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学者姓名：王秀云
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Abstract ：
Nitrate electroreduction to ammonia holds great promise in sustainable green ammonia synthesis, yet faces a dearth of competent electrocatalysts adapted to varying nitrate concentration, and inadequate ammonia fixation. Herein, we present a high-performance Ag single-atom-decorated Cu2O nanowire catalyst (Ag1@Cu2O) that exhibits concentration-universal high-rate nitrate reduction, achieving >90% to near-unity ammonia faradaic efficiency (FE) across nitrate concentrations from 0.01 to 0.5 M. Notably, at 0.5 M nitrate concentration, it attains a two-ampere-level current density (2.3 A cm-2) at -1 V vs. RHE, resulting in a leading ammonia yield rate of 184.4 mgNH3 h-1 cm-2. In situ studies combined with theoretical calculations elucidate an Ag-Cu inter-site synergistic catalytic mechanism, in which single-atom Ag serves as an accelerator for active hydrogen generation and stabilization on Cu sites to boost the hydrogenation kinetics of N-containing intermediates, thus smoothing the energy barriers for ammonia production via the favorable *NHO pathway. Additionally, Ag1@Cu2O demonstrates near-unity formate FE for formaldehyde oxidation, reaching a 300 mA cm-2 current density at a mere 0.31 V vs. RHE. Motivated by this exceptional bifunctionality, we demonstrate an innovative tandem electrochemical-chemical strategy for upgrading ammonia into high-value ammonium formate by coupled electrolysis of nitrate reduction and formaldehyde oxidation, followed by straightforward chemical combination and isolation. In practice, membrane electrode assembly (MEA) electrolysis at 1.6 V for 100 h successfully outputs 10.7 g of high-purity ammonium formate. Furthermore, the commonality of this strategy is validated by application to various nitrate/aldehyde pairs. This work blazes a new trail for scalable, cost- and energy-efficient green ammonia production and fixation from nitrate reduction.
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| GB/T 7714 | Zhang, Linjie , Cai, Yimeng , Li, Yanghua et al. Unlocking high-current-density nitrate reduction and formaldehyde oxidation synergy for scalable ammonia production and fixation [J]. | ENERGY & ENVIRONMENTAL SCIENCE , 2025 , 18 (6) . |
| MLA | Zhang, Linjie et al. "Unlocking high-current-density nitrate reduction and formaldehyde oxidation synergy for scalable ammonia production and fixation" . | ENERGY & ENVIRONMENTAL SCIENCE 18 . 6 (2025) . |
| APA | Zhang, Linjie , Cai, Yimeng , Li, Yanghua , Sun, Chen , Xiao, Yi , Yang, Yibing et al. Unlocking high-current-density nitrate reduction and formaldehyde oxidation synergy for scalable ammonia production and fixation . | ENERGY & ENVIRONMENTAL SCIENCE , 2025 , 18 (6) . |
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The insufficient availability and activity of interfacial water remain a major challenge for alkaline hydrogen evolution reaction (HER). Here, we propose an "on-site disruption and near-site compensation" strategy to reform the interfacial water hydrogen bonding network via deliberate cation penetration and catalyst support engineering. This concept is validated using tip-like bimetallic RuNi nanoalloys planted on super-hydrophilic and high-curvature carbon nanocages (RuNi/NC). Theoretical simulations suggest that tip-induced localized concentration of hydrated K+ facilitates optimization of interfacial water dynamics and intermediate adsorption. In situ synchrotron X-ray spectroscopy endorses an H* spillover-bridged Volmer-Tafel mechanism synergistically relayed between Ru and Ni. Consequently, RuNi/NC exhibits low overpotential of 12 mV and high durability of 1600 h at 10 mA cm(-2) for alkaline HER, and demonstrates high performance in both water electrolysis and chlor-alkali electrolysis. This strategy offers a microscopic perspective on catalyst design for manipulation of the local interfacial water structure toward enhanced HER kinetics.
