Achieving Selective and Efficient Electrocatalytic Activity for CO2 Reduction Using Immobilized Silver Nanoparticles

被引:603
作者
Kim, Cheonghee [1 ]
Jeon, Hyo Sang [1 ,2 ]
Eom, Taedaehyeong [3 ]
Jee, Michael Shincheon [1 ,4 ]
Kim, Hyungjun [3 ]
Friend, Cynthia M. [5 ]
Min, Byoung Koun [1 ,2 ,6 ]
Hwang, Yun Jeong [1 ,2 ]
机构
[1] Korea Inst Sci & Technol, Clean Energy Res Ctr, Seoul 02792, South Korea
[2] Korea Univ Sci & Technol, Taejon 34113, South Korea
[3] Korea Adv Inst Sci & Technol, Grad Sch Energy Environm Water & Sustainabil EEWS, Taejon 34141, South Korea
[4] Korea Univ, Dept Chem & Biol Engn, Seoul 02841, South Korea
[5] Harvard Univ, Dept Chem & Chem Biol, Cambridge, MA 02138 USA
[6] Korea Univ, Green Sch, Seoul 02841, South Korea
基金
新加坡国家研究基金会;
关键词
RENEWABLE ENERGY; GOLD CLUSTERS; SIZE; CONVERSION;
D O I
10.1021/jacs.5b06568
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Selective electrochemical reduction of CO2, is one of the most sought-after processes because of the potential to convert a harmful greenhouse gas to a useful chemical. We have discovered that immobilized Ag nanoparticles supported on carbon exhibit enhanced Faradaic efficiency and a lower overpotential for selective reduction of CO2, to CO. These electrocatalysts were synthesized directly on the carbon support by a facile one-pot method using a cysteamine anchoring agent resulting in controlled monodispersed particle sizes. These synthesized Ag/C electrodes showed improved activities, specifically decrease of the overpotential by 300 mV at 1 mA/cm(2), and 4-fold enhanced CO Faradaic efficiency at -0.75 V vs RHE with the optimal particle size of 5 nm compared to polycrystalline Ag foil. DFT calculations enlightened that the specific interaction between Ag nanoparticle and the anchoring agents modified the catalyst surface to have a selectively higher affinity to the intermediate COOH over CO, which effectively lowers the overpotential.
引用
收藏
页码:13844 / 13850
页数:7
相关论文
共 31 条
[1]   Silver nanoparticles linked by a Pt-containing organometallic dithiol bridge: study of local structure and interface by XAFS and SR-XPS [J].
Battocchio, C. ;
Fratoddi, I. ;
Fontana, L. ;
Bodo, E. ;
Porcaro, F. ;
Meneghini, C. ;
Pis, I. ;
Nappini, S. ;
Mobilio, S. ;
Russo, M. V. ;
Polzonetti, G. .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2014, 16 (23) :11719-11728
[2]   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
[3]   Aqueous CO2 Reduction at Very Low Overpotential on Oxide-Derived Au Nanoparticles [J].
Chen, Yihong ;
Li, Christina W. ;
Kanan, Matthew W. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2012, 134 (49) :19969-19972
[4]   Size-Dependent Electrocatalytic Reduction of CO2 over Pd Nanoparticles [J].
Gao, Dunfeng ;
Zhou, Hu ;
Wang, Jing ;
Miao, Shu ;
Yang, Fan ;
Wang, Guoxiong ;
Wang, Jianguo ;
Bao, Xinhe .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2015, 137 (13) :4288-4291
[5]   Carbon Dioxide Capture from the Air Using a Polyamine Based Regenerable Solid Adsorbent [J].
Goeppert, Alain ;
Czaun, Miklos ;
May, Robert B. ;
Prakash, G. K. Surya ;
Olah, George A. ;
Narayanan, S. R. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2011, 133 (50) :20164-20167
[6]   Colloidally Synthesized Monodisperse Rh Nanoparticles Supported on SBA-15 for Size- and Pretreatment-Dependent Studies of CO Oxidation [J].
Grass, Michael E. ;
Joo, Sang Hoon ;
Zhang, Yawen ;
Somorjai, Gabor A. .
JOURNAL OF PHYSICAL CHEMISTRY C, 2009, 113 (20) :8616-8623
[7]   Sustainable hydrocarbon fuels by recycling CO2 and H2O with renewable or nuclear energy [J].
Graves, Christopher ;
Ebbesen, Sune D. ;
Mogensen, Mogens ;
Lackner, Klaus S. .
RENEWABLE & SUSTAINABLE ENERGY REVIEWS, 2011, 15 (01) :1-23
[8]   Atomic and electronic structure of gold clusters:: understanding flakes, cages and superatoms from simple concepts [J].
Hakkinen, Hannu .
CHEMICAL SOCIETY REVIEWS, 2008, 37 (09) :1847-1859
[9]   Understanding Trends in the Electrocatalytic Activity of Metals and Enzymes for CO2 Reduction to CO [J].
Hansen, Heine A. ;
Varley, Joel B. ;
Peterson, Andrew A. ;
Norskov, Jens K. .
JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 2013, 4 (03) :388-392
[10]   Insights into the electrocatalytic reduction of CO2 on metallic silver surfaces [J].
Hatsukade, Toru ;
Kuhl, Kendra P. ;
Cave, Etosha R. ;
Abram, David N. ;
Jaramillo, Thomas F. .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2014, 16 (27) :13814-13819