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表面硫酸化在介导镍改性二氧化铈催化剂的酸度和氧化能力以催化消除有机氯化物中的作用。

The role of surface sulfation in mediating the acidity and oxidation ability of nickel modified ceria catalyst for the catalytic elimination of chlorinated organics.

作者信息

Wang Xinwei, Jiang Weiyu, Yin Rongqiang, Sun Pengfei, Lu Yunhao, Wu Zhongbiao, Weng Xiaole

机构信息

State Key Laboratory of Silicon Materials and School of Materials Science and Engineering and College of Environmental and Resource Sciences, Zhejiang University, 310058 Hangzhou, PR China.

Zhejiang Province Key Laboratory of Quantum Technology and Device, Department of Physics, Zhejiang University, 310027 Hangzhou, PR China.

出版信息

J Colloid Interface Sci. 2020 Aug 15;574:251-259. doi: 10.1016/j.jcis.2020.04.047. Epub 2020 Apr 14.

DOI:10.1016/j.jcis.2020.04.047
PMID:32330751
Abstract

Surface sulfation has shown to be an effective way in modifying the acidity and oxygen mobility of metal oxide catalysts. Both of the properties were crucial in the catalytic elimination of chlorinated organics from industrial source of emission. Herein, sulfation of a dry-mixed NiO/CeO catalyst was conducted. The catalyst was subsequently utilized for eliminating chlorobenzene (CB) under a simulated realistic condition. A range of analytical techniques, including XRD, XPS, in situ DRIFT and NH-DRIFT were employed to elucidate the sulfation effect on the physiochemical property and reaction activity of NiO/CeO. Enhanced Lewis acidity and enriched surface oxygen vacancies originating from the interaction of sulfates and metal ions were observed, which led to improved conversion efficiency and CO (CO + CO) selectivity in CB oxidation. In particular, qualitative analyses of reaction byproducts in the off-gas indicated that sulfation modification did not cause severe electrophilic chlorination of NiO/CeO, and resulted in limited production of polychlorinated byproducts and less secondary pollution of the catalyst.

摘要

表面硫酸化已被证明是一种改变金属氧化物催化剂酸度和氧迁移率的有效方法。这两种性质对于从工业排放源催化消除氯代有机物至关重要。在此,对干混NiO/CeO催化剂进行了硫酸化处理。随后将该催化剂用于在模拟实际条件下消除氯苯(CB)。采用了一系列分析技术,包括XRD、XPS、原位DRIFT和NH-DRIFT,以阐明硫酸化对NiO/CeO的物理化学性质和反应活性的影响。观察到由于硫酸盐与金属离子的相互作用而增强的路易斯酸度和富集的表面氧空位,这导致了CB氧化中转化效率和CO(CO + CO)选择性的提高。特别是,对废气中反应副产物的定性分析表明,硫酸化改性不会导致NiO/CeO发生严重的亲电氯化反应,并且多氯代副产物的产生有限,催化剂的二次污染较少。

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