Synthesis and carbon monoxide purification performance of ZSM-5 molecular sieve Co-doped Mn/V catalytic material

IF 8.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Separation and Purification Technology Pub Date : 2024-11-07 DOI:10.1016/j.seppur.2024.130327
Gang Zhou, Hui Zhen, Yongliang Zhang, Gang Li, Xueqiang Lv, Xinyuan Zhang
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Abstract

Trackless, rubber-tired, diesel-powered vehicles are widely used in the mining industry. In recent years, the use of high-performance catalysts to remove carbon monoxide (CO) from diesel vehicle exhaust has attracted much attention. In this paper, a series of manganese-vanadium doped ZSM-5 molecular sieve catalysts were prepared by an impregnation method. The structures of the catalysts were characterized and experiments were conducted to evaluate their performance. The CO catalytic oxidation performance experiments revealed that Mn0.6-V0.4-ZSM-5 had the best performance, with a conversion rate of 97.5 % at 300 °C. The catalyst was also tested for water resistance and stability. Kinetic measurements were performed and the fitted activation energy was 22.68 kJ/mol. Characterization studies revealed that the surface defects formed by Mn and V doping provided a large number of active sites and oxygen vacancies for CO oxidation, increased the number of adsorbed oxygen species on the surface, and enhanced the redox capacity through the interaction of Mn4+ and V5+ to improve the catalytic oxidation performance of the catalyst. The adsorption configurations, adsorption energy (Ebin), and formation energy of oxygen vacancies of CO at different adsorption sites and different active fractions were calculated with density functional theory. The Ebin of CO on Mn2V2O7, the active fraction of Mn0.6-V0.4-ZSM-5, was −1.29 eV, which was the most stable adsorption configuration. This configuration had good oxygen mobility, and was conducive to CO catalysis, confirming the characterization and performance experiments.
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ZSM-5 分子筛 Co 掺杂 Mn/V 催化材料的合成及一氧化碳净化性能
采矿业广泛使用无轨橡胶轮胎柴油动力车辆。近年来,使用高性能催化剂去除柴油车尾气中的一氧化碳(CO)备受关注。本文采用浸渍法制备了一系列掺杂锰钒的 ZSM-5 分子筛催化剂。对催化剂的结构进行了表征,并通过实验对其性能进行了评估。一氧化碳催化氧化性能实验表明,Mn0.6-V0.4-ZSM-5 的性能最好,在 300 °C 时的转化率为 97.5%。此外,还对催化剂的耐水性和稳定性进行了测试。进行了动力学测量,拟合活化能为 22.68 kJ/mol。表征研究表明,Mn 和 V 掺杂形成的表面缺陷为 CO 氧化提供了大量的活性位点和氧空位,增加了表面吸附氧物种的数量,并通过 Mn4+ 和 V5+ 的相互作用增强了氧化还原能力,从而提高了催化剂的催化氧化性能。利用密度泛函理论计算了 CO 在不同吸附位点和不同活性组分上的吸附构型、吸附能(Ebin)和氧空位的形成能。CO 在 Mn2V2O7(Mn0.6-V0.4-ZSM-5 的活性组分)上的 Ebin 为-1.29 eV,是最稳定的吸附构型。这种构型具有良好的氧气流动性,有利于 CO 催化,证实了表征和性能实验结果。
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来源期刊
Separation and Purification Technology
Separation and Purification Technology 工程技术-工程:化工
CiteScore
14.00
自引率
12.80%
发文量
2347
审稿时长
43 days
期刊介绍: Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.
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