RuO<i><sub>x</sub></i>分散性导致的活性氧异化与氯苯氧化相关性

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Abstract TiCeO_x bimetallic catalysts were prepared as catalyst carries. And the Ru-supported catalysts with different dispersions were synthesized by the methods of Ru³⁺ impregnation reduction (bottom to up) and Ru colloid solution thermal diffusion (top to down) methods. In the catalyst RuTiCeO_x-N prepared by Ru³⁺ immersion reduction method, Ru species exist in the form of RuO_x nanoclusters. In the catalyst RuTiCeO_x-A prepared by Ru colloid solution thermal diffusion, Ru species exist in the form of single-atom dispersion. The different dispersion states of Ru species lead to the difference of active oxygen species and acid sites involved in chlorobenzene (CB) oxidation. Chemisorbed oxygen and surface lattice oxygen could be the dominating active oxygen species for RuTiCeO_x-N and RuTiCeO_x-A, respectively. And due to the chemisorption of CB, that could be transformed into hydroxyl radical (-OH) to be involved in the catalytic reaction. Catalyst RuTiCeO_x-A performed better with the complete conversion of CB at 300℃ and 24h of durability test without deactivation. That could be attributed to the synergy between its resulted active oxygen species and multiple acid sites (strong and weak).

Key words： catalyst carries noble metals clusters single-atom dispersion oxygen species hydroxyl

Received: 23 September 2024

PACS:

X511

Corresponding Authors: 梁美生,责任作者,教授,liangmeisheng@tyut.edu.cn E-mail: liangmeisheng@tyut.edu.cn

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	CHEN Xi
	JIA Zi-liang
	WANG Meng-xue
	WANG Peng
	JI Xin-tong
	QIAO Xin-ru
	GUO Dong-rui
	LIANG Mei-sheng

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CHEN Xi,JIA Zi-liang,WANG Meng-xue等. Correlation between chlorobenzene oxidation and active oxygen species induced by the dispersity of RuO_x[J]. CHINA ENVIRONMENTAL SCIENCECE, 2025, 45(4): 1820-1832.

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http://www.zghjkx.com.cn/EN/ OR http://www.zghjkx.com.cn/EN/Y2025/V45/I4/1820

