Effect of transition metal oxide doping on catalytic activity of titania for the oxidation of 1,2-dichloroethane

Effect of transition metal oxide doping on catalytic activity of titania for the oxidation of 1,2-dichloroethane
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过渡金属氧化物掺杂对二氧化钛催化1,2-二氯乙烷氧化活性的影响

DOI:
10.1016/j.cattod.2019.12.011
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发表时间:
2019-12
期刊:
影响因子:
5.3
通讯作者:
Hongxing Dai
Hongxing Dai
中科院分区:
化学2区
文献类型:
--
作者:
Xing Zhang;Yuxi Liu;Jiguang Deng;Lin Jing;Xiaohui Yu;Zhuo Han;Hongxing Dai

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采用共沉淀法制备了过渡金属氧化物(MOx;M = Cr、Mn、Fe、Ni、Cu)掺杂二氧化钛固溶体催化剂(10wt% MOx-TiO2,记为10MOx-TiO2)。采用 XRD、TPR、TPD、XPS、TPSR 和原位 DRIFTS 技术表征材料的理化性质,并评价其对 1,2-二氯乙烷(1,2-DCE)氧化的催化活性。 MOx的引入增强了氧分子的吸附和活化、表面晶格氧的迁移性和低温还原性。 10MOx-TiO2催化剂表现出良好的性能,其中10CrOx-TiO2表现出最高的催化活性(反应速率 = 2.35 × 10−7mol/(gcats)和表观活化能(Ea)=35 kJ/mol,空速 = 40,000 mL/(g·h))和良好的耐腐蚀性基于TPSR和原位DRIFTS表征的结果,还讨论了10CrOx-TiO2上1,2-DCE氧化的机理。结论是强酸性和氧化还原能力、高吸附氧浓度以及TiO2和CrOx之间的强相互作用是10CrOx-TiO2具有良好性能的原因。
Transition metal oxides (MOx; M = Cr, Mn, Fe, Ni, Cu)-doped titania solid solution catalysts (10 wt% MOx–TiO2, denoted as 10MOx–TiO2) were prepared by the coprecipitation method. The techniques of XRD, TPR, TPD, XPS, TPSR, and in situ DRIFTS were used to characterize physicochemical properties of the materials, and their catalytic activities were evaluated for the oxidation of 1,2-dichloroethane (1,2-DCE). The introduction of MOxenhanced adsorption and activation of oxygen molecules, mobility of surface lattice oxygen, and low-temperature reducibility. The 10MOx–TiO2catalysts showed good performance, with 10CrOx–TiO2exhibiting the highest catalytic activity (reaction rate = 2.35 × 10−7mol/(gcats) and apparent activation energy (Ea) =35 kJ/mol at space velocity = 40,000 mL/(g h)) and good resistance to chlorine poisoning, The mechanism of 1,2-DCE oxidation over 10CrOx–TiO2was also discussed based on the results of TPSR and in situ DRIFTS characterization. It is concluded that strong acidity and redox ability, high adsorbed oxygen species concentration, and strong interaction between TiO2and CrOxwere accountable for the good performance of 10CrOx–TiO2.
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