燃料化学学报（中英文）2025，Vol.53Issue(6)：872-882,11.DOI:10.3724/2097-213X.2024.JFCT.0040
Cu-Pd/CP双金属催化剂电催化丙酮自缩合反应的研究
Investigation of electrocatalysis for acetone self-condensation using Cu-Pd/CP bimetallic catalyst
摘要
Abstract
Organic electrosynthesis is an important green and low-carbon method for upgrading short-chain biomass platform molecules into high-value-added chemicals.The development of efficient,cost-effective,and easily synthesized electrocatalysts is crucial for organic electrosynthesis reactions.In this study,a three-dimensional self-supporting Cu-Pd/CP bimetallic electrocatalyst was prepared using an electrodeposition method,with carbon paper(CP)as the substrate.The catalyst's performance and influencing factors in the electrocatalytic acetone self-condensation reaction were systematically investigated.Acetone,as a biomass-derived compound,primarily produces diacetone alcohol(DAA)in its self-condensation reaction,which has important applications in the chemical industry.However,traditional thermal catalysis methods suffer from high energy consumption and low efficiency.Electrocatalysis,with its mild reaction conditions,high controllability,and environmental friendliness,provides a new catalytic pathway for acetone self-condensation.In this study,the structure and composition of the Cu-Pd/CP catalyst were analyzed in detail using characterization techniques such as XRD,SEM,TEM,and XPS.The results revealed that the Cu-Pd bimetallic structure provides rich catalytic active sites,higher surface roughness,and synergy between the two metals,all of which contribute to the excellent catalytic performance of Cu-Pd/CP in the electrocatalytic acetone self-condensation reaction.Experimental results show that under optimal conditions,the Cu-Pd/CP bimetallic catalyst achieved a 28.11％acetone conversion rate and a 22.61％DAA yield,significantly outperforming traditional methods and other catalysts.A small amount of Pd promoted the formation of free radical anion intermediates during electrocatalysis,while Cu facilitated the coupling condensation reaction.The synergy between these two metals is key to the high catalytic activity of Cu-Pd/CP.Additionally,the study found that the electropolymerization current,reaction potential,and reaction temperature significantly influenced the reaction,providing valuable insights for the design of efficient catalysts for acetone electrochemical condensation reactions and industrial applications.In terms of the influence of catalyst materials,the Cu-Pd/CP bimetallic catalyst exhibited the highest response current and active surface area,indicating its most favorable performance in electrocatalytic acetone self-condensation.The study of electropolymerization current showed that appropriate Cu and Pd metal loadings,as well as the Cu/Pd mass ratio,are beneficial for the reaction,while excessive Cu content promotes DAA dehydration and excessive condensation of acetone.The experimental results on reaction potential showed that the DAA yield follows a volcano-type trend with respect to the reaction potential,reaching a peak at-2 V.However,with further increase in potential,the DAA yield decreased,likely due to faster reaction kinetics at higher potentials,which promoted the further dehydration of the condensation products.The temperature experiments indicated that at 25 ℃,the DAA yield and acetone conversion rate were highest,but as the temperature increased,both the DAA yield and acetone conversion rate decreased.Regarding catalyst stability,the Cu-Pd/CP bimetallic electrocatalyst was subjected to a 5 h electrolysis experiment at-2 V for acetone self-condensation.The results showed a decay in current density after approximately 12000 s.XRD analysis revealed that after cycling,Cu metal leaching occurred,and part of the Cu metal or CuO was detached into the solution.It is speculated that Pd metal also underwent leaching and loss.The LSV curves before and after stability testing indicated that after long-term electrolysis,the current density decreased significantly across the entire potential range,indicating a marked decline in catalyst activity.SEM images showed that the catalyst surface experienced metal detachment or dissolution and agglomeration,leading to morphological changes.In conclusion,this study successfully developed an efficient and easily synthesized Cu-Pd/CP bimetallic electrocatalyst and explored the catalytic mechanism and influencing factors in acetone self-condensation.These findings provide valuable references for the design of efficient catalysts for acetone electrochemical condensation reactions and their industrial applications,while also offering new insights into the upgrading and conversion of biomass-derived compounds.关键词
电催化/自缩合/丙酮/双金属催化剂Key words
electrocatalysis/self-condensation/acetone/bimetallic catalyst分类
化学化工引用本文复制引用
于方正,包桂蓉,罗嘉,潘浩伟,殷啸天,高鹏,吉学武,谈诚..Cu-Pd/CP双金属催化剂电催化丙酮自缩合反应的研究[J].燃料化学学报（中英文）,2025,53(6):872-882,11.基金项目
The project was supported by National Natural Science Foundation of China(52466014)and Yunnan Major Scientific and Technological Projects(202302AG050011). 国家自然科学基金(52466014)和云南省重大科技项目(202302AG050011)资助 （52466014）
