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学者姓名：万宇驰
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Abstract ：
Nitrate electroreduction is promising for achieving effluent waste-water treatment and ammonia production with respect to the global nitrogen balance. However, due to the impeded hydrogenation process, high overpotentials need to be surmounted during nitrate electroreduction, causing intensive energy consumption. Herein, a hydroxide regulation strategy is developed to optimize the interfacial H2O behavior for accelerating the hydrogenation conversion of nitrate to ammonia at ultralow overpotentials. The well-designed Ru & horbar;Ni(OH)(2) electrocatalyst shows a remarkable energy efficiency of 44.6% at +0.1 V versus RHE and a nearly 100% Faradaic efficiency for NH3 synthesis at 0 V versus RHE. In situ characterizations and theoretical calculations indicate that Ni(OH)(2) can regulate the interfacial H2O structure with a promoted H2O dissociation process and contribute to the spontaneous hydrogen spillover process for boosting NO3 (-) electroreduction to NH3 at Ru sites. Furthermore, the assembled rechargeable Zn-NO3 (-)/ethanol battery system exhibits an outstanding long-term cycling stability during the charge-discharge tests with the production of high-value-added ammonium acetate, showing great potential for simultaneously achieving nitrate removal, energy conversion, and chemical synthesis. This work can not only provide a guidance for interfacial H2O regulation in extensive hydrogenation reactions but also inspire the design of a novel hybrid flow battery with multiple functions.
Keyword ：
ammonia synthesis ammonia synthesis hydrogen spillover hydrogen spillover interfacial H2O regulation interfacial H2O regulation nitrate electroreduction nitrate electroreduction rechargeable hybrid flow battery rechargeable hybrid flow battery ultralow overpotentials ultralow overpotentials
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| GB/T 7714 | Wan, Yuchi , Pei, Maojun , Tang, Yixiang et al. Interfacial Water Regulation for Nitrate Electroreduction to Ammonia at Ultralow Overpotentials [J]. | ADVANCED MATERIALS , 2025 , 37 (8) . |
| MLA | Wan, Yuchi et al. "Interfacial Water Regulation for Nitrate Electroreduction to Ammonia at Ultralow Overpotentials" . | ADVANCED MATERIALS 37 . 8 (2025) . |
| APA | Wan, Yuchi , Pei, Maojun , Tang, Yixiang , Liu, Yao , Yan, Wei , Zhang, Jiujun et al. Interfacial Water Regulation for Nitrate Electroreduction to Ammonia at Ultralow Overpotentials . | ADVANCED MATERIALS , 2025 , 37 (8) . |
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Abstract ：
Currently, ammonia is an important chemical in modern society, widely used in agriculture and energy-conversion fields. However, there are existing energy-consumption and environmental problems in the traditional process of ammonia synthesis. At present, electrochemical nitrate reduction reaction (NO3-RR) uses renewable electricity as power to achieve simultaneous nitrate removal and ammonia generation, providing an efficient, green and clean platform for sustainable ammonia synthesis. As an ideal model material for electrochemistry research, two-dimensional (2D) materials with tunable surface properties and electronic structure have aroused immense interest in electrocatalysis applications. The atomic-layer structure of 2D materials can significantly affect their physical/chemical properties, while size and surface characteristics are important aspects to be considered for designing and synthesizing efficient catalysts to achieve the high performance of the electrocatalytic NO3-RR application. In this review, we discuss the fundamentals of electrocatalytic nitrate reduction to ammonia including reaction mechanisms and basic research methods. Moreover, synthetic methods and design strategies of 2D-material electrocatalysts are introduced and specific applications of 2D material in electrocatalytic NO3-RR are demonstrated. Furthermore, future perspectives are proposed to inspire novel attempts for new 2D materials applications across broad fields.
