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Progress in electrocatalytic nitrate reduction for green energy: Catalyst engineering, mechanisms, and techno-economic feasibility

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Journal of Energy Chemistry 2024年第8期95卷 380-406页

作者： Hafiz Muhammad Adeel Sharif Hafiz Muhammad Farooq Khan Sadeeq Ullah Yuwei Wang Muhammad Ahmad Bo Yang Changping Li Muhammad Bilal Asif Research Center for Eco-Environmental Engineering Dongguan University of Technology College of Chemistry and Engineering Shenzhen University FMH College of Medicine and Dentistry School of Environment and Civil Engineering Research Center for Eco-Environment Engineering Dongguan University of Technology Advanced Membranes and Porous Materials Center (AMPMC) Physical Sciences and Engineering (PSE) King Abdullah University of Science and Technology (KAUST)

Ammonia（NH3） is an irreplaceable chemical that has been widely demanded to keep the sustainable development of modern society.However,its industrial production consumes a huge amount of energy and releases extraordinary greenhouse gases（GHGs）,leading to various environmental issues.Achieving the green production of ammonia is a great challenge,which has been extensively pursued in the last decade.In this review,the most promising strategy,electrochemical nitrate reduction reaction（e-NO3RR）,is comprehensively investigated to give a complete understanding of its development and mechanism and provide guidance for future directions.However,owing to the complex reactions and limited selectivity,a comprehensive understanding of the mechanisms is crucial to further development and commercialization.Moreover,NO3-RR is a promising strategy for simultaneous water treatment and NH3production.A detailed overview of the recent progress in NO3-RR for NH3production with nontransition and transition metal based electrocatalysts is summarized.In addition,critical advanced techniques,future challenges,and prospects are discussed to guide future research on transition metal-based catalysts for commercial NH3synthesis by NO3-reduction.

关键词： Ammonia synthesis Electrolysis Green energy nitrate reduction Pollution to solution Transition metal catalysts

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Enhancing the electrocatalytic performance of nitrate reduction to ammonia by in-situ nitrogen leaching

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Chinese Chemical Letters 2024年第2期35卷 564-569页

作者： Mimi Fu Yini Mao Hua Wang Wei Luo Yimin Jiang Wei Shen Ming Li Rongxing He College of Chemistry and Chemical Engineering Southwest UniversityChongqing 400715China

Electrochemical nitrate reduction reaction (NITRR) is regarded as a “two birds-one stone” method for the treatment of nitrate contaminant in polluted water and the synthesis of valuable ammonia, which is retarded by the lack of highly reactive and selective electrocatalysts .Herein, for the first time, nickel foam supported Co_(4) N was designed as a high-performance NITRR catalyst by an in-situ nonmetal leaching-induced strategy.At the optimal potential, the Co_(4) N/NF catalyst achieves ultra-high Faraday efficiency and NH_(3) selectivity of 95.4% and 99.4%, respectively.Ex situ X-ray absorption spectroscopy (XAS), together with other experiments powerfully reveal that the nitrogen vacancies produced by nitrogen leaching are stable and play a key role in boosting nitrate reduction to ammonia.Theoretical calculations confirm that Co_(4) N with abundant nitrogen vacancies can optimize the adsorption energies of NO_(3)^(-) and intermediates, lower the free energy (Δ G ) of the potential-determining step (*NH_(3) to NH_(3) ) and inhibit the formation of N-containing byproducts.In addition, we also conclude that the nitrogen vacancies can stabilize the adsorbed hydrogen, making H_(2) quite difficult to produce, and lowering ΔG from *NO to *NOH, which facilitates the selective reduction of nitrate.This study reveals significant insights about the in-situ nonmetal leaching to enhance the NITRR activity.

关键词： Co4N nitrate reduction In-situ nonmetal leaching Nitrogen vacancy Mechanism

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Ru-Ni alloy nanosheets as tandem catalysts for electrochemical reduction of nitrate to ammonia

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Nano Research 2024年第6期17卷 4815-4824页

作者： Xingchao You Jiawei Xu Zechao Zhuang Junkai Xia Suwen Wang Haiyan Wei Yongfu Li Yanjiang Cai Hai Xiang Bing Yu State Key Laboratory of Subtropical Silviculture Zhejiang A&F UniversityHangzhou 311300China Ecological-Environment&Health College(EEHC) Zhejiang A&F UniversityHangzhou 311300China Jiangsu Key Laboratory of Numerical Simulation of Large Scale Complex Systems and School of Chemistry and Materials Science Nanjing Normal UniversityNanjing 210023China Department of Chemistry Tsinghua UniversityBeijing 100084China Department of Chemical Engineering Columbia UniversityNew YorkNY 10027USA

