Oxo dicopper anchored on carbon nitride for selective oxidation of methane

Pengfei Xie (), Jing Ding, Zihao Yao, Tiancheng Pu, Peng Zhang, Zhennan Huang, Canhui Wang, Junlei Zhang, Noah Zecher-Freeman, Han Zong, Dashui Yuan, Shengwei Deng, Reza Shahbazian-Yassar and Chao Wang ()
Additional contact information
Pengfei Xie: Johns Hopkins University
Jing Ding: Johns Hopkins University
Zihao Yao: Zhejiang University of Technology
Tiancheng Pu: Johns Hopkins University
Peng Zhang: Zhengzhou University
Zhennan Huang: University of Illinois
Canhui Wang: Johns Hopkins University
Junlei Zhang: Johns Hopkins University
Noah Zecher-Freeman: Johns Hopkins University
Han Zong: Johns Hopkins University
Dashui Yuan: Nanjing Tech University
Shengwei Deng: Zhejiang University of Technology
Reza Shahbazian-Yassar: University of Illinois
Chao Wang: Johns Hopkins University

Nature Communications, 2022, vol. 13, issue 1, 1-10

Abstract: Abstract Selective conversion of methane (CH4) into value-added chemicals represents a grand challenge for the efficient utilization of rising hydrocarbon sources. We report here dimeric copper centers supported on graphitic carbon nitride (denoted as Cu2@C3N4) as advanced catalysts for CH4 partial oxidation. The copper-dimer catalysts demonstrate high selectivity for partial oxidation of methane under both thermo- and photocatalytic reaction conditions, with hydrogen peroxide (H2O2) and oxygen (O2) being used as the oxidizer, respectively. In particular, the photocatalytic oxidation of CH4 with O2 achieves >10% conversion, and >98% selectivity toward methyl oxygenates and a mass-specific activity of 1399.3 mmol g Cu−1h−1. Mechanistic studies reveal that the high reactivity of Cu2@C3N4 can be ascribed to symphonic mechanisms among the bridging oxygen, the two copper sites and the semiconducting C3N4 substrate, which do not only facilitate the heterolytic scission of C-H bond, but also promotes H2O2 and O2 activation in thermo- and photocatalysis, respectively.

Date: 2022
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DOI: 10.1038/s41467-022-28987-1

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