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通过猝灭诱导钙钛矿氧化物的表面调制以提高催化氧化活性。

Quenching-induced surface modulation of perovskite oxides to boost catalytic oxidation activity.

作者信息

Wu Peng, Chen Tingyu, Jin Xiaojing, Zhao Shuaiqi, Chong Yanan, Li Yifei, Lin Jiajin, Li Anqi, Zhao Yun, Qiu Yongcai, Ye Daiqi

机构信息

Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control, School of Environment and Energy, South China University of Technology, Guangzhou 510006, China.

Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control, School of Environment and Energy, South China University of Technology, Guangzhou 510006, China; State Key Laboratory of Luminescent Materials and Devices, South China University of Technology, Guangzhou, China.

出版信息

J Hazard Mater. 2022 Jul 5;433:128765. doi: 10.1016/j.jhazmat.2022.128765. Epub 2022 Apr 4.

DOI:10.1016/j.jhazmat.2022.128765
PMID:35390616
Abstract

Quenching is a powerful method for modulating surface structures of metal oxide nanocatalysts to achieve high catalytic oxidation activities, but it is still challenging. Herein, a catalyst of ultrafine CoO nanoparticles decorated on Co-doped LaMnO (CoO/LaCoMnO) is synthesized via one-step quenching perovskite-type LaMnO nanocatalyst into an aqueous solution of cobalt nitrate, which exhibits significantly improved catalytic performance with toluene (1000 ppm) conversion of 90% at 269 °C under the gas hourly space velocity of 72000 mL g h. The high catalytic activity correlates with large surface area, abundant oxygen vacancies and good reducibility. Furthermore, density functional theory calculations disclose that Co doping and interfacial effect of CoO/LaCoMnO can achieve lower C-H bond activation energy. These findings provide a unique and effective route towards surface modification of nanocatalysts.

摘要

淬火是一种用于调节金属氧化物纳米催化剂表面结构以实现高催化氧化活性的强大方法,但它仍然具有挑战性。在此,通过将钙钛矿型LaMnO纳米催化剂一步淬火到硝酸钴水溶液中,合成了一种负载在Co掺杂的LaMnO上的超细CoO纳米颗粒催化剂(CoO/LaCoMnO),在气体时空速为72000 mL g⁻¹ h⁻¹的条件下,该催化剂在269℃时对甲苯(1000 ppm)的转化率为90%,表现出显著提高的催化性能。高催化活性与大表面积、丰富的氧空位和良好的还原性相关。此外,密度泛函理论计算表明,Co掺杂和CoO/LaCoMnO的界面效应可以实现更低的C-H键活化能。这些发现为纳米催化剂的表面改性提供了一条独特而有效的途径。

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