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| GB/T 7714 | Zhang, Linjie , Hu, Haihui , Sun, Chen et al. Bimetallic nanoalloys planted on super-hydrophilic carbon nanocages featuring tip-intensified hydrogen evolution electrocatalysis [J]. | NATURE COMMUNICATIONS , 2024 , 15 (1) . |
| MLA | Zhang, Linjie et al. "Bimetallic nanoalloys planted on super-hydrophilic carbon nanocages featuring tip-intensified hydrogen evolution electrocatalysis" . | NATURE COMMUNICATIONS 15 . 1 (2024) . |
| APA | Zhang, Linjie , Hu, Haihui , Sun, Chen , Xiao, Dongdong , Wang, Hsiao-Tsu , Xiao, Yi et al. Bimetallic nanoalloys planted on super-hydrophilic carbon nanocages featuring tip-intensified hydrogen evolution electrocatalysis . | NATURE COMMUNICATIONS , 2024 , 15 (1) . |
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氨是重要的化肥原料,也是颇具潜力的氢能源载体,对于可再生能源的储存、运输和终端利用至关重要.然而,传统Haber-Bosch工艺合成氨的反应条件苛刻,需要高温高压条件,并消耗大量化石能源及排放大量二氧化碳.可再生能源电解水制氢耦合温和合成氨新技术(eHB),不仅能实现可再生能源电力的"消纳和调峰",而且可进行低成本、跨地域长距离存储运输,并可将"绿氨"与氢能产业相结合.然而,现有的高温高压合成氨催化剂与eHB工艺相不匹配,因此,迫切需要开发温和条件下高效合成氨催化剂技术,以实现可再生能源电力电解制氢体系和合成氨技术互补融合.目前,虽然助剂对于Ru基纳米簇(≥l nm)合成氨催化剂的影响规律已得到了广泛研究,但它们对于Ru原子簇催化剂的作用机制尚不清楚,需要进一步揭示. 本文考察了Ba及Ce助剂对Ru原子簇催化剂的影响规律,并分析了其作用机制.首先,通过简单的浸渍法将Ba和/或Ce物种掺杂到Ru原子簇催化剂(2 wt％Ru ACCs),制得Ba/Ce/2 wt％Ru ACCs催化剂;然后,通过一系列实验考察了这些催化剂的合成氨性能,并利用多种表征手段对其进行了深入分析.合成氨性能测试结果表明,添加Ba和Ce助剂后,2 wt％Ru ACCs催化剂的合成氨速率明显提高,在400℃和1 MPa下,Ba/Ce/2 wt％Ru ACCs催化剂的合成氨反应速率达到56.2 mmolNH3 gcat-1 h1,是2 wt％Ru ACCs的7.5倍,且催化剂表现出较好的稳定性,在稳定运行140 h后活性未见明显降低.球差校正电子显微镜和X射线吸收精细结构谱结果表明,负载Ba和/或Ce后,Ru以Ru3原子簇形式存在.X射线吸收近边结构谱和X射线光电子能谱结果表明,Ru与Ba及Ce物种之间存在较强的簇-金属氧化物助剂电子相互作用,可促进电子转移到Ru物种,形成富电子状态的Ru,进而促使电子转移到N2的π*反键轨道,提高温和条件下合成氨反应速率.利用25％N2+75％D2气氛下的原位红外光谱研究催化剂的合成氨反应机理,结果表明,在Ba/Ce/2 wt％Ru ACCs催化剂表面同时检测到N2D2物种和N2Dx物种的振动吸收峰,说明添加Ba和/或Ce物种没有改变Ru原子簇催化剂活化N2的方式,N2仍是通过加氢的路径合成氨. 综上,本文考察了助剂对Ru原子簇的影响规律,揭示了其作用机制,为设计高效的温和条件合成氨催化剂提供参考.