Keyword ：
2D materials 2D materials ammonia synthesis ammonia synthesis design strategies design strategies electrochemical nitrate reduction electrochemical nitrate reduction property modulation property modulation
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| GB/T 7714 | Bai, Bobing , Wan, Yuchi , Yan, Wei et al. 2D materials design and property modulation for electrocatalytic nitrate reduction to ammonia [J]. | 2D MATERIALS , 2025 , 12 (2) . |
| MLA | Bai, Bobing et al. "2D materials design and property modulation for electrocatalytic nitrate reduction to ammonia" . | 2D MATERIALS 12 . 2 (2025) . |
| APA | Bai, Bobing , Wan, Yuchi , Yan, Wei , Zhang, Jiujun . 2D materials design and property modulation for electrocatalytic nitrate reduction to ammonia . | 2D MATERIALS , 2025 , 12 (2) . |
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Abstract ：
Electrocatalytic nitrate reduction (NO3-RR) holds significant potential for clean NH3 synthesis and the treatment of industrial effluents, effectively converting waste into a valuable resource. However, the catalyst reconstruction mechanism remains ambiguous, and the influence of interfacial hydrogen bonds on NO3-RR performance remains underexplored. Herein, a Cr-doping strategy was developed to regulate the interfacial hydrogen-bonded interactions on Co-based dynamic electrocatalysts to improve electrocatalytic NO3-RR activity. In situ XRD, in situ Raman spectroscopy and theoretical calculations indicated that Cr doping could modulate the reconstruction process of Co-based materials, achieving a dynamic balance between Co(OH)2 and Co. Moreover, molecular dynamics simulations and density functional theory calculations, combined with in situ infrared spectroscopy, revealed that the strong hydrogen-bonding interactions between interfacial H2O and the Cr-doped Co(OH)2 surface could drag more free H2O from the rigid H2O network and facilitate H2O dissociation, forming active hydrogen to accelerate the NO3-RR pathway on metallic Co sites. As a result, the Cr-doped Co-based dynamic electrocatalyst displayed a superior NH3 faradaic efficiency of 97.36% and a high NH3 yield rate of 58.92 mg h-1 cm-2, outperforming the state-of-the-art electrocatalysts. This work can further inspire the design of dynamic electrocatalysts and the modulation of the interfacial microenvironment for promoting effective electrochemical hydrogenation reactions.
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| GB/T 7714 | Wan, Yuchi , Tang, Yixiang , Zuo, Yinze et al. Interfacial hydrogen-bond modulation of dynamic catalysts for nitrate electroreduction to ammonia [J]. | ENERGY & ENVIRONMENTAL SCIENCE , 2025 , 18 (15) : 7460-7469 . |
| MLA | Wan, Yuchi et al. "Interfacial hydrogen-bond modulation of dynamic catalysts for nitrate electroreduction to ammonia" . | ENERGY & ENVIRONMENTAL SCIENCE 18 . 15 (2025) : 7460-7469 . |
| APA | Wan, Yuchi , Tang, Yixiang , Zuo, Yinze , Sun, Kaian , Zhuang, Zewen , Zheng, Yun et al. Interfacial hydrogen-bond modulation of dynamic catalysts for nitrate electroreduction to ammonia . | ENERGY & ENVIRONMENTAL SCIENCE , 2025 , 18 (15) , 7460-7469 . |
