Kuai Long, Liu Li, Tao Qingmei, Yu Nan, Kan Erjie, Sun Na, Liu Shoujie, Geng Baoyou
College of Chemistry and Materials Science, The Key Laboratory of Electrochemical Clean Energy of An-hui Higher Education Institutes, Anhui Provincial Engineering Laboratory for New-Energy Vehicle Battery Energy-Storage Materials, Anhui Normal University, Jiuhua South Road, Wuhu, 241002, China.
School of Chemical and Environmental Engineering, Anhui Laboratory of Clean Catalytic Engineering, Anhui Polytechnic University, Beijing Middle Road, Wuhu, 241000, China.
Angew Chem Int Ed Engl. 2022 Nov 7;61(45):e202212338. doi: 10.1002/anie.202212338. Epub 2022 Oct 7.
The two-dimensional nanosheets are conducive to not only endow opened surfaces for loading active metal atoms but also boost the mass transfer for the heterogeneous reactions. The challenge is how to load and stabilize single-atoms on nanosheets in high-areal densities. This work reports an efficient micro-gas blasting (MGB) strategy to access versatile noble metal single-atoms/metal oxide nanosheets, including Ir /CoO , Pd /CeO , etc. Especially for Pt/CeO nanosheets (Pt /CeO -S), the Pt loading is increased to 15 at%. The Pt /CeO -S catalysts from MGB are revealed to possess superior reactivity and tolerance in the model reaction of water-gas shift (WGS). The Pt /CeO -S catalyst exhibit 2-3 times reactivity that of their thicker counterpart, single-atom Pt /CeO microspheric catalyst. Moreover, the single-atom sites in Pt /CeO -S (1-10 %) catalysts are stable in a harsh WGS reaction condition of 10 % CO. This work thus paves a way to access the practical single-atom catalysts.
二维纳米片不仅有利于为负载活性金属原子提供开放表面,还能促进多相反应的传质。挑战在于如何以高面密度在纳米片上负载并稳定单原子。这项工作报道了一种高效的微气体喷射(MGB)策略,用于制备多种贵金属单原子/金属氧化物纳米片,包括Ir/CoO、Pd/CeO等。特别是对于Pt/CeO纳米片(Pt/CeO -S),Pt负载量提高到了15原子%。通过MGB制备的Pt/CeO -S催化剂在水煤气变换(WGS)模型反应中表现出优异的反应活性和耐受性。Pt/CeO -S催化剂的反应活性是其较厚的对应物——单原子Pt/CeO微球催化剂的2至3倍。此外,Pt/CeO -S(1 - 10%)催化剂中的单原子位点在10% CO的苛刻WGS反应条件下是稳定的。因此,这项工作为获得实用的单原子催化剂铺平了道路。