Catalytic oxidation of <i>o</i>-chlorophenol over Co<sub>2</sub>XAl (X= Co, Mg, Ca, Ni) hydrotalcite-derived mixed oxide catalysts

doi:10.1007/s11783-020-1284-3

Front. Environ. Sci. Eng.

2020, Vol. 14

Issue (6) : 105 https://doi.org/10.1007/s11783-020-1284-3

RESEARCH ARTICLE

Catalytic oxidation of o-chlorophenol over Co₂XAl (X= Co, Mg, Ca, Ni) hydrotalcite-derived mixed oxide catalysts

Na Li^1,², Xin Xing^1,², Yonggang Sun^1,², Jie Cheng²(

), Gang Wang¹, Zhongshen Zhang², Zhengping Hao^1,²(

)

¹. Key Laboratory of Environmental Nanotechnology and Health Effects, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China
². National Engineering Laboratory for VOCs Pollution Control Material & Technology, Research Center for Environmental Material and Pollution Control Technology, University of Chinese Academy of Sciences, Beijing 101408, China

Download: PDF(1203 KB) HTML
Export: BibTeX | EndNote | Reference Manager | ProCite | RefWorks

Abstract

• Superior catalytic activity observed for o-chlorophenol oxidation on Co₂MgAlO.

• The reducibility, oxygen species and basicity influenced catalytic activity.

• The organic by-products were generated in o-chlorophenol catalytic oxidation.

A cobalt-based hydrotalcite-like compound was prepared using a constant-pH coprecipitation method. Cobalt-transition metal oxides (Co₂XAlO, X= Co, Mg, Ca and Ni) were investigated for the deep catalytic oxidation of o-chlorophenol as a typical heteroatom contaminant containing chlorine atoms. The partial substitution of Co by Mg, Ca or Ni in the mixed oxide can promote the catalytic oxidation of o-chlorophenol. The Co₂MgAlO catalyst presented the best catalytic activity, and could maintain 90% o-chlorophenol conversion at 167.1°C, compared only 27% conversion for the Co₃AlO catalyst. The results demonstrated that the high activity could be attributed to its increased low-temperature reducibility, rich active oxygen species and excellent oxygen mobility. In the existence of acid and base sites, catalysts with strong basicity also showed preferred activity. The organic by-products generated during the o-chlorophenol catalytic oxidation over Co₂MgAlO catalyst included carbon tetrachloride, trichloroethylene, 2,4-dichlorophenol, and 2,6-dichloro-p-benzoquinon, et al. This work provides a facile method for the preparation of Co-based composite oxide catalysts, which represent promising candidates for typical chlorinated and oxygenated volatile organic compounds.

Keywords Hydrotalcite-derived mixed oxides o-chlorophenol Catalytic oxidation Organic by-products

Corresponding Author(s): Jie Cheng,Zhengping Hao

Issue Date: 28 June 2020

Cite this article:

Na Li,Xin Xing,Yonggang Sun, et al. Catalytic oxidation of o-chlorophenol over Co₂XAl (X= Co, Mg, Ca, Ni) hydrotalcite-derived mixed oxide catalysts[J]. Front. Environ. Sci. Eng., 2020, 14(6): 105.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-020-1284-3
https://academic.hep.com.cn/fese/EN/Y2020/V14/I6/105

Fig.1 XRD patterns of Co₂XAl-HTs precursors (a) and Co₂XAlO catalysts (b).

Tab.1 T₅₀, T₉₀, reaction rates (r) at 120°C and textural properties of the Co₂XAlO catalysts

Fig.2 Nitrogen adsorption/desorption isotherms curves (a) and pore size distribution (b) of the Co₂XAlO catalysts.

Fig.3 The catalytic performances (a) and Arrhenius plots (ln (r × 10⁶) vs 1000/T) (b).

Tab.2 Organic by-products over Co₂MgAlO catalyst at 400°C

Fig.4 FT-IR spectra of the Co₂XAlO catalysts.

Fig.5 H₂-TPR (a), O₂-TPD-MS (b), Co 2p (c) and O 1s (d) XPS spectra of Co₂XAlO.

Fig.6 NH₃-TPD-MS (a) and CO₂-TPD-MS (b) profiles of the Co₂XAlO catalysts.

