非晶TiO2修饰CuBi2O4光阴极增强其光电化学产氢活性

doi:10.1016/S1872-2067(18)63127-4

催化学报 ›› 2018, Vol. 39 ›› Issue (10): 1704-1710.DOI: 10.1016/S1872-2067(18)63127-4

非晶TiO₂修饰CuBi₂O₄光阴极增强其光电化学产氢活性

朱相林^a, 管子涵^a, 王朋^a, 张倩倩^a, 戴瑛^b, 黄柏标^a

a 山东大学晶体材料国家重点实验室, 山东济南 250100;
b 山东大学物理学院, 山东济南 250100

收稿日期:2018-04-28 修回日期:2018-05-30 出版日期:2018-10-18 发布日期:2018-08-03
通讯作者: 王朋, 黄柏标
基金资助:
国家自然科学基金（51602179，21333006，21573135，11374190）；国家基础研究计划（973计划，2013CB632401）.

Amorphous TiO₂-modified CuBi₂O₄ Photocathode with enhanced photoelectrochemical hydrogen production activity

Xianglin Zhu^a, Zihan Guan^a, Peng Wang^a, Qianqian Zhang^a, Ying Dai^b, Baibiao Huang^a

a State Key Laboratory of Crystal Materials, Shandong University, Jinan 250100, Shandong, China;
b School of Physics, Shandong University, Jinan 250100, Shandong, China

Received:2018-04-28 Revised:2018-05-30 Online:2018-10-18 Published:2018-08-03
Contact: 10.1016/S1872-2067(18)63127-4
Supported by:
This work was supported by the National Natural Science Foundation of China (51602179, 21333006, 21573135, 11374190) and the National Basic Research Program of China (973 Program, 2013CB632401).

摘要/Abstract

摘要：

光催化作为太阳能利用领域的研究热点引起了广泛的关注.其中，光电化学技术能够通过分解水提供清洁的氢能源，因此被认为是一种潜在的新能源制造方式.在光电化学分解水产氢的过程中，最重要的是高效光电极的制备.一系列n型半导体材料已被广泛地报道并用作光阳极，如BiVO₄，ZnO，Fe₂O₃等.然而对于光阴极材料，其可选择性则较少.CuBi₂O₄是一种天然矿物，具有廉价易得以及化学性质稳定的特性，而且是一种p型半导体材料，因此能够用于制备光阴极；另外因为其强的可见光响应（1.70eV），所以具有广泛的应用前景.目前对于CuBi₂O₄光阴极研究主要集中在合成和理论计算方面，而对于如何促进界面处的载流子分离研究较少.
本文通过一种简单的电沉积方法成功制备出CuBi₂O₄光阴极，然后利用非晶TiO₂和助催化剂Pt进行修饰后将其用于光电化学产氢.由于形成了CuBi₂O₄/TiO₂ p-n结，因此其光阴极活性得到增强.新的Pt/TiO₂/CuBi₂O₄光阴极在0.60V偏压处的光电流为0.35mA/cm²，其数值约为Pt/CuBi₂O₄光阴极的两倍.XRD结果表明，我们制备的CuBi₂O₄为纯相且结晶性较好，其表面修饰的TiO₂为非晶相的.SEM结果表明，CuBi₂O₄电极层由100-150nm的颗粒构成.紫外-可见吸收光谱表明，制备的CuBi₂O₄光电极拥有良好的可见光吸收性质，而且TiO₂修饰未对CuBi₂O₄的光吸收产生明显的影响.XPS结果表明，修饰TiO₂并未对CuBi₂O₄电极造成成分上的破坏.光电化学测试表明，修饰TiO₂层厚度和结晶性会影响光电极的最终活性.修饰四层TiO₂和退火200℃的样品具有最好的活性.
另外稳定性测试也表明，修饰非晶TiO₂的CuBi₂O₄光阴极具有良好的稳定性.在IPCE测试中，Pt/TiO₂/CuBi₂O₄光阴极在其光响应范围内均比Pt/CuBi₂O₄光阴极表现出更高的效率.阻抗结果测试中Pt/TiO₂/CuBi₂O₄光阴极具有更小的阻抗，这表明其载流子传输更加高效.在Mott-Shetty测试中，Pt/TiO₂/CuBi₂O₄和Pt/CuBi₂O₄光阴极都表现出p型半导体性质，但是Pt/TiO₂/CuBi₂O₄具有更负的平带电位，这表明修饰的TiO₂仍具有n型半导体材料的特性，并与p型的CuBi₂O₄形成p-n结，从而促进了载流子分离效率.

关键词: 光电化学产氢, CuBi₂O₄, 非晶TiO₂, p-n结, 载流子分离

Abstract:

In this study, CuBi₂O₄ photocathodes were prepared using a simple electrodeposition method for photoelectrochemical (PEC) hydrogen production. The prepared photocathodes were modified with amorphous TiO₂ and a Pt co-catalyst, which resulted in the formation of CuBi₂O₄/TiO₂ p-n heterojunctions, and enhanced the activities of the as-prepared photocathodes. The novel Pt/TiO₂/CuBi₂O₄ photocathode exhibited a photocurrent of 0.35 mA/cm² at 0.60 V vs. Reversible Hydrogen Electrode (RHE), which was nearly twice that of the Pt/CuBi₂O₄ photocathode. The present study provides a facile method for increasing the efficiency of photocathodes and provides meaningful guidance for the preparation of high-performance CuBi₂O₄ photocathodes.

Key words: Photoelectrochemical hydrogen production, CuBi₂O₄, Amorphous TiO₂, p-n heterojunction, Carriers' separation

朱相林, 管子涵, 王朋, 张倩倩, 戴瑛, 黄柏标. 非晶TiO₂修饰CuBi₂O₄光阴极增强其光电化学产氢活性[J]. 催化学报, 2018, 39(10): 1704-1710.

Xianglin Zhu, Zihan Guan, Peng Wang, Qianqian Zhang, Ying Dai, Baibiao Huang. Amorphous TiO₂-modified CuBi₂O₄ Photocathode with enhanced photoelectrochemical hydrogen production activity[J]. Chinese Journal of Catalysis, 2018, 39(10): 1704-1710.

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非晶TiO₂修饰CuBi₂O₄光阴极增强其光电化学产氢活性

Amorphous TiO₂-modified CuBi₂O₄ Photocathode with enhanced photoelectrochemical hydrogen production activity

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