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铜改性黄铁矿催化剂的CO2电催化还原性能研究

杨予辰 杨应举 刘晶 熊勃

杨予辰, 杨应举, 刘晶, 熊勃. 铜改性黄铁矿催化剂的CO2电催化还原性能研究[J]. 燃料化学学报. doi: 10.19906/j.cnki.JFCT.2022025
引用本文: 杨予辰, 杨应举, 刘晶, 熊勃. 铜改性黄铁矿催化剂的CO2电催化还原性能研究[J]. 燃料化学学报. doi: 10.19906/j.cnki.JFCT.2022025
YANG Yu-chen, YANG Ying-ju, LIU Jing, XIONG Bo. Copper modification of pyrite for CO2 electrochemical reduction[J]. Journal of Fuel Chemistry and Technology. doi: 10.19906/j.cnki.JFCT.2022025
Citation: YANG Yu-chen, YANG Ying-ju, LIU Jing, XIONG Bo. Copper modification of pyrite for CO2 electrochemical reduction[J]. Journal of Fuel Chemistry and Technology. doi: 10.19906/j.cnki.JFCT.2022025

铜改性黄铁矿催化剂的CO2电催化还原性能研究

doi: 10.19906/j.cnki.JFCT.2022025
基金项目: 中央高校基本科研基金(2019kfyRCPY021)资助
详细信息
    通讯作者:

    liujing27@mail.hust.edu.cn; Tel: 027-87542417

  • 中图分类号: TK16

Copper modification of pyrite for CO2 electrochemical reduction

Funds: Fundamental Research Funds for the Central Universities (2019kfyRCPY021)
  • 摘要: CO2电催化还原合成高附加值燃料为CO2转化利用提供了一条可持续发展的途径。然而,开发具有优异催化活性和产物选择性的电催化剂仍面临巨大的挑战。本研究制备了铜改性黄铁矿催化剂CuxFe1-xS2,采用XRD、XPS、SEM等表征分析方法研究了催化剂的物理化学性质,并研究了催化剂的CO2电催化还原活性和产物选择性。实验结果表明,Cu掺杂可以调控催化剂纳米片的尺寸,同时可以抑制FeS2在空气中的氧化。Cu0.33Fe0.67S2比FeS2表现出更好的催化反应活性,在−1.5−−1.6 V vs. RHE,CO2电催化还原的含碳产物法拉第效率为50.8%,电流密度为23.8 mA/cm2。相比于FeS2催化剂,电流密度提高了71.2%。Cu0.09Fe0.91S2在−1.3 V vs. RHE下生成C3H6的法拉第效率为21.8%,显著高于目前文献中已报道的数值。因此,CuxFe1-xS2是一种比较有前景的CO2电催化还原催化剂。
  • 图  1  催化剂制备流程图

    Figure  1  Flow chart of catalyst preparation

    图  2  CuxFe1-xS2催化剂的XRD衍射图谱

    Figure  2  XRD patterns of CuxFe1-xS2 catalysts

    图  3  CuxFe1-xS2催化剂的SEM图:(a) FeS2;(b) Cu0.05Fe0.95S2;(c) Cu0.09Fe0.91S2;(d) Cu0.17Fe0.83S2;(e) Cu0.33Fe0.67S2

    Figure  3  SEM images of CuxFe1-xS2 catalysts: (a) FeS2; (b) Cu0.05Fe0.95S2; (c) Cu0.09Fe0.91S2; (d) Cu0.17Fe0.83S2; (e) Cu0.33Fe0.67S2

    图  4  FeS2样品的Fe 2p、S 2p和FeS2样品的XPS光谱谱图

    Figure  4  (a) Fe 2p XPS spectrum of FeS2 sample; (b) S 2p XPS spectrum of FeS2 sample; (c) XPS survey spectrum of FeS2 sample

    图  5  Cu0.33Fe0.67S2样品的XPS光谱和样品的S 2p 、Fe 2p、Cu 2p XPS光谱谱图

    Figure  5  (a) XPS survey spectrum of Cu0.33Fe0.67S2 sample; (b) S 2p XPS spectrum of Cu0.33Fe0.67S2 sample; (c) Fe 2p XPS spectrum of Cu0.33Fe0.67S2 sample; (d) Cu 2p XPS spectrum of Cu0.33Fe0.67S2 sample

    图  6  CuxFe1-xS2催化剂在CO2饱和的0.2 moL/L KHCO3和0.1 moL/L NaOH混合溶液中的(a) CV、 LSV曲线

    Figure  6  (a) CV curve; (b) LSV curve of CuxFe1-xS2 catalyst in CO2-saturated mixed solution of 0.2 moL/L KHCO3 and 0.1 moL/L NaOH

    图  7  FeS2和Cu0.33Fe0.67S2催化剂的稳定性测试

    Figure  7  Stability of FeS2 and Cu0.33Fe0.67S2 catalyst at −1.2 V vs. RHE

    图  8  Cu掺杂量对CO和C2H6法拉第效率的影响

    Figure  8  Influence of different Cu doping loadings on the Faraday efficiency of CO and C2H6

    (a): CO Faraday efficiency; (b): C2H6 Faraday efficiency

    图  9  H2、CO、C2H6、C3H6的法拉第效率

    Figure  9  Selectivity of H2, CO, C2H6 and C3H6 under different reaction voltages: (a) −1.2 V vs. RHE; (b) −1.3 V vs. RHE; (c) −1.4 V vs. RHE; (d) −1.5 V vs. RHE

    表  1  Cu基催化剂上CO2电催化还原产生C2+产物的法拉第效率

    Table  1  Summary of CO2RR towards C2+ Faradaic efficiency on different catalysts

    CatalystE/ (V vs. RHE)Faradaic efficiency/%Ref.
    ethanepropenepropanol
    Cu2O derived Cu nanoparticle−1.106.0[18]
    Ag-Cu2OPS−1.201.6[20]
    Cu nanowire array−1.108.0[21]
    Cu(100) single electrode−1.001.5[22]
    18-nm Cu−1.035.4[23]
    Nanoporous Cu−0.674.5[24]
    Surface reconstructed Cu−2.605.0[25]
    Plasma-Cu nanocubes−1.009.0[19]
    Cu0.33Fe0.67S2−1.6023.9this work
    Cu0.09Fe0.91S2−1.3021.8this work
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  • 收稿日期:  2021-12-28
  • 录用日期:  2022-03-25
  • 修回日期:  2022-03-24
  • 网络出版日期:  2022-04-22

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