Copper modification of pyrite for CO2 electrochemical reduction
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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法拉第效率。因此,CuxFe1−xS2是一种比较有前景的CO2电催化还原催化剂。Abstract: CO2 electrocatalytic reduction to synthesize highly value-added fuels provides a sustainable path for CO2 conversion and utilization. Nevertheless, the development of electrocatalysts with high catalytic activity and product selectivity remains a major challenge. In this work, copper-doped FeS2 catalysts (CuxFe1−xS2) were prepared for CO2 electrochemical reduction. The physicochemical properties of the catalysts were studied by XRD, XPS, SEM and other characterization analysis methods. Experimental results show that Cu doping can control the size of the catalyst nanosheets and inhibit the oxidation of FeS2 in the air. Cu0.33Fe0.67S2 shows better catalytic activity for CO2 electrocatalytic reduction than FeS2. In the potential range of (−1.5) − (−1.6) V vs. RHE, the total efficiency of carbon-containing products of CO2 electrocatalytic reduction is 50.8% and its current density is 23.8 mA/cm2, which increases by 71.2% compared with FeS2 catalyst. The Faradaic efficiency of Cu0.09Fe0.91S2 to produce C3H6 at −1.3 V vs. RHE is 21.8%, which is significantly higher than the value reported in the current literature. Thus, CuxFe1−xS2 is regarded as an excellent electrocatalyst for CO2 reduction.
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Key words:
- carbon dioxide /
- electrocatalytic reduction /
- pyrite /
- catalyst
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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
Catalyst E/ (V vs. RHE) Faradaic efficiency/% Ref. ethane propene propanol Cu2O derived Cu nanoparticle −1.10 6.0 [18] Ag-Cu2OPS −1.20 1.6 [20] Cu nanowire array −1.10 8.0 [21] Cu(100) single electrode −1.00 1.5 [22] 18 nm Cu −1.03 5.4 [23] Nanoporous Cu −0.67 4.5 [24] Surface reconstructed Cu −2.60 5.0 [25] Plasma-Cu nanocubes −1.00 9.0 [19] Cu0.33Fe0.67S2 −1.60 23.9 this work Cu0.09Fe0.91S2 −1.30 21.8 this work -
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