TY - JOUR
T1 - Oxo dicopper anchored on carbon nitride for selective oxidation of methane
AU - Xie, Pengfei
AU - Ding, Jing
AU - Yao, Zihao
AU - Pu, Tiancheng
AU - Zhang, Peng
AU - Huang, Zhennan
AU - Wang, Canhui
AU - Zhang, Junlei
AU - Zecher-Freeman, Noah
AU - Zong, Han
AU - Yuan, Dashui
AU - Deng, Shengwei
AU - Shahbazian-Yassar, Reza
AU - Wang, Chao
N1 - Publisher Copyright:
© 2022, The Author(s).
PY - 2022/12
Y1 - 2022/12
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85126301324&partnerID=8YFLogxK
U2 - 10.1038/s41467-022-28987-1
DO - 10.1038/s41467-022-28987-1
M3 - 文章
C2 - 35296655
AN - SCOPUS:85126301324
SN - 2041-1723
VL - 13
JO - Nature Communications
JF - Nature Communications
IS - 1
M1 - 1375
ER -