Graphene Chainmail Shelled Dilute Ni─Cu Alloy for Selective and Robust Aqueous Phase Catalytic Hydrogenation

Author:

Yuan Haifeng1,Hong Mei1ORCID,Huang Xianzhen1,Qiu Weitao1,Dong Feng1,Zhou Yu1,Chen Yanpeng2,Gao Jinqiang1,Yang Shihe13

Affiliation:

1. Guangdong Provincial Key Lab of Nano‐Micro Materials Research, School of Advanced Materials, Shenzhen Graduate School Peking University Shenzhen Shenzhen Guangdong 518055 China

2. Shenzhen Key Laboratory of Organic Pollution Prevention and Control, Environmental Science and Engineering Research Center Harbin Institute of Technology (Shenzhen) Shenzhen Guangdong 518055 China

3. Insitute of Biomedical Engineering Shenzhen Bay Laboratory Shenzhen Guangdong 518055 China

Abstract

AbstractCost‐effective non‐noble metal‐based catalysts for selective hydrogenation with excellent activity, selectivity, and durability are still the holy grail. Herein, an oxygen‐doped carbon (OC) chainmail encapsulated dilute Cu–Ni alloy is developed by simple pyrolysis of Cu/Ni‐metal–organic framework. The CuNi0.05@OC catalyst displays superior performance for atmospheric pressure transfer hydrogenation of p‐chloronitrobenzene and p‐nitrophenol, and for hydrogenation of furfural, all in water and with exceptional durability. Comprehensive characterizations confirm the close interactions between the diluted Ni sites, the base Cu, and optimized three‐layered graphene chainmail. Theoretical calculations demonstrate that the properly tuned lattice strain and Schottky junction can adjust electron density to facilitate specific adsorption on the active centers, thus enhancing the catalytic activity and selectivity, while the OC shell also offers robust protection. This work provides a simple and environmentally friendly strategy for developing practical heterogeneous catalysts that bring the synergistic effect into play between dilute alloy and functional carbon wrapping.

Funder

National Natural Science Foundation of China

Shenzhen Science and Technology Innovation Program

Publisher

Wiley

Subject

General Physics and Astronomy,General Engineering,Biochemistry, Genetics and Molecular Biology (miscellaneous),General Materials Science,General Chemical Engineering,Medicine (miscellaneous)

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