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分级结构AgAu纳米合金用于高效电催化乙醇氧化
引用本文:王彩琴,Danil Bukhvalov,M.Cynthia Goh,杜玉扣,杨小飞.分级结构AgAu纳米合金用于高效电催化乙醇氧化[J].催化学报,2022,43(3):851-861.
作者姓名:王彩琴  Danil Bukhvalov  M.Cynthia Goh  杜玉扣  杨小飞
作者单位:南京林业大学理学院,材料物理化学研究所,江苏南京210037,中国;多伦多大学化学系,多伦多,加拿大,南京林业大学理学院,材料物理化学研究所,江苏南京210037,中国,多伦多大学化学系,多伦多,加拿大,苏州大学材料与化学化工学部,江苏苏州215123,中国
基金项目:江苏省自然科学基金(BK20190762);南京林业大学杰出青年基金(JC2019002).
摘    要:乙醇由于具有无毒、理论能量密度高、易存储等优点,被广泛用于直接醇类燃料电池研究.乙醇电氧化是直接醇类燃料电池中重要的阳极反应,通常涉及C1和C2反应路径.C1路径中乙醇分子主要转化成二氧化碳,但该过程涉及C-C键断裂,会有COad和CH(x)ad等中间体产生;C2路径中乙醇分子转化成乙醛,最终转化成乙酸或乙酸根.为提升...

关 键 词:AgAu纳米杂合材料  多级纳米结构  表面缺陷  密度泛函理论  乙醇电氧化

Hierarchical AgAu alloy nanostructures for highly efficient electrocatalytic ethanol oxidation
Caiqin Wang,Danil Bukhvalov,M.Cynthia Goh,Yukou Du,Xiaofei Yang.Hierarchical AgAu alloy nanostructures for highly efficient electrocatalytic ethanol oxidation[J].Chinese Journal of Catalysis,2022,43(3):851-861.
Authors:Caiqin Wang  Danil Bukhvalov  MCynthia Goh  Yukou Du  Xiaofei Yang
Institution:(College of Science&Institute of Materials Physics and Chemistry,Nanjing Forestry University,Nanjing 210037,Jiangsu,China;Department of Chemistry,University of Toronto,Toronto,Canada;College of Chemistry,Chemical Engineering and Materials Science,Soochow University,Suzhou 215123,Jiangsu,China)
Abstract:The ethanol oxidation reaction is a significant anodic reaction for direct alcohol fuel cells.The most commonly used catalysts for this reaction are Pt‐based materials;however,Pt‐based electrocatalysts cause carbon monoxide poisoning with intermediates before the complete transformation of alcohol to CO2.Herein,we present hierarchical AgAu bimetallic nanoarchitectures for ethanol electrooxidation,which were fabricated via a partial galvanic reduction reaction between Ag and HAuCl4.The ethanol electrooxidation performance of the optimal AgAu nanohybrid was increased to 1834 mA mg?1,which is almost 10 times higher than that of the pristine Au catalyst(190 mA mg?1)in alkaline solutions.This was achieved by introducing Ag into the Au catalyst and controlling the time of the replacement reaction.The heterostructure also presents a higher current density than that of commercial Pt/C(1574 mA mg?1).Density functional theory calculations revealed that the enhanced activity and stability may stem from unavoidable defects on the surface of the integrated AgAu nanoarchitectures.Ethanol oxidation reactions over these defects are more energetically favorable,which facilitates the oxidative removal of carbonaceous poison and boosts the combination with radicals on adjacent Au active sites.
Keywords:AgAu nanohybrids  Hierarchical nanostructures  Defected surface  DFT calculation  Ethanol electrooxidation
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