Iron Nanoparticles Tuned to Catalyze CO2 Electroreduction in Acidic Solutions through Chemical Microenvironment Engineering

被引:57
作者
Fan, Qun [1 ]
Bao, GuangXu [1 ]
Chen, Xiaoyi [1 ]
Meng, Yichen [1 ]
Zhang, Sheng [1 ,2 ,3 ]
Ma, Xinbin [1 ,2 ,3 ]
机构
[1] Tianjin Univ, Sch Chem Engn & Technol, Key Lab Green Chem Technol, Minist Educ, Tianjin 300072, Peoples R China
[2] Zhejiang Inst Tianjin Univ, Ningbo 315201, Peoples R China
[3] Joint Sch Natl Univ Singapore & Tianjin Univ, Fuzhou 350207, Peoples R China
关键词
chemical microenvironment; CO2 electrochemical reduction; Fe nanoparticles; acidic electrolyte; ATR-FTIR; N-DOPED CARBON; ELECTROCHEMICAL REDUCTION; OXYGEN REDUCTION; ACTIVE-SITES; FE; EVOLUTION; DIOXIDE; AU;
D O I
10.1021/acscatal.2c01890
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Electrochemical CO2 reduction reaction (CO2RR) is an attractive solution to close the anthropogenic carbon cycle and store intermittent renewable energy in value-added chemicals and fuels. While Fe nanoparticles are typically employed as catalysts for hydrogen evolution reaction (HER, a competing reaction against CO2RR), herein, efficient CO2 electroreduction is achieved through tuning their chemical microenvironment. Porous carbon layers were deposited on these Fe nanoparticles, which creates a hydrophobic environment to enrich local CO2 concentration and suppress water penetration and thus HER in the micropores. This strategy successfully turns Fe nanoparticles into an excellent CO2RR catalyst with over 90% CO Faradaic efficiency. Due to the unique local chemical environment created above, high CO selectivity could be maintained even in acidic electrolytes, which provides a promising approach to address the notorious issue of carbonate precipitation in widely used alkaline solutions for CO2 electrolyzers.
引用
收藏
页码:7517 / 7523
页数:7
相关论文
共 46 条
  • [1] Active Sites of Au and Ag Nanoparticle Catalysts for CO2 Electroreduction to CO
    Back, Seoin
    Yeom, Min Sun
    Jung, Yousung
    [J]. ACS CATALYSIS, 2015, 5 (09): : 5089 - 5096
  • [2] Electrochemical CO2 Reduction: A Classification Problem
    Bagger, Alexander
    Ju, Wen
    Sofia Varela, Ana
    Strasser, Peter
    Rossmeisl, Jan
    [J]. CHEMPHYSCHEM, 2017, 18 (22) : 3266 - 3273
  • [3] Suppression of Hydrogen Evolution in Acidic Electrolytes by Electrochemical CO2 Reduction
    Bondue, Christoph J.
    Graf, Matthias
    Goyal, Akansha
    Koper, Marc T. M.
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2021, 143 (01) : 279 - 285
  • [4] Ligand Engineering in Nickel Phthalocyanine to Boost the Electrocatalytic Reduction of CO2
    Chen, Kejun
    Cao, Maoqi
    Lin, Yiyang
    Fu, Junwei
    Liao, Hanxiao
    Zhou, Yajiao
    Li, Hongmei
    Qiu, Xiaoqing
    Hu, Junhua
    Zheng, Xusheng
    Shakouri, Mohsen
    Xiao, Qunfeng
    Hu, Yongfeng
    Li, Jun
    Liu, Jilei
    Cortes, Emiliano
    Liu, Min
    [J]. ADVANCED FUNCTIONAL MATERIALS, 2022, 32 (10)
  • [5] Fe and N Co-Doped Porous Carbon Nanospheres with High Density of Active Sites for Efficient CO2 Electroreduction
    Chen, Yubin
    Zou, Liangliang
    Liu, Hong
    Chen, Chi
    Wang, Qi
    Gu, Meng
    Yang, Bo
    Zou, Zhiqing
    Fang, Jianhui
    Yang, Hui
    [J]. JOURNAL OF PHYSICAL CHEMISTRY C, 2019, 123 (27) : 16651 - 16659
  • [6] Activation of Ni Particles into Single Ni-N Atoms for Efficient Electrochemical Reduction of CO2
    Fan, Qun
    Hou, Pengfei
    Choi, Changhyeok
    Wu, Tai-Sing
    Hong, Song
    Li, Fang
    Soo, Yun-Liang
    Kang, Peng
    Jung, Yousung
    Sun, Zhenyu
    [J]. ADVANCED ENERGY MATERIALS, 2020, 10 (05)
  • [7] Observational determination of surface radiative forcing by CO2 from 2000 to 2010
    Feldman, D. R.
    Collins, W. D.
    Gero, P. J.
    Torn, M. S.
    Mlawer, E. J.
    Shippert, T. R.
    [J]. NATURE, 2015, 519 (7543) : 339 - +
  • [8] Atomic structures of iron-based single-crystalline nanowires crystallized inside multi-walled carbon nanotubes as revealed by analytical electron microscopy
    Golberg, D
    Mitome, M
    Müller, C
    Tang, C
    Leonhardt, A
    Bando, Y
    [J]. ACTA MATERIALIA, 2006, 54 (09) : 2567 - 2576
  • [9] Simultaneous determination of composition and thickness of thin iron-oxide films from XPS Fe 2p spectra
    Graat, PCJ
    Somers, MAJ
    [J]. APPLIED SURFACE SCIENCE, 1996, 100 : 36 - 40
  • [10] Atomically dispersed Fe3+ sites catalyze efficient CO2 electroreduction to CO
    Gu, Jun
    Hsu, Chia-Shuo
    Bai, Lichen
    Chen, Hao Ming
    Hu, Xile
    [J]. SCIENCE, 2019, 364 (6445) : 1091 - +