Low-temperature efficient catalytic oxidation of acetonitrile over Cu and Ce co-doped perovskite-type LaMnO3 catalyst

被引:0
作者
Wei, Yanyu [1 ]
Li, Yonghong [1 ]
机构
[1] Tianjin Univ, Sch Chem Engn & Technol, Minist Educ, Key Lab Green Chem Technol, Tianjin 300350, Peoples R China
基金
中国国家自然科学基金;
关键词
Perovskite catalysts; Acetonitrile oxidation; Cu-Ce co-doping; Low-temperature catalysis; Dual-path reaction mechanism; ENHANCED ACTIVITY; MIXED OXIDES; NO; PERFORMANCE; COMBUSTION; REDUCTION; MN; ACRYLONITRILE; ADSORPTION; REMOVAL;
D O I
10.1016/j.apcata.2025.120250
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
This work develops Cu and Ce co-doped LaMnO3 perovskite catalysts via sol-gel synthesis for low-temperature catalytic oxidation of toxic acetonitrile. Optimized La0.9Ce0.1Mn0.9Cu0.1O3 achieved 90 % acetonitrile conversion at 215 degrees C with N-2 selectivity > 98 %, surpassing monometallic counterparts. Structural analysis revealed that Cu/Ce co-doping induced lattice distortion and oxygen vacancy formation, enhancing O-2 activation and Mn3 +/Mn4+ redox cycling. In-situ DRIFT studies unveiled a dual reaction pathway: hydrolysis-dominated conversion to acetamide/NH3 at low temperatures (<200 degrees C) and oxidation-driven -NCO intermediate formation at elevated temperatures. Significantly, NH3 generated from hydrolysis participated in in-situ selective catalytic reduction of NOx to N-2, minimizing secondary pollution. The catalyst maintained robust stability under industrial conditions (GHSV = 300,000 h(-1)) after thermal cycling. This work provides mechanistic insights into perovskite-mediated nitrile degradation and demonstrates a design strategy for energy-efficient emission control systems targeting industrial HCN/acrylonitrile pollutants.
引用
收藏
页数:17
相关论文
共 62 条
[1]   Three-dimensionally ordered macroporous La0.6Sr0.4MnO3 with high surface areas: Active catalysts for the combustion of methane [J].
Arandiyan, Hamidreza ;
Dai, Hongxing ;
Deng, Jiguang ;
Liu, Yuxi ;
Bai, Bingyang ;
Wang, Yuan ;
Li, Xinwei ;
Xie, Shaohua ;
Li, Junhua .
JOURNAL OF CATALYSIS, 2013, 307 :327-339
[2]   Study of the hydrolysis of acetonitrile using different Bronsted acid models:: Zeolite-type and HCl(H2O)x clusters [J].
Barbosa, LAMM ;
van Santen, RA .
JOURNAL OF CATALYSIS, 2000, 191 (01) :200-217
[3]   Photo-redox reactions of dicarboxylates and α-hydroxydicarboxylates at the surface of Fe(III)(hydr)oxides followed with in situ ATR-FTIR spectroscopy [J].
Borer, Paul ;
Hug, Stephan J. .
JOURNAL OF COLLOID AND INTERFACE SCIENCE, 2014, 416 :44-53
[4]   Removal and recovery of nitriles from gaseous streams: An IR study of acetonitrile adsorption on and desorption from inorganic solids [J].
Busca, Guido ;
Montanari, Tania ;
Bevilacqua, Maria ;
Finocchio, Elisabetta .
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS, 2008, 320 (1-3) :205-212
[5]   The influence of nonstoichiometry on LaMnO3 perovskite for catalytic NO oxidation [J].
Chen, Jiahao ;
Shen, Meiqing ;
Wang, Xinquan ;
Qi, Gongshin ;
Wang, Jun ;
Li, Wei .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2013, 134 :251-257
[6]   DRIFT Study on Cerium-Tungsten/Titiania Catalyst for Selective Catalytic Reduction of NOx with NH3 [J].
Chen, Liang ;
Li, Junhua ;
Ge, Maofa .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2010, 44 (24) :9590-9596
[7]   Enhanced activity for catalytic oxidation of 1,2-dichloroethane over Al-substituted LaMnO3 perovskite catalysts [J].
Chen, Shu-Xia ;
Wang, Yu ;
Jia, Ai-Ping ;
Liu, Huan-Huan ;
Luo, Meng-Fei ;
Lu, Ji-Qing .
APPLIED SURFACE SCIENCE, 2014, 307 :178-188
[8]   INFRARED SPECTROSCOPIC STUDY OF ACRYLONITRILE ADSORBED ON MORDENITE ZEOLITES .1. SURFACE INTERACTION OF C=N TRIPLE BOND [J].
CHONG, PJ ;
CURTHOYS, G .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS I, 1981, 77 :1639-1648
[9]   Adsorption and photochemistry of CH3CN and CH3CONH2 on powdered TiO2 [J].
Chuang, CC ;
Wu, WC ;
Lee, MX ;
Lin, JL .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2000, 2 (17) :3877-3882
[10]   Recent Advances in the Catalytic Oxidation of Volatile Organic Compounds: A Review Based on Pollutant Sorts and Sources [J].
He, Chi ;
Cheng, Jie ;
Zhang, Xin ;
Douthwaite, Mark ;
Pattisson, Samuel ;
Hao, Zhengping .
CHEMICAL REVIEWS, 2019, 119 (07) :4471-4568