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

Zhang, Chenhao; Yang, Shize; Wu, Jingjie; Liu, Mingjie; Yazdi, Sadegh; Ren, Muqing; Sha, Junwei; Zhong, Jun; Nie, Kaiqi; Jalilov, Almaz S.; Li, Zhenyuan; Li, Huaming; Yakobson, Boris I.; Wu, Qin; Ringe, Emilie; Xu, Hui; Ajayan, Pulickel M.; Tour, James M.

doi:10.1002/aenm.201703487

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

Journal Article · Sun Mar 25 00:00:00 EDT 2018 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.201703487· OSTI ID:1433979

Zhang, Chenhao ^[1]; Yang, Shize ^[2]; Wu, Jingjie ^[3]; Liu, Mingjie ^[4]; Yazdi, Sadegh ^[3]; Ren, Muqing ^[1]; Sha, Junwei ^[1]; Zhong, Jun ^[5]; Nie, Kaiqi ^[5]; Jalilov, Almaz S. ^[1]; Li, Zhenyuan ^[3]; Li, Huaming ^[6]; Yakobson, Boris I. ^[7]; Wu, Qin ^[8]; Ringe, Emilie ^[9]; Xu, Hui ^[10]; Ajayan, Pulickel M. ^[11];

^[11]

Rice Univ., Houston, TX (United States). Dept. of Chemistry
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
Rice Univ., Houston, TX (United States). Dept. of Materials Science and NanoEngineering
Rice Univ., Houston, TX (United States). Dept. of Materials Science and NanoEngineering; Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
Soochow Univ., Suzhou (China). Inst. of Functional Nano and Soft Materials
Jiangsu Univ., Zhenjiang (China). Inst. for Energy Research
Rice Univ., Houston, TX (United States). Dept. of Chemistry. Smalley-Curl Inst. The NanoCarbon Center
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
Rice Univ., Houston, TX (United States). Dept. of Chemistry. Dept. of Materials Science and NanoEngineering
Rice Univ., Houston, TX (United States). Dept. of Materials Science and NanoEngineering; Jiangsu Univ., Zhenjiang (China). Inst. for Energy Research
Rice Univ., Houston, TX (United States). Dept. of Chemistry. Dept. of Materials Science and NanoEngineering. Smalley-Curl Inst. The NanoCarbon Center

Electrochemical reduction of CO2 provides an opportunity to reach a carbon-neutral energy recycling regime, in which CO2 emissions from fuel use are collected and converted back to fuels. The reduction of CO2 to CO is the first step toward the synthesis of more complex carbon-based fuels and chemicals. Therefore, understanding this step is crucial for the development of high-performance electrocatalyst for CO2 conversion to higher order products such as hydrocarbons. Here, atomic iron dispersed on nitrogen-doped graphene (Fe/NG) is synthesized as an efficient electrocatalyst for CO2 reduction to CO. Fe/NG has a low reduction overpotential with high Faradic efficiency up to 80%. The existence of nitrogen-confined atomic Fe moieties on the nitrogen-doped graphene layer is confirmed by aberration-corrected high-angle annular dark-field scanning transmission electron microscopy and X-ray absorption fine structure analysis. The Fe/NG catalysts provide an ideal platform for comparative studies of the effect of the catalytic center on the electrocatalytic performance. The CO2 reduction reaction mechanism on atomic Fe surrounded by four N atoms (Fe–N4) embedded in nitrogen-doped graphene is further investigated through density functional theory calculations, revealing a possible promotional effect of nitrogen doping on graphene.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Rice Univ., Houston, TX (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); US Air Force Office of Scientific Research (AFOSR); American Chemical Society Petroleum Research Fund (United States)

Grant/Contract Number:: SC0012704; FA9550-12-1-0035; FA9550-14-1-0111; 56256 DNI5; DE‐SC0012704; AC05-00OR22725

OSTI ID:: 1433979

Alternate ID(s):: OSTI ID: 1429531; OSTI ID: 1435178

Report Number(s):: BNL-203515-2018-JAAM

Journal Information:: Advanced Energy Materials, Vol. 8, Issue 19; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 345 works

