Discovery of single-atom alloy catalysts for CO2-to-methanol reaction by density functional theory calculations

被引:29
作者
Li, Meng [1 ]
Hua, Bin [1 ]
Wang, Lu-Cun [1 ]
Zhou, Zheng [1 ,2 ]
Stowers, Kara J. [2 ]
Ding, Dong [1 ]
机构
[1] Idaho Natl Lab, Energy & Environm Sci & Technol, Idaho Falls, ID 83415 USA
[2] Brigham Young Univ, Dept Chem & Biochem, C100 BNSN Bldg, Provo, UT 84604 USA
关键词
CO2-to-methanol; Single-atom alloy; Density functional theory; Charge redistribution; ELASTIC BAND METHOD; CO2; CONVERSION; HYDROGENATION; METHANOL; REDUCTION; ENERGY; TECHNOLOGY; DYNAMICS; INDUSTRY;
D O I
10.1016/j.cattod.2020.04.059
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
The transformations of CO2 molecules into valuable products are of increasing interest due to the negative impact of anthropogenic CO2 emissions on global warming. The CO2-to-methanol hydrogenation is an economically profitable reaction of carbon fixation, but it still steps away from widespread industrialization because of the lack of efficient and selective catalysts. Recently, single-atom alloy (SAA) catalysts have been developed to work remarkably in CO2 hydrogenation reactions. Doping isolated single atoms into metallic catalyst can dramatically alter the catalytic performance of the host. We have performed a screening discovery on Ru and 6 RuX (X = Fe, Co, Ni, Cu, Ir and Pt) SAAs using density functional theory (DFT) computations. We considered 13 possible elementary reactions in 4 possible reaction pathways on Ru and all RuX surfaces. In the computed mechanisms, we found that the formation of *H2COOH and *HCOO intermediates plays a critical role in determining catalysts' activities. Doping Co and Pt isolated single atoms into Ru surface can thermodynamically and kinetically facilitate these intermediates formation processes, eventually promoting the production of methanol. The combination of weak binding and enhanced charge redistribution on RuCo and RuPt surfaces give them improved catalytic activities over pure Ru. This work will ultimately facilitate the discovery and development of SAAs for CO2 to methanol, serving as guidance to experiments and theoreticians alike.
引用
收藏
页码:403 / 409
页数:7
相关论文
共 43 条
[1]   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
[2]  
Ahmad K, 2019, INTEGR GREEN CHEM SU, P57, DOI [10.1002/9781119509868.ch3, DOI 10.1002/9781119509868.CH3]
[3]   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
[4]   Selective solar-driven reduction of CO2 to methanol using a catalyzed p-GaP based photoelectrochemical cell [J].
Barton, Emily E. ;
Rampulla, David M. ;
Bocarsly, Andrew B. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2008, 130 (20) :6342-+
[5]   A review of technology and policy deep decarbonization pathway options for making energy-intensive industry production consistent with the Paris Agreement [J].
Bataille, Chris ;
Ahman, Max ;
Neuhoff, Karsten ;
Nilsson, Lars J. ;
Fischedick, Manfred ;
Lechtenboehmer, Stefan ;
Solano-Rodriquez, Baltazar ;
Denis-Ryan, Amandine ;
Stiebert, Seton ;
Waisman, Henri ;
Sartor, Oliver ;
Rahbar, Shahrzad .
JOURNAL OF CLEANER PRODUCTION, 2018, 187 :960-973
[6]   Catalysis for CO2 conversion: a key technology for rapid introduction of renewable energy in the value chain of chemical industries [J].
Centi, Gabriele ;
Quadrelli, Elsje Alessandra ;
Perathoner, Siglinda .
ENERGY & ENVIRONMENTAL SCIENCE, 2013, 6 (06) :1711-1731
[7]   Using a One-Electron Shuttle for the Multielectron Reduction of CO2 to Methanol: Kinetic, Mechanistic, and Structural Insights [J].
Cole, Emily Barton ;
Lakkaraju, Prasad S. ;
Rampulla, David M. ;
Morris, Amanda J. ;
Abelev, Esta ;
Bocarsly, Andrew B. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2010, 132 (33) :11539-11551
[8]   CO2GeoNet actions in Europe for advancing CCUS through global cooperation [J].
Czernichowski-Lauriol, Isabelle ;
Berenblyum, Roman ;
Bigi, Sabina ;
Car, Marjeta ;
Gastine, Marie ;
Persoglia, Sergio ;
Poulsen, Niels ;
Schmidt-Hattenberger, Cornelia ;
Stead, Rowena ;
Vincent, Ceri J. ;
Wildenborg, Ton .
APPLIED ENERGY SYMPOSIUM AND FORUM, CARBON CAPTURE, UTILIZATION AND STORAGE, CCUS 2018, 2018, 154 :73-79
[9]   A novel low-thermal-budget approach for the co-production of ethylene and hydrogen via the electrochemical non-oxidative deprotonation of ethane [J].
Ding, Dong ;
Zhang, Yunya ;
Wu, Wei ;
Chen, Dongchang ;
Liu, Meilin ;
He, Ting .
ENERGY & ENVIRONMENTAL SCIENCE, 2018, 11 (07) :1710-1716
[10]   A-site deficient perovskite with nano-socketed Ni-Fe alloy particles as highly active and durable catalyst for high-temperature CO2 electrolysis [J].
Ding, Shaochen ;
Li, Meng ;
Pang, Wanying ;
Hua, Bin ;
Duan, Nanqi ;
Zhang, Ya-Qian ;
Zhang, Sheng-Nian ;
Jin, Zhehui ;
Luo, Jing-Li .
ELECTROCHIMICA ACTA, 2020, 335