CeMn复合氧化物的制备及氯苯催化氧化性能

doi:10.11896/cldb.23050133

Abstract
Figure/Table
References
Related Citation (15)

Download:

Full Text ( PDF ) (9976KB)
Export: BibTeX | EndNote (RIS)

Abstract Chlorobenzene, as a chlorobenzene ring substance, has high biological toxicity and chemical stability, is difficult to degrade, and needs urgent treatment. Among many treatment technologies, catalytic oxidation has a good application prospect because of its deep degradation ability. In this study, based on the rare earth metal oxide CeO₂, which is rich in resources, the effects of different preparation methods and doping of different transition metal elements on the catalytic oxidation of chlorobenzene were investigated. The physicochemical properties and reaction paths of the catalyst were analyzed and the results showed that compared with the direct calcination, acetic acid+hydrothermal, urea hydrolysis+hydrothermal methods, the CeO₂ catalyst prepared by NaOH precipitation+hydrothermal method has better performance. The study of doping with different elements (Mn, Fe, Co) found that the chlorobenzene oxidation activity of Ce-Mn catalyst was significantly improved, and the catalytic conversion rate was 95% at 450 ℃ containing H₂O (5vol%, the same below). The analysis showed that Mn doping significantly increased the acidic sites and REDOX sites on the surface of the catalyst, and the Brønsted/Lewis (B/L) acid ratio was increased from 0.259 to 0.419, which promoted more electron cycling (Ce⁴⁺/Ce³⁺) and reactive oxidizing species mobility (O_α↔O_β). Chlorobenene molecules adsorbed on the active site (acid site or oxygen vacancy) on the catalyst surface underwent nucleophilic substitution reaction, dechlorinated to form phenol. Under the action of reactive oxygen species, chlorobenene gradually opened to intermediate species such as acetate, and finally converted to small molecular products such as CO₂, H₂O and HCl.

Key words： CeMn oxide hydrothermal method element doping chlorobenzene degradation catalytic oxidation reaction pathway

Published: 25 August 2024 Online: 2024-09-10

CLC number:

X511

Fund:National Key R & D Program of China (2023YFB3810800), National Natural Science Foundation of China (U20A20130), and Special Fund for Basic Scientific Research of Central Universities (FRF-EYIT-23-07).

	Service
	E-mail this article
	Add to my bookshelf
	Add to citation manager
	E-mail Alert
	RSS
	Articles by authors
	LUO Ning
	GAO Fengyu
	CHEN Du
	ZHANG Chenxiao
	DUAN Erhong
	ZHAO Shunzheng
	YI Honghong
	TANG Xiaolong

Cite this article:

LUO Ning,GAO Fengyu,CHEN Du, et al. Preparation of CeMn Composite Oxide and Catalytic Oxidation of Chlorobenzene[J]. Materials Reports, 2024, 38(16): 23050133-9.

URL:

http://www.mater-rep.com/EN/10.11896/cldb.23050133 OR http://www.mater-rep.com/EN/Y2024/V38/I16/23050133

