DOI: 10.1016/j.scib.2020.11.002
论文题名: Interlayer engineering of molybdenum disulfide toward efficient electrocatalytic hydrogenation
作者: Tan J. ; Zhang W. ; Shu Y. ; Lu H. ; Tang Y. ; Gao Q.
刊名: Science Bulletin
ISSN: 20959273
出版年: 2021
卷: 66, 期: 10 起始页码: 1003
结束页码: 1012
语种: 英语
中文关键词: Binding energy
; Electrocatalytic hydrogenation
; Interlayer engineering
; Molybdenum disulfide
; Surface hydrophobicity
英文关键词: Ammonia
; Chemisorption
; Electrocatalysts
; Hydrogenation
; Hydrophobicity
; Layered semiconductors
; Precious metals
; Sulfur compounds
; Diffusion limitations
; Electrocatalytic hydrogenation
; Electrochemical synthesis
; Electronic configuration
; Faradaic efficiencies
; Langmuir Hinshelwood mechanism
; Surface hydrophobicity
; Sustainable production
; Molybdenum compounds
英文摘要: Electrocatalytic hydrogenation (ECH) enables the sustainable production of chemicals under ambient condition; however, suffers from serious competition with hydrogen (H2) evolution and the use of precious metals as electrocatalysts. Herein, molybdenum disulfide is for the first time developed as an efficient and noble-metal-free catalyst for ECH via in situ intercalation of ammonia or alkyl-amine cations. This interlayer engineering regulates phase transition (2H → 1 T), and effectively ameliorates electronic configurations and surface hydrophobicity to promote the ECH of biomass-derived oxygenates, while prohibiting H2 evolution. The optimal one intercalated by dimethylamine (MoS2-DMA) is capable of hydrogenating furfural (FAL) to furfuryl alcohol with high Faradaic efficiency of 86.3%–73.3% and outstanding selectivity of >95.0% at −0.25 to −0.65 V (vs. RHE), outperforming MoS2 and other conventional metals. Such prominent performance stems from the enhanced chemisorption and surface hydrophobicity. The chemisorption of H intermediate and FAL, synchronously strengthened on the edge-sites of MoS2-DMA, accelerates the surface elementary step following Langmuir-Hinshelwood mechanism. Moreover, the improved hydrophobicity benefits FAL affinity to overcome diffusion limitation. Discovering the effective modulation of MoS2 from a typical H2 evolution electrocatalyst to a promising candidate for ECH, this study broadens the scope to exploit catalysts used for electrochemical synthesis. © 2020 Science China Press Citation statistics:
资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/170399
Appears in Collections: 气候变化与战略
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作者单位: College of Chemistry and Materials Science, Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and Applications, Jinan University, Guangzhou, 510632, China; Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Laboratory of Advanced Materials and Collaborative Innovation Center of Chemistry for Energy Materials (iCHEM), Fudan University, Shanghai, 200433, China
Recommended Citation:
Tan J.,Zhang W.,Shu Y.,et al. Interlayer engineering of molybdenum disulfide toward efficient electrocatalytic hydrogenation[J]. Science Bulletin,2021-01-01,66(10)