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用于促进光催化CO还原的具有铟空位的全光谱响应金属ZnInS中载流子动力学的定量评估

Quantitative Evaluation of Carrier Dynamics in Full-Spectrum Responsive Metallic ZnInS with Indium Vacancies for Boosting Photocatalytic CO Reduction.

作者信息

He Yiqiang, Chen Cailing, Liu Yuxin, Yang Yilin, Li Chunguang, Shi Zhan, Han Yu, Feng Shouhua

机构信息

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, People's Republic of China.

Advanced Membranes and Porous Materials Center, Physical Sciences and Engineering Division, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Saudi Arabia.

出版信息

Nano Lett. 2022 Jun 22;22(12):4970-4978. doi: 10.1021/acs.nanolett.2c01666. Epub 2022 Jun 9.

Abstract

The influence of defects on quantitative carrier dynamics is still unclear. Therefore, full-spectrum responsive metallic ZnInS (V-rich-ZIS) rich in indium vacancies and exhibiting high CO photoreduction efficiency was synthesized for the first time. The influence of the defects on the carrier dynamic parameters was studied quantitatively; the results showed that the minority carrier diffusion length () is closely related to the catalytic performance. In situ infrared spectroscopy and theoretical calculations revealed that the presence of indium vacancies lowers the energy barrier for CO to CO conversion via the COOH* intermediate. Hence, the high rate of CO evolution reaches 298.0 μmol g h, a nearly 28-fold enhancement over that with ZnInS (V-poor-ZIS), which is not rich in indium vacancies. This work fills the gaps between the catalytic performance of defective photocatalysts and their carrier dynamics and may offer valuable insight for understanding the mechanism of photocatalysis and designing more efficient defective photocatalysts.

摘要

缺陷对载流子动力学定量的影响仍不清楚。因此,首次合成了富含铟空位且具有高CO光还原效率的全光谱响应金属ZnInS(富V-ZIS)。定量研究了缺陷对载流子动力学参数的影响;结果表明,少数载流子扩散长度()与催化性能密切相关。原位红外光谱和理论计算表明,铟空位的存在降低了通过COOH*中间体将CO转化为CO的能垒。因此,CO的高析出速率达到298.0 μmol g h,比不含铟空位的ZnInS(贫V-ZIS)提高了近28倍。这项工作填补了缺陷光催化剂的催化性能与其载流子动力学之间的空白,并可能为理解光催化机理和设计更高效的缺陷光催化剂提供有价值的见解。

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