Developing electrocatalysts that exhibit both high activity and ammonia selectivity for nitrate reduction is a significant and demanding challenge,primarily due to the complex nature of the multiple-electron reduction process involved.An encouraging approach involves coupling highly active precious metals with transition metals to enhance catalytic performance through synergy.Here,we report a ruthenium-nickel alloy catalyst with nanosheets(Ru-Ni NSs)structure that achieves a remarkable ammonia Faradaic efficiency of approximately 95.93%,alongside a yield rate of up to 6.11 g·h^(−1)·cm^(−2).Moreover,the prepared Ru-Ni NSs exhibit exceptional stability during continuous nitrate reduction in a flow reactor for 100 h,maintaining a Faradaic efficiency of approximately 90%and an ammonia yield of 37.4 mg·L^(−1)·h^(−1)using 0.05 M nitrate alkaline electrolyte.Mechanistic studies reveal that the catalytic process follows a two-step pathway,in which HONO serves as a migration intermediate.The presence of a partially oxidized Ru(002)surface enhances the adsorption of nitrate and facilitates the release of the migration intermediate by adjusting the strength of the electrostatic and covalent interactions between the adsorbate and the surface,respectively.On the other hand,the Ni(111)surface promotes the utilization of the migration intermediate and requires less energy for NH_(3)desorption.This tandem process contributes to a high catalytic activity of Ru-Ni NSs towards nitrate reduction.

关键词： alloy catalyst nitrate reduction ammonia synthesis Faradaic efficiency

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Electron engineering of nickel phosphide for Ni^(δ+) in electrochemical nitrate reduction to ammonia

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Nano Research 2024年第6期17卷 4864-4871页

作者： Jie Hu Hao Huang Miao Yu Shuang Wang Jinping Li College of Environmental Science and Engineering Taiyuan University of TechnologyJinzhong 030600China School of Sustainable Energy Materials and Science Jinhua Advanced Research InstituteJinhua 321000China Shanxi Key Laboratory of Gas Energy Efficient and Clean Utilization Taiyuan University of TechnologyTaiyuan 030024China

The electrochemical reduction of nitrate to ammonia(ENRA)provides an efficient approach to remove nitrate pollution and achieve ammonia production simultaneously.Herein,inspired by bio-enzyme in denitrifying bacteria,a carbon-coated nickel phosphide(NiPC)nanosheet derived from metal-organic frameworks(MOFs)is proposed as an efficient catalyst for ENRA.Through electron engineering,controllable Ni^(δ+)in nickel phosphide is achieved by regulating the degree of phosphating,which enhances its activity for the hydrogenation of nitrate.As the result,Niδ+becomes one of dominating factors determining the efficiency of the ENRA reaction in nickel phosphide.The optimal NiPC catalyst exhibits impressive property toward ENRA:NH_(4)^(+)Faraday efficiency of 96.68%,NH4+selectivity of 99.04%,and nitrate conversion rate of 90.43%under low nitrate concentration(200 mg·L^(−1)).This work opens a new avenue for the design of next-generation catalysts through electron engineering for ENRA.

关键词： electron engineering transition metal phosphide nitrate reduction ammonia production metal-organic frameworks

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Electrosynthesis of hydroxylamine from nitrate reduction in water

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Science China Chemistry 2023年第6期66卷 1758-1762页

作者： Xianen Lan Chuanqi Cheng Chengying Guo Minghao Guo Tieliang Li Yongmeng Wu Yifu Yu Bin Zhang Institute of Molecular Plus Department of ChemistrySchool of ScienceTianjin UniversityTianjin 300072China Institute of New Energy Materials School of Materials Science and EngineeringTianjin UniversityTianjin 300072China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China

Hydroxylamine(NH_(2)OH),a vital but unstable industrial feedstock,is presently prepared under harsh conditions that cause environmental and energy concerns.Here,we report an electrochemical method to prepare oximes,which serve as precursors for NH_(2)OH after facile hydrolysis.The carbon-supported amorphous Mn electrocatalyst delivers a current density of~100 mA cm^(-2) with a Faradaic efficiency of 40.92%and a yield rate of 0.251 mmol cm^(-2)h^(-1) for formaldoxime(CH_(2)NOH)generation by using nitrate and formaldehyde as reactants.Formaldoxime can be easily released to produce NH_(2)OH via hydrolysis.Impressively,this method exhibits an economic advantage over conventional manufacturing based on techno-economic analysis.A series of control experiments,in situ characterizations,and theoretical simulations unveil the reaction mechanism via the spontaneous reaction between an aldehyde and*NH_(2)OH intermediate derived from nitrate electroreduction.The high activity of Mn originates from its inhibitory effects on the further reduction of key*NH_(2)OH intermediate.This strategy opens a sustainable and green way for NH_(2)OH synthesis under mild conditions using renewable energy.

