气候变化领域集成服务门户(CCPortal): Nitrate reduction to ammonium: From CuO defect engineering to waste NOx-to-NH3 economic feasibility

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DOI	10.1039/d1ee00594d
	Nitrate reduction to ammonium: From CuO defect engineering to waste NOx-to-NH3 economic feasibility
	Daiyan R.; Tran-Phu T.; Kumar P.; Iputera K.; Tong Z.; Leverett J.; Khan M.H.A.; Asghar Esmailpour A.; Jalili A.; Lim M.; Tricoli A.; Liu R.-S.; Lu X.; Lovell E.; Amal R.
发表日期	2021
ISSN	17545692
起始页码	3588
结束页码	3598
卷号	14 期号:6
英文摘要	Critical to the feasibility of electrochemical reduction of waste NOx(NOxRR), as a sustainable pathway and to close the NOxcycle for the emerging NH3economy, is the requirement of inexpensive, scalable and selective catalysts that can generate NH4+with high yield, as indicated by our economic modelling. To this end, we carry out density functional theory (DFT) calculations to investigate the possible contribution of oxygen vacancy (OV) defects in NOxRR catalysis, discovering that an increase in defect density within CuO is leading to a decrease in adsorption energy for NO3−reactants. Using these findings as design guidelines, we develop defective CuO nanomaterials using flame spray pyrolysis (FSP) and mild plasma treatment, that can attain a NH4+yield of 520 μmol cm−2h−1at a cell voltage of 2.2 V within a flow electrolyser with good stability over 10 h of operation. Through our mechanistic investigation, we establish the beneficial role of oxygen vacancy defects (with one free electron) in CuO for NOxRR and we reveal a direct correlation of oxygen vacancy density with the NH4+yield, arising from improved NO3−adsorption, as evidenced from our theoretical calculations. Our findings on defect engineering to improve NH4+yield and its economic feasibility display the potential of NOxRR as an alternative pathway to generate green NH3, which can also serve as an energy vector for the emerging hydrogen economy and close the NOxcycle. © The Royal Society of Chemistry 2021.
英文关键词	Ammonia; Copper oxides; Defects; Density functional theory; Design for testability; Electrolytic reduction; Electrons; Flame spraying; Hydrogen economy; Nitrogen oxides; Oxygen; Plasma applications; Plasma stability; Spray pyrolysis; Adsorption energies; Defect engineering; Economic feasibilities; Economic modelling; Electrochemical reductions; Oxygen vacancy defects; Selective catalysts; Theoretical calculations; Oxygen vacancies; adsorption; catalyst; design; fuel cell; hydrogen; nanomaterial; nitrate; oxygen; plasma; pyrolysis; spray
语种	英语
来源期刊	Energy & Environmental Science
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/190643
作者单位	Particles and Catalysis Research Laboratories and School of Chemical Engineering, UNSW Sydney, Sydney, NSW 2052, Australia; Nanotechnology Research Laboratory, Faculty of Engineering University of SydneyNSW 2006, Australia; Nanotechnology Research Laboratory, Research School of Chemistry, College of Science, Australian National University, Canberra, ACT 2601, Australia; Department of Chemistry, National Taiwan University, Taipei, 106, Taiwan
推荐引用方式 GB/T 7714	Daiyan R.,Tran-Phu T.,Kumar P.,et al. Nitrate reduction to ammonium: From CuO defect engineering to waste NOx-to-NH3 economic feasibility[J],2021,14(6).
APA	Daiyan R..,Tran-Phu T..,Kumar P..,Iputera K..,Tong Z..,...&Amal R..(2021).Nitrate reduction to ammonium: From CuO defect engineering to waste NOx-to-NH3 economic feasibility.Energy & Environmental Science,14(6).
MLA	Daiyan R.,et al."Nitrate reduction to ammonium: From CuO defect engineering to waste NOx-to-NH3 economic feasibility".Energy & Environmental Science 14.6(2021).