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Defect-Mediated Electron–Hole Separation in One-Unit-Cell ZnIn2S4 Layers for Boosted Solar-Driven CO2 Reduction
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 ZnIn 2 S 4 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 ZnIn 2 S 4 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 ZnIn 2 S 4 layers with rich zinc vacancies exhibit a carbon monoxide formation rate of 33.2 μmol g –1 h –1, roughly 3.6 times higher than that of the one-unit-cell ZnIn 2 S 4 layers with poor zinc vacancies, while the former’s photocatalytic activity shows negligible loss after 24 h photocatalysis. This present work uncovers the role of defects in affecting electron–hole separation at atomic level, opening new opportunities for achieving highly efficient solar CO 2 reduction performances.
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Metadata
- Authors
- Jiao, X., Chen, Z., Li, X., Sun, Y., Gao, S., Yan, W., Wang, C., Zhang, Q., Lin, Y., Luo, Y., & Xie, Y.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2017-05-23
- Volume
- 139
- Issue
- 22
- Pages
- 7586-7594
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2614741941
- Cited by
- 1,049
- References
- 38
- FWCI
- 22.56
- Type
- journal article
- Language
- en
- Open access
- closed
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