1	B Y Bai, J H Li (2014). Positive effects of K+ ions on three-dimensional mesoporous Ag/Co3O4 catalyst for HCHO oxidation. ACS Catalysis, 4(8): 2753–2762 https://doi.org/10.1021/cs5006663
2	N Blanch-Raga, A E Palomares, J Martínez-Triguero, G Fetter, P Bosch (2013). Cu mixed oxides based on hydrotalcite-like compounds for the oxidation of trichloroethylene. Industrial & Engineering Chemistry Research, 52(45): 15772–15779 https://doi.org/10.1021/ie4024935
3	N Blanch-Raga, A E Palomares, J Martínez-Triguero, M Puche, G Fetter, P Bosch (2014). The oxidation of trichloroethylene over different mixed oxides derived from hydrotalcites. Applied Catalysis B: Environmental, 160–161: 129–134 https://doi.org/10.1016/j.apcatb.2014.05.014
4	P H Bolt, F H P M Habraken, J W Geus (1998). Formation of nickel, cobalt, copper, and iron aluminates from a- and l-alumina-supported oxides: A comparative study. Journal of Solid State Chemistry, 135(1): 59–69 https://doi.org/10.1006/jssc.1997.7590
5	T Cai, H Huang, W Deng, Q G Dai, W Liu, X Y Wang (2015). Catalytic combustion of 1,2-dichlorobenzene at low temperature over Mn-modified Co3O4 catalysts. Applied Catalysis B: Environmental, 166–167: 393–405 https://doi.org/10.1016/j.apcatb.2014.10.047
6	C A Chagas, E F de Souza, R L Manfro, S M Landi, M M V M Souza, M Schmal (2016). Copper as promoter of the NiO-CeO2 catalyst in the preferential CO oxidation. Applied Catalysis B: Environmental, 182: 257–265 https://doi.org/10.1016/j.apcatb.2015.09.033
7	J Cheng, J J Yu, X P Wang, L D Li, J J Li, Z P Hao (2008). Novel CH4 combustion catalysts derived from Cu-Co/X-Al (X= Fe, Mn, La, Ce) hydrotalcite-like compounds. Energy & Fuels, 22(4): 2131–2137 https://doi.org/10.1021/ef8000168
8	Q G Dai, W Wang, X Y Wang, G Z Lu (2017). Sandwich-structured CeO2@ZSM-5 hybrid composites for catalytic oxidation of 1,2-dichloroethane: An integrated solution to coking and chlorine poisoning deactivation. Applied Catalysis B: Environmental, 203: 31–42 https://doi.org/10.1016/j.apcatb.2016.10.009
9	C S Evans, B Dellinger (2005). Surface-mediated formation of polybrominated dibenzo-p-dioxins and dibenzofurans from the high-temperature pyrolysis of 2-bromophenol on a CuO/silica surface. Environmental Science & Technology, 39(13): 4857–4863 https://doi.org/10.1021/es048057z
10	Y F Gu, T Cai, X H Gao, H Q Xia, W Sun, J Zhao, Q G Dai, X Y Wang (2019). Catalytic combustion of chlorinated aromatics over WOx/CeO2 catalysts at low temperature. Applied Catalysis B: Environmental, 248: 264–276 https://doi.org/10.1016/j.apcatb.2018.12.055
11	L J Guo, N Jiang, J Li, K F Shang, N Lu, Y Wu (2018). Abatement of mixed volatile organic compounds in a catalytic hybrid surface/packed-bed discharge plasma reactor. Frontiers of Environmental Science & Engineering, 12(2): 15 https://doi.org/10.1007/s11783-018-1017-z
12	J K Han, L T Jia, B Hou, D B Li, Y Liu, Y C Liu (2015). Catalytic properties of CoAl2O4/Al2O3 supported cobalt catalysts for Fischer-Tropsch synthesis. Journal of Fuel Chemistry and Technology, 43(7): 846–851 https://doi.org/10.1016/S1872-5813(15)30025-6
13	C He, J Cheng, X Zhang, M Douthwaite, S Pattisson, Z P Hao (2019). Recent advances in the catalytic oxidation of volatile organic compounds: A review based on pollutant sorts and sources. Chemical Reviews, 119(7): 4471–4568 https://doi.org/10.1021/acs.chemrev.8b00408
14	C E Hetrick, J Lichtenberger, M D Amiridis (2008). Catalytic oxidation of chlorophenol over V2O5/TiO2 catalysts. Applied Catalysis B: Environmental, 77(3–4): 255–263 https://doi.org/10.1016/j.apcatb.2007.07.022
15	H Hu, S X Cai, H R Li, L Huang, L Y Shi, D S Zhang (2015). Mechanistic aspects of deNOx processing over TiO2 supported Co–Mn oxide catalysts: Structure–activity relationships and in situ DRIFTs analysis. ACS Catalysis, 5(10): 6069–6077 https://doi.org/10.1021/acscatal.5b01039
16	Y C Huang, W J Fan, B Long, H B Li, W T Qiu, F Y Zhao, Y X Tong, H B Ji (2016a). Alkali-modified non-precious metal 3D-NiCo2O4 nanosheets for efficient formaldehyde oxidation at low temperature. Journal of Materials Chemistry. A, Materials for Energy and Sustainability, 4(10): 3648–3654 https://doi.org/10.1039/C5TA09370H
17	Y C Huang, K H Ye, H B Li, W J Fan, F Y Zhao, Y M Zhang, H B Ji (2016b). A highly durable catalyst based on CoxMn3–xO4 nanosheets for low-temperature formaldehyde oxidation. Nano Research, 9(12): 3881–3892 https://doi.org/10.1007/s12274-016-1257-9
18	M S Kamal, S A Razzak, M M Hossain (2016). Catalytic oxidation of volatile organic compounds (VOCs): A review. Atmospheric Environment, 140: 117–134 https://doi.org/10.1016/j.atmosenv.2016.05.031
