张宁
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祝贺课题组与刘东教授合作,在《Science Advances》上发表有关晶格氧活化介导甲烷有氧氧化偶联的研究论文,第一作者为博士生翟广耀!
Title: Highly efficient, selective, and stable photocatalytic methane coupling to ethane enabled by lattice oxygen looping
Abstract: Light-driven oxidative coupling of methane (OCM) for multi-carbon (C2+) product evolution is a promising approach toward the sustainable production of value-added chemicals, yet remains challenging due to its low intrinsic activity. Here, we demonstrate the integration of bismuth oxide (BiOx) and gold (Au) on titanium dioxide (TiO2) substrate to achieve a high conversion rate, product selectivity, and catalytic durability toward photocatalytic OCM through rational catalytic site engineering. Mechanistic investigations reveal that the lattice oxygen in BiOx is effectively activated as the localized oxidant to promote methane dissociation, while Au governs the methyl transfer to avoid undesirable overoxidation and promote carbon─carbon coupling. The optimal Au/BiOx-TiO2 hybrid delivers a conversion rate of 20.8 millimoles per gram per hour with C2+ product selectivity high to 97% in the flow reactor. More specifically, the veritable participation of lattice oxygen during OCM is chemically looped by introduced dioxygen via the Mars-van Krevelen mechanism, endowing superior catalyst stability.
论文链接:https://www.science.org/doi/10.1126/sciadv.ado4390