Keyword ：
N2活化 N2活化 助剂 助剂 原子簇 原子簇 合成氨 合成氨 电子相互作用 电子相互作用
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| GB/T 7714 | 张天华 , 胡海慧 , 李嘉欣 et al. 簇-金属氧化物助剂电子相互作用调控的Ru原子簇催化剂用于温和条件下合成氨反应 [J]. | 催化学报 , 2024 , 60 (5) : 209-218 . |
| MLA | 张天华 et al. "簇-金属氧化物助剂电子相互作用调控的Ru原子簇催化剂用于温和条件下合成氨反应" . | 催化学报 60 . 5 (2024) : 209-218 . |
| APA | 张天华 , 胡海慧 , 李嘉欣 , 高迎龙 , 李玲玲 , 张明远 et al. 簇-金属氧化物助剂电子相互作用调控的Ru原子簇催化剂用于温和条件下合成氨反应 . | 催化学报 , 2024 , 60 (5) , 209-218 . |
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Ammonia (NH3) is closely related to the fields of food and energy that humans depend on. The exploitation of advanced catalysts for NH3 synthesis has been a research hotspot for more than one hundred years. Previous studies have shown that the Ru B5 sites (step sites on the Ru (0001) surface uniquely arranged with five Ru atoms) and Fe C7 sites (iron atoms with seven nearest neighbors) over nanoparticle catalysts are highly reactive for N2-to-NH3 conversion. In recent years, single-atom and cluster catalysts, where the B5 sites and C7 sites are absent, have emerged as promising catalysts for efficient NH3 synthesis. In this review, we focus on the recent advances in single-atom and cluster catalysts, including single-atom catalysts (SACs), single-cluster catalysts (SCCs), and bimetallic-cluster catalysts (BCCs), for thermocatalytic NH3 synthesis at mild conditions. In addition, we discussed and summarized the unique structural properties and reaction performance as well as reaction mechanisms over single-atom and cluster catalysts in comparison with traditional nanoparticle catalysts. Finally, the challenges and prospects in the rational design of efficient single-atom and cluster catalysts for NH3 synthesis were provided. Recent advances in single-atom and cluster catalysts, including single-atom catalysts (SACs), single-cluster catalysts (SCCs), and bimetallic-cluster catalysts (BCCs), for thermocatalytic NH3 synthesis at mild conditions.
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| GB/T 7714 | Peng, Xuanbei , Zhang, Mingyuan , Zhang, Tianhua et al. Single-atom and cluster catalysts for thermocatalytic ammonia synthesis at mild conditions [J]. | CHEMICAL SCIENCE , 2024 , 15 (16) : 5897-5915 . |
| MLA | Peng, Xuanbei et al. "Single-atom and cluster catalysts for thermocatalytic ammonia synthesis at mild conditions" . | CHEMICAL SCIENCE 15 . 16 (2024) : 5897-5915 . |
| APA | Peng, Xuanbei , Zhang, Mingyuan , Zhang, Tianhua , Zhou, Yanliang , Ni, Jun , Wang, Xiuyun et al. Single-atom and cluster catalysts for thermocatalytic ammonia synthesis at mild conditions . | CHEMICAL SCIENCE , 2024 , 15 (16) , 5897-5915 . |
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The development of effective Ru catalyst for ammonia synthesis is of important practical value and scientific significance because of the wide application of ammonia as a fertilizer and its promising applications in the renewable energy. Generally, ZrO2 was regarded as an inferior support for Ru catalyst used in ammonia synthesis. Here we prepare ZrO2 with monoclinic phase and carbon species from ZrCl4 fol-lowing the preparation route of UiO-66 as well as ammonia treatment. Owing to the presence of a larger amount of hydrogen adsorption as well as the easier desorption of hydrogen species, the ill effect of hydrogen species on the nitrogen adsorption-desorption and ammonia synthesis can be effectively alleviated. The resulting ZrO2-supported Ru catalyst showed 4 times higher ammonia synthesis activity than the conventional Ru/ZrO2 obtained from zirconium nitrate. (C) 2022 Published by Elsevier B.V. on behalf of Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences.