19	P Li, C He, J Cheng, C Y Ma, B J Dou, Z P Hao (2011). Catalytic oxidation of toluene over Pd/Co3AlO catalysts derived from hydrotalcite-like compounds: Effects of preparation methods. Applied Catalysis B: Environmental, 101(3–4): 570–579 https://doi.org/10.1016/j.apcatb.2010.10.030
20	Q Li, M Meng, Z Q Zou, X G Li, Y Q Zha (2009). Simultaneous soot combustion and nitrogen oxides storage on potassium-promoted hydrotalcite-based CoMgAlO catalysts. Journal of Hazardous Materials, 161(1): 366–372 https://doi.org/10.1016/j.jhazmat.2008.03.103
21	S D Li, H S Wang, W M Li, X F Wu, W X Tang, Y F Chen (2015). Effect of Cu substitution on promoted benzene oxidation over porous CuCo-based catalysts derived from layered double hydroxide with resistance of water vapor. Applied Catalysis B: Environmental, 166–167: 260–269 https://doi.org/10.1016/j.apcatb.2014.11.040
22	J G Liu, M Y Ding, T J Wang, L L Ma (2012). Promoting effect of cobalt addition on higher alcohols synthesis over copper-based catalysts. Advanced Materials Research, 550–553: 270–275 https://doi.org/10.4028/www.scientific.net/AMR.550-553.270
23	Y Lou, L Wang, Z Y Zhao, Y H Zhang, Z G Zhang, G Z Lu, Y Guo, Y L Guo (2014). Low-temperature CO oxidation over Co3O4-based catalysts: Significant promoting effect of Bi2O3 on Co3O4 catalyst. Applied Catalysis B: Environmental, 146: 43–49 https://doi.org/10.1016/j.apcatb.2013.06.007
24	W J Lu, Y Abbas, M F Mustafa, C Pan, H T Wang (2019). A review on application of dielectric barrier discharge plasma technology on the abatement of volatile organic compounds. Frontiers of Environmental Science & Engineering, 13(2): 30 https://doi.org/10.1007/s11783-019-1108-5
25	M Salavati-Niasari, N Mir, F Davar (2009). Synthesis and characterization of Co3O4 nanorods by thermal decomposition of cobalt oxalate. Journal of Physics and Chemistry of Solids, 70(5): 847–852 https://doi.org/10.1016/j.jpcs.2009.04.006
26	Z N Shi, P Yang, F Tao, R X Zhou (2016). New insight into the structure of CeO2–TiO2 mixed oxides and their excellent catalytic performances for 1,2-dichloroethane oxidation. Chemical Engineering Journal, 295: 99–108 https://doi.org/10.1016/j.cej.2016.03.032
27	X F Tang, J M Hao, J H Li (2009). Complete oxidation of methane on Co3O4–SnO2 catalysts. Frontiers of Environmental Science & Engineering in China, 3(3): 265–270 https://doi.org/10.1007/s11783-009-0019-2
28	M J Tian, C He, Y K Yu, H Pan, L Smith, Z Y Jiang, N B Gao, Y F Jian, Z P Hao, Q Zhu (2018). Catalytic oxidation of 1,2-dichloroethane over three-dimensional ordered meso-macroporous Co3O4/La0.7Sr0.3Fe0.5Co0.5O3: Destruction route and mechanism. Applied Catalysis A, General, 553: 1–14 https://doi.org/10.1016/j.apcata.2018.01.013
29	Z Y Tian, P H Tchoua Ngamou, V Vannier, K Kohse-Höinghaus, N Bahlawane (2012). Catalytic oxidation of VOCs over mixed Co–Mn oxides. Applied Catalysis B: Environmental, 117–118: 125–134 https://doi.org/10.1016/j.apcatb.2012.01.013
30	L L Yang, G R Liu, M H Zheng, Y Y Zhao, R Jin, X L Wu, Y Xu (2017). Molecular mechanism of dioxin formation from chlorophenol based on electron paramagnetic resonance spectroscopy. Environmental Science & Technology, 51(9): 4999–5007 https://doi.org/10.1021/acs.est.7b00828
31	P Yang, S S Yang, Z N Shi, Z H Meng, R X Zhou (2015). Deep oxidation of chlorinated VOCs over CeO2-based transition metal mixed oxide catalysts. Applied Catalysis B: Environmental, 162: 227–235 https://doi.org/10.1016/j.apcatb.2014.06.048
32	L P Zeng, K Z Li, F Huang, X Zhu, H C Li (2016). Effects of Co3O4 nanocatalyst morphology on CO oxidation: Synthesis process map and catalytic activity. Chinese Journal of Catalysis, 37(6): 908–922 https://doi.org/10.1016/S1872-2067(16)62460-9
33	C H Zhang, C Wang, S Gil, A Boreave, L Retailleau, Y L Guo, J L Valverde, A Giroir-Fendler (2017). Catalytic oxidation of 1,2-dichloropropane over supported LaMnOx oxides catalysts. Applied Catalysis B: Environmental, 201: 552–560 https://doi.org/10.1016/j.apcatb.2016.08.038
34	X Zhang, Z Wang, Y Y Tang, N L Qiao, Y Li, S Q Qu, Z P Hao (2015). Catalytic behaviors of combined oxides derived from Mg/AlxFe1–x–Cl layered double hydroxides for H2S selective oxidation. Catalysis Science & Technology, 5(11): 4991–4999 https://doi.org/10.1039/C5CY00689A
35	Z Z Zhu, G Z Lu, Z G Zhang, Y Guo, Y L Guo, Y Q Wang (2013). Highly active and stable Co3O4/ZSM-5 catalyst for propane oxidation: Effect of the preparation method. ACS Catalysis, 3(6): 1154–1164 https://doi.org/10.1021/cs400068v

