Single Atomic Cu-N Catalytic Sites for Highly Active and Selective Hydroxylation of Benzene to Phenol.

iScience

State Key Laboratory of Fine Chemicals, PSU-DUT Joint Center for Energy Research, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, P. R. China. Electronic address:

Published: December 2019

AI Article Synopsis

  • A new single-atom catalyst with Cu-N moieties (Cu-N/HCNS) has been developed for efficiently converting benzene to phenol, achieving a turnover number (TON) of 6,935, which is significantly higher than previous versions.
  • The catalyst demonstrates outstanding phenol selectivity (about 99%) and stability compared to traditional Cu nanoparticles and nanoclusters.
  • Research indicates that the unique coordination of Cu-N enhances the catalyst's activity for hydroxylation reactions due to lower energy barriers, suggesting new possibilities for designing effective single-atom catalysts in the future.

Article Abstract

Searching for an efficient single-atom catalyst for benzene hydroxylation to phenol is of critical importance, but it still remains a challenge. Herein, a single-atom catalyst with unique Cu-N moieties (Cu-N/HCNS) was prepared and confirmed by HAADF-STEM and EXAFS. Turnover number (TON) over Cu-N/HCNS (6,935) is 3.4 times of Cu-N/HCNS (2,034) under the same reaction conditions, and both exhibit much higher phenol selectivity (close to 99%) and stability compared with Cu nanoparticles and nanoclusters. Experiments and DFT calculations reveal that atomically dispersed Cu species are active sites for benzene hydroxylation to phenol, and the Cu-N is more active than Cu-N owing to its much lower energy barrier concerning the activation of HO led by its unique coordination state of local atomic structure. We envision that this work opens a new window for modulating coordination environments of single metallic atoms in catalysis design.

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Source
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6880104PMC
http://dx.doi.org/10.1016/j.isci.2019.11.010DOI Listing

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