Keyword ：
Ammonia synthesis Ammonia synthesis Carbon Carbon Hydrogen adsorption-desorption Hydrogen adsorption-desorption Ru catalyst Ru catalyst ZrO2 ZrO2
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| GB/T 7714 | Zhang, Chuanfeng , Shi, Siyu , Fang, Biyun et al. Zirconia prepared from UIO-66 as a support of Ru catalyst for ammonia synthesis [J]. | CHINESE CHEMICAL LETTERS , 2023 , 34 (1) . |
| MLA | Zhang, Chuanfeng et al. "Zirconia prepared from UIO-66 as a support of Ru catalyst for ammonia synthesis" . | CHINESE CHEMICAL LETTERS 34 . 1 (2023) . |
| APA | Zhang, Chuanfeng , Shi, Siyu , Fang, Biyun , Ni, Jun , Lin, Jianxin , Wang, Xiuyun et al. Zirconia prepared from UIO-66 as a support of Ru catalyst for ammonia synthesis . | CHINESE CHEMICAL LETTERS , 2023 , 34 (1) . |
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Ammonia(NH3)decomposition to release COx-free hydrogen(H2)over non-noble catalysts has gained increasing attention.In this study,three nanostructured CeO2 with different morphologies,viz.rod(R),sphere(Sph),and spindle(Spi),were fabricated and served as supports for Ni/CeO2 catalyst.The CeO2 supports are different in particle sizes,specific surface area and porosity,resulting in the formation of Ni nanoparticles with distinguished sizes and dispersions.The surface properties of the Ni/CeO2 catalysts are not only distinct but also influential,affecting the adsorption and desorption of NH3,N2,and/or H2 molecules.The Ni/CeO2-R catalyst shows superior catalytic activity compared to the other two,owing to its smaller Ni crystallite size and larger BET surface area.The most abundant strong basic sites are observed for Ni/CeO2-Spi catalyst based on its exposed CeO2(110)planes,which facilitates the donation of electrons to the Ni particles,benefiting the associative desorption of N atoms.Thus,Ni/CeO2-Spi shows higher catalytic activity than Ni/CeO2-Sph,despite their almost identical Ni crystallite sizes.
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| GB/T 7714 | Chongqi Chen , Xiaoshuang Fan , Chen Zhou et al. Hydrogen production from ammonia decomposition over Ni/CeO2 catalyst:Effect of CeO2 morphology [J]. | 稀土学报（英文版） , 2023 , 41 (7) : 1014-1021 . |
| MLA | Chongqi Chen et al. "Hydrogen production from ammonia decomposition over Ni/CeO2 catalyst:Effect of CeO2 morphology" . | 稀土学报（英文版） 41 . 7 (2023) : 1014-1021 . |
| APA | Chongqi Chen , Xiaoshuang Fan , Chen Zhou , Li Lin , Yu Luo , Chaktong Au et al. Hydrogen production from ammonia decomposition over Ni/CeO2 catalyst:Effect of CeO2 morphology . | 稀土学报（英文版） , 2023 , 41 (7) , 1014-1021 . |
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The development of effective Ru catalyst for ammonia synthesis is of important practical value and sci-entific significance because of the wide application of ammonia as a fertilizer and its promising applica-tions in the renewable energy.Generally,ZrO2 was regarded as an inferior support for Ru catalyst used in ammonia synthesis.Here we prepare ZrO2 with monoclinic phase and carbon species from ZrCl4 fol-lowing the preparation route of UiO-66 as well as ammonia treatment.Owing to the presence of a larger amount of hydrogen adsorption as well as the easier desorption of hydrogen species,the ill effect of hydrogen species on the nitrogen adsorption-desorption and ammonia synthesis can be effectively alle-viated.The resulting ZrO2-supported Ru catalyst showed 4 times higher ammonia synthesis activity than the conventional Ru/ZrO2 obtained from zirconium nitrate.
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| GB/T 7714 | Chuanfeng Zhang , Siyu Shi , Biyun Fang et al. Zirconia prepared from UIO-66 as a support of Ru catalyst for ammonia synthesis [J]. | 中国化学快报（英文版） , 2023 , 34 (1) : 461-464 . |
| MLA | Chuanfeng Zhang et al. "Zirconia prepared from UIO-66 as a support of Ru catalyst for ammonia synthesis" . | 中国化学快报（英文版） 34 . 1 (2023) : 461-464 . |
| APA | Chuanfeng Zhang , Siyu Shi , Biyun Fang , Jun Ni , Jianxin Lin , Xiuyun Wang et al. Zirconia prepared from UIO-66 as a support of Ru catalyst for ammonia synthesis . | 中国化学快报（英文版） , 2023 , 34 (1) , 461-464 . |
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Ammonia (NH3) synthesis with hydrogen (H2) produced from renewable energy is a promising route to reduce carbon footprints and the dependence on fossil fuels. However, the development of highly efficient and stable catalyst for NH3 synthesis under mild conditions is a challenge. Herein, a series of boron nitride (BN)-supported Ru catalysts were synthesized, and the NH3 synthesis rate was enhanced significantly after the introduce of Ce. The developed RuCe2.4/BN catalyst with a Ce/Ru molar ratio of 2.4 exhibited the optimal NH3 synthesis rate of 14.6 mmolNH3 gcat−1 h−1 at 400 °C and 1.0 MPa, which was ∼21-fold that of the catalyst prepared without Ce. In situ diffuse reflectance infrared Fourier transform spectroscopy of CO adsorption and X-ray photoemission spectroscopy coupled with electron energy loss spectroscopy revealed that the d-d electronic interaction between Ru and CeO2 can be differentially adjusted by a change in the Ce/Ru molar ratio. An appropriate amount of Ce could enhance the electronic interaction between the CeOy overlayer and Ru entities. Also, the CeOy overlayer acted as an “electron shuttle” and enhanced the charge transfer from Ce to the surface of Ru atoms. Finally, electron donation occurred from the surface abundancy of Ru atoms to N2 molecule through a d-π* interaction. Moreover, the introduction of excessive Ce could block Ru active sites, weaken the electron transfer and, therefore, decrease the NH3 synthesis rate. © 2023 The Royal Society of Chemistry.
