Low Overpotential for Electrochemically Reducing CO2 to CO on Nitrogen-Doped Graphene Quantum Dots-Wrapped Single-Crystalline Gold Nanoparticles,ACS Energy Letters

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Low Overpotential for Electrochemically Reducing CO2 to CO on Nitrogen-Doped Graphene Quantum Dots-Wrapped Single-Crystalline Gold Nanoparticles
ACS Energy Letters ( IF 19.3 ) Pub Date : 2018-03-20 00:00:00 , DOI: 10.1021/acsenergylett.8b00261
Jiaju Fu ₁ , Yu Wang ₂ , Juan Liu ₁ , Kaikai Huang ₁ , Ying Chen ₁ , Yafei Li ₂ , Jun-Jie Zhu ₁

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Electrochemically converting the overemitted CO₂ from fossil fuel combustion back into the natural carbon cycle has become a hot spot in recent years. However, surfactants on synthesized nanocatalysts have negative effects on the activity and selectivity. Herein, we transferred the surfactants on single-crystalline gold nanoparticles into N-doped graphene quantum dots (NGQDs) by a hydrothermal method, which not only cleared the Au surfaces but also enhanced the catalytic activity for converting CO₂ into CO at ultralow potentials. The highest faradaic efficiency reaches 93% at −0.25 V vs RHE, and CO production starts from as low as −0.15 V, which is much lower than other Au-based nanocatalysts. DFT calculations were applied to investigate the mechanism and indicate that the synergistic effect between gold and NGQDs is a key to increasing activity.

中文翻译：

氮掺杂石墨烯量子点包裹单晶金纳米粒子上电化学还原CO ₂为CO的低过电势

近年来，将化石燃料燃烧过程中过量排放的CO ₂电化学转化为自然碳循环已成为热点。然而，合成的纳米催化剂上的表面活性剂对活性和选择性具有负面影响。在本文中，我们通过水热法将单晶金纳米颗粒上的表面活性剂转移到掺N的石墨烯量子点（NGQDs）中，不仅清除了Au表面，而且还增强了转化CO ₂的催化活性。以超低电势进入CO。在相对于RHE的-0.25 V时，最高法拉第效率达到93％，并且CO的产生从低至-0.15 V开始，这远低于其他基于Au的纳米催化剂。DFT计算用于研究机理，并表明金和NGQD之间的协同作用是增加活性的关键。

更新日期：2018-03-20

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