Surface Organometallic Chemistry as a Versatile Strategy for Synthesizing Supported Bimetallic Cluster Catalysts
Surface Organometallic Chemistry as a Versatile Strategy for Synthesizing Supported Bimetallic Cluster Catalysts
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表面有机金属化学作为合成负载型双金属簇催化剂的多功能策略
DOI：
10.1021/acs.jpcc.2c04869
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发表时间：
2022-09
期刊：
影响因子：
--
通讯作者：
Haibo Zhu
中科院分区：
文献类型：
--
作者：
Kunbo Lian;Yuanyuan Yue;Jean-Marie Basset;Xi Liu;Liwei Chen;Cigdem Ozsoy-Keskinbora;Xiaojun Bao;Haibo Zhu
固定在热稳定性和高比表面积载体上的双金属簇合物在多相催化中得到了广泛的应用。与单金属原子簇或大的双金属纳米粒子相比，双金属原子簇由于高比例的表面不饱和配位金属原子产生的调制电子和几何效应以及两个组成金属之间的协同效应而显示出前所未有的催化性能。然而，即使经过60多年的努力，到目前为止，在两种组成金属之间控制合成分布均匀、结构良好的双金属团簇仍然是一个巨大的挑战。在这里，我们提出了一种基于表面有机金属化学概念的通用策略来合成负载型双金属簇合物催化剂，该策略是通过所谓的“双表面有机金属络合物”的加氢来实现的。双表面有机金属络合物中两个表面金属有机碎片的协同分解以及它们与载体的强相互作用使其能够形成均匀分散在不同载体表面的合金化的双金属团簇。这种方法可以作为一种平台技术，用于在诸如氧化铝、二氧化钛和沸石等广泛的载体上制备具有不同组成的各种双金属簇合物。与单金属催化剂相比，双金属簇合物催化剂在苯加氢反应中表现出显著的催化性能，这是由于其表面原子的高度暴露和组成金属之间的协同作用。
Bimetallic clusters anchored on thermally stable and high-surface-area supports have gained a wide range of applications in heterogeneous catalysis. Compared to monometallic clusters or large bimetallic nanoparticles, bimetallic clusters show unprecedented catalytic performances due to the modulated electronic and geometric effects arising from the high fraction of surface unsaturated–coordinated metallic atoms and the synergistic effects between two constituting metals. However, even after more than 60 years of efforts, the controlled synthesis of homogeneously distributed bimetallic clusters with well-alloyed structure between two constituting metals remains a tremendous challenge so far. Herein, we present a versatile strategy based on the surface organometallic chemistry concept for synthesizing supported bimetallic cluster catalysts, which is achieved via the hydrogenation of a so-called “double surface organometallic complex”. The cooperative decomposition of two surface organometallic fragments in the double surface organometallic complex and their strong interaction with the support enable the formation of well-alloyed bimetallic clusters uniformly dispersed at the surfaces of different supports. This approach can serve as a platform technique for producing a variety of bimetallic clusters with varied compositions on a wide range of supports, such as Al2O3, TiO2, and zeolite. The resulting bimetallic cluster catalysts exhibit remarkably enhanced catalytic performance in benzene hydrogenation as compared to their monometallic counterparts because of highly exposed surface atoms and synergistic effects between constituting metals.
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影响因子：
56.9
作者：
Ding, Kunlun;Cullen, David A.;Cao, Dongmei
通讯作者：
Cao, Dongmei
影响因子：
15
作者：
F. Humblot;D. Didillon;F. Lepeltier;J. Candy;J. Corker;O. Clause;F. Bayard;J. Basset
通讯作者：
F. Humblot;D. Didillon;F. Lepeltier;J. Candy;J. Corker;O. Clause;F. Bayard;J. Basset
影响因子：
3.7
作者：
Alper Uzun;Vinesh A. Bhirud;Philip W. Kletnieks-;J. F. Haw;B. Gates
通讯作者：
Alper Uzun;Vinesh A. Bhirud;Philip W. Kletnieks-;J. F. Haw;B. Gates
影响因子：
2.8
作者：
Bonati, Matteo L. M.;Douglas, Thomas M.;Guo, Neng
通讯作者：
Guo, Neng
影响因子：
1.8
作者：
Yanming Xue;Jing Lin;Ying Fan;Jie Li;A. Elsanousi;Xuewen Xu;Dong Liu;Yang Huang;Long Hu;Yan Liu;F. Meng;J. Zou;Chengchun Tang
通讯作者：
Yanming Xue;Jing Lin;Ying Fan;Jie Li;A. Elsanousi;Xuewen Xu;Dong Liu;Yang Huang;Long Hu;Yan Liu;F. Meng;J. Zou;Chengchun Tang