Li Meng, Hu Yue, Wang Dawei, Geng Dongsheng
Beijing Advanced Innovation Center for Materials Genome Engineering, Beijing Key Laboratory for Magneto-Photoelectrical Composite and Interface Science, School of Mathematics and Physics, University of Science and Technology Beijing, 100083, Beijing, P. R. China.
Jiangsu JITRI Molecular Engineering Institute Co., Ltd., 215500, Changshu, P. R. China.
Chem Asian J. 2021 Sep 20;16(18):2694-2701. doi: 10.1002/asia.202100718. Epub 2021 Aug 12.
Silver (Ag)-based materials are considered to be promising materials for electrochemical reduction of CO to produce CO, but the selectivity and efficiency of traditional polycrystalline Ag materials are insufficient; there still exists a great challenge to explore novel modified Ag based materials. Herein, a nanocomposite of Ag and SnO (Ag/SnO ) for efficient reduction of CO to CO is reported. HRTEM and XRD patterns clearly demonstrated the lattice destruction of Ag and the amorphous SnO in the Ag/SnO nanocomposite. Electrochemical tests indicated the nanocomposite containing 15% SnO possesses highest catalytic selectivity featured by a CO faradaic efficiency (FE) of 99.2% at -0.9 V versus reversible hydrogen electrode (vs RHE) and FE>90% for the CO product at a wide potential range from -0.8 V to -1.4 V vs RHE. Experimental characterization and analysis showed that the high catalytic performance is attributed to not only the branched morphology of Ag/SnO nanocomposites (NCs), which endows the maximum exposure of active sites, but also the special adsorption capacity of abundant defect sites in the crystal for *COOH (the key intermediate of CO formation), which improves the intrinsic activity of the catalyst. But equally important, the existed SnO also plays an important role in inhibiting hydrogen evolution reaction (HER) and anchoring defect sites. This work demonstrates the use of crystal defect engineering and synergy in composite to improve the efficiency of electrocatalytic CO reduction reaction (CO RR).
银(Ag)基材料被认为是用于将CO电化学还原以生产CO的有前景的材料,但传统多晶Ag材料的选择性和效率不足;探索新型改性Ag基材料仍然存在巨大挑战。在此,报道了一种用于将CO高效还原为CO的Ag和SnO的纳米复合材料(Ag/SnO)。高分辨透射电子显微镜(HRTEM)和X射线衍射(XRD)图谱清楚地表明了Ag/SnO纳米复合材料中Ag的晶格破坏和非晶态SnO。电化学测试表明,含有15% SnO的纳米复合材料具有最高的催化选择性,其特征在于相对于可逆氢电极(vs RHE)在-0.9 V时CO法拉第效率(FE)为99.2%,并且在相对于RHE从-0.8 V到-1.4 V的宽电位范围内,CO产物的FE>90%。实验表征和分析表明,高催化性能不仅归因于Ag/SnO纳米复合材料(NCs)的分支形态,其赋予了活性位点的最大暴露,还归因于晶体中丰富缺陷位点对*COOH(CO形成的关键中间体)的特殊吸附能力,这提高了催化剂的本征活性。但同样重要的是,存在的SnO在抑制析氢反应(HER)和锚定缺陷位点方面也起着重要作用。这项工作展示了利用晶体缺陷工程和复合材料中的协同作用来提高电催化CO还原反应(CO RR)的效率。