Wei Xiaoqian, Li Zijian, Jang Haeseong, Wang Zhe, Zhao Xuhao, Chen Yunfei, Wang Xuefeng, Kim Min Gyu, Liu Xien, Qin Qing
College of Chemical Engineering, Qingdao University of Science and Technology, Qingdao, 266042, China.
Department of Chemistry, City University of Hong Kong, Hong Kong, 999077, China.
Small. 2024 Jun;20(24):e2311136. doi: 10.1002/smll.202311136. Epub 2023 Dec 26.
Dual-engineering involved of grain boundaries (GBs) and oxygen vacancies (V) efficiently engineers the material's catalytic performance by simultaneously introducing favorable electronic and chemical properties. Herein, a novel SnO nanoplate is reported with simultaneous oxygen vacancies and abundant grain boundaries (V,G-SnO/C) for promoting the highly selective conversion of CO to value-added formic acid. Attributing to the synergistic effect of employed dual-engineering, the V,G-SnO/C displays highly catalytic selectivity with a maximum Faradaic efficiency (FE) of 87% for HCOOH production at -1.2 V versus RHE and FEs > 95% for all C products (CO and HCOOH) within all applied potential range, outperforming current state-of-the-art electrodes and the amorphous SnO/C. Theoretical calculations combined with advanced characterizations revealed that GB induces the formation of electron-enriched Sn site, which strengthens the adsorption of *HCOO intermediate. While GBs and V synergistically lower the reaction energy barrier, thus dramatically enhancing the intrinsic activity and selectivity toward HCOOH.
晶界（GBs）和氧空位（V）的双重工程通过同时引入有利的电子和化学性质，有效地调控了材料的催化性能。在此，报道了一种新型的具有同时存在氧空位和大量晶界的SnO纳米片（V,G-SnO/C），用于促进CO向高附加值甲酸的高选择性转化。由于采用的双重工程的协同效应，V,G-SnO/C表现出高度的催化选择性，在相对于可逆氢电极（RHE）为-1.2 V时，甲酸生成的最大法拉第效率（FE）为87%，并且在所有施加电位范围内，所有含碳产物（CO和HCOOH）的FE均>95%，优于当前最先进的电极和非晶态SnO/C。理论计算结合先进表征表明，晶界诱导了富电子Sn位点的形成，这增强了*HCOO中间体的吸附。同时，晶界和氧空位协同降低了反应能垒，从而显著提高了对甲酸的本征活性和选择性。
