螯合剂对MnCr2O4尖晶石催化剂选择性催化还原活性的影响及其机理

IF 4.5 3区 工程技术 Q2 ENGINEERING, CHEMICAL
Fenghe Sheng, De Fang, Sensheng Hou, Feng He, Junlin Xie
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引用次数: 0

摘要

选用四乙酸乙二胺、柠檬酸、葡萄糖、蔗糖4种不同的螯合剂,采用溶胶-凝胶法制备尖晶石结构的MnCr2O4催化剂。在所制备的催化剂中,比表面积最大的MnCr2O4-S-700表现出最好的催化性能,其T80温度窗为200-260℃,220℃时脱硝率高达91.6%。氢温度程序还原、氨温度程序解吸和x射线光电子能谱分析结果表明,MnCr2O4-S-700具有更多的化学吸附氧Oα以及活性位点(Mn3+ + Mn4+)和(Cr3+ + Cr5+),从而提高了MnCr2O4-S-700的酸性和氧化还原能力。Mn和Cr元素之间存在丰富的电子转移(Cr5+ + Mn3+→Cr3+ + Mn4+),增强了催化剂的氧化还原能力。根据原位漫反射红外变换光谱,MnCr2O4-S-700催化剂不仅遵循Langmuir-Hinshelwood机理,而且遵循Eley-Rideal机理。研究了螯合剂在尖晶石催化剂上与NH3的络合作用机理。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Effect of chelating agents on selective catalytic reduction activity and mechanism for MnCr2O4 spinel catalyst

Four different chelating agents, ethylenediamine tetraacetic acid, citric acid, glucose, and sucrose, were selected to synthesize MnCr2O4 catalysts (spinel structure) with sol-gel method. Among the prepared catalysts, MnCr2O4-S-700, which had the largest specific surface area, showed the best catalytic performance, with a T80 temperature window of 200–260 °C and a denitrification rate of up to 91.6% at 220 °C. Hydrogen temperature programmed reduction, ammonia temperature programmed desorption, and X-ray photoelectron spectroscopy results showed that MnCr2O4-S-700 possessed more chemisorbed oxygen Oα as well as active sites (Mn3+ + Mn4+) and (Cr3+ + Cr5+), which improved acidity and redox capacity. There was abundant electron transfer between Mn and Cr elements (Cr5+ + Mn3+ → Cr3+ + Mn4+), enhancing the redox capacity of catalysts. According to the in situ diffuse reflectance infrared transform spectroscopy spectra, it could be concluded that the MnCr2O4-S-700 catalyst followed not only the Langmuir-Hinshelwood mechanism but also the Eley-Rideal mechanism. This work displays the effect of the complexation mechanism of chelating agents on the SCR reaction with NH3 over spinel catalysts.

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来源期刊
CiteScore
7.60
自引率
6.70%
发文量
868
审稿时长
1 months
期刊介绍: Frontiers of Chemical Science and Engineering presents the latest developments in chemical science and engineering, emphasizing emerging and multidisciplinary fields and international trends in research and development. The journal promotes communication and exchange between scientists all over the world. The contents include original reviews, research papers and short communications. Coverage includes catalysis and reaction engineering, clean energy, functional material, nanotechnology and nanoscience, biomaterials and biotechnology, particle technology and multiphase processing, separation science and technology, sustainable technologies and green processing.
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