Computational Approaches to the Chemical Conversion of Carbon Dioxide

被引:155
作者
Cheng, Daojian [1 ]
Negreiros, Fabio R. [2 ]
Apra, Edoardo [3 ]
Fortunelli, Alessandro [2 ]
机构
[1] Beijing Univ Chem Technol, Div Mol & Mat Simulat, State Key Lab Organ Inorgan Composites, Beijing 100029, Peoples R China
[2] CNR, IPCF, I-56124 Pisa, Italy
[3] Pacific NW Natl Lab, William R Wiley Environm Mol Sci Lab Battelle, Richland, WA 99352 USA
基金
中国国家自然科学基金; 欧洲研究理事会;
关键词
catalysts; density functional theory; hydrogenation; reaction mechanisms; reduction; WATER-GAS-SHIFT; DENSITY-FUNCTIONAL THEORY; CATALYZED ELECTROCHEMICAL REDUCTION; TRANSITION-METAL CATALYSTS; CO2; HYDROGENATION; METHANOL SYNTHESIS; REACTION-MECHANISM; FORMIC-ACID; PHOTOCATALYTIC CONVERSION; RUTHENIUM(II)-CATALYZED HYDROGENATION;
D O I
10.1002/cssc.201200872
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The conversion of CO2 into fuels and chemicals is viewed as an attractive route for controlling the atmospheric concentration and recycling of this greenhouse gas, but its industrial application is limited by the low selectivity and activity of the current catalysts. Theoretical modeling, in particular density functional theory (DFT) simulations, provides a powerful and effective tool to discover chemical reaction mechanisms and design new catalysts for the chemical conversion of CO2, overcoming the repetitious and time/labor consuming trial-and-error experimental processes. In this article we give a comprehensive survey of recent advances on mechanism determination by DFT calculations for the catalytic hydrogenation of CO2 into CO, CH4, CH3OH, and HCOOH, and CO2 methanation, as well as the photo- and electrochemical reduction of CO2. DFT-guided design procedures of new catalytic systems are also reviewed, and challenges and perspectives in this field are outlined.
引用
收藏
页码:944 / 965
页数:22
相关论文
共 219 条
[1]   Reduction of CO2 on a Tricarbonyl Rhenium(I) Complex: Modeling a Catalytic Cycle [J].
Agarwal, Jay ;
Johnson, Richard P. ;
Li, Gonghu .
JOURNAL OF PHYSICAL CHEMISTRY A, 2011, 115 (13) :2877-2881
[2]   Iridium catalyzed hydrogenation of CO2 under basic conditions-Mechanistic insight from theory [J].
Ahlquist, Marten S. G. .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2010, 324 (1-2) :3-8
[3]   Toward computational screening in heterogeneous catalysis: Pareto-optimal methanation catalysts [J].
Andersson, MP ;
Bligaard, T ;
Kustov, A ;
Larsen, KE ;
Greeley, J ;
Johannessen, T ;
Christensen, CH ;
Norskov, JK .
JOURNAL OF CATALYSIS, 2006, 239 (02) :501-506
[4]   Electrocatalytic CO2 Conversion to Oxalate by a Copper Complex [J].
Angamuthu, Raja ;
Byers, Philip ;
Lutz, Martin ;
Spek, Anthony L. ;
Bouwman, Elisabeth .
SCIENCE, 2010, 327 (5963) :313-315
[5]  
[Anonymous], 2009, ANGEW CHEM INT ED, V48, P1467
[6]  
[Anonymous], 2010, ANGEW CHEM INT ED, V49, P9822
[7]  
[Anonymous], 2007, ANGEW CHEM INT ED, V46, P7324
[8]   Carbon supports for low-temperature fuel cell catalysts [J].
Antolini, Ermete .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2009, 88 (1-2) :1-24
[9]  
Auerbach S. M., 2003, HDB ZEOLITE SCI TECH
[10]   Epitaxy, truncations, and overhangs in palladium nanoclusters adsorbed on MgO(001) [J].
Barcaro, G. ;
Fortunelli, A. ;
Rossi, G. ;
Nita, F. ;
Ferrando, R. .
PHYSICAL REVIEW LETTERS, 2007, 98 (15)