Efficient metal borate catalysts for oxidative dehydrogenation of propane

被引:14
作者
Qian, Heming [1 ]
Sun, Fulin [1 ]
Zhang, Wei [1 ]
Huang, Chao [2 ]
Wang, Yingjun [1 ]
Fang, Kegong [2 ]
机构
[1] Northeast Petr Univ, Coll Chem & Chem Engn, Daqing 163318, Peoples R China
[2] Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Peoples R China
关键词
SILICA-SUPPORTED BORON; CRYSTAL-STRUCTURE; OXIDE CATALYSTS; LIGHT ALKANES; NITRIDE; B-11; GLASSES; PERFORMANCE; SELECTIVITY; OLEFINS;
D O I
10.1039/d1cy01792f
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Boron-based catalysts have attracted attention in recent years, due to their high selectivity for light olefins in the catalytic oxidative dehydrogenation of propane (ODHP). But they still face drawbacks such as low activity at mild reaction temperature and more or less boron leaching from the catalyst surface during the reaction. Hence, it is necessary to exploit more efficient boron-based catalysts with higher stability. In this study, metal borate catalysts (CoB4O7 and Ni3B2O6) were prepared by a co-precipitation method and evaluated for the ODHP. Reaction tests showed that both metal borates could catalyze propane dehydrogenation efficiently at 450-540 degrees C with high selectivity and stability. In particular, the CoB4O7 catalyst, after activation at 490 degrees C for 70 h, exhibited rather high stability with propane conversion of 17.6% and an appreciable selectivity for light olefins of 91.4% during the subsequent reaction run. The structural stability and active sites of the metal borate catalysts were investigated by SEM, TEM, XRD, FTIR, ICP-MS and XPS. The results showed that the morphology and crystal structure of the catalysts as well as the composition of bulk and surface elements changed little after reaction, showing excellent structural stability. Besides, the M-B-O (M = Co, Ni) and B-OH species on the catalysts surface were considered to be the active sites, which gradually increased and reached an abundant content without boron leaching during the induction period of the catalysts, affording the high catalytic activity and selectivity for light olefins.
引用
收藏
页码:1996 / 2005
页数:10
相关论文
共 55 条
[31]   HP-KB3O5 Highlights the Structural Diversity of Borates: Corner-Sharing BO3/BO4 Groups in Combination with Edge-Sharing BO4 Tetrahedra [J].
Neumair, Stephanie C. ;
Vanicek, Stefan ;
Kaindl, Reinhard ;
Toebbens, Daniel M. ;
Martineau, Charlotte ;
Taulelle, Francis ;
Senker, Juergen ;
Huppertz, Hubert .
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY, 2011, (27) :4147-4152
[32]   High-pressure synthesis and crystal structure of the lithium borate HP-LiB3O5 [J].
Neumair, Stephanie C. ;
Vanicek, Stefan ;
Kaindl, Reinhard ;
Toebbens, Daniel M. ;
Wurst, Klaus ;
Huppertz, Hubert .
JOURNAL OF SOLID STATE CHEMISTRY, 2011, 184 (09) :2490-2497
[33]   High-Pressure Syntheses, Crystal Structures, and Properties of the Transition Metal Borates β-MB4O7 (M = Fe, Co) [J].
Neumair, Stephanie C. ;
Knyrim, Johanna S. ;
Glaum, Robert ;
Huppertz, Hubert .
ZEITSCHRIFT FUR ANORGANISCHE UND ALLGEMEINE CHEMIE, 2009, 635 (12) :2002-2008
[34]   Oxidative dehydrogenation of propane using layered borosilicate zeolite as the active and selective catalyst [J].
Qiu, Bin ;
Jiang, Fan ;
Lu, Wen-Duo ;
Yan, Bing ;
Li, Wen-Cui ;
Zhao, Zhen-Chao ;
Lu, An-Hui .
JOURNAL OF CATALYSIS, 2020, 385 :176-182
[35]   Crystallographic investigation of the Co-B-O system [J].
Rowsell, JLC ;
Taylor, NJ ;
Nazar, LF .
JOURNAL OF SOLID STATE CHEMISTRY, 2003, 174 (01) :189-197
[36]   Oxidative dehydrogenation of light alkanes to olefins on metal-free catalysts [J].
Sheng, Jian ;
Yan, Bing ;
Lu, Wen-Duo ;
Qiu, Bin ;
Gao, Xin-Qian ;
Wang, Dongqi ;
Lu, An-Hui .
CHEMICAL SOCIETY REVIEWS, 2021, 50 (02) :1438-1468
[37]   Progress in selective oxidative dehydrogenation of light alkanes to olefins promoted by boron nitride catalysts [J].
Shi, Lei ;
Wang, Yang ;
Yan, Bing ;
Song, Wei ;
Shao, Dan ;
Lu, An-Hui .
CHEMICAL COMMUNICATIONS, 2018, 54 (78) :10936-10946
[38]   A viewpoint on catalytic origin of boron nitride in oxidative dehydrogenation of light alkanes [J].
Shi, Lei ;
Wang, Dongqi ;
Lu, An-Hui .
CHINESE JOURNAL OF CATALYSIS, 2018, 39 (05) :908-913
[39]   Edge-hydroxylated Boron Nitride for Oxidative Dehydrogenation of Propane to Propylene [J].
Shi, Lei ;
Wang, Dongqi ;
Song, Wei ;
Shao, Dan ;
Zhang, Wei-Ping ;
Lu, An-Hui .
CHEMCATCHEM, 2017, 9 (10) :1788-1793
[40]   An Amorphous Cobalt Borate Nanosheet-Coated Cobalt Boride Hybrid for Highly Efficient Alkaline Water Oxidation Reaction [J].
Tan, Tan ;
Han, Pengyu ;
Cong, Hengjiang ;
Cheng, Gongzhen ;
Luo, Wei .
ACS SUSTAINABLE CHEMISTRY & ENGINEERING, 2019, 7 (06) :5620-5625