Synthesis of GaN-ZnO/MCM-41 for catalyzing CO<sub>2</sub>-based oxidative dehydrogenation of propane to propene

Related Articles

Guide

Abstract The oxidative dehydrogenation of propane to propene in the presence of CO₂ (CO₂-OPDH) is considered as a desirable route for propene production, and the development of catalyst with high performance is the key to get a breakthrough in this process. Here, the GaN-ZnO/MCM-41 catalysts with dual-function active sites were constructed via a solid-state nitridation method with GaN-ZnO solid solution as the active component supporting on mesoporous MCM-41. Their catalytic performances for CO₂-OPDH reaction were further evaluated. The physicochemical properties of obtained catalysts were characterized by a series of techniques such as X-ray diffraction spectroscopy (XRD), N₂ adsorption-desorption measurements, field-emission scanning electron microscopy equipped with an energy dispersive X-ray instrument (SEM-EDX), transmission electron microscopy (TEM),thermogravimetric-mass spectra (TG-MS) and Raman spectra. It is found that the solid solution catalyst can be successfully prepared in a solid-state nitridation method, the propane dehydrogenation activity of which is superior to that of the supported single-component GaN or ZnO catalysts under the same testing conditions. Among them, the Ga_0.5-Zn_0.5/MCM-41 catalyst delivers a propane conversion of 22% with the selectivity of 92% towards propene at 600 ℃ in the CO₂ atmosphere. This excellent catalytic performance could be attributed to the formation of solid solution structure, which was beneficial to the dispersion of active components and the generation of more active sites. The calcination temperature influenced the structure of solid solution and thus affected its catalytic activity. In addition, CO₂ can not only increase the activity of the catalyst, but also improve its stability by declining the coke formation in PDH reaction.

	Service

	Email this article
	Add to my bookshelf
	Add to citation manager
	Email Alert
	RSS
	Articles by authors
	LIU Haiwei
	SONG Chengxuan
	YU Fang
	SONG Jian
	WANG Zhipeng
	WANG Liyan
	LI Yu
	WANG Pengfei
	CUI Jian

Keywords： gallium nitride zinc oxide solid solution propane dehydrogenation CO₂

Received 2023-03-17;

Fund:

About author:

Cite this article:

LIU Haiwei, SONG Chengxuan, YU Fang, SONG Jian, WANG Zhipeng, WANG Liyan, LI Yu, WANG Pengfei, CUI Jian.Synthesis of GaN-ZnO/MCM-41 for catalyzing CO₂-based oxidative dehydrogenation of propane to propene[J] Chemcial Industry and Engineering, 2023,V40(6): 37-44

