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研究 Cr-Mn 氧化物共改性柱状活性炭对甲苯和 Hg 去除性能的增强作用。

Investigation into enhanced performance of toluene and Hg stimulative abatement over Cr-Mn oxides co-modified columnar activated coke.

机构信息

School of Resources Environment and Safety Engineering, University of South China, Hengyang 421001, China; National & Local Joint Engineering Research Center for Airborne Pollutants Control and Radioactivity Protection in Buildings, Hengyang 421001, China; Key Laboratory of Prefabricated Building Energy Saving Technology of Hunan Province, Hengyang 421001, China.

School of Resources Environment and Safety Engineering, University of South China, Hengyang 421001, China; National & Local Joint Engineering Research Center for Airborne Pollutants Control and Radioactivity Protection in Buildings, Hengyang 421001, China; Key Laboratory of Prefabricated Building Energy Saving Technology of Hunan Province, Hengyang 421001, China; College of Environmental Science and Engineering, Hunan University, Changsha 410082, China.

出版信息

J Environ Sci (China). 2025 Feb;148:88-106. doi: 10.1016/j.jes.2023.09.011. Epub 2023 Sep 18.

Abstract

In this study, a string of Cr-Mn co-modified activated coke catalysts (XCrMn/AC) were prepared to investigate toluene and Hg removal performance. Multifarious characterizations including XRD, TEM, SEM, in situ DRIFTS, BET, XPS and H-TPR showed that 4%CrMn/AC had excellent physicochemical properties and exhibited the best toluene and Hg removal efficiency at 200℃. By varying the experimental gas components and conditions, it was found that too large weight hourly space velocity would reduce the removal efficiency of toluene and Hg. Although O promoted the abatement of toluene and Hg, the inhibitory role of HO and SO offset the promoting effect of O to some extent. Toluene significantly inhibited Hg removal, resulting from that toluene was present at concentrations orders of magnitude greater than mercury's or the catalyst was more prone to adsorb toluene, while Hg almost exerted non-existent influence on toluene elimination. The mechanistic analysis showed that the forms of toluene and Hg removal included both adsorption and oxidation, where the high-valent metal cations and oxygen vacancy clusters promoted the redox cycle of Cr + Mn/Mn ↔ Cr + Mn, which facilitated the conversion and replenishment of reactive oxygen species in the oxidation process, and even the CrMnO spinel structure could provide a larger catalytic interface, thus enhancing the adsorption/oxidation of toluene and Hg. Therefore, its excellent physicochemical properties make it a cost-effective potential industrial catalyst with outstanding synergistic toluene and Hg removal performance and preeminent resistance to HO and SO.

摘要

在这项研究中,制备了一系列 Cr-Mn 共改性的活性炭催化剂 (XCrMn/AC),以研究甲苯和 Hg 的去除性能。多种表征手段,包括 XRD、TEM、SEM、原位 DRIFTS、BET、XPS 和 H-TPR 表明,4%CrMn/AC 具有优异的物理化学性质,在 200℃时表现出最佳的甲苯和 Hg 去除效率。通过改变实验气体成分和条件,发现太大的重量空速会降低甲苯和 Hg 的去除效率。尽管 O 促进了甲苯和 Hg 的去除,但 HO 和 SO 的抑制作用在一定程度上抵消了 O 的促进作用。甲苯显著抑制了 Hg 的去除,这是因为甲苯的浓度比汞的浓度高几个数量级,或者催化剂更容易吸附甲苯,而 Hg 对甲苯的去除几乎没有影响。机理分析表明,甲苯和 Hg 的去除形式包括吸附和氧化,其中高价金属阳离子和氧空位簇促进了 Cr + Mn/Mn↔Cr + Mn 的氧化还原循环,这有利于氧化过程中活性氧物种的转化和补充,甚至 CrMnO 尖晶石结构可以提供更大的催化界面,从而增强甲苯和 Hg 的吸附/氧化。因此,其优异的物理化学性质使其成为一种具有成本效益的潜在工业催化剂,具有出色的协同甲苯和 Hg 去除性能以及对 HO 和 SO 的优异抗性。

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