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Recent advances and challenges of nitrogen/nitrate electro catalytic reduction to ammonia synthesis

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Frontiers in Energy 2024年第2期18卷 128-140页

作者： Junwen CAO Yikun HU Yun ZHENG Wenqiang ZHANG Bo YU Institute of Nuclear and New Energy Technology(INET) Collaborative Innovation Center of Advanced Nuclear Energy TechnologyTsinghua UniversityBeijing 100084China Department of Chemical Engineering University of WaterlooWaterlooOntario N2L 3G1Canada Institute of New Energy Materials and Engineering School of Materials Science and EngineeringFuzhou UniversityFuzhou 350108China

The Haber-Bosch process is the most widely used synthetic ammonia technology at *** its invention,it has provided an important guarantee for global food ***,the traditional Haber-Bosch ammonia synthesis process consumes a lot of energy and causes serious environmental *** the serious pressure of energy and environment,a green,clean,and sustainable ammonia synthesis route is urgently *** synthesis of ammonia is a green and mild new method for preparing ammonia,which can directly convert nitrogen or nitrate into ammonia using electricity driven by solar,wind,or water energy,without greenhouse gas and toxic gas ***,the basic mechanism of the nitrogen reduction reaction(NRR)to ammonia and nitrate reduction reaction(NO_(3)^(-))to ammonia were *** representative approaches and major technologies,such as lithium mediated electrolysis and solid oxide electrolysis cell(SOEC)electrolysis for NRR,high activity catalyst and advanced electrochemical device fabrication for(NO_(3)^(-))RR and electrochemical ammonia synthesis were *** on the above discussion and analysis,the main challenges and development directions for electrochemical ammonia synthesis were further proposed.

关键词： electrochemical ammonia synthesis nitrogen nitrate nitrogen reduction reaction(NRR)to ammonia nitrate reduction reaction(NO_(3)^(-))RR

Mechanochemical route to fabricate an efficient nitrate reduction electrocatalyst

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Nano Research 2024年第6期17卷 4889-4897页

作者： Yunliang Liu Zhiyu Zheng Sobia Jabeen Naiyun Liu Yixian Liu Yuanyuan Cheng Yaxi Li Jingwen Yu Xin Wu Nina Yan Lei Xu Haitao Li Institute for Energy Research School of Energy and Power EngineeringJiangsu UniversityZhenjiang 212013China Jiangsu Engineering Technology Research Center of Biomass Composites and Addictive Manufacturing Institute of Agricultural Facilities and EquipmentJiangsu Academy of Agricultural SciencesNanjing 210014China Key Laboratory for Protected Agricultural Engineering in the Middle and Lower Reaches of Yangtze River Ministry of Agriculture and Rural AffairsNanjing 210014China

The electrochemical nitrate reduction reaction(NO_(3)RR)to ammonia under ambient conditions is a promising approach for addressing elevated nitrate levels in water bodies,but the progress of this reaction is impeded by the complex series of chemical reactions involving electron and proton transfer and competing hydrogen evolution ***,it becomes imperative to develop an electro-catalyst that exhibits exceptional efficiency and remarkable selectivity for ammonia synthesis while maintaining long-term *** the magnetic biochar(Fe-C)has been synthesized by a two-step mechanochemical route after a pyrolysis treatment(450,700,and 1000℃),which not only significantly decreases the particle size,but also exposes more oxygen-rich functional groups on the surface,promoting the adsorption of nitrate and water and accelerating electron transfer to convert it into *** showed that the catalyst(Fe-C-700)has an impressive NH_(3)production rate of 3.5 mol·h^(−1)·gcat^(−1),high Faradaic efficiency of 88%,and current density of 0.37 A·cm^(−2)at 0.8 V *** hydrogen electrode(RHE).In-situ Fourier transform infrared spectroscopy(FTIR)is used to investigate the reaction intermediate and to monitor the *** oxygen functionalities on the catalyst surface activate nitrate ions to form various intermediates(NO_(2),NO,NH_(2)OH,and NH_(2))and reduce the rate determining step energy barrier(*NO_(3)→*NO_(2)).This study presents a novel approach for the use of magnetic biochar as an electro-catalyst in NO_(3)RR and opens the road for solving environmental and energy challenges.

