Interlayer engineering of molybdenum disulfide toward efficient electrocatalytic hydrogenation

• 作者: Jingwen Tan Wenbiao Zhang Yijin Shu Haiyang Lu Yi Tang Qingsheng Gao
• 来源期刊: 科学通报（英文版）
• 年，卷（期）: 2021,（10）
• 所属期刊栏目: ARTICLES
• 页码范围: 1003-1012
• 页数: 10页
• 语种: 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 → 1T),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.