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| GB/T 7714 | Li, L. , Zhang, M. , Zhang, T. et al. Strong Ruδ+-Ce3+ electronic interaction induced by a CeOy overlayer for enhanced low-temperature N2-to-NH3 conversion [J]. | Catalysis Science and Technology , 2023 , 13 (7) : 2134-2141 . |
| MLA | Li, L. et al. "Strong Ruδ+-Ce3+ electronic interaction induced by a CeOy overlayer for enhanced low-temperature N2-to-NH3 conversion" . | Catalysis Science and Technology 13 . 7 (2023) : 2134-2141 . |
| APA | Li, L. , Zhang, M. , Zhang, T. , Gao, Y. , Ni, J. , Zhou, Y. et al. Strong Ruδ+-Ce3+ electronic interaction induced by a CeOy overlayer for enhanced low-temperature N2-to-NH3 conversion . | Catalysis Science and Technology , 2023 , 13 (7) , 2134-2141 . |
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本发明涉及一种用于电化学反应机理研究的图案电极，包括图案电极层、电解质层和阴极层；所述图案电极层为金属镍网格嵌入在电解质表面形成的平面电极层；所述图案电极层和阴极层分别设置于电解质层的正面及背面。本发明采用嵌入镍金属网格法制备的具有夹层结构的电解质支撑纽扣电池片，工艺简单，成本低，进一步提高了研究燃料电池反应机理的便捷性。
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| GB/T 7714 | 王秀云 , 刘顺利 , 罗宇 et al. 一种用于电化学反应机理研究的图案电极的制备方法 : CN202210120430.1[P]. | 2022-02-09 00:00:00 . |
| MLA | 王秀云 et al. "一种用于电化学反应机理研究的图案电极的制备方法" : CN202210120430.1. | 2022-02-09 00:00:00 . |
| APA | 王秀云 , 刘顺利 , 罗宇 , 方辉煌 , 陈崇启 , 江莉龙 . 一种用于电化学反应机理研究的图案电极的制备方法 : CN202210120430.1. | 2022-02-09 00:00:00 . |
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本发明公开了一种过渡金属原子簇催化剂及其制备方法和应用，所述催化剂以氮掺杂碳材料为载体，以过渡金属TM为活性组分，所述过渡金属以TM2原子簇形式负载在所述载体上。本发明制备的过渡金属(Co、Fe和Mn)原子簇催化剂的优点是无需负载其它催化活性组分，其本身呈现原子分散的金属团簇就是活性中心，在低温低压合成氨中呈现出良好的较强的工业应用前景。
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| GB/T 7714 | 王秀云 , 周岩良 , 江莉龙 . 一种过渡金属原子簇催化剂的制备方法及其在温和合成氨中的应用 : CN202110644472.0[P]. | 2021-06-09 00:00:00 . |
| MLA | 王秀云 et al. "一种过渡金属原子簇催化剂的制备方法及其在温和合成氨中的应用" : CN202110644472.0. | 2021-06-09 00:00:00 . |
| APA | 王秀云 , 周岩良 , 江莉龙 . 一种过渡金属原子簇催化剂的制备方法及其在温和合成氨中的应用 : CN202110644472.0. | 2021-06-09 00:00:00 . |
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