Dual-atom Ag2/graphene catalyst for efficient electroreduction of CO2 to CO

Li, Yifan; Chen, Chang; Cao, Rui; Pan, Ziwei; He, Hua; Zhou, Kebin

doi:10.1016/j.apcatb.2020.118747

Dual-atom Ag₂/graphene catalyst for efficient electroreduction of CO₂ to CO

Journal Article · Mon Feb 10 00:00:00 EST 2020 · Applied Catalysis B: Environmental

DOI:https://doi.org/10.1016/j.apcatb.2020.118747· OSTI ID:1616714

Li, Yifan ^[1]; Chen, Chang ^[1]; ^[2]; Pan, Ziwei ^[1]; He, Hua ^[1]; Zhou, Kebin ^[1]

Univ. of Chinese Academy of Sciences, Beijing (China)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)

Electrochemical reduction of CO₂ into value-added carbon compounds offers a promising strategy to mitigate global warming, but present challenges for chemistry due to the poor selectivity and stability of electrocatalysts. In this work, we report a dual-atom Ag₂/graphene catalyst featuring well-defined AgN₃-AgN₃ active site for CO₂ electrochemical reduction. This dual-atom catalyst can drive CO₂ reduction reaction at a potential as high as -0.25 V, and exhibit excellent CO Faradic efficiency up to 93.4 % with a current density of 11.87 mA cm^-2 at -0.7 V and long-term stability, far surpassing the single-atom Ag₁/graphene and the traditional silver nanoparticle catalysts. Finally, DFT calculations reveal that the dual-atom Ag site lowers the barrier for the formation of *COOH by stabilizing the *CO₂ through the concomitant interactions with the C and an O atom of CO₂, resulting in excellent catalytic performance.

View Accepted Manuscript (DOE)

Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: National Natural Science Foundation of China (NNSFC); USDOE

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1616714

Journal Information:: Applied Catalysis B: Environmental, Journal Name: Applied Catalysis B: Environmental Journal Issue: C Vol. 268; ISSN 0926-3373

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (54)

