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Recent development of catalytic strategies for sustainable ammonia production

Chinese Journal of Chemical Engineering 2023年第10期62卷 65-113页

作者： Supeng Yu Ting Xiang Njud SAlharbi Bothaina AAl-aidaroos Changlun Chen Institute of Plasma Physics HFIPSChinese Academy of SciencesHefei 230031China University of Science and Technology of China Hefei 230026China Institute of Energy Hefei Comprehensive National Science Center(Anhui Energy Laboratory)Hefei 230000China Department of Biological Sciences Faculty of ScienceKing Abdulaziz UniversityJeddah 21589Saudi Arabia

Presently,ammonia is an ideal candidate for future clean energy.The Haber-Bosch process has been an essential ammonia production process,and it is one of the most important technological advancements since its invention,sustaining the explosive growth of military munitions industry and fertilizers in the first half of the 20th century.However,the process is facing great challenges:the growing need for ammonia and the demands of environmental protection.High energy consumption and high CO_(2) emissions greatly limit the application of the Haber-Bosch method,and increasing research efforts are devoted to"green"ammonia synthesis.Thermocatalytic,electrocatalytic,and photocatalytic ammonia production under mild conditions and the derived chemical looping and plasma ammonia production methods,have been widely developed.Electrocatalytic and photocatalytic methods,which use low fossil fuels,are naturally being considered as future directions for the development of ammonia production.Although their catalytic efficiency of ammonia generation is not yet sufficient to satisfy the actual demands,considerable progress has been made in terms of regulating structure and morphology of catalyst and improving preparation efficiency.The chemical looping approach of ammonia production differs from the thermocatalytic,electrocatalytic,and photocatalytic methods,and is the method of reusing raw materials.The plasma treatment approach alters the overall ammonia production approach and builds up a new avenue of development in combination with thermal,photocatalytic,and electrocatalytic methods as well.This review discusses several recent effective catalysts for different ammonia production methods and explores mechanisms as well as efficiency of these catalysts for catalytic N2fixation of ammonia.

关键词： Thermocatalytic ammonia production Electrocatalytic,and photocatalytic ammonia production Thermodynamics process Electrochemistry Multiphase reaction

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Enhancing ammonia production rates from electrochemical nitrogen reduction by engineering three-phase boundary with phosphorus-activated Cu catalysts

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Journal of Energy Chemistry 2023年第9期84卷 394-401页

作者： Jeehye Kim Cho Hee Lee Yong Hyun Moon Min Hee Lee Eun Hyup Kim Sun Hee Choi Youn Jeong Jang Jae Sung Lee School of Energy and Chemical Engineering Ulsan National Institute of Science and Technology(UNIST)Ulsan 44919Republic of Korea Department of Chemical Engineering Hanyang UniversitySeoul 04763Republic of Korea Pohang Accelerator Laboratory(PAL) Pohang University of Science and Technology(POSTECH)Pohang 37673Republic of Korea

Electrochemical N_(2) reduction reaction(eNRR) over Cu-based catalysts suffers from an intrinsically low activity of Cu for activation of stable N_(2) molecules and the limited supply of N_(2) to the catalyst due to its low solubility in aqueous electrolytes.Herein,we propose phosphorus-activated Cu electrocatalysts to generate electron-deficient Cu sites on the catalyst surface to promote the adsorption of N_(2) molecules.The eNRR system is further modified using a gas diffusion electrode(GDE) coated with polytetrafluoroethylene(PTFE) to form an effective three-phase boundary of liquid water-gas N_(2)-solid catalyst to facilitate easy access of N_(2) to the catalytic sites.As a result,the new catalyst in the flow-type cell records a Faradaic efficiency of 13.15% and an NH_(3) production rate of 7.69 μg h^(-1) cm^(-2) at-0.2 V_(RHE),which represent 3.56 and 59.2 times increases from those obtained with a pristine Cu electrode in a typical electrolytic cell.This work represents a successful demonstration of dual modification strategies;catalyst modification and N_(2) supplying system engineering,and the results would provide a useful platform for further developments of electrocatalysts and reaction systems.

