IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v14y2023i1d10.1038_s41467-023-40667-2.html
   My bibliography  Save this article

Combining Fe nanoparticles and pyrrole-type Fe-N4 sites on less-oxygenated carbon supports for electrochemical CO2 reduction

Author

Listed:
  • Cai Wang

    (Nankai University)

  • Xiaoyu Wang

    (Nankai University)

  • Houan Ren

    (Nankai University)

  • Yilin Zhang

    (Nankai University)

  • Xiaomei Zhou

    (Nankai University)

  • Jing Wang

    (Nankai University)

  • Qingxin Guan

    (Nankai University)

  • Yuping Liu

    (Nankai University)

  • Wei Li

    (Nankai University)

Abstract

A great challenge for electrochemical CO2 reduction is to improve energy efficiency, which requires reducing overpotential while increasing product Faraday efficiency. Here, we designedly synthesize a hybrid electrocatalyst consisting of Fe nanoparticles, pyrrole-type Fe-N4 sites and less-oxygenated carbon supports, which exhibits a remarkable CO Faraday efficiency above 99% at an ultralow overpotential of 21 mV, reaching the highest cathode energy efficiency of 97.1% to date. The catalyst also can afford a CO selectivity nearly 100% with a high cathode energy efficiency (>90%) at least 100 h. The combined results of control experiments, in situ characterizations and theoretical calculations demonstrate that introducing Fe nanoparticles can reduce the overpotential by accelerating the proton transfer from CO2 to *COOH and lowering the free energy for *COOH formation, constructing pyrrole-type Fe-N4 sites and limiting oxygen species on carbon supports can increase CO Faraday efficiency through inhibiting the H2 evolution, thus achieving energy-efficient electrochemical CO2 reduction to CO.

Suggested Citation

  • Cai Wang & Xiaoyu Wang & Houan Ren & Yilin Zhang & Xiaomei Zhou & Jing Wang & Qingxin Guan & Yuping Liu & Wei Li, 2023. "Combining Fe nanoparticles and pyrrole-type Fe-N4 sites on less-oxygenated carbon supports for electrochemical CO2 reduction," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-40667-2
    DOI: 10.1038/s41467-023-40667-2
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-023-40667-2
    File Function: Abstract
    Download Restriction: no
    File URL: https://libkey.io/10.1038/s41467-023-40667-2?utm_source=ideas
    LibKey link: if access is restricted and if your library uses this service, LibKey will redirect you to where you can use your library subscription to access this item
    ---><---

    References listed on IDEAS

    as
    1. Xin Wan & Qingtao Liu & Jieyuan Liu & Shiyuan Liu & Xiaofang Liu & Lirong Zheng & Jiaxiang Shang & Ronghai Yu & Jianglan Shui, 2022. "Iron atom–cluster interactions increase activity and improve durability in Fe–N–C fuel cells," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    2. Hui Li & Peng Wen & Dominique S. Itanze & Zachary D. Hood & Xiao Ma & Michael Kim & Shiba Adhikari & Chang Lu & Chaochao Dun & Miaofang Chi & Yejun Qiu & Scott M. Geyer, 2019. "RETRACTED ARTICLE: Colloidal silver diphosphide (AgP2) nanocrystals as low overpotential catalysts for CO2 reduction to tunable syngas," Nature Communications, Nature, vol. 10(1), pages 1-10, December.
    3. Kun Zhao & Xiaowa Nie & Haozhi Wang & Shuo Chen & Xie Quan & Hongtao Yu & Wonyong Choi & Guanghui Zhang & Bupmo Kim & Jingguang G. Chen, 2020. "Selective electroreduction of CO2 to acetone by single copper atoms anchored on N-doped porous carbon," Nature Communications, Nature, vol. 11(1), pages 1-10, December.
    4. Hong Bin Yang & Sung-Fu Hung & Song Liu & Kaidi Yuan & Shu Miao & Liping Zhang & Xiang Huang & Hsin-Yi Wang & Weizheng Cai & Rong Chen & Jiajian Gao & Xiaofeng Yang & Wei Chen & Yanqiang Huang & Hao M, 2018. "Atomically dispersed Ni(i) as the active site for electrochemical CO2 reduction," Nature Energy, Nature, vol. 3(2), pages 140-147, February.
    5. Wenchao Ma & Shunji Xie & Xia-Guang Zhang & Fanfei Sun & Jincan Kang & Zheng Jiang & Qinghong Zhang & De-Yin Wu & Ye Wang, 2019. "Promoting electrocatalytic CO2 reduction to formate via sulfur-boosting water activation on indium surfaces," Nature Communications, Nature, vol. 10(1), pages 1-10, December.
    6. Hengpan Yang & Qing Lin & Chao Zhang & Xinyao Yu & Zhong Cheng & Guodong Li & Qi Hu & Xiangzhong Ren & Qianling Zhang & Jianhong Liu & Chuanxin He, 2020. "Carbon dioxide electroreduction on single-atom nickel decorated carbon membranes with industry compatible current densities," Nature Communications, Nature, vol. 11(1), pages 1-8, December.
    Full references (including those not matched with items on IDEAS)