Atomic Resolution of the Structure of a Metal-Support Interface: Triosmium Clusters on MgO(110) Kulkarni, Apoorva; Chi, Miaofang; Ortalan, Volkan Angewandte Chemie International Edition, Vol. 49, Issue 52 https://doi.org/10.1002/anie.201005105	journal	November 2010
Regulation of Coordination Number over Single Co Sites: Triggering the Efficient Electroreduction of CO ₂ Wang, Xiaoqian; Chen, Zhao; Zhao, Xuyan Angewandte Chemie International Edition, Vol. 57, Issue 7 https://doi.org/10.1002/anie.201712451	journal	January 2018
Isolated Diatomic Ni-Fe Metal-Nitrogen Sites for Synergistic Electroreduction of CO ₂ Ren, Wenhao; Tan, Xin; Yang, Wanfeng Angewandte Chemie International Edition, Vol. 58, Issue 21 https://doi.org/10.1002/anie.201901575	journal	April 2019
Highly Selective and Stable Reduction of CO ₂ to CO by a Graphitic Carbon Nitride/Carbon Nanotube Composite Electrocatalyst Lu, Xunyu; Tan, Tze Hao; Ng, Yun Hau Chemistry – A European Journal, Vol. 22, Issue 34 https://doi.org/10.1002/chem.201601674	journal	July 2016
A Core-Shell-Structured Silver Nanowire/Nitrogen-Doped Carbon Catalyst for Enhanced and Multifunctional Electrofixation of CO ₂ Yang, Heng-Pan; Zhang, Han-Wen; Wu, Yu ChemSusChem, Vol. 11, Issue 22 https://doi.org/10.1002/cssc.201801612	journal	September 2018
Semiempirical GGA-type density functional constructed with a long-range dispersion correction Grimme, Stefan Journal of Computational Chemistry, Vol. 27, Issue 15, p. 1787-1799 https://doi.org/10.1002/jcc.20495	journal	January 2006
Highly electrically conductive adhesives using silver nanoparticle (Ag NP)-decorated graphene: the effect of NPs sintering on the electrical conductivity improvement Meschi Amoli, Behnam; Trinidad, Josh; Hu, Anming Journal of Materials Science: Materials in Electronics, Vol. 26, Issue 1 https://doi.org/10.1007/s10854-014-2440-y	journal	November 2014
Highly efficient and selective CO2 electro-reduction with atomic Fe-C-N hybrid coordination on porous carbon nematosphere Zhong, Haixia; Meng, Fanlu; Zhang, Qi Nano Research, Vol. 12, Issue 9 https://doi.org/10.1007/s12274-019-2339-2	journal	April 2019
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set Kresse, G.; Furthmüller, J. Computational Materials Science, Vol. 6, Issue 1, p. 15-50 https://doi.org/10.1016/0927-0256(96)00008-0	journal	July 1996
Aberration-corrected scanning transmission electron microscopy in single-atom catalysis: Probing the catalytically active centers Liu, Jingyue Chinese Journal of Catalysis, Vol. 38, Issue 9 https://doi.org/10.1016/S1872-2067(17)62900-0	journal	September 2017
Facile synthesis of single-nickel-atomic dispersed N-doped carbon framework for efficient electrochemical CO2 reduction Lu, Peilong; Yang, Yijun; Yao, Jiannian Applied Catalysis B: Environmental, Vol. 241 https://doi.org/10.1016/j.apcatb.2018.09.025	journal	February 2019
Cu-Pd alloy nanoparticles as highly selective catalysts for efficient electrochemical reduction of CO2 to CO Mun, Yeongdong; Lee, Seunghyun; Cho, Ara Applied Catalysis B: Environmental, Vol. 246 https://doi.org/10.1016/j.apcatb.2019.01.021	journal	June 2019
Searching for magnetism in pyrrolic N-doped graphene synthesized via hydrothermal reaction Li, Jiayuan; Li, Xinghua; Zhao, Penghui Carbon, Vol. 84 https://doi.org/10.1016/j.carbon.2014.12.024	journal	April 2015
Facile synthesis silver nanoparticles on different xerogel supports as highly efficient catalysts for the reduction of p-nitrophenol Feng, Jin; Fan, Dongliang; Wang, Qiang Colloids and Surfaces A: Physicochemical and Engineering Aspects, Vol. 520 https://doi.org/10.1016/j.colsurfa.2017.02.041	journal	May 2017
Directly synthesized silver nanoparticles on gas diffusion layers by electrospray pyrolysis for electrochemical CO2 reduction Chae, Sang Youn; Lee, Si Young; Joo, Oh-Shim Electrochimica Acta, Vol. 303 https://doi.org/10.1016/j.electacta.2019.02.046	journal	April 2019
Silver(I) complexes with phthalazine and quinazoline as effective agents against pathogenic Pseudomonas aeruginosa strains Glišić, Biljana Đ.; Senerovic, Lidija; Comba, Peter Journal of Inorganic Biochemistry, Vol. 155 https://doi.org/10.1016/j.jinorgbio.2015.11.026	journal	February 2016
Identification of binuclear Co2N5 active sites for oxygen reduction reaction with more than one magnitude higher activity than single atom CoN4 site Xiao, Meiling; Zhang, Hao; Chen, Yongting Nano Energy, Vol. 46 https://doi.org/10.1016/j.nanoen.2018.02.025	journal	April 2018
