气候变化领域集成服务门户(CCPortal): Unique interfacial thermodynamics of few-layer 2D MoS2 for (photo)electrochemical catalysis

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DOI	10.1039/c9ee00513g
	Unique interfacial thermodynamics of few-layer 2D MoS2 for (photo)electrochemical catalysis
	Carroll G.M.; Zhang H.; Dunklin J.R.; Miller E.M.; Neale N.R.; Van De Lagemaat J.
发表日期	2019
ISSN	17545692
起始页码	1648
结束页码	1656
卷号	12 期号:5
英文摘要	The electronic structure of few-layer MoS2 is studied by in situ and operando spectroelectrochemistry in conditions relevant to its use as an electrocatalyst. We show that electron injection into the conduction band is coupled with a redshift of the exciton resonance, the magnitude of which depends on the number of vertical MoS2 layers. In addition, the applied electric field/electronic doping imparts uniaxial tensile strain evidenced by broadening Raman signals, indicating that under conditions of electrocatalysis, the system is structurally different from equilibrium. We demonstrate that field/carrier induced changes to the electronic structure of MoS2 alter the band edge positions which changes the fundamental thermodynamic driving force for charge transfer. This property is a function of the applied potential, an effect unique to 2D semiconductors. The dynamic band edge potentials change the relevant interfacial energetics for charge transfer and have strong implications for the mechanistic understanding of (photo)catalytic fuel-forming reactions using two-dimensional systems. © 2019 The Royal Society of Chemistry.
英文关键词	Catalysis; Charge transfer; Electric fields; Electrocatalysis; Electrocatalysts; Electronic structure; Layered semiconductors; Molybdenum compounds; Raman spectroscopy; Semiconductor doping; Spectroelectrochemistry; Tensile strain; Thermodynamics; Applied potentials; Electrochemical catalysis; Exciton resonances; Interfacial energetics; Interfacial thermodynamics; Thermodynamic driving forces; Two-dimensional systems; Uniaxial tensile strain; Sulfur compounds; catalysis; catalyst; electric field; electrochemical method; electrokinesis; operations technology; thermodynamics
语种	英语
来源期刊	Energy & Environmental Science
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/189918
作者单位	Chemistry and Nanoscience Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO 80401, United States
推荐引用方式 GB/T 7714	Carroll G.M.,Zhang H.,Dunklin J.R.,et al. Unique interfacial thermodynamics of few-layer 2D MoS2 for (photo)electrochemical catalysis[J],2019,12(5).
APA	Carroll G.M.,Zhang H.,Dunklin J.R.,Miller E.M.,Neale N.R.,&Van De Lagemaat J..(2019).Unique interfacial thermodynamics of few-layer 2D MoS2 for (photo)electrochemical catalysis.Energy & Environmental Science,12(5).
MLA	Carroll G.M.,et al."Unique interfacial thermodynamics of few-layer 2D MoS2 for (photo)electrochemical catalysis".Energy & Environmental Science 12.5(2019).