[1] SATTLER J J H B, RUIZ-MARTINEZ J, SANTILLAN-JIMENEZ E, et al. Catalytic dehydrogenation of light alkanes on metals and metal oxides[J]. Chemical Reviews, 2014, 114(20): 10613-10653
[2] ZHOU S, ZHOU Y, SHI J, et al. Synthesis of Ce-doped mesoporous γ-alumina with enhanced catalytic performance for propane dehydrogenation[J]. Journal of Materials Science, 2015, 50(11): 3984-3993
[3] SONG Y, LIU G, YUAN Z. N-, P- and B-doped mesoporous carbons for direct dehydrogenation of propane[J]. RSC Advances, 2016, 6(97): 94636-94642
[4] LIU L, ZHU Y P, SU M, et al. Metal-free carbonaceous materials as promising heterogeneous catalysts[J]. ChemCatChem, 2015, 7(18): 2765-2787
[5] LI Z, PETERS A W, BERNALES V, et al. Metal-organic framework supported cobalt catalysts for the oxidative dehydrogenation of propane at low temperature[J]. ACS Central Science, 2017, 3(1): 31-38
[6] 杜凯敏, 范杰. 丙烷氧化脱氢制丙烯研究进展[J]. 化工进展, 2019, 38(6): 2697-2706 DU Kaimin, FAN Jie. Research progress on oxidative dehydrogenation of propane to propene[J]. Chemical Industry and Engineering Progress, 2019, 38(6): 2697-2706(in Chinese)
[7] VU B K, SONG M, AHN I Y, et al. Location and structure of coke generated over Pt-Sn/Al₂O₃ in propane dehydrogenation[J]. Journal of Industrial and Engineering Chemistry, 2011, 17(1): 71-76
[8] ZHANG Y, ZHOU Y, WAN L, et al. Effect of magnesium addition on catalytic performance of PtSnK/γ-Al₂O₃ catalyst for isobutane dehydrogenation[J]. Fuel Processing Technology, 2011, 92(8): 1632-1638
[9] ATANGA M A, REZAEI F, JAWAD A, et al. Oxidative dehydrogenation of propane to propylene with carbon dioxide[J]. Applied Catalysis B: Environmental, 2018, 220: 429-445
[10] KORZYŃSKI M D, DINCǍ M. Oxidative dehydrogenation of propane in the realm of metal-organic frameworks[J]. ACS Central Science, 2017, 3(1): 10-12
[11] PRAKASH N, LEE M H, YOON S, et al. Role of acid solvent to prepare highly active PtSn/θ-Al₂O₃ catalysts in dehydrogenation of propane to propylene[J]. Catalysis Today, 2017, 293/294: 33-41
[12] WANG G, ZHU X, LI C. Recent progress in commercial and novel catalysts for catalytic dehydrogenation of light alkanes[J]. The Chemical Record, 2020, 20(6): 604-616
[13] ZHANG L, WANG Z, SONG J, et al. Facile synthesis of SiO₂ supported GaN as an active catalyst for CO₂ enhanced dehydrogenation of propane[J]. Journal of CO₂ Utilization, 2020, 38: 306-313
[14] CHEN C, HU Z, REN J, et al. ZnO nanoclusters supported on dealuminated zeolite β as a novel catalyst for direct dehydrogenation of propane to propylene[J]. ChemCatChem, 2019, 11(2): 868-877
[15] ZHAO D, LI Y, HAN S, et al. ZnO nanoparticles encapsulated in nitrogen-doped carbon material and silicalite-1 composites for efficient propane dehydrogenation[J]. iScience, 2019, 13: 269-276
[16] WANG G, LI C, SHAN H. Catalytic dehydrogenation of isobutane over a Ga₂O₃/ZnO interface: Reaction routes and mechanism[J]. Catalysis Science & Technology, 2016, 6(9): 3128-3136
[17] MAPA M, SIVARANJANI K, BHANGE D S, et al. Structure, electronic structure, optical, and dehydrogenation catalytic study of (Zn_1-zIn_z)(O_1-xN_x) solid solution[J]. Chemistry of Materials, 2010, 22(2): 565-578
[18] MAEDA K, TAKATA T, HARA M, et al. GaN: ZnO solid solution as a photocatalyst for visible-light-driven overall water splitting[J]. Journal of the American Chemical Society, 2005, 127(23): 8286-8287
[19] LI J, LIU B, YANG W, et al. Solubility and crystallographic facet tailoring of (GaN)_1-x(ZnO)_x pseudobinary solid-solution nanostructures as promising photocatalysts[J]. Nanoscale, 2016, 8(6): 3694-3703
[20] TONGYING P, LU Y, HALL L M G, et al. Control of elemental distribution in the nanoscale solid-state reaction that produces (Ga_1-xZn_x)(N_1-xO_x) nanocrystals[J]. ACS Nano, 2017, 11(8): 8401-8412
[21] LENG B, ZHANG X, CHEN S, et al. Highly efficient visible-light photocatalytic degradation and antibacterial activity by GaN: ZnO solid solution nanoparticles[J]. Journal of Materials Science & Technology, 2021, 94: 67-76
[22] QIN J, LI B, ZHANG W, et al. Synthesis, characterization and catalytic performance of well-ordered mesoporous Ni-MCM-41 with high nickel content[J]. Microporous and Mesoporous Materials, 2015, 208: 181-187
[23] LIU G, ZENG L, ZHAO Z, et al. Platinum-modified ZnO/Al₂O₃ for propane dehydrogenation: Minimized platinum usage and improved catalytic stability[J]. ACS Catalysis, 2016, 6(4): 2158-2162