Nitrogen doped MoS2 and nitrogen doped carbon dots composite catalyst for electroreduction CO2 to CO with high Faradaic efficiency Lv, Kuilin; Suo, Weiqun; Shao, Mingda Nano Energy, Vol. 63 https://doi.org/10.1016/j.nanoen.2019.06.030	journal	September 2019
Raman spectroscopy in graphene Malard, L. M.; Pimenta, M. A.; Dresselhaus, G. Physics Reports, Vol. 473, Issue 5-6, p. 51-87 https://doi.org/10.1016/j.physrep.2009.02.003	journal	April 2009
Synthesis, spectroscopic characterization, DFT calculations and antimicrobial properties of silver(I) complexes of 2,2′-bipyridine and 1,10-phenanthroline Aslam, Sumaira; Isab, Anvarhusein A.; Alotaibi, Mshari A. Polyhedron, Vol. 115 https://doi.org/10.1016/j.poly.2016.04.047	journal	September 2016
Catalysts and Reaction Pathways for the Electrochemical Reduction of Carbon Dioxide Kortlever, Ruud; Shen, Jing; Schouten, Klaas Jan P. The Journal of Physical Chemistry Letters, Vol. 6, Issue 20 https://doi.org/10.1021/acs.jpclett.5b01559	journal	September 2015
Modification of CO ₂ Reduction Activity of Nanostructured Silver Electrocatalysts by Surface Halide Anions Hsieh, Yu-Chi; Betancourt, Luis E.; Senanayake, Sanjaya D. ACS Applied Energy Materials, Vol. 2, Issue 1 https://doi.org/10.1021/acsaem.8b01692	journal	December 2018
Preferentially Oriented Ag Nanocrystals with Extremely High Activity and Faradaic Efficiency for CO ₂ Electrochemical Reduction to CO Peng, Xiong; Karakalos, Stavros G.; Mustain, William E. ACS Applied Materials & Interfaces, Vol. 10, Issue 2 https://doi.org/10.1021/acsami.7b16164	journal	January 2018
High-Performance Carbon Dioxide Electrocatalytic Reduction by Easily Fabricated Large-Scale Silver Nanowire Arrays Luan, Chuhao; Shao, Yang; Lu, Qi ACS Applied Materials & Interfaces, Vol. 10, Issue 21 https://doi.org/10.1021/acsami.8b03461	journal	May 2018
Beyond Copper in CO ₂ Electrolysis: Effective Hydrocarbon Production on Silver-Nanofoam Catalysts Dutta, Abhijit; Morstein, Carina Elisabeth; Rahaman, Motiar ACS Catalysis, Vol. 8, Issue 9 https://doi.org/10.1021/acscatal.8b01738	journal	July 2018
Achieving Highly Efficient, Selective, and Stable CO ₂ Reduction on Nitrogen-Doped Carbon Nanotubes Wu, Jingjie; Yadav, Ram Manohar; Liu, Mingjie ACS Nano, Vol. 9, Issue 5 https://doi.org/10.1021/acsnano.5b01079	journal	April 2015
Proton-Coupled Electron Transfer Huynh, My Hang V.; Meyer, Thomas J. Chemical Reviews, Vol. 107, Issue 11 https://doi.org/10.1021/cr0500030	journal	November 2007
Graphene Oxide: Preparation, Functionalization, and Electrochemical Applications Chen, Da; Feng, Hongbin; Li, Jinghong Chemical Reviews, Vol. 112, Issue 11 https://doi.org/10.1021/cr300115g	journal	August 2012
Catalysis for the Valorization of Exhaust Carbon: from CO ₂ to Chemicals, Materials, and Fuels. Technological Use of CO ₂ Aresta, Michele; Dibenedetto, Angela; Angelini, Antonella Chemical Reviews, Vol. 114, Issue 3 https://doi.org/10.1021/cr4002758	journal	November 2013
Competition between CO ₂ Reduction and H ₂ Evolution on Transition-Metal Electrocatalysts Zhang, Yin-Jia; Sethuraman, Vijay; Michalsky, Ronald ACS Catalysis, Vol. 4, Issue 10 https://doi.org/10.1021/cs5012298	journal	September 2014
Preparation of Graphitic Oxide Hummers, William S.; Offeman, Richard E. Journal of the American Chemical Society, Vol. 80, Issue 6, p. 1339-1339 https://doi.org/10.1021/ja01539a017	journal	March 1958
Achieving Selective and Efficient Electrocatalytic Activity for CO ₂ Reduction Using Immobilized Silver Nanoparticles Kim, Cheonghee; Jeon, Hyo Sang; Eom, Taedaehyeong Journal of the American Chemical Society, Vol. 137, Issue 43 https://doi.org/10.1021/jacs.5b06568	journal	October 2015
Shape-Dependent Electrocatalytic Reduction of CO ₂ to CO on Triangular Silver Nanoplates Liu, Subiao; Tao, Hongbiao; Zeng, Li Journal of the American Chemical Society, Vol. 139, Issue 6 https://doi.org/10.1021/jacs.6b12103	journal	February 2017
Tuning Sn-Catalysis for Electrochemical Reduction of CO ₂ to CO via the Core/Shell Cu/SnO ₂ Structure Li, Qing; Fu, Jiaju; Zhu, Wenlei Journal of the American Chemical Society, Vol. 139, Issue 12 https://doi.org/10.1021/jacs.7b00261	journal	March 2017
Confined Pyrolysis within Metal–Organic Frameworks To Form Uniform Ru ₃ Clusters for Efficient Oxidation of Alcohols Ji, Shufang; Chen, Yuanjun; Fu, Qiang Journal of the American Chemical Society, Vol. 139, Issue 29 https://doi.org/10.1021/jacs.7b05018	journal	July 2017