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Electrocatalytic C-N coupling reaction is regarded as a promising strategy for achieving clean and sustainable urea production by coreducing CO2 and nitrogen species, thus contributing to carbon neutrality and the artificial nitrogen cycle. However, restricted by the sluggish adsorption of reactants, competitive side reactions, and multistep reaction pathways, the electrochemical urea production suffers from a low urea yield rate and low selectivity so far. In order to comprehensively improve urea synthesis performance, it is crucial to develop highly efficient catalysts for electrochemical C-N coupling. In this article, the catalyst-designing strategies, C-N coupling mechanisms, and fundamental research methods are reviewed. For the coreduction of CO2 and different nitrogen species, several prevailing reaction mechanisms are discussed. With the aim of establishing the standard research system, the fundamentals of electrocatalytic urea synthesis research are introduced. The most important catalyst-designing strategies for boosting the electrocatalytic urea production are discussed, including heteroatom doping, vacancy engineering, crystal facet regulation, atom-scale modulation, alloying and heterostructure construction. Finally, the challenges and perspectives are proposed for future industrial applications of electrochemical urea production by C-N coupling. The rational design of efficient heterogeneous electrocatalysts is crucial but still very challenging for sustainable urea production at ambient conditions by coreducing CO2 and nitrogen species. In this review article, design strategies for C-N coupling electrocatalysts are emphasized-for the in-depth understanding of the structure-activity relationship and the establishment of a systematic research framework -toward this emerging field. image
Keyword ：
artificial nitrogen cycle artificial nitrogen cycle carbon neutrality carbon neutrality catalyst-designing strategies catalyst-designing strategies C-N coupling C-N coupling electrocatalytic urea synthesis electrocatalytic urea synthesis
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| GB/T 7714 | Wan, Yuchi , Zheng, Muyun , Yan, Wei et al. Fundamentals and Rational Design of Heterogeneous C-N Coupling Electrocatalysts for Urea Synthesis at Ambient Conditions [J]. | ADVANCED ENERGY MATERIALS , 2024 , 14 (28) . |
| MLA | Wan, Yuchi et al. "Fundamentals and Rational Design of Heterogeneous C-N Coupling Electrocatalysts for Urea Synthesis at Ambient Conditions" . | ADVANCED ENERGY MATERIALS 14 . 28 (2024) . |
| APA | Wan, Yuchi , Zheng, Muyun , Yan, Wei , Zhang, Jiujun , Lv, Ruitao . Fundamentals and Rational Design of Heterogeneous C-N Coupling Electrocatalysts for Urea Synthesis at Ambient Conditions . | ADVANCED ENERGY MATERIALS , 2024 , 14 (28) . |
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Electrocatalytic nitrate reduction reaction (NO3-RR) to ammonia under ambient conditions is expected to be a green process for ammonia synthesis and alleviate water pollution issues. We report a CuO nanoparticles incorporated on nitrogen-doped porous carbon (CuO@NC) catalyst for NO3-RR. Part of Cu(II) is reduced to Cu(I) during the NO3-RR process to construct Cu(I)-Cu(II) pairs, confirmed by in situ X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy. Density functional theory (DFT) calculations indicated that the formation of Cu(I) could provide a reaction path with smaller energy barrier for NO3-RR, while Cu(II) effectively suppressed the competition of hydrogen evolution reaction (HER). As a result, CuO@NC catalyst achieved a Faradaic efficiency of 84.2% at -0.49 V versus reversible hydrogen electrode (RHE), and a NH3 yield rate of 17.2 mg h-1 mgcat.-1 at -0.79 V vs. RHE, higher than the HaberBosch process (<3.4 g h-1 gcat.-1 ). This work may open a new avenue for effective NO3-RR by modulating oxidation states. (c) 2024 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights are reserved, including those for text and data mining, AI training, and similar technologies.