关键词： mechanochemical route magnetic biochar electron transfer nitrate ammonia

Efficient ammonia electrosynthesis from nitrate via a three-step relay mechanism

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Science China Chemistry 2024年第1期67卷 319-320页

作者： Haifeng Jiang Gao-Feng Chen Haihui Wang Beijing Key Laboratory for Membrane Materials and Engineering Department of Chemical EngineeringTsinghua UniversityBeijing 100084China Department of Colloid Chemistry Max-Planck Institute of Colloids and InterfacesPotsdam 14476Germany School of Chemistry and Chemical Engineering South China University of TechnologyGuangzhou 510640China

Electrocatalytically converting nitrate waste to value-added ammonia(NO3−RR)is beneficial to environmental restoration and an attractive candidate for green ammonia production[1].However,developing NO_(3)^(-)RR in an energy-saving way remains a significant challenge due to the slow kinetics inherent in multi-step electron and proton transfer,making previous investigations for NO_(3)^(-)RR generally operate at a large overpotential(<-0.2 V versus reversible hydrogen electrode(RHE))to achieve optimal efficiency and industrial current for NH3 synthesis[2].

关键词： ammonia nitrate kinetics

Enhanced nitrate removal from groundwater using a conductive spacer in flow-electrode capacitive deionization

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Chinese Chemical Letters 2024年第8期35卷 379-382页

作者： Hongjie Guo Qiang Wei Yangyang Wu Wei Qiu Hongliang Li Changyong Zhang College of Mining Engineering Taiyuan University of TechnologyTaiyuan 030024China CAS Key Laboratory of Urban Pollutant Conversion Department of Environmental Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026China CAS Key Laboratory of Mechanical Behavior and Design of Materials Department of Modern MechanicsUniversity of Science and Technology of ChinaHefei 230026China

Flow-electrode capacitive deionization(FCDI)represents a promising approach for ion separation from aqueous ***,the optimization of spacer,particularly for nitrate-contaminated groundwa-ter systems,has often been *** research comprehensively investigates the influence of using a conductive(carbon cloth,CC)spacer on nitrate removal performance within FCDI system,comparing it to a non-conductive(nylon net,NN)*** both CC and NN FCDI systems,it is unsurprisingly that nitrate removal efficiency improved notably with the increasing current density and hydraulic retention time(HRT).Interestingly,the specific energy consumption(SEC)for nitrate removal did not show obvious fluctuations when the current density and HRT varied in both *** the auspiciously optimized process parameters,CC-FCDI attained a 20%superior nitrate removal efficiency relative to NN-FCDI,ac-companied by a notably diminished SEC for CC-FCDI,registering at a mere 28%of *** great improvement can be primarily attributed to the decrement in FCDI internal resistance after using con-ductive spacer,which further confirmed by electrochemical tests such as linear sweep voltammetry(LSV)and electrochemical impedance spectroscopy(EIS).Upon prolonged continuous nitrate removal at the optimized conditions,the CC-FCDI system achieved a consistent 90%nitrate removal efficiency with a low SEC of 2.7-7.8 kWh/kg NO_(3)-N,underscoring its steady ***,this study highlights the pivotal importance of careful spacer design and optimization in realizing energy-efficient groundwater treatment via FCDI.

关键词： Flow-electrode capacitive deionization Carbon cloth nitrate Underground water Ions transport

Analysis of Flowing and Heat Transfer of Commercial Molten nitrate in Porous Foundation Material

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Journal of Thermal Science 2023年第4期32卷 1455-1465页

作者： SHI Hua ZHOU Hao MENG Hanxiao LV Laiquan LIU Tianxiao ZUO Yuhang CEN Kefa State Key Laboratory of Clean Energy Utilization Institute for Thermal Power EngineeringZhejiang UniversityHangzhou310027China

