Yang Qingcheng, Zhao Yang, Meng Linghu, Liu Zhixiao, Lan Jiao, Zhang Yanlong, Duan Huigao, Tan Yongwen
College of Materials Science and Engineering, State Key Laboratory of Advanced Design and Manufacturing for Vehicle Body, Hunan University, Changsha, Hunan, 410082, China.
College of Mechanical and Vehicle Engineering, Hunan University, Changsha, Hunan, 410082, China.
Small. 2022 Apr;18(17):e2107968. doi: 10.1002/smll.202107968. Epub 2022 Mar 22.
Electrochemical reduction of CO into formate product is considered the most practical significance link in the carbon cycle. Developing cheap and efficient electrocatalysts with high selectivity for formate on a wide operated potential window is desirable yet challenging. Herein, nanoporous ordered intermetallic tin-tellurium (SnTe) is synthesized with a greater reduction performance for electrochemical CO to formate reduction compared to bare Sn. This nanoporous SnTe achieves 93% Faradaic efficiency for formate production and maintains over 90% Faradaic efficiency at a wide voltage range from -1.0 to -1.3 V versus reversible hydrogen electrode (RHE), together with 60 h stability. Combining operando Raman spectroscopy studies with density functional theory calculations reveals that strong orbital interaction between Sn and neighboring tellurium (Te) in the intermetallic SnTe can lower the barriers of the oxygen cutoff hydrogenation and desorption steps by promoting the fracture of bond between metal and oxygen, leading to the significant enhancement of formate production.
将CO电化学还原为甲酸盐产物被认为是碳循环中最具实际意义的环节。开发在宽操作电位窗口下对甲酸盐具有高选择性的廉价高效电催化剂是理想的，但具有挑战性。在此，合成了纳米多孔有序金属间化合物锡-碲（SnTe），与裸Sn相比，其对电化学CO还原为甲酸盐具有更高的还原性能。这种纳米多孔SnTe在生成甲酸盐方面实现了93%的法拉第效率，并且在相对于可逆氢电极（RHE）为-1.0至-1.3 V的宽电压范围内保持超过90%的法拉第效率，同时具有60小时的稳定性。将原位拉曼光谱研究与密度泛函理论计算相结合表明，金属间化合物SnTe中Sn与相邻碲（Te）之间的强轨道相互作用可以通过促进金属与氧之间键的断裂来降低氧切断氢化和解吸步骤的势垒，从而导致甲酸盐生成的显著增强。
