Interfacial Engineering Promoting Electrosynthesis of Ammonia over Mo/Phosphotungstic Acid with High Performance

doi:10.1002/adfm.202009151

	Interfacial Engineering Promoting Electrosynthesis of Ammonia over Mo/Phosphotungstic Acid with High Performance
	Liao, Wanru 1; Qi, Lu 1; Wang, Yanlei 2; Qin, Jingyu 2; Liu, Guangyong 2; Liang, Shijing 1; He, Hongyan 2; Jiang, Lilong 1
刊名	ADVANCED FUNCTIONAL MATERIALS
	2021-03-27
页码	9
关键词	ammonia synthesis electrocatalysis high faradaic efficiency interfacial engineering phosphotungstic acid‐ based catalyst
ISSN号	1616-301X
DOI	10.1002/adfm.202009151
英文摘要	Electrochemical 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.
资助项目	National 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研究方向	Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics
语种	英语
出版者	WILEY-V C H VERLAG GMBH
WOS记录号	WOS:000633508900001
资助机构	National Natural Science Foundation of China ; Youth Innovation Promotion Association of CAS
内容类型	期刊论文
源URL	[http://ir.ipe.ac.cn/handle/122111/48055]
专题	中国科学院过程工程研究所
通讯作者	Liang, Shijing; He, Hongyan
作者单位	1.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
推荐引用方式 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.