Bi Fukun, Wei Jiafeng, Zhou Zhuoxuan, Zhang Yaofei, Gao Bin, Liu Ning, Xu Jingcheng, Liu Baolin, Huang Yuandong, Zhang Xiaodong
School of Environment and Architecture, University of Shanghai for Science and Technology, Shanghai 200093, China.
School of Health Science and Engineering, University of Shanghai for Science and Technology, Shanghai 200093, China.
JACS Au. 2025 Jan 8;5(1):363-380. doi: 10.1021/jacsau.4c01146. eCollection 2025 Jan 27.
The synthesis of high-performance catalysts for volatile organic compounds (VOCs) degradation under humid conditions is essential for their practical industrial application. Herein, a codoping strategy was adopted to synthesize the N-CoO-C catalyst with N, C codoping for low-temperature ethyl acetate (EA) degradation under humid conditions. Results showed that N-CoO-C exhibited great catalytic activity ( = 177 °C) and water resistance (5.0 vol% HO, = 178 °C) for EA degradation. Characterization results suggested that the C, N codoping weakened the Co-O bond strength, increased surface Co and O species, and improved the low-temperature redox ability and the mobility of lattice oxygen species, which boosted the catalytic performance of N-CoO-C for EA degradation. Meanwhile, the N-doping-induced oxygen vacancies could interact with water vapor to generate extra active oxygen species, which enhanced the water resistance. Importantly, based on a series of characterization technologies, in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), and theoretical calculations, the synergistic effect of C, N codoping was systematically investigated and elucidated. The C doping induced the increase of surface area and the weakening of Co-O bond strength, which improved EA adsorption and lattice oxygen species activation to dissociate and oxidize EA, forming the key intermediate, acetate acid. N doping enhanced the adsorption and activation of gaseous oxygen species to form active oxygen species, attacking and breaking the C-C bond in acetate acid to accelerate EA deep oxidation, which synergistically facilitated EA degradation.
合成用于在潮湿条件下降解挥发性有机化合物（VOCs）的高性能催化剂对于其实际工业应用至关重要。在此，采用共掺杂策略合成了具有N、C共掺杂的N-CoO-C催化剂，用于在潮湿条件下低温降解乙酸乙酯（EA）。结果表明，N-CoO-C对EA降解表现出优异的催化活性（T90 = 177 °C）和耐水性（5.0 vol% H2O，T90 = 178 °C）。表征结果表明，C、N共掺杂削弱了Co-O键强度，增加了表面Co和O物种，提高了低温氧化还原能力和晶格氧物种的迁移率，从而提高了N-CoO-C对EA降解的催化性能。同时，N掺杂诱导的氧空位可与水蒸气相互作用产生额外的活性氧物种，增强了耐水性。重要的是，基于一系列表征技术、原位漫反射红外傅里叶变换光谱（DRIFTS）和理论计算，系统地研究和阐明了C、N共掺杂的协同效应。C掺杂导致表面积增加和Co-O键强度减弱，改善了EA吸附和晶格氧物种活化，使EA解离和氧化，形成关键中间体乙酸。N掺杂增强了气态氧物种的吸附和活化以形成活性氧物种，攻击并断裂乙酸中的C-C键以加速EA深度氧化，协同促进了EA降解。
