介孔锰-钴-钛对邻二甲苯降解的催化性能:实际条件下的机理研究

IF 7.2 2区 工程技术 Q1 CHEMISTRY, APPLIED
Qiqi Shi , Yujing Zhang , Xiao Zhang , Boxiong Shen , Kai Ren , Hanming Wu
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引用次数: 0

摘要

在低温条件下催化燃烧工业烟气中的挥发性有机化合物仍然是一项挑战。在此,我们采用溶热策略开发了一种用于降解邻二甲苯的介孔锰-钴-钛催化剂。优化后的 Mn0.1Co-TiO2 催化剂具有纳米花结构,比表面积为 83.1 m2/g,介孔体积为 0.1191 cm3/g。掺杂锰调节了锰和钴之间的电子相互作用,促进了 MnCo2O4.5 相的形成,增加了催化剂中 Co3+ 和 Mn4+ 的含量。Mn0.1Co-TiO2 催化剂的还原能力从 170 ℃ 提高到 644 ℃,最大 H2 消耗量为 4.56 mmol/g。Mn0.1Co-TiO2 催化剂在 193 ℃、60,000 h-1 的 GHSV 条件下实现了 50%的邻二甲苯转化率,而通过浸渍法制备的同等催化剂需要 315 ℃ 才能实现 50%的邻二甲苯转化率。在 NO 存在的情况下,生成的 NO2 加快了邻二甲苯的转化,因为它促进了更多 Mn4+-O-Co3+ 活性位点的生成以及马来酸盐和乙酸盐等中间产物的积累。NH3 和 H2O 对邻二甲苯的转化有轻微的抑制作用,但催化剂丰富的介孔和氧化还原能力减弱了这种抑制作用。SO2 气体在催化剂表面造成非活性硫酸盐和化学失活,从而导致苯醌产物的过量生成。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Catalytic performance of mesoporous Mn-Co-Ti for o-xylene degradation: Mechanistic study under practical conditions

Catalytic performance of mesoporous Mn-Co-Ti for o-xylene degradation: Mechanistic study under practical conditions

Catalytic combustion of volatile organic compounds from industrial flue gases at low temperatures remains a challenge. Herein, we developed a mesoporous Mn-Co-Ti catalyst for o-xylene degradation by a solvothermal strategy. The optimized Mn0.1Co-TiO2 catalyst possessed a nanoflower structures with a surface area of 83.1 m2/g and mesoporous volume of 0.1191 cm3/g. Mn-doping modulated the electronic interactions between Mn and Co, which promoted the formation of MnCo2O4.5 phase and increased Co3+ and Mn4+ content of the catalyst. The Mn0.1Co-TiO2 catalyst had an improved reduction capacity from 170 to 644 °C, with a maximum H2 consumption of 4.56 mmol/g. The Mn0.1Co-TiO2 catalyst achieved 50% o-xylene conversion at 193 °C at a GHSV of 60,000 h−1, whereas the equivalent catalyst prepared by impregnation required 315 °C for 50% o-xylene conversion. In the presence of NO, the generated NO2 accelerated o-xylene conversion because it promoted the generation of more Mn4+-O-Co3+ active sites and accumulation of intermediates such as maleate and acetate species. NH3 and H2O had slight inhibitory effects on o-xylene conversion, which were attenuated by abundant mesopores and redox ability of catalyst. SO2 gas caused inactive sulfates and chemical deactivation on catalyst surface, thus leading to excessive formation of benzoquinone products.

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来源期刊
Fuel Processing Technology
Fuel Processing Technology 工程技术-工程:化工
CiteScore
13.20
自引率
9.30%
发文量
398
审稿时长
26 days
期刊介绍: Fuel Processing Technology (FPT) deals with the scientific and technological aspects of converting fossil and renewable resources to clean fuels, value-added chemicals, fuel-related advanced carbon materials and by-products. In addition to the traditional non-nuclear fossil fuels, biomass and wastes, papers on the integration of renewables such as solar and wind energy and energy storage into the fuel processing processes, as well as papers on the production and conversion of non-carbon-containing fuels such as hydrogen and ammonia, are also welcome. While chemical conversion is emphasized, papers on advanced physical conversion processes are also considered for publication in FPT. Papers on the fundamental aspects of fuel structure and properties will also be considered.
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