Defect-Mediated Electron-Hole Separation in One-Unit-Cell ZnIn2 S4 Layers for Boosted Solar-Driven CO2 Reduction

Journal of the American Chemical Society
Xingchen JiaoYi Xie

Abstract

The effect of defects on electron-hole separation is not always clear and is sometimes contradictory. Herein, we initially built clear models of two-dimensional atomic layers with tunable defect concentrations, and hence directly disclose the defect type and distribution at atomic level. As a prototype, defective one-unit-cell ZnIn2S4 atomic layers are successfully synthesized for the first time. Aberration-corrected scanning transmission electron microscopy directly manifests their distinct zinc vacancy concentrations, confirmed by positron annihilation spectrometry and electron spin resonance analysis. Density-functional calculations reveal that the presence of zinc vacancies ensures higher charge density and efficient carrier transport, verified by ultrafast photogenerated electron transfer time of ∼15 ps from the conduction band of ZnIn2S4 to the trap states. Ultrafast transient absorption spectroscopy manifests the higher zinc vacancy concentration that allows for ∼1.7-fold increase in average recovery lifetime, confirmed by surface photovoltage spectroscopy and PL spectroscopy analysis, which ensures promoted carrier separation rates. As a result, the one-unit-cell ZnIn2S4 layers with rich zinc vacancies exhibit a carbon ...Continue Reading

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Citations

Jul 19, 2018·Dalton Transactions : an International Journal of Inorganic Chemistry·Jing HuangHaining Tian
Aug 18, 2018·Dalton Transactions : an International Journal of Inorganic Chemistry·Wei ShaoXiaodong Zhang
Nov 23, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Jian-Peng DongLi-Ya Wang
Nov 21, 2019·Angewandte Chemie·Hao ZhangRuqiang Zou
Jun 6, 2019·Beilstein Journal of Nanotechnology·Jingshuai ChenJi-Ming Song
Sep 15, 2020·Dalton Transactions : an International Journal of Inorganic Chemistry·Wenhao XingJiyong Yao
Aug 14, 2019·Advanced Science·Zaiyong JiangGeoffrey A Ozin
Sep 30, 2020·Dalton Transactions : an International Journal of Inorganic Chemistry·Wen-Jin YinLi-Min Liu
May 26, 2018·Chemical Society Reviews·Oleksandr StroyukNikolai Gaponik
May 23, 2020·Advanced Science·Jie YinChun-Hua Yan

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