Zheng Xiaohai, Zhang Guanqing, Yao Zheng, Zheng Yong, Shen Lijuan, Liu Fujian, Cao Yanning, Liang Shijing, Xiao Yihong, Jiang Lilong
National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, Fujian 350002, PR China.
National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, Fujian 350002, PR China; Fujian Key Laboratory of Pollution Control & Resource Reuse, College of Environmental Science and Engineering, Fujian Normal University, Fuzhou, Fujian 350007, PR China.
J Hazard Mater. 2021 Jun 5;411:125180. doi: 10.1016/j.jhazmat.2021.125180. Epub 2021 Jan 19.
In the present work, we report a facile oxalate-derived hydrothermal method to fabricate α-, β- and δ-MnO catalysts with hierarchically porous structure and study the phase-dependent behavior for selective oxidation of HS over MnO catalysts. It was disclosed that the oxygen vacancy, reducibility and acid property of MnO are essentially determined by the crystalline phase. Systematic experiments demonstrate that δ-MnO is superior in active oxygen species, activation energy and HS adsorption capacity among the prepared catalysts. As a consequence, δ-MnO nanosphere with a hierarchically porous structure shows high activity and stability with almost 100% HS conversion and sulfur selectivity at 210 °C, better than majority of reported Mn-based materials. Meanwhile, hierarchically porous structure of δ-MnO nanosphere alleviates the generation of by-product SO and sulfate, promoting the adoptability of Mn-based catalysts in industrial applications.
在本工作中，我们报道了一种简便的草酸盐衍生水热法来制备具有分级多孔结构的α-、β-和δ-MnO催化剂，并研究MnO催化剂上HS选择性氧化的相依赖行为。结果表明，MnO的氧空位、还原性和酸性本质上由晶相决定。系统实验表明，在制备的催化剂中，δ-MnO在活性氧物种、活化能和HS吸附容量方面表现优异。因此，具有分级多孔结构的δ-MnO纳米球在210℃时表现出高活性和稳定性，HS转化率几乎达到100%，硫选择性良好，优于大多数已报道的锰基材料。同时，δ-MnO纳米球的分级多孔结构减轻了副产物SO和硫酸盐的生成，促进了锰基催化剂在工业应用中的适用性。
