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Tailored nitrogen-defect induced by diels-alder reaction for enhanced electrochemical hydrogen evolution reaction
Yuan, Menglei1; Zhang, Lei2; Wang, Tianxin3; Liu, Yiming3; Li, Qiongguang4; Wu, Jinxiong5; Chen, Junwu6; Zhang, Jintong7; Yang, Hailun8; Zhang, Guangjin9
2023-03-01
Source PublicationJOURNAL OF COLLOID AND INTERFACE SCIENCE
ISSN0021-9797
Volume633Pages:754-763
AbstractElectrocatalytic water splitting in an alkaline medium is recognized as the promising technology to sustainably generate clean hydrogen energy via hydrogen evolution reaction (HER), while the sluggish water dissociation and subsequent *H adsorption steps greatly retarded the reaction kinetics and efficiency of the overall hydrogen evolution process. Whilst nitrogen (N)-doped carbon-based materials are attractive candidates for promoting HER activity, the facile fabrication and gaining a deeper insight into the electrocatalytic mechanism are still challenging. Herein, inspired by the Diels-Alder reaction, we precisely tailored six-membered pyridinic N and five-membered pyrrolic N sites at the edge of the carbon substrates. Comprehensive analysis validates that the participation of pyridinic N (electron-withdrawing) and pyrrolic N (electron-releasing) will induce the charge rearrangements, and further generate local electrophilic and nucleophilic domains in adjacent carbon rings, which guarantees the occurrence of water dissociation to generate protons and the subsequent adsorption of *H intermediates through elec-trostatic interactions, thereby facilitating the overall reaction kinetics. To this end, the optimal NC-ZnCl2- 25 % electrocatalysts present excellent alkaline HER activity (l10 = 45 mV, Tafel slop of 37.7 mV dec-1) superior to commercial Pt/C. (c) 2022 Elsevier Inc. All rights reserved.
KeywordTunable nitrogen-defect Diels-Alder reaction Carbon materials Charge redistribution Alkaline HER
DOI10.1016/j.jcis.2022.11.093
Language英语
WOS KeywordOXYGEN REDUCTION REACTION ; ACTIVE-SITES ; CARBON ; PH ; ELECTROCATALYSTS ; EFFICIENT ; GRAPHENE ; CATALYST ; NANOPARTICLES ; PERFORMANCE
Funding ProjectNational Natural Science Founda-tion of China ; National Key R&D Program of China ; Fundamental Research Funds for the Central Universities ; Natural Science Foundation of Shaanxi Province ; Regional Joint Fund of Guangdong Province ; [22178361] ; [21908228] ; [52101271] ; [2020YFA0710200] ; [G2022KY05111] ; [2021JQ-094] ; [2020A1515111017]
WOS Research AreaChemistry
WOS SubjectChemistry, Physical
Funding OrganizationNational Natural Science Founda-tion of China ; National Key R&D Program of China ; Fundamental Research Funds for the Central Universities ; Natural Science Foundation of Shaanxi Province ; Regional Joint Fund of Guangdong Province
WOS IDWOS:000901458400007
PublisherACADEMIC PRESS INC ELSEVIER SCIENCE
Citation statistics
Document Type期刊论文
Identifierhttp://ir.ipe.ac.cn/handle/122111/56337
Collection中国科学院过程工程研究所
Corresponding AuthorLi, Qiongguang; Yang, Hailun; Zhang, Guangjin
Affiliation1.Northwestern Polytech Univ, Sch Mat Sci & Engn, State Key Lab Solidificat Proc, Xian 710072, Peoples R China
2.Northwestern Polytech Univ, Sch Chem & Chem Engn, Key Lab Special Funct & Smart Polymer Mat, Minist Ind & Informat Technol, Xian 710129, Peoples R China
3.Northwestern Polytech Univ, Queen Mary Univ London Engn Sch, Xian 710129, Peoples R China
4.Anhui Jianzhu Univ, Sch Mat & Chem Engn, Hefei 230601, Peoples R China
5.Yili Normal Univ, Sch Chem & Environm Sci, Univ & Coll Key Lab Nat Prod Chem & Applicat Xinji, Yining 835000, Peoples R China
6.Ecole Polytech Fed Lausanne EPFL, Inst Chem Sci & Engn, CH-1015 Lausanne, Switzerland
7.Powertight Biotechnol Hangzhou Co Ltd, Hangzhou 311122, Peoples R China
8.SINOPEC Res Inst Petr Proc Co Ltd, Beijing 100083, Peoples R China
9.Chinese Acad Sci, Inst Proc Engn, CAS Key Lab Green Proc & Engn, Beijing 100190, Peoples R China
Recommended Citation
GB/T 7714
Yuan, Menglei,Zhang, Lei,Wang, Tianxin,et al. Tailored nitrogen-defect induced by diels-alder reaction for enhanced electrochemical hydrogen evolution reaction[J]. JOURNAL OF COLLOID AND INTERFACE SCIENCE,2023,633:754-763.
APA Yuan, Menglei.,Zhang, Lei.,Wang, Tianxin.,Liu, Yiming.,Li, Qiongguang.,...&Zhang, Guangjin.(2023).Tailored nitrogen-defect induced by diels-alder reaction for enhanced electrochemical hydrogen evolution reaction.JOURNAL OF COLLOID AND INTERFACE SCIENCE,633,754-763.
MLA Yuan, Menglei,et al."Tailored nitrogen-defect induced by diels-alder reaction for enhanced electrochemical hydrogen evolution reaction".JOURNAL OF COLLOID AND INTERFACE SCIENCE 633(2023):754-763.
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