A strain-engineered self-intercalation Ta9Se12 based bifunctional single atom catalyst for oxygen evolution and reduction reactions

A self-intercalation Ta9Se12 supported Pd SAC was evidenced to be a promising bifunctional catalyst for OER and ORR under strain. [Display omitted] •The Ta intercalation can effectively improve the stability and activity of supported SACs.•Some intercalated SACs with high performance were identified...

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Vydáno v:Applied surface science Ročník 602; s. 154378
Hlavní autoři: Huang, Hai-Cai, Wang, Ting-Ting, Li, Jun, Chen, Jing, Bu, Yuxiang, Cheng, Shi-Bo
Médium: Journal Article
Jazyk:angličtina
Vydáno: Elsevier B.V 15.11.2022
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ISSN:0169-4332, 1873-5584
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Abstract A self-intercalation Ta9Se12 supported Pd SAC was evidenced to be a promising bifunctional catalyst for OER and ORR under strain. [Display omitted] •The Ta intercalation can effectively improve the stability and activity of supported SACs.•Some intercalated SACs with high performance were identified for OER and ORR, respectively.•Pd-Ta9Se12 was evidenced to be a promising bifunctional catalyst under a 3 % tensile strain.•Charge transfer to the surface is the origin for the enhancement of stability and activity of SAC. Seeking and designing stable, high-efficiency, and economical bifunctional catalysts for the metal-air battery is challenging but of great significance towards the conversion and storage of renewable energy. In this study, based on first principles calculations, the oxygen evolution (OER) and oxygen reduction reaction (ORR) catalytic performance of different transition-metal (TM) atoms embedded into the surface of the self-intercalation structure Ta9Se12 (TM-Ta9Se12) were evaluated. The results demonstrate that the self-intercalated Ta-layer obviously improves the stability and catalytic activity of the system. Remarkably, Pd-Ta9Se12 under a tensile strain of 3 % was identified as an efficient bifunctional catalyst for OER and ORR with overpotentials of 0.65 and 0.42 V, respectively. Mechanistically, the intercalation structure of Ta9Se12 leads to a charge accumulation in the inner layer. But divertingly, under an external force, the charge in the inner layer will diffuse to the surface. This curious phenomenon can provide the possibility for directional and continuous regulation of the catalytic performance of the catalysts. This work elucidates a new approach for designing high-efficient and stable bifunctional SACs for OER and ORR.
AbstractList A self-intercalation Ta9Se12 supported Pd SAC was evidenced to be a promising bifunctional catalyst for OER and ORR under strain. [Display omitted] •The Ta intercalation can effectively improve the stability and activity of supported SACs.•Some intercalated SACs with high performance were identified for OER and ORR, respectively.•Pd-Ta9Se12 was evidenced to be a promising bifunctional catalyst under a 3 % tensile strain.•Charge transfer to the surface is the origin for the enhancement of stability and activity of SAC. Seeking and designing stable, high-efficiency, and economical bifunctional catalysts for the metal-air battery is challenging but of great significance towards the conversion and storage of renewable energy. In this study, based on first principles calculations, the oxygen evolution (OER) and oxygen reduction reaction (ORR) catalytic performance of different transition-metal (TM) atoms embedded into the surface of the self-intercalation structure Ta9Se12 (TM-Ta9Se12) were evaluated. The results demonstrate that the self-intercalated Ta-layer obviously improves the stability and catalytic activity of the system. Remarkably, Pd-Ta9Se12 under a tensile strain of 3 % was identified as an efficient bifunctional catalyst for OER and ORR with overpotentials of 0.65 and 0.42 V, respectively. Mechanistically, the intercalation structure of Ta9Se12 leads to a charge accumulation in the inner layer. But divertingly, under an external force, the charge in the inner layer will diffuse to the surface. This curious phenomenon can provide the possibility for directional and continuous regulation of the catalytic performance of the catalysts. This work elucidates a new approach for designing high-efficient and stable bifunctional SACs for OER and ORR.
ArticleNumber 154378
Author Li, Jun
Bu, Yuxiang
Huang, Hai-Cai
Cheng, Shi-Bo
Wang, Ting-Ting
Chen, Jing
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  email: shibocheng@sdu.edu.cn
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crossref_primary_10_3390_molecules30071505
crossref_primary_10_1002_smtd_202402196
crossref_primary_10_1016_j_apsusc_2022_155846
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Keywords Bifunctional catalysts
Self-intercalation
Single-atom catalysts
Oxygen evolution reaction
Charge transfer
Oxygen reduction reaction
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Snippet A self-intercalation Ta9Se12 supported Pd SAC was evidenced to be a promising bifunctional catalyst for OER and ORR under strain. [Display omitted] •The Ta...
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StartPage 154378
SubjectTerms Bifunctional catalysts
Charge transfer
Oxygen evolution reaction
Oxygen reduction reaction
Self-intercalation
Single-atom catalysts
Title A strain-engineered self-intercalation Ta9Se12 based bifunctional single atom catalyst for oxygen evolution and reduction reactions
URI https://dx.doi.org/10.1016/j.apsusc.2022.154378
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