The leakage accident of molten salt in the thermal storage tank will cause the shutdown and enormous economic losses of Concentrated Solar Power *** study investigates the heat transfer and flow characteristic of commercial molten nitrates leaking in the thermal state porous foundation *** migration width and depth of three molten nitrates,Solar Salt(60 wt%NaNO_(3)-40 wt%KNO_(3)),Hitec XL(7 wt%NaNO_(3)-45 wt%KNO_(3)-48 wt%Ca(NO_(3))_(2))and Hitec(7 wt%NaNO_(3)-53 wt%KNO_(3)-40 wt%NaNO_(2)),are obtained at different operating *** results indicate that the temperature rising rate of foundation material in the nitrate leaking process has a trend of first increasing rapidly and then decreasing,and then it increases slightly as the depth *** temperature rising rate increases obviously with increasing operating temperature of the molten *** the increase of the operating temperature,the distances from the storage tank bottom to solid salt in foundation and the total migration depths both increase obviously,while the average migrating widths change *** the same operating temperature,the temperature rising rate of the foundation material where Hitec XL and Hitec salt leak is significantly greater than that with Solar Salt,which is closely related to the melting points of molten *** migration depth of Hitec is 95.03%greater than that of Solar Salt and 19.11%larger than that of Hitec XL at the operating temperature of 300℃.Compared with Hitec XL,the leakage of Hitec with a smaller viscosity has a larger temperature rising rate and a wider and deeper transporting range during the leakage *** work could guide the installation locations of the leak detection devices for high temperature storage tank and the environmental treatment of leaking accident.

关键词： nitrate foundation material leaking flow heat transfer

Selective photo-reduction of nitrate to nitrogen with a two-step process by a KBH_(4)/Cu(II)modified CuFe_(2)O_(4)photocatalyst

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Nano Research 2023年第7期16卷 10462-10475页

作者： Li Cai Jinrui Guo Ting Liu Jing Tian Zhaoli Wang Yong Liu Mohamed SHamdy Xuping Sun College of Chemistry and Materials Science Sichuan Normal UniversityChengdu 610066China Chengdu Academy of Environmental Sciences Chengdu 610072China Key Laboratory of Treatment for Special Wastewater of Sichuan Province Higher Education System Chengdu 610066China Catalysis Research Group(CRG) Department of ChemistryCollege of ScienceKing Khalid UniversityP.O.Box 9004Abha 61413Saudi Arabia Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 610054China

nitrate(NO_(3)^(-))removal by photochemical-reduction has received extensive ***,the low selectivity of NO_(3)^(-)reduction to N_(2)hinders the application of this *** this study,a novel Cu@Fe-Cu-CuFe_(2)O_(4)-x photocatalyst was prepared by modifying CuFe_(2)O_(4)with KBH4 and Cu(II),and used to selectively reduce NO_(3)^(-)to N_(2)with a two-step reduction *** step(1),with Cu@Fe-Cu-CuFe_(2)O_(4)-x/ultraviolet(UV)system,91.0%NO_(3)^(-)was reduced to 52.3%NO_(2)-and 39.4%N_(2)within 60 *** rapid removal of NO_(3)^(-)was due to the synergistic effect of oxygen vacancies,Fe-Cu corrosion cell,and CuFe_(2)O_(4)*** step(2),H_(2)C_(2)O_(4)and H_(2)O_(2)were introduced into the effluent of step(1)to promote CO_(2)·-formation via Fe(II)and Fe(III)catalysis and UV radiation,which boosted the selective reduction of NO_(2)-to N_(2).When H_(2)C_(2)O_(4)and H_(2)O_(2)dosages were both 4.0 mmol·L^(-1)and the reaction time was 30 min,the removal efficiency of NO_(2)-achieved 100%and the selectivity of N_(2)was 83.0%.Overall,the two-step reduction process achieved 95.0%NO_(3)^(-)removal efficiency and 90.1%N_(2)selectivity with initial NO_(3)^(-)concentration of 30 mg·N·L^(-1).In addition,the denitrification mechanism of the two-step reduction process was tentatively proposed.

