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Support effect boosting the electrocatalytic N-2 reduction activity of Ni2P/N,P-codoped carbon nanosheet hybrids
Yuan, Menglei1,2; Zhang, Honghua1,2; Gao, Denglei1,2; He, Hongyan1,2; Sun, Yu3; Lu, Peilong1,2; Dipazir, Sobia1,2; Li, Qiongguang1,2; Zhou, Le1,2; Li, Shuwei1; Liu, Zhanjun2,4; Yang, Junhan1,2; Xie, Yongbing1,2; Zhao, He1,2; Zhang, Guangjin1,2
2020-02-07
Source PublicationJOURNAL OF MATERIALS CHEMISTRY A
ISSN2050-7488
Volume8Issue:5Pages:2691-2700
AbstractElectrochemical reduction of N-2 into NH3 (N2RR) under ambient conditions has emerged as a sustainable approach alternative to the Haber-Bosch process. However, the more favored H+ reduction in aqueous electrolytes can lead to low faradaic efficiency for NH3 production. Thus, designing electrocatalysts to suppress proton reduction is the key to improve the activities towards the N2RR. As an efficient strategy for modulating the associated electronic properties of surface catalysts, the support effect is drawing growing attention. Sparked by the support effect, Ni2P nanoparticles supported by N,P co-doped carbon nanosheets (Ni2P/N,P-C) were synthesized and found to have a higher affinity for N-2 molecules than for H+ which makes it a good candidate for the N2RR. The prepared catalyst showed an NH3 yield rate of 34.4 mu g h(-1) mg(Ni2P)(-1) at -0.2 V vs. the reversible hydrogen electrode (RHE) with a faradaic efficiency of 17.21% in 0.1 M HCl (22.89% and 57.2 mu g h(-1) mg(Ni2P)(-1) in 0.2 M PBS; 19.82% and 90.1 mu g h(-1) mg(Ni2P)(-1) in 0.1 M KOH), which is higher than the best values ever reported for noble-metal free catalysts in aqueous solution under ambient conditions. Importantly, the N,P-C substrate in this work is regarded as an electronic storage medium that regulates the electronic distribution of Ni2P/N,P-C when N-2 is chemically adsorbed at the Ni site, playing a vital role in inhibiting the adsorption of H and promoting the adsorption and activation of N-2 molecules. This work not only gives a new insight into understanding the transformation of the HER to the N2RR, but also provides a guideline for the development of highly active non-noble-metal catalysts.
DOI10.1039/c9ta09920d
Language英语
WOS KeywordELECTROCHEMICAL AMMONIA-SYNTHESIS ; DINITROGEN REDUCTION ; NITROGEN REDUCTION ; AMBIENT CONDITIONS ; OXYGEN VACANCIES ; RATIONAL DESIGN ; WATER ; FIXATION ; NITRIDE ; CONVERSION
Funding ProjectKey Program for International S&T Cooperation Projects of China from the Ministry of Science and Technology of China[2018YFE0124600] ; National Natural Science Foundation of China[U1662121] ; Youth Innovation Promotion Association of CAS
WOS Research AreaChemistry ; Energy & Fuels ; Materials Science
WOS SubjectChemistry, Physical ; Energy & Fuels ; Materials Science, Multidisciplinary
Funding OrganizationKey Program for International S&T Cooperation Projects of China from the Ministry of Science and Technology of China ; National Natural Science Foundation of China ; Youth Innovation Promotion Association of CAS
WOS IDWOS:000521200000043
PublisherROYAL SOC CHEMISTRY
Citation statistics
Cited Times:10[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.ipe.ac.cn/handle/122111/39871
Collection中国科学院过程工程研究所
Corresponding AuthorZhang, Guangjin
Affiliation1.Chinese Acad Sci, State Key Lab Multiphase Complex Syst, Beijing Key Lab Ion Liquids Clean Proc, CAS Key Lab Green Proc Engn,Inst Proc Engn, Beijing 100190, Peoples R China
2.Univ Chinese Acad Sci, Ctr Mat Sci & Optoelect Engn, Beijing 100049, Peoples R China
3.North Univ China, Sch Sci, Taiyuan 030051, Peoples R China
4.Chinese Acad Sci, Inst Coal Chem, CAS Key Lab Carbon Mat, Taiyuan 030001, Peoples R China
Recommended Citation
GB/T 7714
Yuan, Menglei,Zhang, Honghua,Gao, Denglei,et al. Support effect boosting the electrocatalytic N-2 reduction activity of Ni2P/N,P-codoped carbon nanosheet hybrids[J]. JOURNAL OF MATERIALS CHEMISTRY A,2020,8(5):2691-2700.
APA Yuan, Menglei.,Zhang, Honghua.,Gao, Denglei.,He, Hongyan.,Sun, Yu.,...&Zhang, Guangjin.(2020).Support effect boosting the electrocatalytic N-2 reduction activity of Ni2P/N,P-codoped carbon nanosheet hybrids.JOURNAL OF MATERIALS CHEMISTRY A,8(5),2691-2700.
MLA Yuan, Menglei,et al."Support effect boosting the electrocatalytic N-2 reduction activity of Ni2P/N,P-codoped carbon nanosheet hybrids".JOURNAL OF MATERIALS CHEMISTRY A 8.5(2020):2691-2700.
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