Preparation of RuCeTi catalyst and catalytic oxidation of chlorobenzene
WANG Meng-xue, CHEN Xi, JIA Zi-liang, Li Shu-ning, LIANG Mei-sheng
Shanxi Key Laboratory of Compound Air Pollutions Identification and Control, College of Environmental Science and Engineering, Taiyuan University of Technology, Jinzhong 030600, China
摘要 In this paper, a catalyst support (CeTi) with abundant strong acidic sites was prepared by sol-gel method, and Ru was loaded on to form a RuCeTi catalyst by chemical reduction process using a certain reductant. And that was used for the catalytic oxidation of chlorobenzene (CB). With the help of characterizations like XRD, HRTEM, XPS, H2-TPR, and in-situ DRIFTS, it showed that the interaction between Ru and CeO2 increased the valence state of Ru species, leading to the promotion of redox ability of RuO2 and the deep oxidation of chlorobenzene. Further the abundant strong acidic sites of the CeTi support provided the adsorption sites for CB. The activity tests showed that the CO2 selectivity and durability of RuCeTi were significantly enhanced, with a 98% of selectivity and 24h on-stream test at 1000×10-6 of CB concentration without deactivation. And that could be derived from the synergistic combination of reactive oxygen species and acidic sites.
Abstract:In this paper, a catalyst support (CeTi) with abundant strong acidic sites was prepared by sol-gel method, and Ru was loaded on to form a RuCeTi catalyst by chemical reduction process using a certain reductant. And that was used for the catalytic oxidation of chlorobenzene (CB). With the help of characterizations like XRD, HRTEM, XPS, H2-TPR, and in-situ DRIFTS, it showed that the interaction between Ru and CeO2 increased the valence state of Ru species, leading to the promotion of redox ability of RuO2 and the deep oxidation of chlorobenzene. Further the abundant strong acidic sites of the CeTi support provided the adsorption sites for CB. The activity tests showed that the CO2 selectivity and durability of RuCeTi were significantly enhanced, with a 98% of selectivity and 24h on-stream test at 1000×10-6 of CB concentration without deactivation. And that could be derived from the synergistic combination of reactive oxygen species and acidic sites.
[1] Jia Q H, Xing Y, Zhang G L, et al. Progress of catalytic oxidation of typical chlorined volatile organic compounds (CVOCs): a review [J]. Science of The Total Environment, 2023,865. DOI:10.1016/j.scitotenv. 2022.161063. [2] Jiang Q, Chen B S, Xu J Z. Development and application of catalysts for catalytic ozonation of Cl-VOCs at low temperature: a comprehensive review [J]. Separation and Purification Technology, 2024,333. DOI: 10.1016/j.seppur.2023.125882. [3] Luo N, Gao Y F, Chen D, et al. Research advances in chlorinated benzene-containing compound oxidation catalyzed by metal oxides: activity-enhanced strategies and reaction-facilitated mechanisms [J]. Nanoscale, 2023,15:12157-12174. [4] Chen X, Jia L Z, Liu H Z, et al. Strong metal-support interactions between atomically dispersed Ru and CrOx for improved durability of chlorobenzene oxidation [J]. RSC Advances, 2023,13:3255-3264. [5] Wang Y, Du C, Liu Z, et al. Highly active and durable chlorobenzene oxidation catalyst via porous atomic layer coating of Ru on Pt/Al2O3 [J]. Applied Catalysis B: Environmental, 2023,330.DOI:10.1016/j. apcatb.2023.122648. [6] Kim H, Kim H J, Kim J H, et al. Noble-metal-based catalytic oxidation technology trends for volatile organic compound (VOC) Removal [J]. Catalysts, 2022,12(1):63. [7] Liu L X, Chen L, Zhu Y T, et al. Catalytic oxidation of chlorobenzene over noble metals (Pd, Pt, Ru, Rh) and the distributions of polychlorinated by-products [J]. Journal of Hazardous Materials, 2019,363:90-98. [8] Sun H B, Li Q Q, Su J G, et al. Insights into chlorobenzene catalytic oxidation over noble metal loading {001}-TiO2: the role of NaBH4 and subnanometer Ru undergoing stable Ru0↔Ru4+ circulation [J]. Environmental Science & Technology, 2022,56:16292-16302. [9] Gannoun C, Ghorbel A, Gaigneaux E M. Influence of zirconia addition in TiO2 and TiO2-CeO2aerogels on the textural, structural and catalytic properties of supported vanadia in chlorobenzene oxidation [J]. RSC Advances, 2022,12:10924-10932. [10] Dai G Q, Bai X S, Wang Y X, et al. Catalytic combustion of chlorobenzene over Ru-doped ceria catalysts: mechanism study [J]. Applied Catalysis B: Environmental, 2013,129:580-588. [11] Dai G Q, Bai X S, Wang Y Z, et al. Catalytic combustion of chlorobenzene over Ru-doped ceria catalysts [J]. Applied Catalysis B: Environmental, 2012,126:64-75. [12] Lin W F, Zhang M Z, Li N, et al. How to achieve complete