气候变化领域集成服务门户(CCPortal): Tuning metal single atoms embedded in NxCy moieties toward high-performance electrocatalysis

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DOI	10.1039/d1ee00154j
	Tuning metal single atoms embedded in NxCy moieties toward high-performance electrocatalysis
	Ha M.; Kim D.Y.; Umer M.; Gladkikh V.; Myung C.W.; Kim K.S.
发表日期	2021
ISSN	17545692
起始页码	3455
结束页码	3468
卷号	14 期号:6
英文摘要	Noble nanoparticle (NP)-sized electrocatalysts have been exploited for diverse electrochemical reactions, in particular, for an eco-friendly hydrogen economy such as water splitting. Recently, minimal amounts of single atoms (SAs) are exploited to maximize the active surface area and to tune the catalytic activity by coordinating the SAs in defect sites of N-doped graphene (GN). For the hydrogen evolution reaction (HER) and oxygen evolution/reduction reactions (OER/ORR), we show high-performance 3d-5d transition metal (TM) SA catalysts using density functional theory (DFT) along with machine learning (ML)-based descriptors. We explore the stability and activity of TM-GNfrom the view of structure/coordination, formation energy, structural/electrochemical stability, electronic properties, electrical conductivity, and reaction mechanism, which have not been seriously explored yet. Among various -NnCmmoieties, the -N2C2moieties tend to be more easily formed and show higher electrochemical catalytic performance and longer durability (without aggregation/dissolution) compared with the widely studied pure -C4/C3and -N4/N3moieties. We found that some TM(SA)s favor a new OER/ORR mechanism, completely different from any known mechanism. The ML-based descriptors showing super HER/OER/ORR performances better than those of bench-mark noble metal catalysts are assessed. In the N2C2templates, Ni/Ru/Rh/Pt show low HER overpotentials. Here, the H adsorption sites are shared by both the metal and C (not N), which was undiscussed in most of the previous literature where the H is attached on top of a metal atom. Low OER overpotentials are found for Pt/Ni-N2C2, Ni/Pd-C4, and Rh-N4, while low ORR overpotentials are found for Ir/Rh-N4, Pd-C4, Ru-N3C1and Ni/Pd/Pt-N1C3. The present findings should help in designing high-performance SA catalysts for other various electrocatalytic reactions such as the ammonia evolution reaction. © The Royal Society of Chemistry 2021.
英文关键词	Ammonia; Atoms; Density functional theory; Doping (additives); Electrocatalysis; Electrocatalysts; Electronic properties; Hydrogen economy; Hydrogen evolution reaction; Precious metals; Active surface area; Catalytic performance; Electrical conductivity; Electrocatalytic reactions; Electrochemical reactions; Evolution reactions; Noble metal catalysts; Reaction mechanism; Catalyst activity; adsorption; catalysis; catalyst; durability; electrical conductivity; electrochemistry; hydrogen; machine learning; nanoparticle; performance assessment
语种	英语
来源期刊	Energy & Environmental Science
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/190641
作者单位	Center for Superfunctional Materials, Department of Chemistry, Ulsan National Institute of Science and Technology (UNIST), 50 UNIST-gil, Ulsan, 44919, South Korea; Department of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), 50 UNIST-gil, Ulsan, 44919, South Korea; Yusuf Hamied Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge, CB2 1EW, United Kingdom
推荐引用方式 GB/T 7714	Ha M.,Kim D.Y.,Umer M.,et al. Tuning metal single atoms embedded in NxCy moieties toward high-performance electrocatalysis[J],2021,14(6).
APA	Ha M.,Kim D.Y.,Umer M.,Gladkikh V.,Myung C.W.,&Kim K.S..(2021).Tuning metal single atoms embedded in NxCy moieties toward high-performance electrocatalysis.Energy & Environmental Science,14(6).
MLA	Ha M.,et al."Tuning metal single atoms embedded in NxCy moieties toward high-performance electrocatalysis".Energy & Environmental Science 14.6(2021).