    Most related items

    These are the items that most often cite the same works as this one and are cited by the same works as this one.
    1. Zhibo Yao & Hao Cheng & Yifei Xu & Xinyu Zhan & Song Hong & Xinyi Tan & Tai-Sing Wu & Pei Xiong & Yun-Liang Soo & Molly Meng-Jung Li & Leiduan Hao & Liang Xu & Alex W. Robertson & Bingjun Xu & Ming Ya, 2024. "Hydrogen radical-boosted electrocatalytic CO2 reduction using Ni-partnered heteroatomic pairs," Nature Communications, Nature, vol. 15(1), pages 1-15, December.
    2. Chia-Shuo Hsu & Jiali Wang & You-Chiuan Chu & Jui-Hsien Chen & Chia-Ying Chien & Kuo-Hsin Lin & Li Duan Tsai & Hsiao-Chien Chen & Yen-Fa Liao & Nozomu Hiraoka & Yuan-Chung Cheng & Hao Ming Chen, 2023. "Activating dynamic atomic-configuration for single-site electrocatalyst in electrochemical CO2 reduction," Nature Communications, Nature, vol. 14(1), pages 1-14, December.
    3. Shuo Zhang & Jianghua Wu & Mengting Zheng & Xin Jin & Zihan Shen & Zhonghua Li & Yanjun Wang & Quan Wang & Xuebin Wang & Hui Wei & Jiangwei Zhang & Peng Wang & Shanqing Zhang & Liyan Yu & Lifeng Dong , 2023. "Fe/Cu diatomic catalysts for electrochemical nitrate reduction to ammonia," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    4. Jiajing Pei & Huishan Shang & Junjie Mao & Zhe Chen & Rui Sui & Xuejiang Zhang & Danni Zhou & Yu Wang & Fang Zhang & Wei Zhu & Tao Wang & Wenxing Chen & Zhongbin Zhuang, 2024. "A replacement strategy for regulating local environment of single-atom Co-SxN4−x catalysts to facilitate CO2 electroreduction," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    5. Li Zhang & Xiaoju Yang & Qing Yuan & Zhiming Wei & Jie Ding & Tianshu Chu & Chao Rong & Qiao Zhang & Zhenkun Ye & Fu-Zhen Xuan & Yueming Zhai & Bowei Zhang & Xuan Yang, 2023. "Elucidating the structure-stability relationship of Cu single-atom catalysts using operando surface-enhanced infrared absorption spectroscopy," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    6. Sung-Fu Hung & Aoni Xu & Xue Wang & Fengwang Li & Shao-Hui Hsu & Yuhang Li & Joshua Wicks & Eduardo González Cervantes & Armin Sedighian Rasouli & Yuguang C. Li & Mingchuan Luo & Dae-Hyun Nam & Ning W, 2022. "A metal-supported single-atom catalytic site enables carbon dioxide hydrogenation," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    7. Guifeng Ma & Olga A. Syzgantseva & Yan Huang & Dragos Stoian & Jie Zhang & Shuliang Yang & Wen Luo & Mengying Jiang & Shumu Li & Chunjun Chen & Maria A. Syzgantseva & Sen Yan & Ningyu Chen & Li Peng &, 2023. "A hydrophobic Cu/Cu2O sheet catalyst for selective electroreduction of CO to ethanol," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    8. Jie Ding & Fuhua Li & Xinyi Ren & Yuhang Liu & Yifan Li & Zheng Shen & Tian Wang & Weijue Wang & Yang-Gang Wang & Yi Cui & Hongbin Yang & Tianyu Zhang & Bin Liu, 2024. "Molecular tuning boosts asymmetric C-C coupling for CO conversion to acetate," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    9. Yuzhu Zhou & Quan Zhou & Hengjie Liu & Wenjie Xu & Zhouxin Wang & Sicong Qiao & Honghe Ding & Dongliang Chen & Junfa Zhu & Zeming Qi & Xiaojun Wu & Qun He & Li Song, 2023. "Asymmetric dinitrogen-coordinated nickel single-atomic sites for efficient CO2 electroreduction," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    10. Liuzhuang Xing & Qian Yang & Chen Zhu & Yilian Bai & Yurong Tang & Magnus Rueping & Yunfei Cai, 2023. "Poly(heptazine imide) ligand exchange enables remarkable low catalyst loadings in heterogeneous metallaphotocatalysis," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    11. Jie Yin & Jing Jin & Zhouyang Yin & Liu Zhu & Xin Du & Yong Peng & Pinxian Xi & Chun-Hua Yan & Shouheng Sun, 2023. "The built-in electric field across FeN/Fe3N interface for efficient electrochemical reduction of CO2 to CO," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    12. Eamonn Murphy & Yuanchao Liu & Ivana Matanovic & Martina Rüscher & Ying Huang & Alvin Ly & Shengyuan Guo & Wenjie Zang & Xingxu Yan & Andrea Martini & Janis Timoshenko & Beatriz Roldán Cuenya & Iryna , 2023. "Elucidating electrochemical nitrate and nitrite reduction over atomically-dispersed transition metal sites," Nature Communications, Nature, vol. 14(1), pages 1-15, December.
