Lu Tonglu, Zhang Chunxia, Du Fangyuan, Zhang Changsen, Zhang Ruiqin, Liu Panpan, Li Juexiu
School of Ecology & Environment, Zhengzhou University, Zhengzhou 450001, China.
School of Ecology & Environment, Zhengzhou University, Zhengzhou 450001, China.
J Colloid Interface Sci. 2023 Jul;641:791-802. doi: 10.1016/j.jcis.2023.03.103. Epub 2023 Mar 21.
Advancing the practical application of catalytic oxidation technology demands for illustrating the synchronous conversion behavior of various volatile organic compounds (VOCs) over catalysts. Here, the mutual effects of benzene, toluene and xylene (BTX) were examined for their synchronous conversion on the surface of the MnO nanowire. Competitive adsorption of xylene (absorption energy (E): -0.889 eV) facilitated its prior conversion and impeded the oxidization of toluene and benzene over the catalyst. The turnover frequencies were 0.52 min (benzene), 0.90 min (toluene) and 2.42 min (xylene) for mixed BTX conversion over the MnO. Doping MnO with K, Na and Ca could enhance its ability to oxidize the individual VOCs but did not alter the conversion mechanism of mixed BTX over the catalyst. When reducing the competitive effects in the adsorption of BTX, the oxidation performance of catalysts would depend on their ability to oxidize toluene and benzene. K-MnO showed superior properties, i.e. specific surface area, highly low-valent Mn species, high lattice oxygen content, and abundant oxygen vacancy, and then exhibited superior performance during long-term operation (90% conversion in 800 min). The present study uncovered the co-conversion mechanism of multiple VOCs and significantly leveraged the catalytic oxidization technology for VOCs removal in practical application.
推进催化氧化技术的实际应用需要阐明各种挥发性有机化合物(VOCs)在催化剂上的同步转化行为。在此,研究了苯、甲苯和二甲苯(BTX)在MnO纳米线表面同步转化时的相互影响。二甲苯的竞争性吸附(吸附能(E):-0.889 eV)促进了其优先转化,并阻碍了甲苯和苯在催化剂上的氧化。在MnO上进行混合BTX转化时,周转频率分别为苯0.52 min⁻¹、甲苯0.90 min⁻¹和二甲苯2.42 min⁻¹。用K、Na和Ca掺杂MnO可以提高其氧化单个VOCs的能力,但不会改变混合BTX在催化剂上的转化机理。当减少BTX吸附中的竞争效应时,催化剂的氧化性能将取决于其氧化甲苯和苯的能力。K-MnO表现出优异的性能,即比表面积、高比例的低价态Mn物种、高晶格氧含量和丰富的氧空位,因此在长期运行中表现出优异的性能(800分钟内转化率达到90%)。本研究揭示了多种VOCs的共转化机理,并在实际应用中显著推动了用于去除VOCs的催化氧化技术。