Maximizing the Number of Interfacial Sites in Single-Atom Catalysts for the Highly Selective, Solvent-Free Oxidation of Primary Alcohols
Maximizing the Number of Interfacial Sites in Single-Atom Catalysts for the Highly Selective, Solvent-Free Oxidation of Primary Alcohols
复制标题
最大化单原子催化剂中的界面位点数量，以实现伯醇的高选择性、无溶剂氧化
DOI：
10.1002/anie.201803272
复制
发表时间：
2018-06-25
影响因子：
16.6
通讯作者：
Zhang, Tao
中科院分区：
文献类型：
--
作者：
Li, Tianbo;Liu, Fei;Zhang, Tao
无溶剂氧选择性氧化醇类化合物制备醛类化合物是一个极具吸引力和挑战性的研究领域。金属和氧化物载体之间的界面位置在决定这种非均相催化剂的活性和选择性方面是至关重要的。在此，我们证明了使用负载的单原子催化剂（SAC）导致在该反应中的高活性和选择性。由于在载体上存在单独分散的金属原子，界面位点的数量显著增加，使得SACS的活性比相应的纳米颗粒（NP）催化剂高一个或两个数量级。晶格氧原子在界面处被激活，被发现是更有选择性的比O-2在金属纳米颗粒上激活的醇基板氧化。这项工作表明，第一次，界面的网站的数量是最大限度地在SAC，提供了一个新的途径，通过开发适当的SAC醇氧化和其他反应发生在金属载体的界面网站，提高催化性能。
The solvent-free selective oxidation of alcohols to aldehydes with molecular oxygen is highly attractive yet challenging. Interfacial sites between a metal and an oxide support are crucial in determining the activity and selectivity of such heterogeneous catalysts. Herein, we demonstrate that the use of supported single-atom catalysts (SACs) leads to high activity and selectivity in this reaction. The significantly increased number of interfacial sites, resulting from the presence of individually dispersed metal atoms on the support, renders SACS one or two orders of magnitude more active than the corresponding nanoparticle (NP) catalysts. Lattice oxygen atoms activated at interfacial sites were found to be more selective than O-2 activated on metal NPs in oxidizing the alcohol substrate. This work demonstrates for the first time that the number of interfacial sites is maximized in SACs, providing a new avenue for improving catalytic performance by developing appropriate SACs for alcohol oxidation and other reactions occurring at metal-support interfacial sites.