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A three-dimensional ordered honeycomb nanostructure anchored with Pt-N active sites via self-assembly of a block copolymer: an efficient electrocatalyst towards the oxygen reduction reaction in fuel cells
Wang, Zhida1; Yang, Yi1,2; Wang, Xiaoman1; Lu, Zhuoxin1; Guo, Changqing1; Shi, Yan1; Tan, Hongyi1; Shen, Lisha1; Cao, Shuo3; Yan, Changfeng1,2
Corresponding AuthorWang, Zhida(wangzd@ms.giec.ac.cn) ; Yan, Changfeng(yancf@ms.giec.ac.cn)
2022-06-07
Source PublicationJOURNAL OF MATERIALS CHEMISTRY A
ISSN2050-7488
Volume10Issue:22Pages:12141-12149
AbstractMesoporous Pt-containing nanocomposites with well-organized pores are desirable for fuel cells as well as sensors, electronics, and various chemical reactions. However, it remains challenging to construct three-dimensional (3D) ordered honeycomb-like (OHC) nanostructures with Pt species anchored in the mesopores. Herein, we show for the first time an in situ strategy of developing an N-doped ordered honeycomb (N-OHC) nanopattern with well-dispersed Pt-N-2 moieties by using the self-assembly of a block copolymer (BCP). The as-mentioned Pt including Pt single atoms (SAs) and Pt similar to 2.5 nm ultrafine nanoparticles (NPs) was hierarchically located on the inner walls and the outer surfaces of the N-OHC mesopores (Pt/N-OHC), forming well-dispersed Pt-N active sites and showing efficient catalytic activity towards the oxygen reduction reaction (ORR). By changing the film thickness of the pristine Pt/BCP template, double-layered Pt/N-OHC could be designed and the ORR activity could be correspondingly improved, for which a current density of 1.60 A cm(-2)@0.6 V and a peak power density of 1.07 W cm(-2) were observed at a very low Pt-loading of 0.04 mg cm(-2), better than 1.21 A cm(-2)@0.6 V and 0.79 W cm(-2) of the commercial Pt/C catalyst at a Pt-loading of 0.15 mg cm(-2). The electron donating behavior of Pt-N-2 and the pathway for O-2 reduction were investigated via the density functional theory (DFT) computation. The electron transfer from Pt to N gave rise to the formation of Pt-N covalent bonds, which resulted in a lower d band center and a weaker O adsorption energy and endowed the Pt/N-OHCs with enhanced ORR activity.
Funding OrganizationSTS Regional Key Project of the Chinese Academy of Sciences ; Guangzhou Science and Technology Plan Project
DOI10.1039/d2ta00752e
Indexed BySCI
Language英语
Funding ProjectSTS Regional Key Project of the Chinese Academy of Sciences[KFJ-STS-QYZD-2021-02-003] ; Guangzhou Science and Technology Plan Project[201904010412] ; Guangzhou Science and Technology Plan Project[202002030349] ; Guangzhou Science and Technology Plan Project[202103040002]
WOS Research AreaChemistry ; Energy & Fuels ; Materials Science
WOS SubjectChemistry, Physical ; Energy & Fuels ; Materials Science, Multidisciplinary
WOS IDWOS:000798865000001
PublisherROYAL SOC CHEMISTRY
Citation statistics
Document Type期刊论文
Identifierhttp://ir.imr.ac.cn/handle/321006/174014
Collection中国科学院金属研究所
Corresponding AuthorWang, Zhida; Yan, Changfeng
Affiliation1.Chinese Acad Sci, Guangzhou Inst Energy Convers, CAS Key Lab Renewable Energy, Guangdong Key Lab New & Renewable Energy Res & De, Guangzhou 510640, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100039, Peoples R China
3.Chinese Acad Sci, Inst Met Res, Shenyang 110016, Peoples R China
Recommended Citation
GB/T 7714
Wang, Zhida,Yang, Yi,Wang, Xiaoman,et al. A three-dimensional ordered honeycomb nanostructure anchored with Pt-N active sites via self-assembly of a block copolymer: an efficient electrocatalyst towards the oxygen reduction reaction in fuel cells[J]. JOURNAL OF MATERIALS CHEMISTRY A,2022,10(22):12141-12149.
APA Wang, Zhida.,Yang, Yi.,Wang, Xiaoman.,Lu, Zhuoxin.,Guo, Changqing.,...&Yan, Changfeng.(2022).A three-dimensional ordered honeycomb nanostructure anchored with Pt-N active sites via self-assembly of a block copolymer: an efficient electrocatalyst towards the oxygen reduction reaction in fuel cells.JOURNAL OF MATERIALS CHEMISTRY A,10(22),12141-12149.
MLA Wang, Zhida,et al."A three-dimensional ordered honeycomb nanostructure anchored with Pt-N active sites via self-assembly of a block copolymer: an efficient electrocatalyst towards the oxygen reduction reaction in fuel cells".JOURNAL OF MATERIALS CHEMISTRY A 10.22(2022):12141-12149.
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