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Defect engineering over Co3O4 catalyst for surface lattice oxygen activation and boosted propane total oxidation
Journal of Catalysis ( IF 7.3 ) Pub Date : 2022-06-20 , DOI: 10.1016/j.jcat.2022.06.024
Wenjun Zhu, Xing-bao Wang, Chuang Li, Xiao Chen, Wen-ying Li, Zhongmin Liu, Changhai Liang

Developing efficient and stable catalyst is crucial for the catalytic removal of volatile organic compounds (VOCs). Herein, we report an effective and versatile surface defect engineering for regulation of surface lattice oxygen species in Co3O4 catalyst by alkaline-earth metal doping-etching strategy. The as-synthesized Ca-Co3O4-Ac exhibited remarkable catalytic activity and stability in propane oxidation, with high propane oxidation rate (5.65 × 10−7 mol g−1 s−1) and turnover frequency (TOF, 2.12 × 10−3 s−1) at 210 °C. Simultaneously, the doping-etching strategy could increase the specific surface area, low-temperature reducibility, and oxygen mobility of Co3O4 catalyst. In addition, in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS), density function theory (DFT) calculation, and propane temperature-programmed desorption/surface reaction (C3H8-TPD/TPSR) further revealed that active lattice oxygen species induced by doping-etching strategy promoted the propane activation on the catalyst surface. This work offers a deeper understanding of the reactive oxygen species and provides a feasible strategy for the design of efficient catalysts for practical VOCs removal.



中文翻译:

用于表面晶格氧活化和促进丙烷全氧化的 Co3O4 催化剂的缺陷工程

开发高效稳定的催化剂对于催化去除挥发性有机化合物(VOCs)至关重要。在此,我们报告了一种有效且通用的表面缺陷工程,用于通过碱土金属掺杂蚀刻策略调节 Co 3 O 4催化剂中的表面晶格氧物种。合成后的 Ca-Co 3 O 4 -Ac 在丙烷氧化中表现出显着的催化活性和稳定性,丙烷氧化速率高(5.65 × 10 -7 mol g -1 s -1)和周转频率(TOF,2.12 × 10 -3-1) 在 210 °C。同时,掺杂蚀刻策略可以提高Co 3 O 4催化剂的比表面积、低温还原性和氧迁移率。此外,原位漫反射红外傅里叶变换光谱(in situ DRIFTS)、密度函数理论(DFT)计算和丙烷程序升温脱附/表面反应(C 3 H 8 -TPD/TPSR)进一步揭示了活性晶格氧掺杂蚀刻策略诱导的物种促进了催化剂表面的丙烷活化。这项工作提供了对活性氧的更深入了解,并为设计用于实际 VOCs 去除的高效催化剂提供了可行的策略。

更新日期:2022-06-25
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