关键词： electrosynthesis hydroxylamine nitrate reduction amorphous Mn reaction pathway

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Electrochemical nitrate reduction to produce ammonia integrated into wastewater treatment:Investigations and challenges

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Chinese Chemical Letters 2023年第6期34卷 26-36页

作者： Xinyi Zou Jiawei Xie Changhong Wang Guangming Jiang Kai Tang Chongjun Chen School of Environmental Science and Engineering Suzhou University of Science and TechnologySuzhou 215009China School of Materials Science and Engineering Suzhou University of Science and TechnologySuzhou 215011China Engineering Research Center for Waste Oil Recovery Technology and Equipment Ministry of EducationChongqing Technology and Business UniversityChongqing 400067China Jiangsu Collaborative Innovation Center of Technology and Material of Water Treatment Suzhou 215009China Tianping College of Suzhou University of Science and Technology Suzhou 215009China

nitrate(NO_(3)^(-))is widely found in wastewater,which is harmful to human health and water environmental.Electrochemical reduction can convert NO_(3)^(-)to high value-added ammonia(NH)3)/ammonium(NH_(4)^(+))for pollutant removal and resource recovery.Currently,electrochemical nitrate reduction to produce ammonia(ENRA)is mostly focused on the preparation of high-performance catalysts,while ignoring the prerequisite for industrial application as the stable operation and optimal regulation of the process.Therefore,the review focused on wastewater treatment,based on the mechanism of electrochemical nitrate reduction for ammonia production and reactor construction(reactor,power supply system),then summarized the operation control strategies(such as reduction potential,nitrate concentration,inorganic ions,p H)that should be noted for ENRA.Finally,the challenges(system structure,economy)and prospects(ammonia recovery process,construction of large-scale ENRA system,application of real wastewater)of the field as it moves towards commercialization were discussed.It is hoped that this review will facilitate the scaling up of ENRA in the wastewater treatment field.

关键词： Electrochemistry nitrate reduction Ammonia production Control strategy

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Microwave-assisted synthesis of oxygen vacancy associated TiO_(2)for efficient photocatalytic nitrate reduction

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Chinese Chemical Letters 2022年第8期33卷 3835-3841页

作者： Qian Li Yunni Liu Zhe Wan Haiyan Cao Shao Zhang Yue Zhou Xingyu Ye Xiaoyan Liu Dieqing Zhang The Education Ministry Key Lab of Resource Chemistry Joint International Research Laboratory of Resource ChemistryMinistry of Educationand Shanghai Key Laboratory of Rare Earth Functional MaterialsCollege of Chemistry and Materials ScienceShanghai Normal UniversityShanghai 200234China School of Environmental and Geographical Sciences Shanghai Normal UniversityShanghai 200234China

The solar-driven photocatalytic technology has shown great potential in nitrate(NO_(3)^(-))pollutants reduction,however,it has been greatly hindered by the complex preparation and high cost of photocatalysts.Herein,a relatively low-cost photocatalyst,rutile and anatase mixed phase TiO_(2) was synthesized by a facile microwave-hydrothermal method.Meanwhile,oxygen vacancy is successfully generated,leading to an acidic surface for strong adsorption towards NO_(3)^(-),which further improved the reduction activity.Compared with the commercial P25,a higher NO_(3)^(-) conversion of ca.100%and nitrogen(N_(2)) selectivity of 87%were achieved under UV(365 nm)irradiation within 2 h.This research provides a promising strategy for designing efficient noble metal free photocatalyst in the NO_(3)^(-) reduction.

关键词： Photocatalysis TiO_(2) Oxygen vacancy nitrate reduction

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Biochar amendment alters the partitioning of nitrate reduction by significantly enhancing DNRA in a paddy field

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Biochar 2022年第1期4卷 460-477页

作者： Zhijun Wei Mehmet Senbayram Xu Zhao Chenglin Li Ke Jin Min Wu M.Mizanur Rahman Jun Shan Xiaoyuan Yan State Key Laboratory of Soil and Sustainable Agriculture Changshu National Agro-Ecosystem Observation and Research StationInstitute of Soil ScienceChinese Academy of SciencesNanjing 210008China University of Chinese Academy of Sciences Beijing 100049China Institute of Plant Nutrition and.Soil Science University of HarranSanliurfa 63000Turkey Department of Biotechnology and Genetic Engineering Islamic UniversityKushtia 7003Bangladesh

