RhO2修饰BiVO4薄膜光阳极的制备及其光电催化分解水性能

doi:10.15541/jim20210798

无机材料学报 ›› 2022, Vol. 37 ›› Issue (8): 873-882.DOI: 10.15541/jim20210798

RhO₂修饰BiVO₄薄膜光阳极的制备及其光电催化分解水性能

胡越¹(), 安琳¹, 韩鑫²(), 侯成义¹, 王宏志¹, 李耀刚³, 张青红³()

1.东华大学材料科学与工程学院, 纤维材料改性国家重点实验室, 上海 201620
2.华东理工大学化工学院, 化学工程国家重点实验室, 上海 200237
3.东华大学材料科学与工程学院, 教育部先进玻璃制造技术工程中心, 上海 201620

收稿日期:2022-12-29 修回日期:2022-03-09 出版日期:2022-08-20 网络出版日期:2022-03-10
通讯作者: 张青红, 教授. E-mail: zhangqh@dhu.edu.cn;
韩鑫, 博士. E-mail: hanx.1026@gmail.com
作者简介:胡越(1998-), 女, 硕士研究生. E-mail: yue_hamish@163.com
基金资助:
国家自然科学基金(51572046)

RhO₂ Modified BiVO₄ Thin Film Photoanodes: Preparation and Photoelectrocatalytic Water Splitting Performance

HU Yue¹(), AN Lin¹, HAN Xin²(), HOU Chengyi¹, WANG Hongzhi¹, LI Yaogang³, ZHANG Qinghong³()

1. State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University, Shanghai 201620, China
2. State Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China
3. Engineering Research Center of Advanced Glasses Manufacturing Technology, Ministry of Education, College of Materials Science and Engineering, Donghua University, Shanghai 201620, China

Received:2022-12-29 Revised:2022-03-09 Published:2022-08-20 Online:2022-03-10
Contact: ZHANG Qinghong, professor. E-mail: zhangqh@dhu.edu.cn;
HAN Xin, PhD. E-mail: hanx.1026@gmail.com
About author:HU Yue (1998-), female, Master candidate. E-mail: yue_hamish@163.com
Supported by:
National Natural Science Foundation of China(51572046)

摘要/Abstract

摘要：

钒酸铋是最具有光电催化应用潜力的水分解光电阳极之一, 但由于表面缓慢的动力学反应速率, 其光电催化效率仍不理想。本研究通过浸渍法在BiVO₄薄膜光阳极上负载纳米RhO₂助催化剂, 研究RhO₂负载量对BiVO₄光阳极光电催化性能的影响规律及其机理。晶粒尺寸10~25 nm的RhO₂均匀负载在颗粒尺寸100~250 nm、厚度约为400 nm的BiVO₄光阳极薄膜表面。考虑到贵金属铑的昂贵成本, RhO₂的最佳负载量为质量分数1.65%, 在偏压1.23 V (vs. RHE)、1.0 mol/L Na₂SO₃溶液中(pH8.5)AM 1.5模拟可见光照射下, 光电流密度达3.81 mA·cm^-2, 相较纯BiVO₄提升了10.58倍。在没有有机牺牲剂的条件下, 光阳极同时析出了氢气和氧气, 两者比例接近2 : 1, 产氧速率为8.22 μmol/(h·cm²)。负载RhO₂有效改善了光阳极的表面水氧化动力学, 使光生空穴更快与电解质溶液进行水氧化反应, 抑制光生载流子复合, 从而显著提升光电催化性能。另外, 负载RhO₂后, 空穴更容易从光阳极表面被有效提取到电解质溶液中, 减少其在光阳极表面积累, 从而使BiVO₄/RhO₂(1.65%)光阳极可持续稳定工作10 h以上。

关键词: 钒酸铋, 氧化铑, 助催化剂, 光电催化, 分解水

Abstract:

Bismuth vanadate is one of the most promising photoanodes for photoelectrocatalytic water splitting, however, its photoelectrocatalytic efficiency is still not ideal due to its sluggish kinetic reaction rate. The RhO₂ cocatalyst was loaded on the BiVO₄ thin film photoanode by impregnation method, and the photoelectrochenucal performance of the BiVO₄ photoanode with different RhO₂loadings was studied. RhO₂ with grain size of 10-25 nm was uniformly loaded on the BiVO₄ film with grain size of 100-250 nm and thickness of 400 nm. The BiVO₄photoanode with 1.65% RhO₂ (mass percent) showed the best comprehensive performance, of which the visible-light photocurrent density reached 3.81 mA·cm^-2 under 1.23 V (vs. RHE) in 1.0 mol/L Na₂SO₃ (pH8.5) electrolyte, which was 10.58 times higher than that of bare BiVO₄. In the absence of any sacrificial agent, the photoanodes produced hydrogen and oxygen at the same time at the ratio of close to 2 : 1, and the oxygen production rate was 8.22 µmol/(h·cm²). RhO₂ loading effectively improved the surface water oxidation kinetics, so that photogenerated holes could undergo water oxidation reaction more quickly. Meanwhile, the photogenerated carrier recombination was inhibited, significantly improving the photoelectrocatalytic performance. In addition, since holes were more easily extracted from the surface of photoanode into electrolyte solution in the presence of RhO₂ cocatalyst, reducing accumulation on the surface of the photoanode, the BiVO₄/RhO₂ (1.65%) photoanode achieved excellent stability for more than 10 h.