Design of N-Coordinated Dual-Metal Sites: A Stable and Active Pt-Free Catalyst for Acidic Oxygen Reduction Reaction Wang, Jing; Huang, Zhengqing; Liu, Wei Journal of the American Chemical Society, Vol. 139, Issue 48 https://doi.org/10.1021/jacs.7b10385	journal	November 2017
Design of Single-Atom Co–N ₅ Catalytic Site: A Robust Electrocatalyst for CO ₂ Reduction with Nearly 100% CO Selectivity and Remarkable Stability Pan, Yuan; Lin, Rui; Chen, Yinjuan Journal of the American Chemical Society, Vol. 140, Issue 12 https://doi.org/10.1021/jacs.8b00814	journal	February 2018
Three-dimensional atomic-scale structure of size-selected gold nanoclusters Li, Z. Y.; Young, N. P.; Di Vece, M. Nature, Vol. 451, Issue 7174 https://doi.org/10.1038/nature06470	journal	December 2007
Changing atmospheric CO2 concentration was the primary driver of early Cenozoic climate Anagnostou, Eleni; John, Eleanor H.; Edgar, Kirsty M. Nature, Vol. 533, Issue 7603 https://doi.org/10.1038/nature17423	journal	April 2016
Single-atom catalysis of CO oxidation using Pt1/FeOx Qiao, Botao; Wang, Aiqin; Yang, Xiaofeng Nature Chemistry, Vol. 3, Issue 8 https://doi.org/10.1038/nchem.1095	journal	July 2011
A selective and efficient electrocatalyst for carbon dioxide reduction Lu, Qi; Rosen, Jonathan; Zhou, Yang Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms4242	journal	January 2014
Atomic cobalt on nitrogen-doped graphene for hydrogen generation Fei, Huilong; Dong, Juncai; Arellano-Jiménez, M. Josefina Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms9668	journal	October 2015
Carbon nitride supported Fe2 cluster catalysts with superior performance for alkene epoxidation Tian, Shubo; Fu, Qiang; Chen, Wenxing Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-04845-x	journal	June 2018
Copper atom-pair catalyst anchored on alloy nanowires for selective and efficient electrochemical reduction of CO2 Jiao, Jiqing; Lin, Rui; Liu, Shoujie Nature Chemistry, Vol. 11, Issue 3 https://doi.org/10.1038/s41557-018-0201-x	journal	January 2019
Atomically dispersed Ni(i) as the active site for electrochemical CO2 reduction Yang, Hong Bin; Hung, Sung-Fu; Liu, Song Nature Energy, Vol. 3, Issue 2 https://doi.org/10.1038/s41560-017-0078-8	journal	February 2018
Heterogeneous single-atom catalysis Wang, Aiqin; Li, Jun; Zhang, Tao Nature Reviews Chemistry, Vol. 2, Issue 6 https://doi.org/10.1038/s41570-018-0010-1	journal	May 2018
Metal ion cycling of Cu foil for selective C–C coupling in electrochemical CO2 reduction Jiang, Kun; Sandberg, Robert B.; Akey, Austin J. Nature Catalysis, Vol. 1, Issue 2 https://doi.org/10.1038/s41929-017-0009-x	journal	January 2018
Chemically and electrochemically catalysed conversion of CO2 to CO with follow-up utilization to value-added chemicals Nielsen, Dennis U.; Hu, Xin-Ming; Daasbjerg, Kim Nature Catalysis, Vol. 1, Issue 4 https://doi.org/10.1038/s41929-018-0051-3	journal	April 2018
Electrocatalytic and homogeneous approaches to conversion of CO ₂ to liquid fuels Benson, Eric E.; Kubiak, Clifford P.; Sathrum, Aaron J. Chem. Soc. Rev., Vol. 38, Issue 1 https://doi.org/10.1039/B804323J	journal	January 2009
Isolated Ni single atoms in graphene nanosheets for high-performance CO ₂ reduction Jiang, Kun; Siahrostami, Samira; Zheng, Tingting Energy & Environmental Science, Vol. 11, Issue 4 https://doi.org/10.1039/C7EE03245E	journal	January 2018
How copper catalyzes the electroreduction of carbon dioxide into hydrocarbon fuels Peterson, Andrew A.; Abild-Pedersen, Frank; Studt, Felix Energy & Environmental Science, Vol. 3, Issue 9 https://doi.org/10.1039/c0ee00071j	journal	January 2010
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
The irreversible momentum of clean energy Obama, Barack Science, Vol. 355, Issue 6321 https://doi.org/10.1126/science.aam6284	journal	January 2017

Similar Records

Electrochemical CO₂ Reduction with Atomic Iron-Dispersed on Nitrogen-Doped Graphene

Journal Article · Sat Mar 24 20:00:00 EDT 2018 · Advanced Energy Materials · OSTI ID:1433979

Effect of Chloride Anions on the Synthesis and Enhanced Catalytic Activity of Silver Nanocoral Electrodes for CO ₂ Electroreduction

Journal Article · Fri Sep 04 00:00:00 EDT 2015 · ACS Catalysis · OSTI ID:1354341

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
CO2 electroreduction
dual-atom catalyst
highly efficient
silver

Dual-atom Ag2/graphene catalyst for efficient electroreduction of CO2 to CO

Citation Formats

References (54)

Similar Records

Related Subjects

Dual-atom Ag₂/graphene catalyst for efficient electroreduction of CO₂ to CO