Surface Oxygen Injection in Tin Disulfide Nanosheets for Efficient CO2 Electroreduction to Formate and Syngas

Tao Chen; Tong Liu; Tao Ding; Beibei Pang; Lan Wang; Xiaokang Liu; Xinyi Shen; Sicong Wang; Dan Wu; Dong Liu; Linlin Cao; Qiquan Luo; Wei Zhang; Wenkun Zhu; Tao Yao

doi:10.1007/s40820-021-00703-6

Surface Oxygen Injection in Tin Disulfide Nanosheets for Efficient CO₂ Electroreduction to Formate and Syngas

Nanomicro Lett. 2021 Sep 6;13(1):189. doi: 10.1007/s40820-021-00703-6.

Authors

Tao Chen^{1

2}, Tong Liu¹, Tao Ding¹, Beibei Pang¹, Lan Wang^{1

2}, Xiaokang Liu¹, Xinyi Shen¹, Sicong Wang¹, Dan Wu¹, Dong Liu¹, Linlin Cao¹, Qiquan Luo³, Wei Zhang^{4

5}, Wenkun Zhu⁶, Tao Yao⁷

Affiliations

¹ National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230029, People's Republic of China.
² State Key Laboratory of Environmentally Friendly Energy Materials, School of National Defense Science and Technology, Southwest University of Science and Technology, Mianyang, 621010, People's Republic of China.
³ Institutes of Physical Science and Information Technology, Anhui University, Hefei, 230601, People's Republic of China.
⁴ National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230029, People's Republic of China. zwei2319@mail.ustc.edu.cn.
⁵ School of Materials, Sun Yat-Sen University, Guangzhou, 510275, People's Republic of China. zwei2319@mail.ustc.edu.cn.
⁶ State Key Laboratory of Environmentally Friendly Energy Materials, School of National Defense Science and Technology, Southwest University of Science and Technology, Mianyang, 621010, People's Republic of China. zhuwenkun@swust.edu.cn.
⁷ National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230029, People's Republic of China. yaot@ustc.edu.cn.

Abstract

Surface chemistry modification represents a promising strategy to tailor the adsorption and activation of reaction intermediates for enhancing activity. Herein, we designed a surface oxygen-injection strategy to tune the electronic structure of SnS₂ nanosheets, which showed effectively enhanced electrocatalytic activity and selectivity of CO₂ reduction to formate and syngas (CO and H₂). The oxygen-injection SnS₂ nanosheets exhibit a remarkable Faradaic efficiency of 91.6% for carbonaceous products with a current density of 24.1 mA cm^-2 at -0.9 V vs RHE, including 83.2% for formate production and 16.5% for syngas with the CO/H₂ ratio of 1:1. By operando X-ray absorption spectroscopy, we unravel the in situ surface oxygen doping into the matrix during reaction, thereby optimizing the Sn local electronic states. Operando synchrotron radiation infrared spectroscopy along with theoretical calculations further reveals that the surface oxygen doping facilitated the CO₂ activation and enhanced the affinity for HCOO* species. This result demonstrates the potential strategy of surface oxygen injection for the rational design of advanced catalysts for CO₂ electroreduction.

Keywords: CO2 electroreduction; Formate; Oxygen injection; Syngas; Tin disulfide.