1 Cao K X, Dai X X, Wu Z B, et al. Chinese Chemical Letters, 2021, 32(3), 1206.
2 Li G B, Shen K, Wang L, et al. Applied Catalysis B: Environmental, 2021, 286, 119865.
3 Wu X Q, Han R, Liu Q L, et al. Catalysis Science & Technology, 2021, 11(16), 5374.
4 Kamal M S, Razzak, S A, Hossain M M, et al. Atmospheric Environment, 2016, 140, 117.
5 Liu X L, Chen L, Zhu T Y, et al. Journal of Hazardous Materials, 2019, 363, 90.
6 Dai Q G, Bai S X, Wang J W, et al. Applied Catalysis B: Environmental, 2013, 142-143, 222.
7 Weng X L, Meng Q J, Liu J J, et al. Environmental Science & Technology, 2019, 53(2), 884.
8 Liu L Z, Zhou B, Liu Y W, et al. Journal of Colloid and Interface Science, 2022, 606, 1866.
9 Weng X L, Sun P F, Long Y, et al. Environmental Science & Technology, 2018, 51(14), 8057.
10 Ye G G, Lu Jun, Qian L L, et al. Journal of Saudi Chemical Society, 2021, 25(5), 101229.
11 Wu L Y, He Fei, Luo J Q, et al. RSC Advances, 2017, 43(7), 26952.
12 Hu E D, Zhang W Z, Wu J, et al. Journal of Environmental Chemical Engineering, 2022, 5(10), 108439.
13 Zhao H J, Han W L, Tang Z C, et al. Applied Catalysis B, Environmental, 2020, 276, 119133.
14 Ding J Y, Liu J, Yang Y J, et al. Chemosphere, 2021, 277, 130194.
15 Wang Y, Chen Y, Zhang L, et al. Microporous and Mesoporous Materials, 2020, 308, 110538.
16 Shi Q, Ding L, Long H M, et al. Materials, 2019, 13(1), 125.
17 Wan J, Tao F, Shi Y J, et al. Chemical Engineering Journal, 2021, 433, 133788.
18 Miran H A, Altarawneh M, Jiang Z T, et al. Catalysis Science & Technology, 2017, 7, 3902.
19 Yang S, Zhao H J, Dong F, et al. Molecular Catalysis, 2019, 463, 119.
20 Weng X L, Long Y, Wang W L, et al. Chinese Journal of Catalysis, 2019, 40(5), 638.
21 Chen G, Cai Y P, Zhang H, et al. Environmental Science & Technology, 2021, 55(20), 14204.
22 Chen G, Cai Y P, Zhang H, et al. Chemical Engineering Journal, 2020, 395, 125172.
23 Gu Y F, Cai T, Gao X H, et al. Applied Catalysis B: Environmental, 2019, 248, 264.
24 Hu W K, He F, Chen X, et al. Journal of Nanoparticle Research, 2018, 21(1), 6.
25 Gao F Y, Chen D, Luo N, et al. Chemical Journal of Chinese Universities, 2023, 44(4), 20220690 (in Chinese).
高凤雨, 陈都, 罗宁, 等. 高等学校化学学报, 2023, 44(4), 20220690.
26 Dai Y, Wang X Y, Dai Q G, et al. Applied Catalysis B: Environmental, 2012, 111-112, 141.
27 Sinquin G, Petit C, Libs S, et al. Applied Catalysis B: Environmental, 2001, 32(1-2), 37.
28 Dai Q G, Wang X Y, Lu G Z, et al. Applied Catalysis B: Environmental, 2008, 81(3-4), 192.
29 Gao F Y, Tang X L, Yi H H, et al. Chemical Engineering Journal, 2017, 317, 20.
30 Machida M, Uto M, Kurpgi D, et al. Chemistry of Materials, 2000, 12(10), 3158.
31 Zhan X C, Zhang X Y, Guo Y L, et al. Journal of Rare Earths, 2014, 32(2), 146.
32 Deng W, Tang Q X, Huang S S, et al. Applied Catalysis B: Environmental, 2020, 278, 119336.
33 Zhao J, Xi W J, Tu C S, et al. Applied Catalysis B: Environmental, 2020, 263, 118237.
34 Lu P, Ye L M, Yan X H, et al. Applied Applied Surface Science, 2021, 567, 150836.
35 Lv X L, Cai S C, Chen J, et al. Catalysis Science & Technology, 2021, 11 (13), 4581.
36 Li N, Cheng J, Xing X, et al. Journal of Hazardous Materials, 2020, 393, 122412.
37 Ta-Thi N A, Le T T, Vu V T, et al. Journal of Inorganic and Organometallic Polymers and Materials, 2020, 30 (10), 3886.
38 Aponte A G, Ramírez, M A, Mora Y C, et al. AIMS Materials Science, 2020, 7, 468.
39 Jayakumar C G, Irudayaraj A A, Raj A D, et al. Applied Physics A, 2019, 125, 742.
40 Liu J S, Zhen Y X, Zhang X F, et al. Ceramics International, 2022, 48(2), 1550.
41 Zamiri R, Ahangar H A, Kaushal A, et al. PLoS One, 2015, 10(4), e0122989.
42 Jiang W Y, Yu Y L, Bi F, et al. Environmental Science & Technology, 2019, 53(21), 12657.
43 Wang X W, Jiang W Y, Yin R Q, et al. Journal of Colloid and Interface Science, 2020, 574, 251.
44 Zhu L, Pan S L, Liu Z Y, et al. Industrial & Engineering Chemistry Research, 2020, 59(13), 5686.
45 Alderman S L, Farquar G R, Poliakoff E D, et al. Environmental Science & Technology, 2005, 39(19), 7396.
46 Dai X X, Wang X W, Long Y P, et al. Environmental Science & Technology, 2019, 53(21), 12697.
47 Zhu L, Li X, Liu Z Y, et al. Nanomaterials, 2019, 9(5), 675.
48 Liu J J, Shi X Y, Shan Y L, et al. Environmental Science & Technology, 2018, 52(20), 11769.
49 Liao Y N, Fu M L, Chen L M, et al. Catalysis Today, 2013, 216, 220.
50 Chen B B, Wu B, Yu L M, et al. ACS Catalysis, 2020, 10(11), 6176.
51 Chen J, Chen X, Yan D X, et al. Applied Catalysis B: Environmental, 2019, 250, 396.
52 Zhuang Y Y, Xu Z J, Zhang X R, et al. Separation and Purification Technology, 2022, 294, 121191.
53 Sun P F, Wang W L, Dai X X, et al. Applied Catalysis B: Environmental, 2016, 198, 389.