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Light tuning CO/H_(2)composition on Ag:Unraveling CO_(2)mass transfer and electron-phonon coupling in plasmon-enhanced electrocatalysis

引用

Nano Research 2025年第1期18卷 173-185页

作者： Rui Lin Dong Fan Luca MBerger Thomas Possmayer Yu Zhou Jiexin Zhu Xingbao Chen Wen Luo Lars Allmendinger Andreas Tittl Leonardo de Souza Menezes Guillaume Maurin Shihe Yang and Stefan AMaier Nanoinstitute Munich Faculty of PhysicsLudwig-Maximilians-Universität München80539 MunichGermany Institut Charles Gerhardt Montpellier UMR 5253 CNRS ENSCM UniversitéMontpellierPlace E.Bataillon34090 MontpellierFrance Guangdong Provincial Key Lab of Nano-Micro Material Research School of Advanced MaterialsPeking University Shenzhen Graduate SchoolShenzhen 518055China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Faculty of Chemistry and Pharmacy Ludwig-Maximilians-Universität München81377 MunichGermany Departamento de Física Universidade Federal de Pernambuco50670-901 Recife-PEBrazil School of Physics and Astronomy Monash University Clayton CampusMelbourneVictoria 3800Australia Department of Physics Imperial College LondonSW72AZ LondonUK

Plasmon-enhanced electrocatalysis(PEEC)is an emerging approach to mitigate CO_(2)*** mechanisms behind CO_(2)adsorption and reduction at the catalyst-electrolyte interface in PEEC still need to be further ***,we employ a well-defined Ag nanostructure to elucidate these pivotal *** shining light with wavelengths of 625,525,405 nm on Ag,an adjustable CO/H_(2)ratio from 35 to 1 can be *** reaction pathway changing under plasmonic excitation does not originate from the lowered CO_(2)mass transfer in the vicinity of Ag,as the electrochemical quartz crystal microbalance results unravel that a slightly elevated temperature in bulk electrolyte caused by light irradiation cannot weaken the CO_(2)adsorption at the Ag catalyst-electrolyte *** calculations reveal that optical excitation towards shorter wavelengths leads to a progressive lowered energy barrier for H_(2)formation together with an enhanced energy barrier for^(*)COOH *** thermodynamically suppressed,CO_(2)reduction can still be improved kinetically by optimizing the excitation wavelength and intensity,being accompanied with the enhanced *** absorption spectroscopy results further correlate the higher photocurrent with a prolonged electron-phonon coupling time,verifying that the improvement of CO_(2)reduction kinetics in PEEC can be realized by hot electron harnessing.

关键词： plasmonic catalysis photoelectrochemical CO_(2)reduction CO/H_(2)ratio hot electron generation electronphonon coupling thermal effect

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