关键词： Electrochemical nitrogen reduction reaction ammonia production Phosphorous modified copper electrodes Gas diffusion electrodes Three-phase boundary PTFE coating

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Controlled Growth of Multidimensional Interface for High-Selectivity ammonia production

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CCS Chemistry 2023年第7期5卷 1653-1662页

作者： Xuchen Zheng Yurui Xue Chao Zhang Yuliang Li CAS Key Laboratory of Organic Solids Institute of ChemistryChinese Academy of SciencesBeijing 100190 School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100190 Science Center for Material Creation and Energy Conversion School of Chemistry and Chemical EngineeringInstitute of Frontier and Interdisciplinary ScienceJinan 250100

The efficient production of ammonia by reducing nitrates at room temperature and ambient pressure is a promising alternative to the Haber-Bosch process and can effectively overcome the attendant water pollution issues.Herein,a new idea has been realized for rational and selective construction of the sp-carbon-metal-carbon interface,comprised of electronic-donating triple bonds in graphdiyne and electron-withdrawing iron carbides,for a highly efficient nitrate reduction reaction.The as-prepared sp-carbon-metal-carbon interfacial structures greatly increase the charge transfer ability and electrical conductivity of the system.The proposed concept of incomplete charge transfer has demonstrated significantly high selectivity,activity,and stability in catalytic system.The catalyst exhibits high Faradaic efficiency of over>95%and a NH3 yield rate up to 205.5μmolNH_(3) cm^(-2) h^(-1) in dilute nitrate conditions without any contaminant.

关键词： graphdiyne donor-acceptor interface incomplete charge transfer high selectivity ammonia production

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Accelerating the Activation of NO_(x)^(−)on Ru Nanoparticles for ammonia production by Tuning Their Electron Deficiency

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CCS Chemistry 2022年第11期4卷 3455-3462页

作者： Guang-Yao Zhai Qi-Yuan Li Shi-Nan Zhang Dong Xu Si-Yuan Xia Peng Gao Xiu Lin Yun-Xiao Lin Jin-Huan Cheng Wei-Yao Hu Lu-Han Sun Xin-Hao Li Jie-Sheng Chen School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative MoleculesShanghai Jiao Tong UniversityShanghai 200240 School of Environmental Science and Engineering Shanghai Jiao Tong UniversityShanghai 200240

Stable and portable ammonia(NH3)is a promising,low-cost,and environment-friendly medium for energy storage.How to achieve the rapid production of NH3 from reducing NO_(x)^(−)in aqueous systems and industrial wastewater via electrochemical methods remains the main challenge for practical application on a large scale.The corresponding electrocatalysts as the key materials in electrochemical devices suffer from low activity,especially in neutral systems.In this work,we successfully elevated the activity of the bench-mark Ru electrocatalysts to more than 30 times via construction of rectifying contact of Ru metals and noble carbons.We theoretically predicted and then rationally designed a new type of P-O rich carbon with large work functions as“noble”supports to attract a pronounced number of electrons from Ru metals at the rectifying interface.The resulting electron deficiency of Ru metals largely promotes the pre-adsorption and activation of NO_(x)^(−)anions,providing high Faradaic efficiencies(>96%)and record-high turnover frequency values for universal NO_(2)^(−)and NO_(3)^(−)reduction in neutral solution.

关键词： electrochemical NOx−reduction ammonia production energy storage P-O rich carbon electron deficiency of Ru nanoparticles

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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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Screening of transition metal oxides for electrocatalytic nitrate reduction to ammonia at large currents

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Nano Research 2024年第5期17卷 3902-3910页

作者： Qiongfei Wu Weijie Zhu Dongxu Ma Chao Liang Zhoucheng Wang Hanfeng Liang State Key Laboratory of Physical Chemistry of Solid Surfaces Tan Kah Kee Innovation LaboratoryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China College of Chemical Engineering Tianjin UniversityTianjin 300072China

Electrochemical nitrate reduction reaction(NO_(3)RR)towards ammonia,as an emerging and appealing technology alternative to the energy-intensive Haber-Bosch process and inefficient nitrogen reduction reaction,has recently aroused wide concern and research.However,the current research of the NO_(3)RR towards ammonia lacks the overall performance comparison of various electrocatalysts.Given this,we here make a comparison of 12 common transition metal oxide catalysts for the NO_(3)RR under a high cathodic current density of 0.25 A·cm^(-2),wherein Co_(3)O_(4) catalyst displays the highest ammonia Faradaic efficiency(85.15%)and moderate activity(ca.-0.25 V vs.reversible hydrogen electrode).Other external factors,such as nitrate concentrations in the electrolyte and applied potential ranges,have also been specifically investigated for the NO_(3)RR.