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Synergistic modulation in MX ₂ (where M = Mo or W or V, and X = S or Se) for an enhanced hydrogen evolution reaction Wang, Ran; Han, Jiecai; Zhang, Xinghong Journal of Materials Chemistry A, Vol. 6, Issue 44 https://doi.org/10.1039/c8ta05912h	journal	January 2018
The effect of coordination environment on the kinetic and thermodynamic stability of single-atom iron catalysts Yang, Weijie; Zhao, Mingliang; Ding, Xunlei Physical Chemistry Chemical Physics, Vol. 22, Issue 7 https://doi.org/10.1039/c9cp05349b	journal	January 2020
Pore size effect of graphyne supports on CO ₂ electrocatalytic activity of Cu single atoms Ni, Youxuan; Miao, Licheng; Wang, Jiaqi Physical Chemistry Chemical Physics, Vol. 22, Issue 3 https://doi.org/10.1039/c9cp05624f	journal	January 2020
Surface strategies for catalytic CO ₂ reduction: from two-dimensional materials to nanoclusters to single atoms Wang, Liming; Chen, Wenlong; Zhang, Doudou Chemical Society Reviews, Vol. 48, Issue 21 https://doi.org/10.1039/c9cs00163h	journal	January 2019
Enhancing electroreduction of CO ₂ over Bi ₂ WO ₆ nanosheets by oxygen vacancies Chu, Mengen; Chen, Chunjun; Guo, Weiwei Green Chemistry, Vol. 21, Issue 10 https://doi.org/10.1039/c9gc00479c	journal	January 2019
Metal single-atom coordinated graphitic carbon nitride as an efficient catalyst for CO oxidation Wang, Shiyan; Li, Jiaqi; Li, Qiang Nanoscale, Vol. 12, Issue 1 https://doi.org/10.1039/c9nr07726j	journal	January 2020
Poly-phenylenediamine-derived atomically dispersed Ni sites for the electroreduction of CO ₂ to CO Zheng, Yonglong; Han, Jianyu; Takele, Leta Inorganic Chemistry Frontiers, Vol. 6, Issue 7 https://doi.org/10.1039/c9qi00297a	journal	January 2019
CO ₂ reduction using paper-derived carbon electrodes modified with copper nanoparticles Gomez, Federico J. V.; Chumanov, George; Silva, Maria Fernanda RSC Advances, Vol. 9, Issue 58 https://doi.org/10.1039/c9ra07430a	journal	January 2019
Carbon-based catalysts for electrochemical CO ₂ reduction Jia, Chen; Dastafkan, Kamran; Ren, Wenhao Sustainable Energy & Fuels, Vol. 3, Issue 11 https://doi.org/10.1039/c9se00527g	journal	January 2019
Electrochemical CO ₂ reduction: from nanoclusters to single atom catalysts Lü, Fang; Bao, Haihong; Mi, Yuying Sustainable Energy & Fuels, Vol. 4, Issue 3 https://doi.org/10.1039/c9se00776h	journal	January 2020
Single-atom catalysts for electrochemical clean energy conversion: recent progress and perspectives Li, Huining; Zhu, Han; Zhuang, Zechao Sustainable Energy & Fuels, Vol. 4, Issue 3 https://doi.org/10.1039/c9se01004a	journal	January 2020
1D/2D nitrogen-doped carbon nanorod arrays/ultrathin carbon nanosheets: outstanding catalysts for the highly efficient electroreduction of CO ₂ to CO Zhu, Ying; Lv, Kuilin; Wang, Xingpu Journal of Materials Chemistry A, Vol. 7, Issue 24 https://doi.org/10.1039/c9ta02353d	journal	January 2019
Emerging nanostructured carbon-based non-precious metal electrocatalysts for selective electrochemical CO ₂ reduction to CO Wang, Xinyue; Zhao, Qidong; Yang, Bin Journal of Materials Chemistry A, Vol. 7, Issue 44 https://doi.org/10.1039/c9ta09681g	journal	January 2019
Novel folic acid complex derived nitrogen and nickel co-doped carbon nanotubes with embedded Ni nanoparticles as efficient electrocatalysts for CO ₂ reduction Wang, Xuewan; Wu, Dan; Dai, Chengzhi Journal of Materials Chemistry A, Vol. 8, Issue 10 https://doi.org/10.1039/c9ta12238a	journal	January 2020
Fe-porphyrin carbon matrix as a bifunctional catalyst for oxygen reduction and CO ₂ reduction from theoretical perspective Liu, Shize; Cheng, Lin; Wang, Wencheng Molecular Physics, Vol. 117, Issue 14 https://doi.org/10.1080/00268976.2018.1544673	journal	November 2018
Electrochemical CO2 Reduction to CO Catalyzed by 2D Nanostructures Hiragond, Chaitanya B.; Kim, Hwapyong; Lee, Junho Catalysts, Vol. 10, Issue 1 https://doi.org/10.3390/catal10010098	journal	January 2020
Controlling Nitrogen Doping in Graphene with Atomic Precision: Synthesis and Characterization Granzier-Nakajima, Tomotaroh; Fujisawa, Kazunori; Anil, Vivek Nanomaterials, Vol. 9, Issue 3 https://doi.org/10.3390/nano9030425	journal	March 2019
Aqueous CO ₂ Reduction with High Efficiency Using α‐Co(OH) ₂ ‐Supported Atomic Ir Electrocatalysts Sun, Xiaofu; Chen, Chunjun; Liu, Shoujie Angewandte Chemie, Vol. 131, Issue 14 https://doi.org/10.1002/ange.201900981	journal	February 2019
Carbon‐Rich Nonprecious Metal Single Atom Electrocatalysts for CO ₂ Reduction and Hydrogen Evolution Wang, Tingting; Zhao, Qidong; Fu, Yuanyuan Small Methods, Vol. 3, Issue 10 https://doi.org/10.1002/smtd.201900210	journal	May 2019
Carbon Nanotubes Synthesis from CO ₂ Based on the Molten Salts Electrochemistry: Effect of Alkaline Earth Carbonate Additives on the Diameter of the Carbon Nanotubes Li, Zhida; Wang, Guanzhong; Zhang, Wenyong Journal of The Electrochemical Society, Vol. 166, Issue 10 https://doi.org/10.1149/2.0861910jes	journal	January 2019

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

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