Co-Fe Clusters Supported on N-Doped Graphitic Carbon as Highly Selective Catalysts for Reverse Water Gas Shift Reaction

被引:24
作者
Peng, Lu [1 ]
Jurca, Bogdan [2 ]
Primo, Ana [1 ]
Gordillo, Alvaro [3 ]
Parvulescu, Vasile, I [2 ]
Garcia, Hermenegildo [1 ]
机构
[1] Univ Politecn Valencia, CSIC, Inst Univ Tecnol Quim, Valencia 46022, Spain
[2] Univ Bucharest, Fac Chem, Dept Organ Chem & Biochem & Catalysis, Bucharest 030016, Romania
[3] BASF SE, D-67056 Ludwigshafen, Germany
关键词
heterogeneous catalysis; CO2; utilization; reverse water gas shift; graphene as support; selective Co-Fe alloy nanoparticles; DEFECTIVE GRAPHENE; HYDROGENATION; CHITOSAN; NANOPARTICLES; NANOCLUSTERS; PERFORMANCE; KINETICS; BIOMASS; SINGLE; OXIDE;
D O I
10.1021/acssuschemeng.1c01401
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Graphitic carbons are suitable supports of metal nanoparticles with catalytic activity. In the present study, the preparation of N-doped graphitic carbon supporting clusters of Fe-Co alloys starting from biomass waste is reported. These sub-nanometric Co-Fe clusters supported on N-doped graphitic carbon at a metal loading below 0.2 wt % exhibit high activity for the selective hydrogenation of CO2 to CO. Operating at 500 degrees C and 10 bar with an H-2/CO2 molar ratio of 7 and a space velocity of 600 h(-1), a conversion of 56% with a selectivity of over 98% to CO, and remarkable stability over 30 h operation was obtained. Interestingly, analogous catalysts based on N-doped graphitic carbon with much higher Co-Fe loadings and an average particle size range of 1-5 nm exhibit only half of this activity, with similar CO selectivity. This contrasting behavior reveals the dramatic effect of the particle size on the catalytic activity. In comparison, SiO2 as support under similar conditions affords CH4 as the main product.
引用
收藏
页码:9264 / 9272
页数:9
相关论文
共 44 条
[11]   Binding of Pt Nanoclusters to Point Defects in Graphene: Adsorption, Morphology, and Electronic Structure [J].
Fampiou, Ioanna ;
Ramasubramaniam, Ashwin .
JOURNAL OF PHYSICAL CHEMISTRY C, 2012, 116 (11) :6543-6555
[12]   Supported Catalysts for CO2 Methanation: A Review [J].
Frontera, Patrizia ;
Macario, Anastasia ;
Ferraro, Marco ;
Antonucci, PierLuigi .
CATALYSTS, 2017, 7 (02)
[13]   Difference in the selectivity of CO and CO2 methanation reactions [J].
Fujita, SI ;
Takezawa, N .
CHEMICAL ENGINEERING JOURNAL, 1997, 68 (01) :63-68
[14]   Support effects in metal catalysis: a study of the behavior of unsupported and silica-supported cobalt catalysts in the hydrogenation of CO2 at atmospheric pressure [J].
Garbarino, Gabriella ;
Cavattoni, Tullio ;
Riani, Paola ;
Busca, Guido .
CATALYSIS TODAY, 2020, 345 :213-219
[15]   Kinetic study of the reverse water-gas shift reaction over CuO/ZnO/Al2O3 catalysts [J].
Gines, MJL ;
Marchi, AJ ;
Apesteguia, CR .
APPLIED CATALYSIS A-GENERAL, 1997, 154 (1-2) :155-171
[16]   Facile fabrication of MOF-derived octahedral CuO wrapped 3D graphene network as binder-free anode for high performance lithium-ion batteries [J].
Ji, Dong ;
Zhou, Hu ;
Tong, Yongli ;
Wang, Jinpei ;
Zhu, Meizhou ;
Chen, Tianhui ;
Yuan, Aihua .
CHEMICAL ENGINEERING JOURNAL, 2017, 313 :1623-1632
[17]   N-Doped Defective Graphene from Biomass as Catalyst for CO2 Hydrogenation to Methane [J].
Jurca, Bogdan ;
Bucur, Cristina ;
Primo, Ana ;
Concepcion, Patricia ;
Parvulescu, Vasile I. ;
Garcia, Hermenegildo .
CHEMCATCHEM, 2019, 11 (03) :985-990
[18]   CATALYSIS Active sites for CO2 hydrogenation to methanol on Cu/ZnO catalysts [J].
Kattel, Shyam ;
Ramirez, Pedro J. ;
Chen, Jingguang G. ;
Rodriguez, Jose A. ;
Liu, Ping .
SCIENCE, 2017, 355 (6331) :1296-+
[19]   The synthesis of a hybrid graphene-nickel/manganese mixed oxide and its performance in lithium-ion batteries [J].
Latorre-Sanchez, Marcos ;
Atienzar, Pedro ;
Abellan, Gonzalo ;
Puche, Marta ;
Fornes, Vicente ;
Ribera, Antonio ;
Garcia, Hermenegildo .
CARBON, 2012, 50 (02) :518-525
[20]   A short review of recent advances in CO2 hydrogenation to hydrocarbons over heterogeneous catalysts [J].
Li, Wenhui ;
Wang, Haozhi ;
Jiang, Xiao ;
Zhu, Jie ;
Liu, Zhongmin ;
Guo, Xinwen ;
Song, Chunshan .
RSC ADVANCES, 2018, 8 (14) :7651-7669