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用于羰基硫和二硫化碳同时催化水解的金属氧化物负载活性炭纤维催化剂的表面特性。

Surface characterization of metal oxides-supported activated carbon fiber catalysts for simultaneous catalytic hydrolysis of carbonyl sulfide and carbon disulfide.

机构信息

Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming 650500, China.

Faculty of Chemical Engineering, Kunming University of Science and Technology, Kunming 650500, China.

出版信息

J Environ Sci (China). 2020 Oct;96:44-54. doi: 10.1016/j.jes.2020.03.019. Epub 2020 May 5.

Abstract

The sol-gel method was used to synthesize a series of metal oxides-supported activated carbon fiber (ACF) and the simultaneous catalytic hydrolysis activity of carbonyl sulfide (COS) and carbon disulfide (CS) at relatively low temperatures of 60°C was tested. The effects of preparation conditions on the catalyst properties were investigated, including the kinds and amount of metal oxides and calcination temperatures. The activity tests indicated that catalysts with 5 wt.% Ni after calcining at 400°C (Ni(5)/ACF(400)) had the best performance for the simultaneous catalytic hydrolysis of COS and CS. The surface and structure properties of prepared ACF were characterized by scanning electron microscope-energy disperse spectroscopy (SEM-EDS), Brunauer-Emmett-Teller (BET), X-ray diffraction (XRD), carbon dioxide-temperature programmed desorption (CO-TPD) and diffuse reflectance Fourier transform infrared reflection (DRFTIR). And the metal cation defects were researched by electron paramagnetic resonance (EPR) method. The characterization results showed that the supporting of Ni on the ACF made the ACF catalyst show alkaline and increased the specific surface area and the number of micropores, then improved catalytic hydrolysis activity. The DRFTIR results revealed that -OH species could facilitate the hydrolysis of COS and CS; -COO and -C-O species could facilitate the oxidation of catalytic hydrolysate HS. And the EPR results showed that high calcination temperature conditions provide more active reaction center for the COS and CS adsorption.

摘要

采用溶胶-凝胶法合成了一系列金属氧化物负载的活性炭纤维(ACF),并在相对较低的 60°C 温度下测试了羰基硫(COS)和二硫化碳(CS)的同时催化水解活性。考察了制备条件对催化剂性能的影响,包括金属氧化物的种类和用量以及煅烧温度。活性测试表明,在 400°C 下煅烧的 5wt%Ni 的催化剂(Ni(5)/ACF(400))对 COS 和 CS 的同时催化水解具有最佳性能。采用扫描电子显微镜-能谱(SEM-EDS)、比表面积测试(BET)、X 射线衍射(XRD)、二氧化碳程序升温脱附(CO-TPD)和漫反射傅里叶变换红外反射(DRFTIR)对制备的 ACF 的表面和结构性质进行了表征。采用电子顺磁共振(EPR)方法研究了金属阳离子缺陷。表征结果表明,Ni 负载在 ACF 上使 ACF 催化剂呈碱性,并增加了比表面积和微孔数量,从而提高了催化水解活性。DRFTIR 结果表明,-OH 物种可以促进 COS 和 CS 的水解;-COO 和 -C-O 物种可以促进催化水解产物 HS 的氧化。EPR 结果表明,高温煅烧条件为 COS 和 CS 的吸附提供了更多的活性反应中心。

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