Integration of Quantum Confinement and Alloy Effect to Modulate Electronic Properties of RhW Nanocrystals for Improved Catalytic Performance toward CO2 Hydrogenation

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• 作者：Wenbo Zhang ; Liangbing Wang ; Haoyu Liu ; Yiping Hao ; Hongliang Li ; Munir Ullah Khan ; Jie Zeng
• 刊名：Nano Letters
• 出版年：2017
• 出版时间：February 8, 2017
• 年：2017
• 卷：17
• 期：2
• 页码：788-793
• 全文大小：465K
• ISSN：1530-6992

文摘

The d-band center and surface negative charge density generally determine the adsorption and activation of CO<sub>2sub>, thus serving as important descriptors of the catalytic activity toward CO<sub>2sub> hydrogenation. Herein, we engineered the d-band center and negative charge density of Rh-based catalysts by tuning their dimensions and introducing non-noble metals to form an alloy. During the hydrogenation of CO<sub>2sub> into methanol, the catalytic activity of Rh<sub>75sub>W<sub>25sub> nanosheets was 5.9, 4.0, and 1.7 times as high as that of Rh nanoparticles, Rh nanosheets, and Rh<sub>73sub>W<sub>27sub> nanoparticles, respectively. Mechanistic studies reveal that the remarkable activity of Rh<sub>75sub>W<sub>25sub> nanosheets is owing to the integration of quantum confinement and alloy effect. Specifically, the quantum confinement in one dimension shifts up the d-band center of Rh<sub>75sub>W<sub>25sub> nanosheets, strengthening the adsorption of CO<sub>2sub>. Moreover, the alloy effect not only promotes the activation of CO<sub>2sub> to form CO<sub>2sub><sup>δ−sup> but also enhances the adsorption of intermediates to facilitate further hydrogenation of the intermediates into methanol.