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

Highlights

• 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.

Abstract

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.

Graphical abstract

Keywords

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

References

[1] Bai B Y, Li J H (2014). Positive effects of K⁺ ions on three-dimensional mesoporous Ag/Co₃O₄ catalyst for HCHO oxidation. ACS Catalysis, 4(8): 2753–2762

[2] Blanch-Raga N, Palomares A E, Martínez-Triguero J, Fetter G, Bosch P (2013). Cu mixed oxides based on hydrotalcite-like compounds for the oxidation of trichloroethylene. Industrial & Engineering Chemistry Research, 52(45): 15772–15779

[3] Blanch-Raga N, Palomares A E, Martínez-Triguero J, Puche M, Fetter G, Bosch P (2014). The oxidation of trichloroethylene over different mixed oxides derived from hydrotalcites. Applied Catalysis B: Environmental, 160–161: 129–134

[4] Bolt P H, Habraken F H P M, Geus J W (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

[5] Cai T, Huang H, Deng W, Dai Q G, Liu W, Wang X Y (2015). Catalytic combustion of 1,2-dichlorobenzene at low temperature over Mn-modified Co₃O₄ catalysts. Applied Catalysis B: Environmental, 166–167: 393–405

[6] Chagas C A, de Souza E F, Manfro R L, Landi S M, Souza M M V M, Schmal M (2016). Copper as promoter of the NiO-CeO₂ catalyst in the preferential CO oxidation. Applied Catalysis B: Environmental, 182: 257–265

[7] Cheng J, Yu J J, Wang X P, Li L D, Li J J, Hao Z P (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

[8] Dai Q G, Wang W, Wang X Y, Lu G Z (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

[9] Evans C S, Dellinger B (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

[10] Gu Y F, Cai T, Gao X H, Xia H Q, Sun W, Zhao J, Dai Q G, Wang X Y (2019). Catalytic combustion of chlorinated aromatics over WO_x/CeO₂ catalysts at low temperature. Applied Catalysis B: Environmental, 248: 264–276

[11] Guo L J, Jiang N, Li J, Shang K F, Lu N, Wu Y (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

[12] Han J K, Jia L T, Hou B, Li D B, Liu Y, Liu Y C (2015). Catalytic properties of CoAl₂O₄/Al₂O₃ supported cobalt catalysts for Fischer-Tropsch synthesis. Journal of Fuel Chemistry and Technology, 43(7): 846–851

[13] He C, Cheng J, Zhang X, Douthwaite M, Pattisson S, Hao Z P (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

[14] Hetrick C E, Lichtenberger J, Amiridis M D (2008). Catalytic oxidation of chlorophenol over V₂O₅/TiO₂ catalysts. Applied Catalysis B: Environmental, 77(3–4): 255–263

[15] Hu H, Cai S X, Li H R, Huang L, Shi L Y, Zhang D S (2015). Mechanistic aspects of deNO_x processing over TiO₂ supported Co–Mn oxide catalysts: Structure–activity relationships and in situ DRIFTs analysis. ACS Catalysis, 5(10): 6069–6077

[16] Huang Y C, Fan W J, Long B, Li H B, Qiu W T, Zhao F Y, Tong Y X, Ji H B (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

[17] Huang Y C, Ye K H, Li H B, Fan W J, Zhao F Y, Zhang Y M, Ji H B (2016b). A highly durable catalyst based on Co_xMn_3–xO₄ nanosheets for low-temperature formaldehyde oxidation. Nano Research, 9(12): 3881–3892

[18] Kamal M S, Razzak S A, Hossain M M (2016). Catalytic oxidation of volatile organic compounds (VOCs): A review. Atmospheric Environment, 140: 117–134

[19] Li P, He C, Cheng J, Ma C Y, Dou B J, Hao Z P (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

[20] Li Q, Meng M, Zou Z Q, Li X G, Zha Y Q (2009). Simultaneous soot combustion and nitrogen oxides storage on potassium-promoted hydrotalcite-based CoMgAlO catalysts. Journal of Hazardous Materials, 161(1): 366–372

