期刊
ACS APPLIED MATERIALS & INTERFACES
卷 13, 期 15, 页码 17429-17438出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c22284
关键词
impeller; hierarchical structures; Pd; Suzuki reaction; biphenyl
资金
- National Natural Science Foundation of China [21872018, 21902020, 22072011]
- Fundamental Research Funds for the Central Universities [DUT20GJ208, DUT20RC(3)022]
- Natural Science Foundation of Liaoning Province [2020-MS-11]
- U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences [DE-AC0276SF00515]
The integration of catalytic production and separation of biphenyl (with a purity of 99.7%) was successfully achieved by combining Suzuki cross-coupling reactions and crystallization separation. A hierarchical-structured impeller loaded with Pd nanoparticles on Ni(OH)(2) nanosheets catalyzed the reactions with high turnover frequency (TOF) value of 25,976 h(-1) and a yield of 99.5%. X-ray absorption fine structure (XAFS) analysis revealed that enhanced catalytic activity was due to electron transfer between the Pd nanoparticles and Ni(OH)(2).
Suzuki cross-coupling reactions catalyzed by palladium are authoritative protocols in fine-chemical synthesis. Mass transfer and catalyst activity are both significant factors affecting the reaction efficiency in heterogeneous reactions. Although the holistic catalysts hold great promise in heterogeneous reactions due to the enhanced mass transport and convenient recycling, the unsatisfied catalytic activity has impeded further large-scale applications. In addition, another pronounced barrier is the product separation in the intricate system. Here, the catalytic production and separation of biphenyl (purity of 99.7%) were achieved by integrating the Suzuki cross-coupling reactions and the crystallization separation for the first time. A hierarchical-structured impeller with Pd nanoparticles (NPs) loaded on the Ni(OH)(2) nanosheets was prepared to catalyze the Suzuki reactions for bromobenzene, which exhibits a high turnover frequency (TOF) value of 25,976 h(-1) and a yield of 99.5%. The X-ray absorption fine structure (XAFS) analysis has unveiled that the electron transfer between the Pd NPs and Ni(OH)(2) accounts for the greatly enhanced catalytic activity. The findings inspire new insights toward rational engineering of highly efficient holistic catalysts for Suzuki reaction, and the innovative integrated technology offers an avenue for the separation and collection of products.
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