Water Enables Lattice Oxygen Activation of Transition Metal Oxides for Volatile Organic Compound Oxidation
Water Enables Lattice Oxygen Activation of Transition Metal Oxides for Volatile Organic Compound Oxidation
复制标题
水能够使过渡金属氧化物晶格氧活化，从而氧化挥发性有机化合物
DOI：
10.1021/acscatal.2c03552
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发表时间：
2022-09-01
期刊：
影响因子：
12.9
通讯作者：
Liu, Xiao
中科院分区：
文献类型：
--
作者：
Gu, Huayu;Lan, Jintong;Liu, Xiao
少量的水可以增强挥发性有机化合物（VOCs）对过渡金属氧化物（TMOs）的催化燃烧活性，但其内在机制仍存在争议。在此，我们从理论上和实验上系统地证明了水分子可以不断激活过渡金属氧化物的晶格氧以形成羟基物种。生成的羟基物种的氧原子与周围金属原子的键合强度较弱，由于其较强的亲核性，很容易从表面逸出并攻击VOCs的缺电子碳原子，留下丰富的氧空位作为后续分子氧活化的活性位点。这项工作有助于我们深入了解水在过渡金属氧化物晶格氧活化中的作用，并为与水相关的催化，如催化VOC燃烧、水分解、水煤气变换反应和腐蚀等提供方向。
A small amount of water can enhance the catalytic combustion activity of volatile organic compounds (VOCs) on transition metal oxides (TMOs), but its intrinsic mechanism is still controversial. Herein, we systematically demonstrate that water molecules can constantly activate lattice oxygen of transition metal oxides to form hydroxyl species theoretically and experimentally. The oxygen atoms of the generated hydroxyl species possess a weak bonding strength with circumjacent metal atoms to easily escape from the surface and attack electron-deficient carbon atoms of VOCs due to their comparatively stronger nucleophilicity, leaving abundant oxygen vacancies as the active sites for subsequent molecular oxygen activation. This work helps us deeply understand the role of water in lattice oxygen activation of transition metal oxides and provides direction for water-related catalysis, such as catalytic VOC combustion, water splitting, water-gas shift reactions, and corrosion.