[1] 徐功达,司涵,黄琼,等.过渡金属改性的Cr-Ce-O催化剂氧化CB性能[J].中国环境科学, 2021,41(7):3184-3192. Xu Gongda, Si Han, Huang Qiong, et al. Catalytic oxidation of chlorobenzene over Cr-Ce-O catalysts modified by transition metals[J]. China Environmental Science, 2021,41(7):3184-3192.
[2] Liu H, Yang J, Jia Y Y, et al. Significant improvement of catalytic performance for chlorinated volatile organic compound oxidation over RuO_x supported on acid-etched Co₃O₄[J]. Environmental Science& Technology, 2021,55(15):10734-10743.
[3] Dai Q G, Bais X, Wang X Y, et al. Catalytic combustion of chlorobenzene over Ru-doped ceria catalysts:Mechanism study[J]. Applied Catalysis B:Environment, 2013,129:580-588.
[4] Huang H, Dai Q G, Wang X Y. Morphology effect of Ru/CeO₂ catalysts for the catalytic combustion of chlorobenzene[J]. Applied Catalysis B:Environment, 2014,158:96-105.
[5] Deng W, Jia Z, Gao B, et al. Effect of preparation method on the performance of porous RuO_x/Co₃O₄ catalysts for 1, 2-dichloroethane oxidation[J]. Applied Catalysis A:General, 2021,624:118300.
[6] Zheng Z, Yang Y, Li H, et al. Effect of multi-pollutant on the catalytic oxidation of dichloromethane over RuO₂-WO₃/Sn_0.2Ti_0.8O₂ catalyst[J]. Fuel, 2020,278:118207.
[7] Wang Y, Cheny, Zhang L, et al. Total catalytic oxidation of chlorinated aromatics over bimetallic Pt-Ru supported on hierarchical HZSM-5zeolite[J]. Microporous and Mesoporous Materials, 2020,308:110538.
[8] Lao Y, Zhu N, Jiang X, et al. Effect of Ru on the activity of Co₃O₄ catalysts for chlorinated aromatics oxidation[J]. Catalysis Science& Technology, 2018,8(18):4797-4811.
[9] Xie B, Wei Z, Ding M, et al. Enhanced Ru-O-Ce interaction by solid solution structure of Ru-Ce_xZr₁_-_xO₂ catalysts for efficient catalytic combustion of vinyl chloride[J]. Applied Catalysis B:Environment and Energy, 2024,350:123926.
[10] Wang J, Liu X L, Zeng J L, et al. Catalytic oxidation of trichloroethylene over TiO₂ supported ruthenium catalysts[J]. Catalysis Communications, 2016,76:13-18.
[11] Dai Q, Wu J, Deng W, et al. Comparative studies of P/CeO₂ and Ru/CeO₂ catalysts for catalytic combustion of dichloromethane:From effects of H₂O to distribution of chlorinated by-products[J]. Applied Catalysis B:Environmental, 2019,249:9-18.
[12] Shen K, Gao B, Xia H, et al. Oxy-anionic doping:A new strategy for improving selectivity of Ru/CeO₂ with synergetic versatility and thermal stability for catalytic oxidation of chlorinated volatile organic compounds[J]. Environmental Science& Technology, 2022,56(12):8854-8863.
[13] Huang Y, Tian M, Jiang Z, et al. Inserting Cr₂O₃ dramatically promotes RuO₂/TiO₂ catalyst for low-temperature 1,2-dichloroethane deep destruction:Catalytic performance and synergy mechanism[J]. Applied Catalysis B:Environmental, 2022,304:121002.
[14] Zhao J, Xi W J, Tu C S, et al. Catalytic oxidation of chlorinated VOCs over Ru/Ti_xSn₁_-_x catalysts[J]. Applied Catalysis B:Environment, 2020,263:118237.
[15] Sun B H, Li Q Q, Su G J, 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(22):16292-16302.
[16] Wu L K, Deng J G, Liu Y X, et al. Enhanced removal efficiency of multicomponent VOCs over the Sn-doped silicalite-1-supported Ru single-atom catalysts by constructing tightly coupled redox and acidic sites[J]. Applied Catalysis B:Environmental, 2024,351:123910.
[17] Lyu S, Cheng Q, Liu Y, et al. Dopamine sacrificial coating strategy driving formation of highly active surface-exposed Ru sites on Ru/TiO₂ catalysts in Fischer-Tropsch synthesis[J]. Applied Catalysis B:Environmental, 2020,278:119261.
[18] Xu K, Hu X C, Ma C, et al. Spectroscopic investigation of the structural transformation of Ru in the Ru/CeO₂ catalyst[J]. Catalysis Science& Technology, 2023,13(21):6254-6263.
[19] Abdel-Mageed A M, Widmann D, Olesen S E, et al. Selective CO Methanation on Highly active Ru/TiO₂ catalysts:Identifying the physical origin of the observed activation/deactivation and loss in selectivity[J]. ACS Catalysis, 2018,8(6):5399-5414.
[20] 梁文俊,朱玉雪,石秀娟,等.Ce掺杂对Ru/TiO₂催化CB性能的影响[J].化工学报, 2020,71(8):3585-3593. Liang Wenjun, Zhu Yuxue, Shi Xiujuan, et al. Effect of Ce doping on catalytic chlorobenzene performance of Ru/TiO₂ catalysts[J]. CIESC Journal, 2020,71(8):3585-3593.
[21] Nakaji Y, Kobayashi D, Nakagawa Y, et al. Mechanism of formation of highly dispersed metallic ruthenium particles on ceria support by heating and reduction[J]. The Journal of Physical Chemistry C, 2019, 123(34):20817-20828.
[22] 王保文,张港,刘同庆,等.CeO₂/CuFe₂O₄氧载体CH₄化学链重整耦合CO₂热催化还原研究[J].化工学报, 2022,73(12):5414-5426. Wang Baowen, Zhang Gang, Liu Tongqing, et al. Research on chemical looping reforming of CH₄ by CeO₂ doped CuFe₂O₄ oxygen carrier coupled with CO₂ thermocatalytic reduction[J]. CIESC Journal, 2022,73(12):5414-5426.
[23] Chen X, Wang X, Jia Z, et al. Weakened Mn-O bond in Mn-Ce catalysts through K doping induced oxygen activation for boosting benzene oxidation at low temperatures[J]. Journal of Colloid and Interface Science, 2024,666:88-100.
[24] Chen X, Jia Z, Liu Z, et al. Strong metal-support interactions between atomically dispersed Ru and CrO_x for improved durability of chlorobenzene oxidation[J]. RSC Advances, 2023,13(5):3255-3264.
