Zhang Yuning, Xu Hai, Niu Dongfang, Zhang Xinsheng, Zhang Yayun
State Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237, P. R. China.
ChemSusChem. 2021 Jul 6;14(13):2769-2779. doi: 10.1002/cssc.202100541. Epub 2021 Apr 29.
Sn-based electrocatalysts have shown great potential in the future industrial application of CO electroreduction (CO ER) to C products due to their non-toxicity and low price. However, it is a great challenge to fabricate a Sn-based electrocatalytic system with high performance and stability. Herein, grafted pyridine was innovatively coupled with SnO to construct an organic-inorganic composite (SnO /Py-CNTO) for highly efficient CO ER. The detailed studies showed that pyridine and protonated pyridine coexist on the surface of SnO /Py-CNTO, and both play distinctive roles in promoting the selectivity of CO ER. Benefiting from the merits, SnO /Py-CNTO delivered an excellent faradaic efficiency (FE) of 96 % for CO ER at -1.29 V where the HCOOH production with 85 % FE dominated, and good stability for 32 h electrolysis. The theoretical calculations showed that protonated pyridine not only facilitates the CO adsorption and HCOOH desorption, but also significantly reduces the limiting potential for the conversion of CO to HCOOH.
基于锡的电催化剂因其无毒且价格低廉,在未来将CO电还原(CO ER)为含碳产物的工业应用中显示出巨大潜力。然而,制备具有高性能和稳定性的基于锡的电催化体系是一项巨大挑战。在此,将接枝吡啶与SnO创新性地偶联,构建了一种用于高效CO ER的有机-无机复合材料(SnO /Py-CNTO)。详细研究表明,吡啶和质子化吡啶共存于SnO /Py-CNTO表面,且二者在促进CO ER的选择性方面发挥着独特作用。得益于这些优点,SnO /Py-CNTO在-1.29 V下对CO ER的法拉第效率(FE)高达96%,此时以85% FE的甲酸生成占主导,并且在32小时的电解过程中具有良好的稳定性。理论计算表明,质子化吡啶不仅促进了CO的吸附和甲酸的脱附,还显著降低了CO转化为甲酸的极限电位。