Electrochemical CO2 Reduction to Formic Acid at Low Overpotential and with High Faradaic Efficiency on Carbon-Supported Bimetallic Pd-Pt Nanoparticles

Electrochemical CO2 Reduction to Formic Acid at Low Overpotential and with High Faradaic Efficiency on Carbon-Supported Bimetallic Pd-Pt Nanoparticles
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DOI:
10.1021/acscatal.5b00602
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发表时间:
2015-07-01
期刊:
影响因子:
12.9
通讯作者:
Koper, Marc T. M.
Koper, Marc T. M.
中科院分区:
化学1区
文献类型:
--
作者:
Kortlever, Ruud;Peters, Ines;Koper, Marc T. M.

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CO2的电化学还原最近引起了人们的极大兴趣,因为它是一种用于储存可再生能源的可能反应。在这里,我们报告的PdxPt(100-x)/C纳米粒子的合成和它们的电催化性能的CO2还原为甲酸,与它们的活性相比,逆氧化的甲酸CO2。我们发现PdxPt(100-x)/C纳米颗粒具有非常低的起始电位,用于将CO2还原为约100 - 200的甲酸。0 V vs RHE,其接近该反应的理论平衡电势0.02 V vs RHE。此外,Pd 70 Pt 30/C催化剂在相对于RHE的-0.4V下电解1小时后显示出88%的对甲酸的法拉第效率,平均电流密度类似于5 mA/cm(2)。因此,与最近报道的催化剂相比,该催化剂显示出对甲酸的竞争性或甚至更好的法拉第效率,在显著更低的过电位下,同时避免了用先前报道的Pd基催化剂观察到的强烈失活。
The electrochemical reduction of CO2 has attracted significant interest recently, as it is a possible reaction for the storage of renewable energy. Here, we report on the synthesis of PdxPt(100-x)/C nanoparticles and their electrocatalytic properties for the reduction of CO2 to formic acid, compared with their activity for the reverse oxidation of formic acid to CO2. We find that PdxPt(100-x)/C nanoparticles have a very low onset potential for the reduction of CO2 to formic acid of ca. 0 V vs RHE, which approaches the theoretical equilibrium potential of 0.02 V vs RHE for this reaction. Furthermore, the Pd70Pt30/C catalyst shows a faradaic efficiency of 88% toward formic acid after 1 h of electrolysis at -0.4 V vs RHE with an average current density of similar to 5 mA/cm(2). Therefore, this catalyst shows a competing or even better faradaic efficiency toward formic acid compared to recently reported catalysts, at a substantially lower overpotential, while avoiding a strong deactivation that was observed with previously reported Pd-based catalysts.