光催化
反应性(心理学)
无定形固体
异质结
材料科学
质子化
载流子
路易斯酸
钛
纳米技术
氧化钛
化学工程
光化学
催化作用
化学
有机化学
光电子学
医学
离子
替代医学
病理
工程类
冶金
作者
Zhao Li,Chengliang Mao,Qijun Pei,Paul N. Duchesne,Teng He,Meikun Xia,Jintao Wang,Lu Wang,Rui Song,Abdinoor A. Jelle,Debora Motta Meira,Qingjie Ge,Kulbir Kaur Ghuman,Le He,Xiaohong Zhang,Geoffrey A. Ozin
标识
DOI:10.1038/s41467-022-34798-1
摘要
Abstract Light harvesting, separation of charge carriers, and surface reactions are three fundamental steps that are essential for an efficient photocatalyst. Here we show that these steps in the TiO 2 can be boosted simultaneously by disorder engineering. A solid-state reduction reaction between sodium and TiO 2 forms a core-shell c-TiO 2 @a-TiO 2-x (OH) y heterostructure, comprised of HO-Ti-[O]-Ti surface frustrated Lewis pairs (SFLPs) embedded in an amorphous shell surrounding a crystalline core, which enables a new genre of chemical reactivity. Specifically, these SFLPs heterolytically dissociate dihydrogen at room temperature to form charge-balancing protonated hydroxyl groups and hydrides at unsaturated titanium surface sites, which display high reactivity towards CO 2 reduction. This crystalline-amorphous heterostructure also boosts light absorption, charge carrier separation and transfer to SFLPs, while prolonged carrier lifetimes and photothermal heat generation further enhance reactivity. The collective results of this study motivate a general approach for catalytically generating sustainable chemicals and fuels through engineered disorder in heterogeneous CO 2 photocatalysts.
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