elimination of Cl-VOCs: a critical review on byproducts formation and inhibition strategies during catalytic oxidation [J]. Chemical Engineering Journal, 2021,404. DOI: 10.1016/j.cej.2020.126534. [13] Wang J, Liu L X, Zeng L J, et al. Catalytic oxidation of trichloroethylene over TiO2 supported ruthenium catalysts [J]. Catalysis Communications, 2016,76:13-18. [14] Wang J, Zhao N H, Liu L X, et al. Study on the catalytic properties of Ru/TiO2 catalysts for the catalytic oxidation of (chloro)-aromatics [J]. Catalysis Letters, 2019,149:2004-2014. [15] Ye M, Chen L, Liu L X, et al. Catalytic oxidation of chlorobenzene over Ruthenium-Ceria bimetallic catalysts [J]. Catalysts, 2018,8:116. [16] Dai G Q, Bai X S, Wang W J, et al. The effect of TiO2 doping on catalytic performances of Ru/CeO2 catalysts during catalytic combustion of chlorobenzene [J]. Applied Catalysis B: Environmental, 2013,142-143:222-233. [17] Huang H, Dai G Q, Wang Y X. Morphology effect of Ru/CeO2 catalysts for the catalytic combustion of chlorobenzene [J]. Applied Catalysis B: Environmental, 2014,158-159:96-105. [18] Qin X X, Chen Y X, Chen M, et al. Highly efficient Ru/CeO2 catalysts for formaldehyde oxidation at low temperature and the mechanistic study [J]. Catalysis Science & Technology, 2021,11:1914-1921. [19] Shi J Y, Wang L J, Zhou X R. Pt-support interaction and nanoparticle size effect in Pt/CeO2-TiO2 catalysts for low temperature VOCs removal [J]. Chemosphere, 2021,265.DOI:10.1016/j.chemosphere. 2020.129127. [20] Zheng K, Li F Y, Liu B, et al. Ti-doped CeO2 stabilized single-atom rhodium catalyst for selective and stable CO2 hydrogenation to ethanol [J]. Angewandte Chemie International Edition, 2022,61.DOI:10.1002/anie.202210991. [21] Yang P, Yang S S, Shi N Z, et al. Deep oxidation of chlorinated VOCs over CeO2-based transition metal mixed oxide catalysts [J]. Applied Catalysis B: Environmental, 2015,162:227-235. [22] Santara B, Giri P K, Imakita K, et al. Evidence of oxygen vacancy induced room temperature ferromagnetism in solvothermally synthesized undoped TiO2 nanoribbons [J]. Nanoscale, 2013,5.DOI: 10.1039/c3nr00799e. [23] Deng W, Dai G Q, Lao J Y, et al. Low temperature catalytic combustion of 1,2-dichlorobenzene over CeO2-TiO2 mixed oxide catalysts [J]. Applied Catalysis B: Environmental, 2016,181:848-861. [24] Sun X X, Yang Sh, Liu X, et al. The enhancement of benzene total oxidation over RuxCeO2 catalysts at low temperature: the significance of Ru incorporation [J]. Science of The Total Environment, 2023,902. DOI: 10.1016/j.scitotenv.2023.165574. [25] 徐达功,思 涵,黄 琼,等.过渡金属改性的Cr-Ce-O催化剂氧化氯苯性能 [J]. 中国环境科学, 2021,41(7):3184-3192. Xu D G, Si H, Huang Q, et al. Catalytic oxidation of chlorobenzene over Cr-Ce-O catalysts modified by transition metals [J]. China Environmental Science, 2021,41(7):3184-3192. [26] 文佳鑫.高活性钌催化剂的制备及其催化氧化氯代芳烃性能研究 [D]. 天津:河北工业大学, 2021. Wen X J. Study on the preparation and catalytic performance of high-activity ruthenium fod chlorinated aromatic hydrocarbons oxidation [D]. Tianjin: Hebei University of Technology, 2021. [27] Ilaria L, Albert C, Jordi Llorca. Catalytic ammonia decomposition for hydrogen production on Ni, Ru and Ni-Ru supported on CeO2[J]. ScienceDirect, 2019,44:12693-12707. [28] Morgan D J. Resolving ruthenium: XPS studies of common ruthenium materials [J]. Surface and Interface Analysis, 2015,47:1072-1079. [29] Liang J W, Zhu X Y, Ren D S, et al. Catalytic combustion of chlorobenzene at low temperature over Ru-Ce/TiO2: high activity and high selectivity [J]. Applied Catalysis A: General, 2021,623. DOI: 10.1016/j.apcata.2021.118257. [30] Yang P, Zuo F S, Shi N Z, et al. Elimination of 1,2-dichloroethane over (Ce,Cr)xO2/MOy catalysts (M = Ti, V, Nb, Mo, W and La) [J]. Applied Catalysis B: Environmental, 2016,191:53-61. [31] Yang P, Zuo F S, Zhou X R. Synergistic catalytic effect of (Ce,Cr)xO2 and HZSM-5 for elimination of chlorinated organic pollutants [J]. Chemical Engineering Journal, 2017,323:160-170. [32] Li B G, Wang L, Wen Y C, et al. Deep insight into the catalytic removal mechanism of a multi-active center catalyst for chlorobenzene: an experiment and density functional theory study [J]. Catalysis Science & Technology, 2020,10:6879-6891. [33] Cao X K, Dai X X, Wu B Z, et al. Unveiling the importance of reactant mass transfer in environmental catalysis: taking catalytic chlorobenzene oxidation as an example [J]. Chinese Chemical Letters, 2021,32:1206-1209. [34] Sun F P, Wang L W, Dai X X, et al. Mechanism study on catalytic oxidation of chlorobenzene over MnxCe1-xO2/H-ZSM5catalysts under dry and humid conditions [J]. Applied Catalysis B: Environmental, 2016,198:389-397.