Using 15N tracer technique,we investigated the potential rates of denitrification,anaerobic ammonium oxidation,dis-similatory nitrate reduction to ammonium(DNRA),and their partitioning among nitrate reduction,as well as the N_(2)O emission rates in a paddy soil receiving various biochar(0%,0.03%,0.1%,0.5%,and 1.0%;w/w)and straw(0.1%)over six consecutive years.Results showed that except for the 1.0%amendment treatment,biochar significantly(Preduction of N_(2)O to N_(2).The promoting effects of biochar on DNRA rates and DNRA/(denitrification+DNRA)ratios were attributed to the increased carbon availability and the altered nitrate reducer communities.Collectively,our study suggests that biochar amendment in the paddy soil is helpful for N conservation by favoring nitrate partitioning toward DNRA process,which deepens our understanding of how biochar mediates N cycling in the paddy field.

关键词： nitrate reduction nitrate partitioning N_(2)O Biochar Paddy field

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Efficient nitrate electroreduction over Mn-doped Cu catalyst via regulating N-containing intermediates adsorption configuration

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Science China Chemistry 2024年第6期67卷 1969-1975页

作者： Limin Wu Shunhan Jia Libing Zhang Ruhan Wang Jiaqi Feng Xiaofu Sun Buxing Han Beijing National Laboratory for Molecular Sciences CAS Laboratory of Colloid and Interface and ThermodynamicsCAS Research/Education Center for Excellence in Molecular SciencesCenter for Carbon Neutral ChemistryInstitute of ChemistryChinese Academy of SciencesBeijing100190China School of Chemical Sciences University of Chinese Academy of SciencesBeijing100049China College of Chemical Engineering and Environment China University of PetroleumBeijing102249China Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai200062China

The electrochemical reduction of NO_(3)^(-)to NH_(3)holds promise for economic and environmental benefits,presenting an energyefficient alternative to the traditional Haber-Bosch method.However,challenges exist due to its sluggish kinetics,multiple intermediates,and various reaction pathways.In this study,Mn-doped-Cu catalyst was synthesized and employed for electrochemical NO_(3)^(-)-to-NH_(3)conversion.The doping of Mn into Cu resulted in exceptional performance,achieving a FE of 95.8%and an NH_(3)yield rate of 0.91 mol g^(-1)h^(-1)at-0.6 V in a neutral electrolyte at low NO_(3)^(-)concentration.Detailed experimental studies and theoretical calculations revealed that the Mn dopant enhanced the kinetic rate of NO_(2)~--to-NH_(3)and induced a distinct configuration of*NO.This alteration decreased the energy barrier of*NO-to-*NOH,consequently promoting the conversion of NO_(3)^(-)-to-NH_(3).

关键词： nitrate reduction electrocatalysis ammonia synthesis N-intermediate green chemistry

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Kinetics and corrosion products of aqueous nitrate reduction by iron powder without reaction conditions control

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Journal of Environmental Sciences 2009年第8期21卷 1028-1035页

作者： FAN Xiaomeng GUAN Xiaohong MA Jun AI Hengyu School of Municipal and Environmental Engineering Harbin Institute of Technology Harbin 150090 China College of Chemical and Environmental Engineering Harbin University of Science and Technology Harbin 150080 China

Although considerable research has been conducted on nitrate reduction by zero-valent iron powder （Fe^0）, these studies were mostly operated under anaerobic conditions with invariable pH that was unsuitable for practical application. Without reaction conditions （dissolved oxygen or reaction pH） control, this work aimed at subjecting the kinetics of denitrification by microscale Fe^0 （160-200 mesh） to analysis the factors affecting the denitrification of nitrate and the composition of iron reductive products coating upon the iron surface. Results of the kinetics study have indicated that a higher initial concentration of nitrate would yield a greater reaction rate constant. The reduction rate of nitrate increased with increasing Fe^0 dosage. The reaction can be described as a pseudo-first order reaction with respect to nitrate concentration or Fe^0 dosage. Experimental results also suggested that nitrate reduction by microscale Fe^0 without reaction condition control primarily was an acid-driven surface-mediated process, and the reaction order was 0.65 with respect to hydrogen ion concentration. The analyses of X-ray diffractometry and X-ray photoelectron spectroscopy indicated that a black coating, consisted of Fe2O3, Fe3O4 and FeO（OH）, was formed on the surface of iron grains as an iron corrosion product when the system initial pH was lower than 5. The proportion of FeO（OH） increased as reaction time went on, whereas the proportion of Fe3O4 decreased.

关键词： kinetics nitrate reduction zero-valent iron corrosion products pH

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