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Interfacial Engineering Promoting Electrosynthesis of Ammonia over Mo/Phosphotungstic Acid with High Performance
Liao, Wanru1; Qi, Lu1; Wang, Yanlei2; Qin, Jingyu2; Liu, Guangyong2; Liang, Shijing1; He, Hongyan2; Jiang, Lilong1
2021-03-27
Source PublicationADVANCED FUNCTIONAL MATERIALS
ISSN1616-301X
Pages9
AbstractElectrochemical nitrogen reduction reaction (eNRR) is recognized as a promising approach for ammonia synthesis, which is, however, impeded by the inert nitrogen and the unavoidable competing hydrogen evolution reaction (HER). Here, a Mo-PTA@CNT electrocatalyst in which Mo species are anchored on the fourfold hollow sites of phosphotungstic acid (PTA) and closely embedded in multi-walled carbon nanotubes (CNT) for immobilization is designed and synthesized. Interestingly, the catalyst presents a high ammonia yield rate of 51 +/- 1 mu g h(-1) mg(cat.)(-1) and an excellent Faradaic efficiency of 83 +/- 1% at -0.1 V versus RHE under ambient conditions. The concentrations of NH4+ are also quantitatively calculated by H-1 NMR spectra and ion chromatography. Isotopic labeling identifies that the N atom of the formed NH3 originates from N-2. The controlled experiments confirm a strong interaction between Mo-PTA and N-2 with an adsorption energy of 50.46 kJ mol(-1) and activation energy of 21.36 kJ mol(-1). More importantly, due to CNT's gas storage and hydrophobicity properties, there is a fourfold increase in N-2 content. The concentration of H2O is reduced by more than half at the interface of the electrode. Thus, the activity of eNRR can be significantly improved with ultrahigh electron selectivity.
Keywordammonia synthesis electrocatalysis high faradaic efficiency interfacial engineering phosphotungstic acid‐ based catalyst
DOI10.1002/adfm.202009151
Language英语
Funding ProjectNational Natural Science Foundation of China[22078063] ; National Natural Science Foundation of China[21825801] ; National Natural Science Foundation of China[21922813] ; Youth Innovation Promotion Association of CAS[2017066]
WOS Research AreaChemistry ; Science & Technology - Other Topics ; Materials Science ; Physics
WOS SubjectChemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter
Funding OrganizationNational Natural Science Foundation of China ; Youth Innovation Promotion Association of CAS
WOS IDWOS:000633508900001
PublisherWILEY-V C H VERLAG GMBH
Citation statistics
Document Type期刊论文
Identifierhttp://ir.ipe.ac.cn/handle/122111/48056
Collection中国科学院过程工程研究所
Corresponding AuthorLiang, Shijing; He, Hongyan
Affiliation1.Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Peoples R China
2.Chinese Acad Sci, State Key Lab Multiphase Complex Syst, Beijing Key Lab Ion Liquids Clean Proc, Inst Proc Engn,CAS Key Lab Green Proc & Engn, Beijing 100190, Peoples R China
Recommended Citation
GB/T 7714
Liao, Wanru,Qi, Lu,Wang, Yanlei,et al. Interfacial Engineering Promoting Electrosynthesis of Ammonia over Mo/Phosphotungstic Acid with High Performance[J]. ADVANCED FUNCTIONAL MATERIALS,2021:9.
APA Liao, Wanru.,Qi, Lu.,Wang, Yanlei.,Qin, Jingyu.,Liu, Guangyong.,...&Jiang, Lilong.(2021).Interfacial Engineering Promoting Electrosynthesis of Ammonia over Mo/Phosphotungstic Acid with High Performance.ADVANCED FUNCTIONAL MATERIALS,9.
MLA Liao, Wanru,et al."Interfacial Engineering Promoting Electrosynthesis of Ammonia over Mo/Phosphotungstic Acid with High Performance".ADVANCED FUNCTIONAL MATERIALS (2021):9.
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