TY - JOUR AU - Chen, Tao AU - Liu, Tong AU - Ding, Tao AU - Pang, Beibei AU - Wang, Lan AU - Liu, Xiaokang AU - Shen, Xinyi AU - Wang, Sicong AU - Wu, Dan AU - Liu, Dong AU - Cao, Linlin AU - Luo, Qiquan AU - Zhang, Wei AU - Zhu, Wenkun AU - Yao, Tao PY - 2021/09/06 Y2 - 2024/03/29 TI - Surface Oxygen Injection in Tin Disulfide Nanosheets for Efficient CO2 Electroreduction to Formate and Syngas JF - Nano-Micro Letters JA - Nano-Micro Lett VL - 13 IS - SE - Articles DO - 10.1007/s40820-021-00703-6 UR - https://nmlett.org/index.php/nml/article/view/955 SP - 189 AB - <p>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 SnS<sub>2</sub> nanosheets, which showed effectively enhanced electrocatalytic activity and selectivity of CO<sub>2</sub> reduction to formate and syngas (CO and H<sub>2</sub>). The oxygen-injection SnS<sub>2</sub> nanosheets exhibit a remarkable Faradaic efficiency of 91.6% for carbonaceous products with a current density of 24.1&nbsp;mA&nbsp;cm<sup>−2</sup> at −0.9&nbsp;V vs RHE, including 83.2% for formate production and 16.5% for syngas with the CO/H<sub>2</sub> ratio of 1:1. By <em>operando</em> X-ray absorption spectroscopy, we unravel the in situ surface oxygen doping into the matrix during reaction, thereby optimizing the Sn local electronic states. <em>Operando</em> synchrotron radiation infrared spectroscopy along with theoretical calculations further reveals that the surface oxygen doping facilitated the CO<sub>2</sub> 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 CO<sub>2</sub> electroreduction.</p><p>Highlights:</p><p>1 A surface oxygen-injection strategy is proposed to synergistically modulate the electronic structure of the SnS<sub>2</sub> nanosheets, thereby regulating the oxophilicity of the catalyst surface.<br>2 The surface oxygen doping facilitates the CO<sub>2</sub> activation and enhances the affinity for HCOO* species.<br>3 The oxygen-injection SnS<sub>2</sub> nanosheets exhibit a remarkable Faradaic efficiency of 91.6% for carbonaceous products with a current density of 24.1 mA cm<sup>−2</sup> at -0.9 V vs RHE.</p> ER -