关键词： nitrate nitrite photochemical-reduction denitrification photocatalysis

nitrate confers rice adaptation to high ammonium by suppressing its uptake but promoting its assimilation

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Molecular Plant 2023年第12期16卷 1871-1874页

作者： Yu Yan Zhihua Zhang Huwei Sun Xiujie Liu Junpeng Xie Yahong Qiu Tuanyao Chai Chengcai Chu Bin Hu College of Life Sciences University of Chinese Academy of SciencesBeijing 100049China State Key Laboratory of Plant Genomics Institute of Genetics and Developmental BiologyInnovation Academy for Seed DesignChinese Academy of SciencesBeijing 100101China Jilin Province Engineering Laboratory of Plant Genetic Improvement College of Plant ScienceJilin UniversityChangchun 130062China Guangdong Laboratory for Lingnan Modern Agriculture College of AgricultureSouth China Agricultural UniversityGuangzhou 510642China Key Laboratory for Enhancing Resource Use Efficiency of Crops in South China Ministry of Agriculture and Rural AffairsSouth China Agricultural UniversityGuangzhou510642China

Dear Editor,earEaltor,Nitrogen(N)is the most important macronutrient driving plant growth and *** higher plants,inorganic N including nitrate(NO_(3)^(-))and ammonium(NH_(4)^(+))are predominant N sources(Hu et al.,2023).nitrate needs to be firstly reduced into ammonium to implement its assimilation,thus requiring a higher energy consumption than ammonium,making ammonium more cost effective for ***,ammonium usually causes severe growth retardation of plants under high concentration,which is known as ammonium *** concentrations of nitrate and ammonium greatly vary in different soil *** is the major inorganic N form in dry land,while ammonium accounts for thehighest proportion of inorganic N in the paddy field,where nitrification is suppressed(Haynes and Goh,1978).Although nitrogen is generally one of the most important contributing factors for yield increase,irrational fertilization strategies can cause negative effects.

关键词： ammonium nitrate inorganic

The nitrate-responsive transcription factor Md NLP7 regulates callus formation by modulating auxin response

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农业科学学报:英文版 2023年第10期22卷 3022-3033页

作者： LI Tong FENG Zi-quan ZHANG Ting-ting YOU Chun-xiang ZHOU Chao WANG Xiao-fei Apple Technology Innovation Center of Shandong Province/Shandong Collaborative Innovation Center of Fruit&Vegetable Quality and Efficient Production/National Key Laboratory of Wheat Improvement/College of Horticulture Science and Engineering Shandong Agricultural UniversityTai’an 271018P.R.China National Key Laboratory of Wheat Improvement/College of Life Sciences Shandong Agricultural UniversityTai’an 271018P.R.China

Under appropriate culture conditions,plant cells can regenerate new organs or even whole *** novo organ regeneration is an excellent biological system,which usually requires additional growth regulators,including auxin and *** is an essential nutrient element for plant vegetative and reproductive *** has been reported that nitrate is involved in auxin biosynthesis and transport throughout the growth and development of *** this study,we demonstrated that the ectopic expression of the MdNLP7 transcription factor in Arabidopsis could regulate the regeneration of root ***7 mainly participated in the regulation of callus formation,starting with pericycle cell division,and mainly affected auxin distribution and accumulation in the regulation ***,MdNLP7 upregulated the expression of genes related to auxin biosynthesis and transport in the callus formation *** results demonstrated that MdNLP7 may play a role in the nitrate-modulated regeneration of root ***,the results revealed that nitrate–auxin crosstalk is required for de novo callus initiation and clarified the mechanisms of organogenesis.

关键词： MdNLP7 callus initiation auxin nitrate pericycle shoot regeneration

Fromα-keto acids to nitrile oxides enabled by copper nitrate:a facile access to fused isoxazolines

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Organic Chemistry Frontiers 2022年第3期9卷 676-681页

作者： Yuping Zhu Tianqi Liu Bingxin Liu Houguang Shi Qitao Tan Bin Xu Department of Chemistry Affiliated Nantong Hospital of Shanghai University(The Sixth People’s Hospital of Nantong)Shanghai Engineering Research Center of Organ RepairInnovative Drug Research CenterSchool of MedicineShanghai UniversityShanghai 200444China State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

α-Keto acids were unprecedentedly employed as novel precursors of nitrile oxides on treatment with copper nitrate,which reacted with maleimides via[3+2]dipolar cycloaddition leading to pharmacologically interesting fused *** approach offers a unique strategy and complementary method for the convenient generation of alkyl substituted nitrile oxides.

关键词： nitrate fused oxides