[21] Li S D, Wang H S, Li W M, Wu X F, Tang W X, Chen Y F (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

[22] Liu J G, Ding M Y, Wang T J, Ma L L (2012). Promoting effect of cobalt addition on higher alcohols synthesis over copper-based catalysts. Advanced Materials Research, 550–553: 270–275

[23] Lou Y, Wang L, Zhao Z Y, Zhang Y H, Zhang Z G, Lu G Z, Guo Y, Guo Y L (2014). Low-temperature CO oxidation over Co₃O₄-based catalysts: Significant promoting effect of Bi₂O₃ on Co₃O₄ catalyst. Applied Catalysis B: Environmental, 146: 43–49

[24] Lu W J, Abbas Y, Mustafa M F, Pan C, Wang H T (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

[25] Salavati-Niasari M, Mir N, Davar F (2009). Synthesis and characterization of Co₃O₄ nanorods by thermal decomposition of cobalt oxalate. Journal of Physics and Chemistry of Solids, 70(5): 847–852

[26] Shi Z N, Yang P, Tao F, Zhou R X (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

[27] Tang X F, Hao J M, Li J H (2009). Complete oxidation of methane on Co₃O₄–SnO₂ catalysts. Frontiers of Environmental Science & Engineering in China, 3(3): 265–270

[28] Tian M J, He C, Yu Y K, Pan H, Smith L, Jiang Z Y, Gao N B, Jian Y F, Hao Z P, Zhu Q (2018). Catalytic oxidation of 1,2-dichloroethane over three-dimensional ordered meso-macroporous Co₃O₄/La_0.7Sr_0.3Fe_0.5Co_0.5O₃: Destruction route and mechanism. Applied Catalysis A, General, 553: 1–14

[29] Tian Z Y, Tchoua Ngamou P H, Vannier V, Kohse-Höinghaus K, Bahlawane N (2012). Catalytic oxidation of VOCs over mixed Co–Mn oxides. Applied Catalysis B: Environmental, 117–118: 125–134

[30] Yang L L, Liu G R, Zheng M H, Zhao Y Y, Jin R, Wu X L, Xu Y (2017). Molecular mechanism of dioxin formation from chlorophenol based on electron paramagnetic resonance spectroscopy. Environmental Science & Technology, 51(9): 4999–5007

[31] Yang P, Yang S S, Shi Z N, Meng Z H, Zhou R X (2015). Deep oxidation of chlorinated VOCs over CeO₂-based transition metal mixed oxide catalysts. Applied Catalysis B: Environmental, 162: 227–235

[32] Zeng L P, Li K Z, Huang F, Zhu X, Li H C (2016). Effects of Co₃O₄ nanocatalyst morphology on CO oxidation: Synthesis process map and catalytic activity. Chinese Journal of Catalysis, 37(6): 908–922

[33] Zhang C H, Wang C, Gil S, Boreave A, Retailleau L, Guo Y L, Valverde J L, Giroir-Fendler A (2017). Catalytic oxidation of 1,2-dichloropropane over supported LaMnO_x oxides catalysts. Applied Catalysis B: Environmental, 201: 552–560

[34] Zhang X, Wang Z, Tang Y Y, Qiao N L, Li Y, Qu S Q, Hao Z P (2015). Catalytic behaviors of combined oxides derived from Mg/Al_xFe_1–x–Cl layered double hydroxides for H₂S selective oxidation. Catalysis Science & Technology, 5(11): 4991–4999

[35] Zhu Z Z, Lu G Z, Zhang Z G, Guo Y, Guo Y L, Wang Y Q (2013). Highly active and stable Co₃O₄/ZSM-5 catalyst for propane oxidation: Effect of the preparation method. ACS Catalysis, 3(6): 1154–1164

Acknowledgements

This work is financially supported by the National Natural Science Foundation of China (Grant Nos. 21677160 and 21477149) and Beijing Municipal Science & Technology Commission (Nos. Z181100000118003 and Z181100005418011).

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://doi.org/10.1007/s11783-020-1284-3 and is accessible for authorized users.

RIGHTS & PERMISSIONS

2020 Higher Education Press