期刊
ACS CATALYSIS
卷 10, 期 14, 页码 7753-7762出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c00177
关键词
metal-organic framework; photothermal effect; alloy nanocrystals; plasmonic; selective catalysis
资金
- National Natural Science Foundation of China [21725101, 21871244, 21673213, 21521001]
- International Partnership Program of CAS [211134KYSB20190109]
- Fundamental Research Funds for the Central Universities [WK2060030029]
- Fujian Institute of Innovation (CAS)
Selective semihydrogenation of alkynes has been a long-term and significant target, yet it remains a great challenge. Herein, bimetallic nanoparticles in a metal-organic framework (MOF), i.e., CuPd@ZIF-8 composite, featuring a cubic CuPd core and a porous ZIF-8 shell, have been rationally fabricated for this end. Given the unique physicochemical properties, the Cu nanocubes can not only convert solar energy into heat to accelerate the reaction but also serve as the seed for in situ formation of Pd nanoparticles (NPs) on their external surface to regulate the chemoselectivity of Pd active sites. The additional growth of the MOF shell is helpful to stabilize the CuPd core and offer regioselectivity via the steric hindrance effect. Ammonia borane provides active hydrogen species to significantly boost the hydrogenation and ensure the high selectivity. As a result, the CuPd@MOF exhibits high efficiency, featuring a turnover frequency (TOF, 6799 min(-1)) of 5-10(5) times higher than that in previous reports, and high chemo- and regioselectivity toward the semihydrogenation of alkynes, in the presence of NH3BH3 as a hydrogen source, under visible-light irradiation at ambient temperature.
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