Quantitative Evaluation of Carrier Dynamics in Full-Spectrum Responsive Metallic ZnIn2S4 with Indium Vacancies for Boosting Photocatalytic CO2 Reduction

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

doi:10.1021/acs.nanolett.2c01666

Quantitative Evaluation of Carrier Dynamics in Full-Spectrum Responsive Metallic ZnIn2S4 with Indium Vacancies for Boosting Photocatalytic CO2 Reduction

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

Research output: Contribution to journal › Article › peer-review

75 Scopus citations

Abstract

The influence of defects on quantitative carrier dynamics is still unclear. Therefore, full-spectrum responsive metallic ZnIn2S4 (VIn-rich-ZIS) rich in indium vacancies and exhibiting high CO2 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 (LD) 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 CO2 to CO conversion via the COOH* intermediate. Hence, the high rate of CO evolution reaches 298.0 μmol g–1 h–1, a nearly 28-fold enhancement over that with ZnIn2S4 (VIn-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.

Original language	English (US)
Journal	Nano letters
DOIs	https://doi.org/10.1021/acs.nanolett.2c01666
State	Published - Jun 9 2022

Bibliographical note

KAUST Repository Item: Exported on 2022-06-13
Acknowledgements: This work was financially supported by the National Natural Science Foundation of China (21621001), the Foundation of Science and Technology Development of Jilin Province, China (20200801004GH) and 111 Project (B17020).

ASJC Scopus subject areas

Bioengineering
General Materials Science
General Chemistry
Mechanical Engineering
Condensed Matter Physics

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10.1021/acs.nanolett.2c01666

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@article{baddb02357e04cd69a33bc6955b9f129,

title = "Quantitative Evaluation of Carrier Dynamics in Full-Spectrum Responsive Metallic ZnIn2S4 with Indium Vacancies for Boosting Photocatalytic CO2 Reduction",

abstract = "The influence of defects on quantitative carrier dynamics is still unclear. Therefore, full-spectrum responsive metallic ZnIn2S4 (VIn-rich-ZIS) rich in indium vacancies and exhibiting high CO2 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 (LD) 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 CO2 to CO conversion via the COOH* intermediate. Hence, the high rate of CO evolution reaches 298.0 μmol g–1 h–1, a nearly 28-fold enhancement over that with ZnIn2S4 (VIn-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.",

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

note = "KAUST Repository Item: Exported on 2022-06-13 Acknowledgements: This work was financially supported by the National Natural Science Foundation of China (21621001), the Foundation of Science and Technology Development of Jilin Province, China (20200801004GH) and 111 Project (B17020).",

year = "2022",

month = jun,

day = "9",

doi = "10.1021/acs.nanolett.2c01666",

language = "English (US)",

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T1 - Quantitative Evaluation of Carrier Dynamics in Full-Spectrum Responsive Metallic ZnIn2S4 with Indium Vacancies for Boosting Photocatalytic CO2 Reduction

AU - He, Yiqiang

AU - Chen, Cailing

AU - Liu, Yuxin

AU - Yang, Yilin

AU - Li, Chunguang

AU - Shi, Zhan

AU - Han, Yu

AU - Feng, Shouhua

N1 - KAUST Repository Item: Exported on 2022-06-13 Acknowledgements: This work was financially supported by the National Natural Science Foundation of China (21621001), the Foundation of Science and Technology Development of Jilin Province, China (20200801004GH) and 111 Project (B17020).

PY - 2022/6/9

Y1 - 2022/6/9

N2 - The influence of defects on quantitative carrier dynamics is still unclear. Therefore, full-spectrum responsive metallic ZnIn2S4 (VIn-rich-ZIS) rich in indium vacancies and exhibiting high CO2 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 (LD) 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 CO2 to CO conversion via the COOH* intermediate. Hence, the high rate of CO evolution reaches 298.0 μmol g–1 h–1, a nearly 28-fold enhancement over that with ZnIn2S4 (VIn-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.

AB - The influence of defects on quantitative carrier dynamics is still unclear. Therefore, full-spectrum responsive metallic ZnIn2S4 (VIn-rich-ZIS) rich in indium vacancies and exhibiting high CO2 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 (LD) 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 CO2 to CO conversion via the COOH* intermediate. Hence, the high rate of CO evolution reaches 298.0 μmol g–1 h–1, a nearly 28-fold enhancement over that with ZnIn2S4 (VIn-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.

UR - http://hdl.handle.net/10754/678903

UR - https://pubs.acs.org/doi/10.1021/acs.nanolett.2c01666

U2 - 10.1021/acs.nanolett.2c01666

DO - 10.1021/acs.nanolett.2c01666

M3 - Article

C2 - 35678583

SN - 1530-6984

JO - Nano letters

JF - Nano letters

ER -

Quantitative Evaluation of Carrier Dynamics in Full-Spectrum Responsive Metallic ZnIn2S4 with Indium Vacancies for Boosting Photocatalytic CO2 Reduction

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