Zhao Shu, Chen Fang, Duan Sibin, Shao Bin, Li Tianbo, Tang Hailian, Lin Qingquan, Zhang Junying, Li Lin, Huang Jiahui, Bion Nicolas, Liu Wei, Sun Hui, Wang Ai-Qin, Haruta Masatake, Qiao Botao, Li Jun, Liu Jingyue, Zhang Tao
Department of Chemistry and Key Laboratory of Organic Optoelectronics & Molecular Engineering of the Ministry of Education, Tsinghua University, 100084, Beijing, China.
Beijing Guyue New Materials Research Institute, Beijing University of Technology, 100124, Beijing, China.
Nat Commun. 2019 Aug 23;10(1):3824. doi: 10.1038/s41467-019-11871-w.
The interfacial sites of supported metal catalysts are often critical in determining their performance. Single-atom catalysts (SACs), with every atom contacted to the support, can maximize the number of interfacial sites. However, it is still an open question whether the single-atom sites possess similar catalytic properties to those of the interfacial sites of nanocatalysts. Herein, we report an active-site dependent catalytic performance on supported gold single atoms and nanoparticles (NPs), where CO oxidation on the single-atom sites is dramatically promoted by the presence of HO whereas on NPs' interfacial sites the promoting effect is much weaker. The remarkable HO promoting effect makes the Au SAC two orders of magnitude more active than the commercial three-way catalyst. Theoretical studies reveal that the dramatic promoting effect of water on SACs originates from their unique local atomic structure and electronic properties that facilitate an efficient reaction channel of CO + OH.
负载型金属催化剂的界面位点在决定其性能方面往往至关重要。单原子催化剂（SAC）中每个原子都与载体接触，能够使界面位点的数量最大化。然而，单原子位点是否具有与纳米催化剂界面位点相似的催化性能仍是一个悬而未决的问题。在此，我们报道了负载型金单原子和纳米颗粒（NP）的活性位点依赖性催化性能，其中单原子位点上的CO氧化因HO的存在而显著促进，而在NP的界面位点上促进作用则弱得多。显著的HO促进作用使金单原子催化剂的活性比商用三元催化剂高两个数量级。理论研究表明，水对SAC的显著促进作用源于其独特的局部原子结构和电子性质，这有利于形成CO + OH的高效反应通道。
