Chen Tao, Liu Tong, Ding Tao, Pang Beibei, Wang Lan, Liu Xiaokang, Shen Xinyi, Wang Sicong, Wu Dan, Liu Dong, Cao Linlin, Luo Qiquan, Zhang Wei, Zhu Wenkun, Yao Tao
National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230029, People's Republic of China.
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.
Nanomicro Lett. 2021 Sep 6;13(1):189. doi: 10.1007/s40820-021-00703-6.
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 nanosheets, which showed effectively enhanced electrocatalytic activity and selectivity of CO reduction to formate and syngas (CO and H). The oxygen-injection SnS nanosheets exhibit a remarkable Faradaic efficiency of 91.6% for carbonaceous products with a current density of 24.1 mA cm at -0.9 V vs RHE, including 83.2% for formate production and 16.5% for syngas with the CO/H 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 CO 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 electroreduction.
表面化学修饰是一种很有前景的策略，可通过调整反应中间体的吸附和活化来提高活性。在此，我们设计了一种表面注氧策略来调节SnS纳米片的电子结构，该策略有效提高了将CO还原为甲酸盐和合成气（CO和H）的电催化活性和选择性。在相对于可逆氢电极（RHE）为-0.9 V时，注氧的SnS纳米片对含碳产物表现出91.6%的显著法拉第效率，电流密度为24.1 mA cm²，其中甲酸盐生成的法拉第效率为83.2%，合成气（CO/H比为1:1）的法拉第效率为16.5%。通过原位X射线吸收光谱，我们揭示了反应过程中原位表面氧掺杂进入基体，从而优化了Sn的局部电子态。原位同步辐射红外光谱结合理论计算进一步表明，表面氧掺杂促进了CO的活化并增强了对HCOO*物种的亲和力。这一结果证明了表面注氧对于合理设计用于CO电还原的先进催化剂的潜在策略。
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