路易斯酸
甲烷氧化偶联
光催化
甲烷
层状结构
联轴节(管道)
氧化磷酸化
材料科学
光化学
化学
化学物理
催化作用
结晶学
有机化学
生物化学
冶金
作者
Ziyu Chen,Yutao Ye,Xiaoyi Feng,Yan Wang,Xiaowei Han,Yu Zhu,Shiqun Wu,Senyao Wang,Wan Yang,Lingzhi Wang,Jinlong Zhang
标识
DOI:10.1038/s41467-023-37663-x
摘要
Abstract Photocatalytic methane conversion requires a strong polarization environment composed of abundant activation sites with the robust stretching ability for C-H scissoring. High-density frustrated Lewis pairs consisting of low-valence Lewis acid Nb and Lewis base Nb-OH are fabricated on lamellar Nb 2 O 5 through a thermal-reduction promoted phase-transition process. Benefitting from the planar atomic arrangement of lamellar Nb 2 O 5 , the frustrated Lewis pairs sites are highly exposed and accessible to reactants, which results in a superior methane conversion rate of 1456 μmol g −1 h −1 for photocatalytic non-oxidative methane coupling without the assistance of noble metals. The time-dependent DFT calculation demonstrates the photo-induced electron transfer from LA to LB sites enhances their intensities in a concerted way, promoting the C-H cleavage through the coupling of LA and LB. This work provides in-depth insight into designing and constructing a polarization micro-environment for photocatalytic C-H activation of methane without the assistance of noble metals.
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