关键词： nitrate reduction reaction ammonia production transition metal oxides Co_(3)O_(4)

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A core-shell copper oxides-cobalt oxides heterostructure nanowire arrays for nitrate reduction to ammonia with high yield rate

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Green Energy & Environment 2023年第6期8卷 1619-1629页

作者： Hui Liu Jingsha Li Feng Du Luyun Yang Shunyuan Huang Jingfeng Gao Changming Li Chunxian Guo Institute of Advanced Cross-field Science College of Life ScienceQingdao UniversityQingdao266071China Institute of Materials Science and Devices School of Materials Science and EngineeringSuzhou University of Science and TechnologySuzhou215011China Jiangsu Key Laboratory for Micro and Nano Heat Fluid Flow Technology and Energy Application Collaborative Innovation Center of Water Treatment Technology&MaterialChina

Electrochemical nitrate reduction to ammonia(NRA) can realize the green synthesis of ammonia(NH3) at ambient conditions, and also remove nitrate contamination in water. However, the current catalysts for NRA still face relatively low NH3yield rate and poor stability. We present here a core-shell heterostructure comprising cobalt oxide anchored on copper oxide nanowire arrays(CuO NWAs@Co_(3)O_(4)) for efficient NRA. The CuO NWAs@Co_(3)O_(4)demonstrates significantly enhanced NRA performance in alkaline media in comparison with plain CuO NWAs and Co_(3)O_(4)flocs. Especially, at-0.23 V vs. RHE, NH_(3) yield rate of the CuO NWAs@Co_(3)O_(4)reaches 1.915 mmol h^(-1)cm^(-2),much higher than those of CuO NWAs(1.472 mmol h^(-1)cm^(-2)), Co_(3)O_(4)flocs(1.222 mmol h^(-1)cm^(-2)) and recent reported Cu-based catalysts.It is proposed that the synergetic effects of the heterostructure combing atom hydrogen adsorption and nitrate reduction lead to the enhanced NRA performance.

关键词： Electrocatalytic nitrate reduction ammonia production Core–shell heterostructure Copper oxides nanowire arrays Cobalt oxidesﬂocs

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Electrocatalytic reduction of NO to NH_(3) in ionic liquids by P-doped TiO_(2) nanotubes

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Frontiers of Chemical Science and Engineering 2023年第6期17卷 726-734页

作者： Shangcong Zhang Qian Liu Xinyue Tang Zhiming Zhou Tieyan Fan Yingmin You Qingcheng Zhang Shusheng Zhang Jun Luo Xijun Liu College of Electrical and Electronic Engineering Wenzhou UniversityWenzhou 325035China Low Voltage Apparatus Technology Research Centre of Zhejiang Wenzhou UniversityWenzhou 325035China Institute for Advanced Study Chengdu UniversityChengdu 610106China College of Chemistry and Materials Engineering Wenzhou UniversityWenzhou 325035China College of Chemistry Zhengzhou UniversityZhengzhou 450000China Tianjin Key Lab for Photoelectric Materials&Devices School of Materials Science and EngineeringTianjin University of TechnologyTianjin 300384China State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Compesite Structures School of ResourceEnvironments and MaterialsGuangxi UniversityNanning 530004China

Designing advanced and cost-effective electrocatalytic system for nitric oxide(NO)reduction reaction(NORR)is vital for sustainable NH_(3) production and NO removal,yet it is a challenging task.Herein,it is shown that phosphorus(P)-doped titania(TiO_(2))nanotubes can be adopted as highly efficient catalyst for NORR.The catalyst demonstrates impressive performance in ionic liquid(IL)-based electrolyte with a remarkable high Faradaic efficiency of 89%and NH3 yield rate of 425μg·h^(−1)·mg_(cat).^(−1),being close to the best-reported results.Noteworthy,the obtained performance metrics are significantly larger than those for N_(2) reduction reaction.It also shows good durability with negligible activity decay even after 10 cycles.Theoretical simulations reveal that the introduction of P dopants tunes the electronic structure of Ti active sites,thereby enhancing the NO adsorption and facilitating the desorption of ^(*)NH_(3).Moreover,the utilization of IL further suppresses the competitive hydrogen evolution reaction.This study highlights the advantage of the catalyst−electrolyte engineering strategy for producing NH_(3) at a high efficiency and rate.

关键词： nitric oxide reduction reaction electrcatalysis ammonia production phosphorus-doped titania

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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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