Composition-Engineered Heavy-Metal-Free Cu–Ga–Zn–S Nanorods for Efficient Photocatalytic Water Splitting
Composition-Engineered Heavy-Metal-Free Cu–Ga–Zn–S Nanorods for Efficient Photocatalytic Water Splitting
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DOI：
10.1021/acsanm.3c02430
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发表时间：
2023-08
影响因子：
5.9
通讯作者：
Zheming Liu;Hao Fu;Yu Li;Jun Liu;Yanbin Huang;Dongxu Zhu;H. Ye;Chunhe Yang;Zhijie Wang;A. Tang
中科院分区：
文献类型：
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作者：
Zheming Liu;Hao Fu;Yu Li;Jun Liu;Yanbin Huang;Dongxu Zhu;H. Ye;Chunhe Yang;Zhijie Wang;A. Tang
由铜基硫化物组成的半导体光催化剂是一种很有前途的光催化分解水的候选材料，能够产生氢气和氧气。在铜硫化物中掺入额外的锌离子可以显著改变其光学和电学性质，如带隙、载流子转移以及光生电子和空穴对的分离。在这项工作中，我们发展了一种胶体方法来合成具有增强光催化析氢性能的一维(1D)四元系铜镓锌S纳米棒(NRS)。铜-镓-锌-S近红外光谱显示出依赖锌的生长机制，其中锌离子促进了沿[0001]方向的形态伸长。通过控制Ga/Zn投料摩尔比，获得了2101mol.g-1·h-1的最大光催化产氢速率，超过了无锌和富锌的μ。这种改善可以归因于光生载流子的定制寿命、电荷转移电阻以及光生电子和空穴的分离效率，而不是略微改变带隙。值得注意的是，优化的铜-镓-锌-S纳米氧化物在太阳光照射下也表现出阳极光电流和光催化产氧活性。我们的研究提供了一种简便的合成一维Cu-Ga-Zn-S NRS的方法，为开发高效分解水的多功能光催化剂提供了有价值的启示。
Semiconductor photocatalysts composed of copper-based chalcogenides have emerged as promising candidates for photocatalytic water splitting, enabling the production of hydrogen and oxygen. The incorporation of extra Zn cations into copper chalcogenides is found to significantly alter their optical and electronic properties, such as band gap, charge carrier transfer, and the separation of photo-generated electron and hole couples. In this work, we developed a colloidal approach to synthesizing one-dimensional (1D) quaternary Cu–Ga–Zn–S nanorods (NRs) with enhanced photocatalytic hydrogen evolution performance. The Cu–Ga–Zn–S NRs demonstrate a Zn-dependent growth mechanism, where Zn cations promote the morphological elongation along the [0001] direction. Through the control of the Ga/Zn feeding molar ratios in Cu–Ga–Zn–S NRs, we achieved the maximum photocatalytic hydrogen production rate of 2101 μmol·g–1·h–1, surpassing both of the Zn-free and Zn-rich counterparts. Such improvement can be attributed to the tailored lifetime of photo-generated charge carriers, charge transfer resistance, and separation efficiency of photo-generated electrons and holes, instead of a slight alteration of band gap. Notably, the optimal Cu–Ga–Zn–S NRs also show an anodic photocurrent and photocatalytic oxygen production activity under solar irradiation. Our study presents a facile method for preparing 1D Cu–Ga–Zn–S NRs via composition engineering and offers valuable insights to develop multifunctional photocatalysts for efficient water splitting.