Key words: BiVO₄, RhO₂, cocatalyst, photoelectrocatalysis, water splitting

中图分类号:

TQ174

胡越, 安琳, 韩鑫, 侯成义, 王宏志, 李耀刚, 张青红. RhO₂修饰BiVO₄薄膜光阳极的制备及其光电催化分解水性能[J]. 无机材料学报, 2022, 37(8): 873-882.

HU Yue, AN Lin, HAN Xin, HOU Chengyi, WANG Hongzhi, LI Yaogang, ZHANG Qinghong. RhO₂ Modified BiVO₄ Thin Film Photoanodes: Preparation and Photoelectrocatalytic Water Splitting Performance[J]. Journal of Inorganic Materials, 2022, 37(8): 873-882.

图/表 10

图1 不同负载量RhO2修饰的BiVO4光阳极的(a)XRD图谱, 以及(b)Bi4f, (c)V2p 和(d)Rh3d的高分辨率XPS图谱

Fig. 1 (a) XRD patterns and XPS spectra of (b) Bi4f, (c) V2p, (d) Rh3d of all BiVO4/RhO2 photoanodes

图2 纯BiVO4和BiVO4/0.1-RhO2的(a, b)低倍和(c, d)高倍场发射扫描电镜照片, (e) BiVO4/0.1-RhO2高倍场发射扫描电镜照片及其Bi、V、Rh的元素分布图

Fig. 2 (a, b) Low-magnification and (c, d) high-magnification FESEM images of bare BiVO4 surface and BiVO4/0.1-RhO2 photoanodes, and (e) high-magnification SEM image with elemental mappings of the BiVO4/0.1-RhO2 photoanode

图3 (a, b)纯BiVO4和(c, d) BiVO4/0.1-RhO2的(a, c) TEM和(b, d) HRTEM照片

Fig. 3 (a, c) TEM and (b, d) HRTEM images of (a, b) bare BiVO4 and (c, d) BiVO4/0.1-RhO2 photoanodes The inset in (d) is the SAED patterns of the selected area

图4 不同负载量RhO2修饰的BiVO4光阳极的(a) UV-Vis DRS光谱和(b) (αhν) 2 vs hν的tauc图

Fig. 4 (a) UV-Vis DRS spectra and (b) (αhν) 2 vs hν tauc plots of BiVO4/RhO2 photoanodes

图5 不同负载量RhO2修饰的BiVO4光阳极的(a)线性扫描伏安(LSV)曲线和(b)光电流响应曲线, 测试电解液为1.0 mol/L Na2SO3 (pH8.5)

Fig. 5 (a) Liner sweep voltammetry curves and (b) photocurrent response plots of BiVO4/RhO2 photoanodes in 1.0 mol/L Na2SO3 (pH8.5) electrolyte

图6 不同负载量RhO2修饰的BiVO4光阳极的(a)线性扫描伏安(LSV)曲线和(b)光电流响应曲线, 测试电解液为0.5 mol/L Na2SO4 (pH6.8)

Fig. 6 (a) Liner sweep voltammetry curves and (b) photocurrent response plots of all BiVO4/RhO2 photoanodes in 0.5 mol/L Na2SO4 (pH6.8) electrolyte

图7 不同负载量RhO2修饰的BiVO4光阳极的Nyquist图

Fig. 7 Nyquist plots of the BiVO4/RhO2 photoanodes The inset showing the equivalent circuit

图8 可见光照射、外加偏压为1.23 V (vs. RHE)、电解液为1.0 mol/L Na2SO3 (pH8.5)条件下BiVO4/0.1-RhO2光阳极的(a)光电流稳定性和(b)催化前后的XRD图谱

Fig. 8 (a) Photocurrent stability of the BiVO4/0.1-RhO2 photoanode in 1.0 mol/L Na2SO3 (pH8.5) under visible-light illumination, and (b) XRD patterns of the BiVO4/0.1-RhO2 photoanodes before and after illumination, respectively

图9 在可见光激发、外加偏压为1.23 V (vs. RE)、电解液为1.0 mol/L Na2SO3 (pH8.5)条件下BiVO4/0.1-RhO2光阳极的(a)产氢速率曲线和(b)产氧速率曲线

Fig. 9 (a) Hydrogen and (b) oxygen evolution vs. reaction time per illuminated area for bare BiVO4 and BiVO4/RhO2 photoanodes under visible-light irradiation with the electrolyte of 1.0 mol/L Na2SO3 (pH8.5) as hole scavenger

图10 RhO2修饰的BiVO4光阳极在可见光照射下进行光电催化分解水的机理示意图

Fig. 10 Schematic diagram depicting PEC water splitting of the RhO2-modified BiVO4 photoanode under visible light irradiation

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RhO₂修饰BiVO₄薄膜光阳极的制备及其光电催化分解水性能

RhO₂ Modified BiVO₄ Thin Film Photoanodes: Preparation and Photoelectrocatalytic Water Splitting Performance

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