[25] Zheng T, Ma X, Cao J, et al. Effect of B-site element on the structure and catalytic performance for toluene of the 3DOM CeBO₃Catalyst[J]. Inorganic Chemistry, 2023,62(16):6352-6360.
[26] Mukherjee D, Venkataswamy P, Devaiah D, et al. Crucial role of titanium dioxide support in soot oxidation catalysis of manganese doped ceria[J]. Catalysis Science& Technology, 2017,7(14):3045-3055.
[27] Liu L, Liu R, Xu T, et al. Enhanced catalytic oxidation of chlorobenzene over MnO₂ grafted in situ by rare earth oxide:Surface doping induces lattice oxygen activation[J]. Inorganic Chemistry, 2020,59(19):14407-14414.
[28] Chen X, Chen X, Yu E Q, et al. In situ pyrolysis of Ce-MOF to prepare CeO₂ catalyst with obviously improved catalytic performance for toluene combustion[J]. Chemical Engineering Journal, 2018,344:469-479.
[29] Wang J, Yoshida A, Wang P, et al. Catalytic oxidation of volatile organic compound over cerium modified cobalt-based mixed oxide catalysts synthesized by electrodeposition method[J]. Applied Catalysis B:Environmental, 2020,271:118941.
[30] Liu S, Wang H, Wei Y, et al. Core-shell structure effect on CeO₂ and TiO₂ supported WO₃ for the NH₃-SCR process[J]. Molecular Catalysis, 2020,485:110822.
[31] Su Y, Fu K, Pang C, et al. Recent advances of chlorinated volatile organic compounds'oxidation catalyzed by multiple catalysts:reasonable adjustment of acidity and redox properties[J]. Environmental Science& Technology, 2022,56(14):9854-9871.
[32] Lv X, Jiang M, Chen J, et al. Unveiling the lead resistance mechanism and interface regulation strategy of Ru-based catalyst during chlorinated VOCs oxidation[J]. Applied Catalysis B:Environmental, 2022,315:121592.
[33] Huang H, Dai Q, Wang X. Morphology effect of Ru/CeO₂ catalysts for the catalytic combustion of chlorobenzene[J]. Applied Catalysis B:Environmental, 2014,158-159:96-105.
[34] Sun X, Yang S, Liu X, et al. The enhancement of benzene total oxidation over Ru_xCeO₂ catalysts at low temperature:The significance of Ru incorporation[J]. Science of The Total Environment, 2023, 902:165574.
[35] Long Y, Meng Q, Chen M, et al. Selective Ru adsorption on SnO₂/CeO₂ mixed oxides for efficient destruction of multicomponent volatile organic compounds:From laboratory to practical possibility[J]. Environmental Science& Technology, 2022,56(13):9762-9772.
[36] Yu X, Dai L, Deng J, et al. Catalytic performance and intermediates identification of trichloroethylene deep oxidation over Ru/3DOM SnO₂ catalysts[J]. Journal of Catalysis, 2021,400:310-324.
[37] Shi Q, Ding L, Long H M, et al. Study on catalytic combustion of dioxins from iron ore sintering flue gas over Ce-V-Ti Catalysts by XRD and FTIR[J]. Spectroscopy and Spectral Analysis, 2021,41(1):327-332.
[38] Carabineiro S A C, Chen X, Konsolakis M, et al. Catalytic oxidation of toluene on Ce-Co and La-Co mixed oxides synthesized by exotemplating and evaporation methods[J]. Catalysis Today, 2015, 244:161-171.
[39] Dong F, Han W, Guo Y, et al. CeCoO_x-MNS catalyst derived from three-dimensional mesh nanosheet Co-based metal-organic frameworks for highly efficient catalytic combustion of VOCs[J]. Chemical Engineering Journal, 2021,405:126948.
[40] Shi Z, Dong F, Han W, et al. Engineering Co₃O₄@3DOM LaCoO₃ multistage-pore nanoreactor with superior SO₂ resistance for toluene catalytic combustion[J]. Nanoscale, 2024,16:10760-10778.
[41] Wu Y, Wang H, Bai J, et al. Highly efficient low-temperature catalytic degradation of chlorobenzene over MnO_x-CeO₂/γ-Al₂O₃-CNT[J]. Fresenius Environmental Bulletin, 2022,31(8):7639-7645.
[42] Wan J, Yang P, Guo X L, et al. Elimination of 1,2-dichloroethane over (Ce,Cr)_xO₂/Nb₂O₅ catalysts:synergistic performance between oxidizing ability and acidity[J]. Chinese Journal of Catalysis, 2019, 40(7):1100-1108.
[43] Shi Y J, Wang J L, Wang Y Y, et al. Synergistic effect in bimetal Cr-Pt/ZSM-5catalysts with high activity for CVOCs low-temperature removal[J]. Journal of Environmental Chemical Engineering, 2022,10(3):107629.
[44] Dong Y, Ran M C, Zhang X, et al. Promoting effect of polyoxometallic acid modification on the NH₃-SCR performance of Mn-based catalysts[J]. Journal of Environmental Chemical Engineering, 2024,12(3):112823.
[45] Sun Y, He C, Tian M, et al. Catalytic combustion of 1,2-dichloroethane via CC/CCl bond cleavage through core-shell structured CeO₂@TiO₂ catalyst with excellent catalytic performances[J]. Molecular Catalysis, 2024,557:113959.
[46] Zhu D, Liu M, Li S, et al. High efficiency CuO_x/TiO₂-ZrO₂ for chlorobenzenes catalytic oxidation via adjusting surface acidic sites[J]. Applied Surface Science, 2023,639:158134.
[47] Zhu F, Wen J, Guo H, et al. Low-temperature catalytic performance improvement of Ru/TiO₂{001}for o-dichlorobenzene oxidation[J]. Chemical Engineering Journal, 2023,473:145186.
[48] Wang J, Wang X, Liu X, et al. Kinetics and mechanism study on catalytic oxidation of chlorobenzene over V₂O₅/TiO₂ catalysts[J]. Journal of Molecular Catalysis A:Chemical, 2015,402:1-9.
[49] Chai S, Li S, Li W, et al. Fabrication of high loading V₂O₅/TiO₂ catalysts derived from metal-organic framework with excellent activity for chlorobenzene decomposition[J]. Applied Surface Science, 2022,572:151511.