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

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

doi:10.1016/j.jechem.2023.10.014

Journal of Energy Chemistry

2024

DOI: 10.1016/j.jechem.2023.10.014

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

Honggang Huang,

Yao Chen,

Hui Fu

et al.

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Cited by 4 publications

References 62 publications

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Crystal‐Phase‐Engineered High‐Entropy Alloy Aerogels for Enhanced Ethylamine Electrosynthesis from Acetonitrile

Huang,

Chen,

Chang

et al. 2024

Advanced Materials

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Crystal‐phase engineering that promoting the rearrangement of active atoms to form new structural frameworks has achieved excellent result in the field of electrocatalysis and optimized the performance of various electrochemical reactions. Herein, for the first time, we found that the different components in metallic aerogels will affect the crystal‐phase transformation, especially in high‐entropy alloy aerogels (HEAAs), whose crystal‐phase transformation during annealing is more difficult than medium‐entropy alloy aerogels (MEAAs), but they still show better electrochemical performance. Specifically, PdPtCuCoNi HEAAs with the parent phase of face‐centered cubic (FCC) PdCu possess excellent 89.24% of selectivity, 746.82 mmol h−1 g−1cat. of yield rate, and 90.75% of Faraday efficiency for ethylamine during acetonitrile reduction reaction (ARR), while maintaining stability under 50 h of long‐term testing and 10 consecutive electrolysis cycles. The structure‐activity relationship indicates that crystal‐phase regulation from amorphous state to FCC phase promotes the atomic rearrangement in HEAAs, thereby optimizing the electronic structure, and enhancing the adsorption strength of reaction intermediates, improving the catalytic performance. This study provides a new paradigm for developing novel ARR electrocatalysts, and also expands the potential of crystal‐phase engineering in other application areas.This article is protected by copyright. All rights reserved

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Crystal‐Phase‐Engineered High‐Entropy Alloy Aerogels for Enhanced Ethylamine Electrosynthesis from Acetonitrile

Huang,

Chen,

Chang

et al. 2024

Advanced Materials

Self Cite

View full text Add to dashboard Cite

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Ultrathin nickel sulfide nanosheets for sulfur ion electrooxidation assisted acetonitrile electroreduction

Wang,

Zhang,

et al. 2024

Sci. China Chem.

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p–d Orbital Hybridization in Pd₃Sn Metallic Aerogels Boosts Alcohol Electrooxidation

Guan,

Fu,

Zhu

et al. 2024

Chem. Mater.

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Orbital engineering of nanomaterials has been proven to be a compelling strategy, which stimulates the synthesis of palladium (Pd)-based nanomaterials with p−d orbital hybridization and the exploration of their electrocatalytic properties. Herein, Pd 3 Sn metallic aerogels (Pd 3 Sn MAs) with p−d orbital hybridization were reasonably constructed as efficient electrocatalysts for alcohol electrooxidation. In particular, the mass activity and specific activity of Pd 3 Sn MAs for the ethylene glycol oxidation reaction are 1.69 A mg Pd −1 and 3.56 mA cm Pd −2, respectively, superior to Pd MAs and commercial Pd/C. Meanwhile, benefiting from the excellent antipoisoning properties, Pd 3 Sn MAs still maintain satisfactory activity after long-term durability tests. Moreover, the same trend can be observed in reactions such as the methanol oxidation reaction, the ethanol oxidation reaction, and the glycerol oxidation reaction. Furthermore, density functional theory calculations reveal that the p−d orbital hybridization of Pd 3 Sn MAs precisely regulates the electronic structure and d-band center of Pd and also decreases the reaction energy barrier in the rate-determining step, thus reactivating the surface of Pd 3 Sn MAs. This study provides a broad prospect for the design of efficient fuel cell electrocatalysts through orbital engineering.

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

Cited by 4 publications

References 62 publications

Crystal‐Phase‐Engineered High‐Entropy Alloy Aerogels for Enhanced Ethylamine Electrosynthesis from Acetonitrile

Crystal‐Phase‐Engineered High‐Entropy Alloy Aerogels for Enhanced Ethylamine Electrosynthesis from Acetonitrile

Ultrathin nickel sulfide nanosheets for sulfur ion electrooxidation assisted acetonitrile electroreduction

p–d Orbital Hybridization in Pd₃Sn Metallic Aerogels Boosts Alcohol Electrooxidation

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

Cited by 4 publications

References 62 publications

Crystal‐Phase‐Engineered High‐Entropy Alloy Aerogels for Enhanced Ethylamine Electrosynthesis from Acetonitrile

Crystal‐Phase‐Engineered High‐Entropy Alloy Aerogels for Enhanced Ethylamine Electrosynthesis from Acetonitrile

Ultrathin nickel sulfide nanosheets for sulfur ion electrooxidation assisted acetonitrile electroreduction

p–d Orbital Hybridization in Pd3Sn Metallic Aerogels Boosts Alcohol Electrooxidation

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Product

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p–d Orbital Hybridization in Pd₃Sn Metallic Aerogels Boosts Alcohol Electrooxidation