M. Gutiérrez-Roa , D. Sebastián , H. Guzmán , F. Zammillo , M. Gallone , S. Hernández , M.J. Lázaro , S. Pérez-Rodríguez
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引用次数: 0
Abstract
Copper-based bimetallic catalysts have garnered significant attention for CO2 electrochemical CO2 conversion due to their ability to catalytically reduce CO2 to hydrocarbons and alcohols. Herein, a set of CuPt/C catalysts with different Cu:Pt atomic ratios are successfully synthesised through galvanostatic displacement. The progressive incorporation of platinum on Cu/C nanoparticles significantly impacts the CO2 electro-reduction performance in a 0.1 M KHCO3 solution. The results revealed that Cu:Pt atomic ratios of 99:1 and 95:5 enhance formate production at mild potentials (-0.6 V vs. RHE) due to an improved water activation compared to monometallic Cu/C and, thus a higher availability of protons (or adsorbed hydrogen, *H) near the active sites. In contrast, lower Cu:Pt ratios or higher overpotentials result in diminished formate production. This behaviour is likely due to the affinity of Pt for the carbon-bound *COOH intermediate, which favors CO formation over formate. These findings demonstrate that Pt incorporation in Cu/C nanoparticles can alter the CO2 reduction mechanism, providing insights into the design of selective formate-producing catalysts.
铜基双金属催化剂因其催化还原二氧化碳为碳氢化合物和醇的能力而引起了二氧化碳电化学转化的极大关注。本文通过恒流位移法成功合成了一套不同Cu:Pt原子比的CuPt/C催化剂。在0.1 M KHCO3溶液中,铂在Cu/C纳米颗粒上的逐渐掺入显著影响CO2电还原性能。结果表明,与单金属Cu/C相比,Cu:Pt原子比为99:1和95:5的原子比提高了在温和电位下(-0.6 V vs. RHE)生成甲酸的能力,从而提高了活性位点附近质子(或吸附氢,*H)的可用性。相反,较低的Cu:Pt比率或较高的过电位会导致甲酸盐产量减少。这种行为可能是由于Pt对碳结合的*COOH中间体的亲和力,这有利于CO的形成而不是甲酸。这些发现表明,在Cu/C纳米颗粒中掺入Pt可以改变CO2还原机制,为设计选择性甲酸生成催化剂提供了见解。
期刊介绍:
The Journal of CO2 Utilization offers a single, multi-disciplinary, scholarly platform for the exchange of novel research in the field of CO2 re-use for scientists and engineers in chemicals, fuels and materials.
The emphasis is on the dissemination of leading-edge research from basic science to the development of new processes, technologies and applications.
The Journal of CO2 Utilization publishes original peer-reviewed research papers, reviews, and short communications, including experimental and theoretical work, and analytical models and simulations.