    13. Jiaqi Feng & Libing Zhang & Shoujie Liu & Liang Xu & Xiaodong Ma & Xingxing Tan & Limin Wu & Qingli Qian & Tianbin Wu & Jianling Zhang & Xiaofu Sun & Buxing Han, 2023. "Modulating adsorbed hydrogen drives electrochemical CO2-to-C2 products," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    14. Bo-Wen Zhang & Meng-Nan Zhu & Min-Rui Gao & Xiuan Xi & Nanqi Duan & Zhou Chen & Ren-Fei Feng & Hongbo Zeng & Jing-Li Luo, 2022. "Boosting the stability of perovskites with exsolved nanoparticles by B-site supplement mechanism," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    15. Charles E. Creissen & Marc Fontecave, 2022. "Keeping sight of copper in single-atom catalysts for electrochemical carbon dioxide reduction," Nature Communications, Nature, vol. 13(1), pages 1-4, December.
    16. Haozhou Yang & Na Guo & Shibo Xi & Yao Wu & Bingqing Yao & Qian He & Chun Zhang & Lei Wang, 2024. "Potential-driven structural distortion in cobalt phthalocyanine for electrocatalytic CO2/CO reduction towards methanol," Nature Communications, Nature, vol. 15(1), pages 1-14, December.
    17. Jiqing Jiao & Qing Yuan & Meijie Tan & Xiaoqian Han & Mingbin Gao & Chao Zhang & Xuan Yang & Zhaolin Shi & Yanbin Ma & Hai Xiao & Jiangwei Zhang & Tongbu Lu, 2023. "Constructing asymmetric double-atomic sites for synergistic catalysis of electrochemical CO2 reduction," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    18. Bin Li & Jiali Mu & Guifa Long & Xiangen Song & Ende Huang & Siyue Liu & Yao Wei & Fanfei Sun & Siquan Feng & Qiao Yuan & Yutong Cai & Jian Song & Wenrui Dong & Weiqing Zhang & Xueming Yang & Li Yan &, 2024. "Water-participated mild oxidation of ethane to acetaldehyde," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    19. Yilong Zhao & Yunxuan Ding & Wenlong Li & Chang Liu & Yingzheng Li & Ziqi Zhao & Yu Shan & Fei Li & Licheng Sun & Fusheng Li, 2023. "Efficient urea electrosynthesis from carbon dioxide and nitrate via alternating Cu–W bimetallic C–N coupling sites," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    20. Xinyi Ren & Jian Zhao & Xuning Li & Junming Shao & Binbin Pan & Aude Salamé & Etienne Boutin & Thomas Groizard & Shifu Wang & Jie Ding & Xiong Zhang & Wen-Yang Huang & Wen-Jing Zeng & Chengyu Liu & Ya, 2023. "In-situ spectroscopic probe of the intrinsic structure feature of single-atom center in electrochemical CO/CO2 reduction to methanol," Nature Communications, Nature, vol. 14(1), pages 1-10, December.

    More about this item

    Statistics

    Access and download statistics

    Corrections

    All material on this site has been provided by the respective publishers and authors. You can help correct errors and omissions. When requesting a correction, please mention this item's handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-40667-2. See general information about how to correct material in RePEc.

    If you have authored this item and are not yet registered with RePEc, we encourage you to do it here. This allows to link your profile to this item. It also allows you to accept potential citations to this item that we are uncertain about.

    If CitEc recognized a bibliographic reference but did not link an item in RePEc to it, you can help with this form .

    If you know of missing items citing this one, you can help us creating those links by adding the relevant references in the same way as above, for each refering item. If you are a registered author of this item, you may also want to check the "citations" tab in your RePEc Author Service profile, as there may be some citations waiting for confirmation.

    For technical questions regarding this item, or to correct its authors, title, abstract, bibliographic or download information, contact: Sonal Shukla or Springer Nature Abstracting and Indexing (email available below). General contact details of provider: http://www.nature.com .

    Please note that corrections may take a couple of weeks to filter through the various RePEc services.

    IDEAS is a RePEc service. RePEc uses bibliographic data supplied by the respective publishers.