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Engineering Bimetallic Centers in Porous Metal Silicate Materials for Hydrogenation of Furfural at Lower Temperature
ACS Materials Letters ( IF 9.6 ) Pub Date : 2021-07-19 , DOI: 10.1021/acsmaterialslett.1c00309
Jiahui Ye 1, 2 , Siqi Huang 1, 2 , Chuan-De Wu 1
Affiliation  

Discrete metal–organic molecules are an ideal class of hybrid templates for in situ encapsulation of different redox-active metal sites inside porous silicate materials. Herein, we report a proposed strategy for the synthesis of a porous metal silicate (PMS) material (denoted as PMS-2) by employing molecular Cu/Co-benzoate coordination complex as the template. The pore distribution, particle size, and redox metallic site could be systematically controlled by tuning the counterbalance of Cu/Co ions, and the concentrations of benzoic acid and tetraethyl orthosilicate. PMS-2 results in low apparent activation temperature of 50 °C and high turnover frequency of 24.9 h–1 at 110 °C for hydrogenation of furfural, which represents the most active catalyst, compared with the noble metal-free catalysts in the literature. The unique catalytic properties of PMS-2 should be ascribed to the synergistic work between Cu and Co metal sites, high surface area (675 m2g–1) and narrow pore size distribution (∼1.5 nm) for the unique PMS material, which can be further developed for extensive catalytic reactions.

中文翻译:

用于在较低温度下氢化糠醛的多孔金属硅酸盐材料中的工程双金属中心

离散的金属有机分子是一类理想的混合模板,用于原位封装多孔硅酸盐材料内的不同氧化还原活性金属位点。在此,我们报告了通过采用分子 Cu/Co-苯甲酸盐配位配合物作为模板合成多孔金属硅酸盐 (PMS) 材料(表示为 PMS-2)的拟议策略。孔分布、粒径和氧化还原金属位点可以通过调节 Cu/Co 离子的平衡以及苯甲酸和原硅酸四乙酯的浓度来系统地控制。PMS-2 导致 50 °C 的低表观活化温度和 24.9 h –1 的高周转频率与文献中的不含贵金属的催化剂相比,糠醛在 110 °C 下加氢是最活跃的催化剂。PMS-2 的独特催化性能应归因于 Cu 和 Co 金属位点之间的协同作用、高表面积 (675 m 2 g –1 ) 和独特的 PMS 材料的窄孔径分布 (~1.5 nm)。可以进一步开发用于广泛的催化反应。
更新日期:2021-08-02
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