Au-Ag synergistic effect in CF3-ketone alkynylation catalyzed by precise nanoclusters
Au-Ag synergistic effect in CF3-ketone alkynylation catalyzed by precise nanoclusters
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精密纳米团簇催化CF3-酮炔化反应中Au-Ag的协同效应
DOI：
10.1016/j.jcat.2019.08.043
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发表时间：
2019
影响因子：
7.3
通讯作者：
Zhu Manzhou
中科院分区：
文献类型：
--
作者：
Sun Lili;Shen Kangqi;Sheng Hongting;Yun Yapei;Song Yongbo;Pan Dianhui;Du Yuanxin;Yu Haizhu;Chen Mingyang;Zhu Manzhou
尽管双金属纳米材料催化剂得到广泛使用，但对协同效应的分子水平理解尚不清楚，这限制了我们预先设计“定制”双金属催化剂的能力。我们选择双金属 Au1Ag24(SR)18 和 Au25−xAgx(SR)18(x=2–6) 纳米团簇 (NC) 作为模型来研究微观结构和性能之间的关系，并将它们与相应的单金属 NC 进行比较。实验和理论分析表明，Au@Ag内核是Au1Ag24(SR)18催化剂在CF3-酮炔基化反应中具有高活性和超稳定性的必要结构特征。这种结构-活性关系已成功扩展到其他带有Au@Ag内核的双金属体系，例如Au12Ag32(SR)30NC，并被认为构成了未来高性能双金属催化剂智能设计的指导原则。
Despite the widespread use of bimetallic nanomaterial catalysts, a molecular-level understanding of the synergistic effects is unclear, limiting our ability to pre-design “tailor-made” bimetallic catalysts. We chose bimetallic Au1Ag24(SR)18and Au25−xAgx(SR)18(x = 2–6) nanoclusters (NCs) as models to investigate the relationship between microstructure and performance, comparing them with the corresponding monometallic NCs. Experimental and theoretical analyses demonstrated that the Au@Ag kernel was the essential structural feature for high activity and super stability of Au1Ag24(SR)18catalyst in the alkynylation of CF3-ketone. This structure-activity relationship was successfully extended to other bimetallic systems bearing an Au@Ag kernel, such as Au12Ag32(SR)30NC, and is thought to constitute a guiding principle for the intelligent design of high-performance bimetallic catalysts in the future.