首页|d-d Orbital coupling induced by crystal-phase engineering assists acetonitrile electroreduction to ethylamine

d-d Orbital coupling induced by crystal-phase engineering assists acetonitrile electroreduction to ethylamine

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The d-d orbital coupling induced by crystal-phase engineering can effectively adjust the electronic struc-ture of electrocatalysts,thus showing significant catalytic performance,while it has been rarely explored in electrochemical acetonitrile reduction reaction(ARR)to date.Herein,we successfully realize the struc-tural transformation of PdCu metallic aerogels(MAs)from face-centered cubic(FCC)to body-centered cubic(BCC)through annealing treatment.Specifically,the BCC PdCu MAs exhibit excellent ARR perfor-mance with high ethylamine selectivity of 90.91％,Faradaic efficiency of 88.60％,yield rate of 316.0 mmol h-1 g-1Pd1+Cu and long-term stability for consecutive electrolysis within 20 h at-0.55 V vs.rever-sible hydrogen electrode,outperforming than those of FCC PdCu MAs.Under the membrane electrode assembly system,BCC PdCu MAs also demonstrate excellent ethylamine yield rate of 389.5 mmol h-1 g-1PdCu-1 Density functional theory calculation reveals that the d-d orbital coupling in BCC PdCu MAs results in an evident correlation effect for the interaction of Pd and Cu sites,which boosts up the Cu sites electronic activities to enhance ARR performance.Our work opens a new route to develop efficient ARR electrocata-lysts from the perspective of crystalline structure transformation.

d-d Orbital couplingCrystal-phase engineeringMetallic aerogelsAcetonitrile electroreduction reactionEthylamine

Honggang Huang、Yao Chen、Hui Fu、Cun Chen、Hanjun Li、Zhe Zhang、Feili Lai、Shuxing Bai、Nan Zhang、Tianxi Liu

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Key Laboratory of Synthetic and Biological Colloids,Ministry of Education,School of Chemical and Material Engineering,Jiangnan University,Wuxi 214122,Jiangsu,China

Department of Chemistry,KU Leuven,Celestijnenlaan 200F,Leuven 3001,Belgium

College of Chemistry and Chemical Engineering,Qingdao University,Qingdao 266071,Shandong,China

National Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaPostdoctoral Research Foundation of ChinaNatural Science Foundation of Jiangsu ProvinceCentral Laboratory,School of Chemical and Material Engineering,Jiangnan University

52161135302221050872022M721360BK20210446

2024

10.1016/j.jechem.2023.10.014

能源化学
中国科学院大连化学物理研究所 中国科学院成都有机化学研究所

能源化学

CSTPCDEI
影响因子：0.654
ISSN：2095-4956
年,卷(期)：2024.89(2)
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