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Modulation of Molecular Spatial Distribution and Chemisorption with Perforated Nanosheets for Ethanol Electro‐oxidation
Author(s) -
Wang Wenbin,
Zhu YinBo,
Wen Qunlei,
Wang Yutang,
Xia Jun,
Li Caicai,
Chen MingWei,
Liu Youwen,
Li Huiqiao,
Wu HengAn,
Zhai Tianyou
Publication year - 2019
Publication title -
advanced materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 10.707
H-Index - 527
eISSN - 1521-4095
pISSN - 0935-9648
DOI - 10.1002/adma.201900528
Subject(s) - materials science , catalysis , heteroatom , molecule , electrolyte , molecular dynamics , chemical engineering , chemisorption , electrochemistry , ethanol , nanotechnology , organic chemistry , computational chemistry , chemistry , electrode , ring (chemistry) , engineering
Integrating thermodynamically favorable ethanol reforming reactions with hybrid water electrolysis will allow room‐temperature production of high‐value organic products and decoupled hydrogen evolution. However, electrochemical reforming of ethanol has not received adequate attention due to its low catalytic efficiency and poor selectivity, which are caused by the multiple groups and chemical bonds of ethanol. In addition to the thermodynamic properties affected by the electronic structure of the catalyst, the dynamics of molecule/ion dynamics in electrolytes also play a significant role in the efficiency of a catalyst. The relatively large size and viscosity of the ethanol molecule necessitates large channels for molecule/ion transport through catalysts. Perforated CoNi hydroxide nanosheets are proposed as a model catalyst to synergistically regulate the dynamics of molecules and electronic structures. Molecular dynamics simulations directly reveal that these nanosheets can act as a “dam” to enrich ethanol molecules and facilitate permeation through the nanopores. Additionally, the charge transfer behavior of heteroatoms modifies the local charge density to promote molecular chemisorption. As expected, the perforated nanosheets exhibit a small potential (1.39 V) and high Faradaic efficiency for the conversion of ethanol into acetic acid. Moreover, the concept in this work provides new perspectives for exploring other molecular catalysts.