Tian Wenrou, Li Najun, Chen Dongyun, Xu Qingfeng, Li Hua, Yan Chenglin, Lu Jianmei
College of Chemistry, Chemical Engineering and Materials Science, Collaborative Innovation Center of Suzhou Nano Science and Technology, Soochow University, Suzhou, 215123, China.
College of Energy, Soochow University, Suzhou, 215006, China.
Angew Chem Int Ed Engl. 2023 Aug 14;62(33):e202306964. doi: 10.1002/anie.202306964. Epub 2023 Jul 4.
Converting CO into high-value C2 chemicals such as acetate with high selectivity and efficiency is a critical issue in renewable energy storage. Herein, for the first time we present a vibration-driven piezocatalysis with tin(II) monosulfide (SnS) nanobelts for conversion of CO to acetate with 100 % selectivity, and the highest production rate (2.21 mM h ) compared with reported catalysts. Mechanism analysis reveal that the polarized charges triggered by periodic mechanical vibration promote the adsorption and activation of CO . The electron transfer can be facilitated due to built-in electric field, decreased band gap and work function of SnS under stress. Remarkably, reduced distance between active sites leads to charge enrichment on Sn sites, promoting the C-C coupling, reducing the energy barriers of the rate determining step. It puts forward a bran-new strategy for converting CO into high-value C2 products with efficient, low-cost and environment-friendly piezocatalysis utilizing mechanical energy.
将一氧化碳高效且高选择性地转化为高附加值的C2化学品(如醋酸盐)是可再生能源存储中的一个关键问题。在此,我们首次展示了一种利用硫化亚锡(SnS)纳米带的振动驱动压电催化,可将一氧化碳以100%的选择性转化为醋酸盐,与已报道的催化剂相比,其产率最高(2.21 mM h)。机理分析表明,周期性机械振动引发的极化电荷促进了一氧化碳的吸附和活化。由于应力作用下SnS的内建电场、减小的带隙和功函数,电子转移得以促进。值得注意的是,活性位点之间距离的减小导致Sn位点上的电荷富集,促进了碳-碳偶联,降低了速率决定步骤的能垒。它提出了一种全新的策略,即利用机械能通过高效、低成本且环境友好的压电催化将一氧化碳转化为高附加值的C2产物。