Precise Fabrication of Tetrametallic Metal-Organic Frameworks and Multivariate Hybrids for Enhanced Photothermal Tandem Catalysis

doi:10.1007/s40242-024-4044-2

高等学校化学研究 ›› 2024, Vol. 40 ›› Issue (6): 1141-1150.doi: 10.1007/s40242-024-4044-2

Precise Fabrication of Tetrametallic Metal-Organic Frameworks and Multivariate Hybrids for Enhanced Photothermal Tandem Catalysis

FAN Yiwen¹, WANG Yang¹, WANG Huijuan², CHEN Yuzhen¹, LI Zhibo¹

1. Department of Chemistry, College of Chemistry and Chemical Engineering, Qingdao University of Science and Technology, Qingdao 266071, P. R. China;
2. Experimental Center of Engineering and Material Science, University of Science and Technology of China, Hefei 230026, P. R. China

收稿日期:2024-02-27 出版日期:2024-12-01 发布日期:2024-10-26
通讯作者: CHEN Yuzhen,yzchen@qust.edu.cn;LI Zhibo,zbli@qust.edu.cn E-mail:yzchen@qust.edu.cn;zbli@qust.edu.cn
基金资助:
This work was supported by the Excellent Youth Foundation of Natural Science Foundation of Shandong Province, China (No. ZR2020YQ08) and the National Natural Science Foundation of China (No. 22275108).

Precise Fabrication of Tetrametallic Metal-Organic Frameworks and Multivariate Hybrids for Enhanced Photothermal Tandem Catalysis

FAN Yiwen¹, WANG Yang¹, WANG Huijuan², CHEN Yuzhen¹, LI Zhibo¹

1. Department of Chemistry, College of Chemistry and Chemical Engineering, Qingdao University of Science and Technology, Qingdao 266071, P. R. China;
2. Experimental Center of Engineering and Material Science, University of Science and Technology of China, Hefei 230026, P. R. China

Received:2024-02-27 Online:2024-12-01 Published:2024-10-26
Contact: CHEN Yuzhen,yzchen@qust.edu.cn;LI Zhibo,zbli@qust.edu.cn E-mail:yzchen@qust.edu.cn;zbli@qust.edu.cn
Supported by:
This work was supported by the Excellent Youth Foundation of Natural Science Foundation of Shandong Province, China (No. ZR2020YQ08) and the National Natural Science Foundation of China (No. 22275108).

摘要/Abstract

摘要： Multiple metal sites doped in metal-organic frameworks (MOFs) are essential for their promising application in cascade reactions. However, precision synthesis of tetrametallic MOFs with total coordination and regular shapes is challenging due to the different coordination abilities of four metal ions. Herein, a series of tetrametallic MOFs (t-MOFs) with four regular morphologies is successfully constructed by regulating the metal ratio, amount of morphologic modulating reagent or growth time. The t-MOFs can be flexibly oxidized to afford porous metal oxides (M_xCo₃O₄, M=CuZnNi) under air or reduced to carbon-encapsulated CuCoNi under H₂/Ar for different reactions to maximize the value-in-use of MOFs. In particular, the t-MOF@M_xCo₃O₄ obtained upon the surface oxidation of t-MOF well integrates the Lewis-base sites from MOF core with photothermal oxidation activity from M_xCo₃O₄ shell. The hybrid effectively catalyzes the cascade reaction of styrene oxidation coupling Knoevenagel condensation under visible light. Thus, the by-product, benzaldehyde, is successfully converted to easily separated benzylidene malononitrile to finally obtain pure styrene epoxide (SO). In M_xCo₃O₄, Ni species afford good photothermal effect, Cu and Co species provide catalytic activity, and Zn species increase SO selectivity. The host-object coordination and the synergy among objects may greatly boost more complex reactions in the future.

关键词: Metal-organic framework, Multimetallic site, Photothermal catalysis, Cascade reaction, Host-object coordination

Abstract: Multiple metal sites doped in metal-organic frameworks (MOFs) are essential for their promising application in cascade reactions. However, precision synthesis of tetrametallic MOFs with total coordination and regular shapes is challenging due to the different coordination abilities of four metal ions. Herein, a series of tetrametallic MOFs (t-MOFs) with four regular morphologies is successfully constructed by regulating the metal ratio, amount of morphologic modulating reagent or growth time. The t-MOFs can be flexibly oxidized to afford porous metal oxides (M_xCo₃O₄, M=CuZnNi) under air or reduced to carbon-encapsulated CuCoNi under H₂/Ar for different reactions to maximize the value-in-use of MOFs. In particular, the t-MOF@M_xCo₃O₄ obtained upon the surface oxidation of t-MOF well integrates the Lewis-base sites from MOF core with photothermal oxidation activity from M_xCo₃O₄ shell. The hybrid effectively catalyzes the cascade reaction of styrene oxidation coupling Knoevenagel condensation under visible light. Thus, the by-product, benzaldehyde, is successfully converted to easily separated benzylidene malononitrile to finally obtain pure styrene epoxide (SO). In M_xCo₃O₄, Ni species afford good photothermal effect, Cu and Co species provide catalytic activity, and Zn species increase SO selectivity. The host-object coordination and the synergy among objects may greatly boost more complex reactions in the future.

Key words: Metal-organic framework, Multimetallic site, Photothermal catalysis, Cascade reaction, Host-object coordination

FAN Yiwen, WANG Yang, WANG Huijuan, CHEN Yuzhen, LI Zhibo. Precise Fabrication of Tetrametallic Metal-Organic Frameworks and Multivariate Hybrids for Enhanced Photothermal Tandem Catalysis[J]. 高等学校化学研究, 2024, 40(6): 1141-1150.

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Precise Fabrication of Tetrametallic Metal-Organic Frameworks and Multivariate Hybrids for Enhanced Photothermal Tandem Catalysis

Precise Fabrication of Tetrametallic Metal-Organic Frameworks and Multivariate Hybrids for Enhanced Photothermal Tandem Catalysis

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