纳米团簇
材料科学
杂原子
光致发光
光催化
纳米技术
Atom(片上系统)
催化作用
纳米材料
十二面体
纳米晶
化学物理
光化学
结晶学
光电子学
化学
戒指(化学)
嵌入式系统
生物化学
有机化学
计算机科学
作者
Megalamane S. Bootharaju,Chan Woo Lee,Guocheng Deng,Hyeseung Kim,Kangjae Lee,Sang-Hwa Lee,Hogeun Chang,Seongbeom Lee,Yun Mo Sung,Jong Suk Yoo,Nanfeng Zheng,Taeghwan Hyeon
标识
DOI:10.1002/adma.202207765
摘要
While core-shell nanomaterials are highly desirable for realizing enhanced optical and catalytic properties, their synthesis with atomic-level control is challenging. Here, the synthesis and crystal structure of [Au12 Ag32 (SePh)30 ]4- , the first example of selenolated Au-Ag core-shell nanoclusters, comprising a gold icosahedron core trapped in a silver dodecahedron, which is protected by an Ag12 (SePh)30 shell, is presented. The gold core strongly modifies the overall electronic structure and induces synergistic effects, resulting in high enhancements in the stability and near-infrared-II photoluminescence. The Au12 Ag32 and its homometal analog Ag44 , show strong interactions with oxygen vacancies of TiO2 , facilitating the interfacial charge transfer for photocatalysis. Indeed, the Au12 Ag32 /TiO2 exhibits remarkable solar H2 production (6810 µmol g-1 h-1 ), which is ≈6.2 and ≈37.8 times higher than that of Ag44 /TiO2 and TiO2 , respectively. Good stability and recyclability with minimal catalytic activity loss are additional features of Au12 Ag32 /TiO2 . The experimental and computational results reveal that the Au12 Ag32 acts as an efficient cocatalyst by possessing a favorable electronic structure that aligns well with the TiO2 bands for the enhanced separation of photoinduced charge carriers due to the relatively negatively charged Au12 core. These atomistic insights will motivate uncovering of the structure-catalytic activity relationships of other nanoclusters.
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