Discerning the Contributions of Gold Species in Butadiene Hydrogenation: From Single Atoms to Nanoparticles
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作者
Wang, Yi; Zhang, Fan; Wang, Mengru; Mou, Xiaoling; Liu, Shuhui; Jiang, Zheng; Liu, Wei; Lin, Ronghe; Ding, Yunjie
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刊物名称
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
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年、卷、文献号
2022, 61, 1433-7851
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关键词
Wang, Yi; Zhang, Fan; Wang, Mengru; Mou, Xiaoling; Liu, Shuhui; Jiang, Zheng; Liu, Wei; Lin, Ronghe; Ding, Yunjie
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摘要
Identification of the roles of different active sites is vital for the rational design of catalysts. We present a cutting-edge strategy to discern the contributions of different single-atom gold species and nanoparticles in 1,3-butadiene hydrogenation, through coupling of advanced spectroscopic techniques, electron microscopy-based automated image analyses, and steady-state and kinetic studies. While all the carbon-hosted single gold atoms display negligible initial activity, the in situ-evolved gold nanoparticles are highly active. Full metal-species quantification is realized by combining electron-microscopy-based atom recognition statistics and deep-learning-driven nanoparticle segmentation algorithm, allowing the structure-activity correlations for the hybrid catalysts containing different Au architectures to be established. Surface exposure density of Au nanoparticles, as revealed by electron-microscopy-based statistics, is revealed as a new and reliable activity descriptor.