[1]

FSE-20041-OF-LN_suppl_1

Download

[1]	Tiejun Zhang, Jian Li, Hong He, Qianqian Song, Quanming Liang. NO oxidation over Co-La catalysts and NO_x reduction in compact SCR[J]. Front. Environ. Sci. Eng., 2017, 11(2): 4-.
[2]	Nanli QIAO,Xin ZHANG,Chi HE,Yang LI,Zhongshen ZHANG,Jie CHENG,Zhengping HAO. Enhanced performances in catalytic oxidation of o-xylene over hierarchical macro-/mesoporous silica-supported palladium catalysts[J]. Front. Environ. Sci. Eng., 2016, 10(3): 458-466.
[3]	Chang-Mao HUNG, Wen-Liang LAI, Jane-Li LIN. Investigation of fluorescence characterization and electrochemical behavior on the catalysts of nanosized Pt-Rh/γ-Al₂O₃ to oxidize gaseous ammonia[J]. Front Envir Sci Eng, 2013, 7(3): 428-434.
[4]	Longli BO, Jianbo LIAO, Yucai ZHANG, Xiaohui WANG, Quan YANG. CuO/zeolite catalyzed oxidation of gaseous toluene under microwave heating[J]. Front Envir Sci Eng, 2013, 7(3): 395-402.
[5]	Zeinab JAMALZADEH, Mohammad HAGHIGHI, Nazli ASGARI. Synthesis, physicochemical characterizations and catalytic performance of Pd/carbon-zeolite and Pd/carbon-CeO₂ nanocatalysts used for total oxidation of xylene at low temperatures[J]. Front Envir Sci Eng, 2013, 7(3): 365-381.
[6]	ZHOU Yunrui, ZHU Wanpeng, CHEN Xun. Catalytic activity of cerium-doped Ru/AlO during ozonation of dimethyl phthalate[J]. Front.Environ.Sci.Eng., 2008, 2(3): 354-357.
[7]	GUO Ting, BAI Zhipeng, WU Can, ZHU Tan. Influence of environmental temperature and relative humidity on photocatalytic oxidation of toluene on activated carbon fibers coated TiO[J]. Front.Environ.Sci.Eng., 2008, 2(2): 224-229.

Viewed

Full text

Abstract

Cited

Shared

Discussed