 under illumination at 1.23 V vs. a reversible hydrogen electrode, which is more than 2.5 times greater than that of pristine BiVO₄. Moreover, the CoS/BiVO₄photoanode also exhibited considerable improvements in the charge injection yield (75.8% vs. 36.7% for the bare BiVO₄ film) and charge separation efficiency (79.8% vs. 66.8% for the pristine BiVO₄ film). These dramatic enhancements were primarily ascribed to rapid charge-transport kinetics and efficient reduction of the anodic overpotential for oxygen evolution enabled by the surface modification of BiVO₄ by CoS. This study provides valuable suggestions for designing efficient photocatalysts via surface modification to improve the PEC performance.

Key words: Photoelectrochemical water splitting, Bismuth vanadate, Cobalt sulfide, Charge separation and transfer, Photoanode

周志明, 陈金金, 王擎龙, 蒋兴星, 申燕. 硫化钴装饰BiVO₄光阳极提升其光电化学水分解性能[J]. 催化学报, 2022, 43(2): 433-441.

Zhiming Zhou, Jinjin Chen, Qinlong Wang, Xingxing Jiang, Yan Shen. Enhanced photoelectrochemical water splitting using a cobalt-sulfide-decorated BiVO₄ photoanode[J]. Chinese Journal of Catalysis, 2022, 43(2): 433-441.

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图/表 7

Fig. 1. SEM images of BiOI (a), BiVO4 (b), and CoS/BiVO4 (c); (d) TEM image of the CoS/BiVO4 photoanode.

Scheme 1. Schematic of the preparation of the CoS/BiVO4 photoanode.

Fig. 2. High-resolution XPS profiles featuring the O 1s of pure BiVO4 (a), V 2p (b) and Bi 4f (c) of BiVO4 and CoS/BiVO4, and Co 2p of CoS/BiVO4 (d).

Fig. 3. (a) UV-vis diffuse reflectance spectra of the BiVO4 and CoS/BiVO4 photoanodes; (b) Photocurrent-potential curves of the BiVO4 and CoS/BiVO4 photoanodes under AM 1.5 G and chopped illumination; (c) Comparison of the PEC performance of the CoS/BiVO4 photoanode and that of other representative BiVO4-based photocatalysts at 1.23 V vs. RHE; (d) IPCE profiles of the BiVO4 and CoS/BiVO4 photoanodes measured at an applied voltage of 1.23 V vs. RHE.

Fig. 4. Light harvesting efficiency (a), electron flux at AM 1.5G (b), charge separation efficiency (c), and charge injection efficiency (d) of the BiVO4 and CoS/BiVO4 photoanodes.

Fig. 5. Electrochemical impedance spectra of BiVO4 and CoS/BiVO4 photoanodes obtained at 1.23 V vs. RHE under illumination.

Fig. 6. Proposed mechanism of the enhancement in PEC activity of the BiVO4 photoanode via decoration of CoS.

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硫化钴装饰BiVO₄光阳极提升其光电化学水分解性能

Enhanced photoelectrochemical water splitting using a cobalt-sulfide-decorated BiVO₄ photoanode

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