Keyword ：
Ammonia synthesis Ammonia synthesis Cu oxidation state Cu oxidation state Electrochemistry Electrochemistry In situ XPS In situ XPS Nitrate reduction Nitrate reduction
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| GB/T 7714 | Zheng, Muyun , Wan, Yuchi , Yang, Leping et al. In situ construction of Cu(I)-Cu(II) pairs for efficient electrocatalytic nitrate reduction reaction to ammonia [J]. | JOURNAL OF ENERGY CHEMISTRY , 2024 , 100 : 106-113 . |
| MLA | Zheng, Muyun et al. "In situ construction of Cu(I)-Cu(II) pairs for efficient electrocatalytic nitrate reduction reaction to ammonia" . | JOURNAL OF ENERGY CHEMISTRY 100 (2024) : 106-113 . |
| APA | Zheng, Muyun , Wan, Yuchi , Yang, Leping , Ao, Shen , Fu, Wangyang , Zhang, Zhengjun et al. In situ construction of Cu(I)-Cu(II) pairs for efficient electrocatalytic nitrate reduction reaction to ammonia . | JOURNAL OF ENERGY CHEMISTRY , 2024 , 100 , 106-113 . |
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Hydrogen (H2) is an important clean energy carrier due to the merits of high combustion value and zero-carbon emission. Water electrolysis has been regarded as a promising technology for achieving green and sustainable production of H2. However, most of the electrocatalysts for water splitting can only work at low current density with poor long-term durability, and it is difficult to meet the extensive requirements of industrial-scale applications. In this article, challenges including the charge transfer, mass diffusion, and catalyst stability during high-current-density water electrolysis are discussed. With the aim of addressing these issues, various electrocatalyst design strategies including morphology engineering, electronic structure modulation, and surface/interface engineering are summarized in detail. For the purpose of promoting practical applications, recent achievements of practical anion exchange membrane water electrolysis (AEMWE) and proton exchange membrane water electrolysis (PEMWE) technologies are discussed. Finally, outlooks toward future investigations on high-current-density water electrolysis are presented. It is believed that this review will guide the rational design of catalysts with both high activity and high stability for high-current-density water electrolysis, and promote the development of industrial-scale green H2 production. Challenges and design strategies of electrocatalysts for high-current-density water electrolysis.
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| GB/T 7714 | Wan, Yuchi , Zhou, Lingxi , Lv, Ruitao . Rational design of efficient electrocatalysts for hydrogen production by water electrolysis at high current density [J]. | MATERIALS CHEMISTRY FRONTIERS , 2023 , 7 (23) : 6035-6060 . |
| MLA | Wan, Yuchi et al. "Rational design of efficient electrocatalysts for hydrogen production by water electrolysis at high current density" . | MATERIALS CHEMISTRY FRONTIERS 7 . 23 (2023) : 6035-6060 . |
| APA | Wan, Yuchi , Zhou, Lingxi , Lv, Ruitao . Rational design of efficient electrocatalysts for hydrogen production by water electrolysis at high current density . | MATERIALS CHEMISTRY FRONTIERS , 2023 , 7 (23) , 6035-6060 . |
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Abstract ：
Hydrogen (H2) is an important clean energy carrier due to the merits of high combustion value and zero-carbon emission. Water electrolysis has been regarded as a promising technology for achieving green and sustainable production of H2. However, most of the electrocatalysts for water splitting can only work at low current density with poor long-term durability, and it is difficult to meet the extensive requirements of industrial-scale applications. In this article, challenges including the charge transfer, mass diffusion, and catalyst stability during high-current-density water electrolysis are discussed. With the aim of addressing these issues, various electrocatalyst design strategies including morphology engineering, electronic structure modulation, and surface/interface engineering are summarized in detail. For the purpose of promoting practical applications, recent achievements of practical anion exchange membrane water electrolysis (AEMWE) and proton exchange membrane water electrolysis (PEMWE) technologies are discussed. Finally, outlooks toward future investigations on high-current-density water electrolysis are presented. It is believed that this review will guide the rational design of catalysts with both high activity and high stability for high-current-density water electrolysis, and promote the development of industrial-scale green H2 production. Challenges and design strategies of electrocatalysts for high-current-density water electrolysis.
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| GB/T 7714 | Wan, Yuchi , Zhou, Lingxi , Lv, Ruitao . Rational design of efficient electrocatalysts for hydrogen production by water electrolysis at high current density [J]. | MATERIALS CHEMISTRY FRONTIERS , 2023 , 7 (23) : 6035-6060 . |
| MLA | Wan, Yuchi et al. "Rational design of efficient electrocatalysts for hydrogen production by water electrolysis at high current density" . | MATERIALS CHEMISTRY FRONTIERS 7 . 23 (2023) : 6035-6060 . |
| APA | Wan, Yuchi , Zhou, Lingxi , Lv, Ruitao . Rational design of efficient electrocatalysts for hydrogen production by water electrolysis at high current density . | MATERIALS CHEMISTRY FRONTIERS , 2023 , 7 (23) , 6035-6060 . |
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