Oxo dicopper anchored on carbon nitride for selective oxidation of methane.
Oxo dicopper anchored on carbon nitride for selective oxidation of methane.
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DOI：
10.1038/s41467-022-28987-1
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发表时间：
2022-03-16
影响因子：
16.6
通讯作者：
Wang C
中科院分区：
文献类型：
--
作者：
Xie P;Ding J;Yao Z;Pu T;Zhang P;Huang Z;Wang C;Zhang J;Zecher-Freeman N;Zong H;Yuan D;Deng S;Shahbazian-Yassar R;Wang C
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. Selective conversion of methane into value-added chemicals is a promising approach for utilization of hydrocarbon sources. Here the authors develop dimeric copper centers supported on graphitic carbon nitride (denoted as Cu2@C3N4) with >10% conversion and >98% selectivity toward methyl oxygenates in both thermo- and photo- catalytic reactions.
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影响因子：
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通讯作者：
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