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Inspired by the advantages of bi-atom catalysts and recent exciting progresses of nanozymes, by means of density functional theory (DFT) computations, we explored the potential of metal dimers embedded in phthalocyanine monolayers (M2-Pc), which mimics the binuclear centers of methane monooxygenase, as catalysts for methane conversion using H2O2 as an oxidant. In total, 26 transition metal (from group IB to VIIIB) and four main group metal (M = Al, Ga, Sn and Bi) dimers were considered, and two methane conversion routes, namely *O-assisted and *OH-assisted mechanisms were systematically studied. The results show that methane conversion proceeds via an *OH-assisted mechanism on the Ti2-Pc, Zr2-Pc and Ta2-Pc, a combination of *O- and *OH-assisted mechanism on the surface of Sc2-Pc, respectively. Our theoretical work may provide impetus to developing new catalysts for methane conversion and help stimulate further studies on metal dimer catalysts for other catalytic reactions. [ABSTRACT FROM AUTHOR]

Excessive accumulation of carbon dioxide in the atmosphere has become a serious environmental problem due to the increasing consumption of fossil fuels in modern society. Reasonably reducing CO 2 in the atmosphere has become a new research hotspot. Electrocatalytic CO 2 reduction reaction (CO 2 RR) offers an appealing strategy to reduce the atmospheric CO 2 concentration and to produce value-added chemicals simultaneously. In this paper, two-dimensional (2D) N-decorated graphene (NG)-supported bimetallic trimers (Fe 2 M@NG) were designed as triple-atom catalysts (TACs). Theoretical calculations showed that Fe 2 M@NG can effectively activate CO 2 , and among the 23 TACs examined, Fe 2 Ir@NG not only has a good catalytic activity for CO 2 RR (limiting potential is 0.49 V for CH 4 formation) but also limits the competing side reaction of the hydrogen evolution reaction (HER). Our theoretical study not only further extends the triple-atom catalysts, but also opens a new door to boost the sustainable CO 2 conversion., Competing Interests: The authors declare no competing financial interest., (© 2022 The Authors. Published by American Chemical Society.)