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作 者:江善良 汤颖 李畅浩 杨东晓 刘琰 赵祯霞[1] JIANG Shan-liang;TANG Ying;LI Chang-hao;YANG Dong-xiao;LIU Yan;ZHAO Zhen-xia(School of Chemistry and Chemical Engineering,Guangxi University,Nanning 530004,China)
出 处:《广西大学学报(自然科学版)》2022年第6期1651-1661,共11页Journal of Guangxi University(Natural Science Edition)
基 金:国家自然科学基金项目(22178073)。
摘 要:针对日益严重的环境污染问题,采用异质原子掺杂策略构筑富含氧空位的新型双金属锰基氧化物A-MnO_(x)(A=Fe、Ni、Ce、Co、Cu)催化剂,用于光热催化高效降解甲苯。结果表明:富含氧空位的Cu-MnO_(x)具有优异的甲苯催化降解性能,分别是原始MnO_(x)和其他A-MnO_(x)的2.65倍和1.14~1.67倍,并表现出更好的甲苯矿化效果和长期催化稳定性。基于晶体结构表征发现,异质原子能有效嵌入MnO_(x)的晶格并诱导A-MnO_(x)产生大量的晶体缺陷,有利于A-MnO_(x)暴露更多的缺陷孔隙和不饱和金属氧键。同时,A-MnO_(x)存在独特的异质原子桥连δ-MnO2/Mn3O4复合界面,能有效地提升其导电性能和氧化还原能力。光热协同机理研究表明,新型Cu-MnO_(x)的优异光热活性和结构稳定性使其成为VOCs减排领域最有前景的候选材料。In view of the increasingly serious environmental pollution problems, heteroatom doping strategy was proposed to construct novel bimetallic A-MnO_(x)(A=Fe, Ni, Ce, Co, Cu) catalysts with abundant oxygen vacancies(OV) for the effective photothermal catalytic degradation of toluene.Benefited from OV-rich structure, Cu-MnO_(x)realized 2.65 times and 1.14~1.67 times higher photothermal catalytic toluene degradation efficiency than that of MnO_(x)and other A-MnO_(x)respectively.Besides, Cu-MnO_(x)displayed better toluene mineralization and long-term catalytic stability.Based on the crystal characterization, heteroatom was well-bound to the MnO_(x)lattice and induced A-MnO_(x)to produce numerous crystal-defects, which was advantageous for the exposure of more defective pores and unsaturated metal-oxygen(M-O) bonds.Meanwhile, the unique heteroatom-bridged δ-MnO2/Mn3O4polycrystalline interface endowed A-MnO_(x)with superior electrical conductivity and excellent redox ability.The photothermal synergistic mechanism exhibited that the excellent photothermal activity and stability of the newly engineered Cu-MnO_(x)made it the most promising candidate in the field of VOCs abatement.
关 键 词:锰基氧化物 异质原子掺杂 氧空位 芳香类挥发性有机物 光热催化
分 类 号:X511[环境科学与工程—环境工程]
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