Semimetal 1H-SnS2 Enables High-Efficiency Electroreduction of CO2 to CO

Jie Xu; Shuhua Lai; Min Hu; Shangmeng Ge; Ruicong Xie; Fan Li; Dandan Hua; Heng Xu; Huang Zhou; Rui Wu; Jiantao Fu; Yuan Qiu; Jia He; Chao Li; Haoxuan Liu; Yifan Liu; Jiaqiang Sun; Xijun Liu; Jun Luo

doi:10.1002/smtd.202000567

Semimetal 1H-SnS₂ Enables High-Efficiency Electroreduction of CO₂ to CO

Jie Xu, Shuhua Lai, Min Hu, Shangmeng Ge, Ruicong Xie, Fan Li, Dandan Hua, Heng Xu, Huang Zhou, Rui Wu, Jiantao Fu, Yuan Qiu, Jia He, Chao Li, Haoxuan Liu, Yifan Liu, Jiaqiang Sun, Xijun Liu, Jun Luo

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

56 Scopus citations

Abstract

Controlling the selectivity of products in CO₂ fixation is essential to obtain desired products using phase engineering. In this study, stable semimetal 1H-SnS₂ nanosheets are successfully synthesized by hydrogen-assisted low-temperature calcination for the first time. Compared with semiconductor 1T-SnS₂, the 1H-SnS₂ exhibits ultrahigh CO selectivity with a Faradaic efficiency of 98.2% at −0.8 V (vs reversible hydrogen electrode) and a partial current density of 10.9 mA cm⁻² in the electrocatalytic CO₂ reduction reaction. Theoretical calculations indicate that the *COOH intermediate is more stable on 1H-SnS₂ surface than 1T-SnS₂ surface and thus promotes the CO production. This work shows that phase engineering control can be an effective approach to regulate the selectivity of products in CO₂RR of transition metal dichalcogenides.

Original language	English
Article number	2000567
Journal	Small Methods
Volume	4
Issue number	10
DOIs	https://doi.org/10.1002/smtd.202000567
State	Published - Oct 1 2020
Externally published	Yes

Funding

This work was financially supported by National Key R&D Program of China (2017YFA0700104), National Natural Science Foundation of China (Grant Nos. 21601136, 11604241, 21603162, 51971157, and 51761165012), Tianjin Science Fund for Distinguished Young Scholars (19JCJQJC61800), the Yong Elite Scientists Sponsorship Program by Tianjin, and Science & Technology Development Fund of Tianjin Education Commission for Higher Education (2018KJ126). The authors would like to thank Yonghong Tang from Shiyanjia Lab (www.shiyanjia.com) for the UPS test and also acknowledge the National Supercomputing Center in Shenzhen for providing the computational resources and materials studio (DMol3). This work was financially supported by National Key R&D Program of China (2017YFA0700104), National Natural Science Foundation of China (Grant Nos. 21601136, 11604241, 21603162, 51971157, and 51761165012), Tianjin Science Fund for Distinguished Young Scholars (19JCJQJC61800), the Yong Elite Scientists Sponsorship Program by Tianjin, and Science & Technology Development Fund of Tianjin Education Commission for Higher Education (2018KJ126). The authors would like to thank Yonghong Tang from Shiyanjia Lab ( www.shiyanjia.com ) for the UPS test and also acknowledge the National Supercomputing Center in Shenzhen for providing the computational resources and materials studio (DMol). 3

Keywords

CO fixation
electrocatalysis
hydrogen-assisted
metastable 1H-SnS
phase transition engineering

Access to Document

10.1002/smtd.202000567

Cite this

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title = "Semimetal 1H-SnS2 Enables High-Efficiency Electroreduction of CO2 to CO",

abstract = "Controlling the selectivity of products in CO2 fixation is essential to obtain desired products using phase engineering. In this study, stable semimetal 1H-SnS2 nanosheets are successfully synthesized by hydrogen-assisted low-temperature calcination for the first time. Compared with semiconductor 1T-SnS2, the 1H-SnS2 exhibits ultrahigh CO selectivity with a Faradaic efficiency of 98.2% at −0.8 V (vs reversible hydrogen electrode) and a partial current density of 10.9 mA cm−2 in the electrocatalytic CO2 reduction reaction. Theoretical calculations indicate that the *COOH intermediate is more stable on 1H-SnS2 surface than 1T-SnS2 surface and thus promotes the CO production. This work shows that phase engineering control can be an effective approach to regulate the selectivity of products in CO2RR of transition metal dichalcogenides.",

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author = "Jie Xu and Shuhua Lai and Min Hu and Shangmeng Ge and Ruicong Xie and Fan Li and Dandan Hua and Heng Xu and Huang Zhou and Rui Wu and Jiantao Fu and Yuan Qiu and Jia He and Chao Li and Haoxuan Liu and Yifan Liu and Jiaqiang Sun and Xijun Liu and Jun Luo",

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doi = "10.1002/smtd.202000567",

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AU - Xu, Jie

AU - Lai, Shuhua

AU - Hu, Min

AU - Ge, Shangmeng

AU - Xie, Ruicong

AU - Li, Fan

AU - Hua, Dandan

AU - Xu, Heng

AU - Zhou, Huang

AU - Wu, Rui

AU - Fu, Jiantao

AU - Qiu, Yuan

AU - He, Jia

AU - Li, Chao

AU - Liu, Haoxuan

AU - Liu, Yifan

AU - Sun, Jiaqiang

AU - Liu, Xijun

AU - Luo, Jun

PY - 2020/10/1

Y1 - 2020/10/1

N2 - Controlling the selectivity of products in CO2 fixation is essential to obtain desired products using phase engineering. In this study, stable semimetal 1H-SnS2 nanosheets are successfully synthesized by hydrogen-assisted low-temperature calcination for the first time. Compared with semiconductor 1T-SnS2, the 1H-SnS2 exhibits ultrahigh CO selectivity with a Faradaic efficiency of 98.2% at −0.8 V (vs reversible hydrogen electrode) and a partial current density of 10.9 mA cm−2 in the electrocatalytic CO2 reduction reaction. Theoretical calculations indicate that the *COOH intermediate is more stable on 1H-SnS2 surface than 1T-SnS2 surface and thus promotes the CO production. This work shows that phase engineering control can be an effective approach to regulate the selectivity of products in CO2RR of transition metal dichalcogenides.

AB - Controlling the selectivity of products in CO2 fixation is essential to obtain desired products using phase engineering. In this study, stable semimetal 1H-SnS2 nanosheets are successfully synthesized by hydrogen-assisted low-temperature calcination for the first time. Compared with semiconductor 1T-SnS2, the 1H-SnS2 exhibits ultrahigh CO selectivity with a Faradaic efficiency of 98.2% at −0.8 V (vs reversible hydrogen electrode) and a partial current density of 10.9 mA cm−2 in the electrocatalytic CO2 reduction reaction. Theoretical calculations indicate that the *COOH intermediate is more stable on 1H-SnS2 surface than 1T-SnS2 surface and thus promotes the CO production. This work shows that phase engineering control can be an effective approach to regulate the selectivity of products in CO2RR of transition metal dichalcogenides.

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KW - metastable 1H-SnS

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