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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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Exploring advanced electrolysis techniques for attaining scene-adaptive and on-site green H2 production is an imperative matter of utmost practical significance but grand challenge remains. Herein, drawn inspiration from a spontaneous hydrazine-H2O galvanic cell configured on a low-valence Ru single atoms-loaded Mo2C electrode (RuSA/v-Mo2C), an alternative H2 energy solution utilizing self-powered electrochemical hydrazine splitting (N2H4 -> 2H2 + N2) instead of the stereotyped electricity-consumed water splitting for green H2 production is proposed. This solution highlights a pH-decoupled hydrazine-H2O primary battery with notable open-circuit voltage of 1.37 V and energy density up to 358 Wh gN2H4-1, which powerfully propels an alkaline hydrazine splitting cell, leading to bilateral H2 harvest with a remarkable rate of 18 mol h-1 m-2, i.e., 403.2 L h-1 m-2, setting a new record for the self-sustaining electricity-powered H2 production systems. The success of RuSA/v-Mo2C for this solution is further decoded by tandem theoretical and in situ spectroscopic studies, cross-verifying a Ru-Mo dual-site synergy in streamlining the overall energy barriers, thereby enhancing the kinetics of electrode reactions. This pioneering work, showcasing electrochemical H2 production free from both external energy and feedstock inputs, opens up a new horizon on way of the ultimate H2 energy solution.
Keyword ：
electrocatalysis electrocatalysis energy conversion energy conversion hydrazine oxidation hydrazine oxidation hydrogen evolution hydrogen evolution self-powered self-powered
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| GB/T 7714 | Zhang, Linjie , Li, Man , Sun, Chen et al. A Hydrazine-Water Galvanic Cell-Inspired Self-Powered High-Rate Hydrogen Production via Overall Hydrazine Electrosplitting [J]. | ADVANCED FUNCTIONAL MATERIALS , 2025 , 35 (19) . |
| MLA | Zhang, Linjie et al. "A Hydrazine-Water Galvanic Cell-Inspired Self-Powered High-Rate Hydrogen Production via Overall Hydrazine Electrosplitting" . | ADVANCED FUNCTIONAL MATERIALS 35 . 19 (2025) . |
| APA | Zhang, Linjie , Li, Man , Sun, Chen , Wang, Hsiao-Tsu , Xiao, Yi , Ma, Ke et al. A Hydrazine-Water Galvanic Cell-Inspired Self-Powered High-Rate Hydrogen Production via Overall Hydrazine Electrosplitting . | ADVANCED FUNCTIONAL MATERIALS , 2025 , 35 (19) . |
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The major bottlenecks for ammonia (NH3) synthesis under mild conditions are the activation of the extremely inert N N bond (941 kJ mol(-1)) and/or the desorption of NH3 from the catalyst surface. Electron donation from the appropriate promoters is essential to enhance N-2 activation over Fe or Ru catalysts. Nevertheless, despite typical element promoters enhancing the N-2 activation efficiency, they induce strong NH3 binding on the catalyst surface, leading to the need for high temperatures and pressures for the reaction to complete. Herein, we propose the use of a molecular promoter (C-60) to tackle the difficulties. The positioning role of C-60 at a 1 nm scale on small Ru nanoclusters drives the exposure of more terrace sites (geometric effect) and induces d-pi interactions at the Ru-C-60 junctions. The latter electronically modifies the Ru sites (electronic effect), thereby synergistically contributing to N-2 and H-2 activation as well as to the release of NH3 on the Ru sites. The significant electron buffer attribute of C-60 and the strong electronic interaction between Ru and C-60 facilitate a shift of d-band center toward the Fermi level and a decrease of work function, simultaneously satisfying the electronic requirements for N-2 activation enhancement and NH3 binding weakening. Consequently, the C-60-promoted Ru/LaN catalyst exhibits a high NH3 synthesis rate. It is envisioned that our findings have significant implications for the rational search of molecular promoters for high-efficiency NH3 synthesis.
Keyword ：
ammonia synthesis ammonia synthesis electronic structure electronic structure molecular promoter molecular promoter N-2 activation N-2 activation ru catalysts ru catalysts
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| GB/T 7714 | Peng, Xuanbei , Luo, Yongjin , Zhang, Yangyu et al. Dissecting the Essential Role of a Molecular Promoter C60 on a Ru Catalyst for Ammonia Synthesis [J]. | ACS CATALYSIS , 2025 , 15 (4) : 2827-2838 . |
| MLA | Peng, Xuanbei et al. "Dissecting the Essential Role of a Molecular Promoter C60 on a Ru Catalyst for Ammonia Synthesis" . | ACS CATALYSIS 15 . 4 (2025) : 2827-2838 . |
| APA | Peng, Xuanbei , Luo, Yongjin , Zhang, Yangyu , Zhang, Shiyong , Zhang, Mingyuan , Mao, Ruishao et al. Dissecting the Essential Role of a Molecular Promoter C60 on a Ru Catalyst for Ammonia Synthesis . | ACS CATALYSIS , 2025 , 15 (4) , 2827-2838 . |
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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 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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本发明公开一种RuCo合金合成氨催化剂的成型方法。本发明将RuCo/N‑C粉末催化剂、粘结剂、助剂和水混炼，经成型、烤干、干燥、焙烧，得到成型催化剂。本发明研究了成型催化剂的颗粒模型对抗压强度的影响规律，构筑了三叶草、条形和球形等不同颗粒模型催化剂，其中三叶草形催化剂的线压强度可达90.4N/cm、磨耗率仅为0.06％/每公斤，且三叶草形的氨合成性能、表观活性和抗压性能最佳。本发明专利提供的催化剂成型过程中所需的原料廉价且易大规模制备，具有较强的工业应用前景。
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| GB/T 7714 | 王秀云 , 张天华 , 江莉龙 . 一种RuCo合金合成氨催化剂的成型方法 : CN202111616636.5[P]. | 2021-12-27 00:00:00 . |
| MLA | 王秀云 et al. "一种RuCo合金合成氨催化剂的成型方法" : CN202111616636.5. | 2021-12-27 00:00:00 . |
| APA | 王秀云 , 张天华 , 江莉龙 . 一种RuCo合金合成氨催化剂的成型方法 : CN202111616636.5. | 2021-12-27 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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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MXene基热催化合成氨催化剂及其制备方法和应用，所述催化剂以过渡金属和Mo2CTx为活性中心，所述过渡金属负载在所述Mo2CTx上；x代表官能团层数；所述过渡金属选自铁(Fe)、钴(Co)、镍(Ni)、铼(Re)中的一种或多种。本发明通过氢氟酸刻蚀和初湿浸渍的方法，合成了Mo2CTx负载不同过渡金属温和合成氨催化剂，为过渡金属温和条件下热催化合成氨催化剂的研究和使用提供了解决方案。
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| GB/T 7714 | 王秀云 , 王聪颖 , 周岩良 et al. 一种MXene基热催化合成氨催化剂及其制备和应用 : CN202210211034.X[P]. | 2022-03-04 00:00:00 . |
| MLA | 王秀云 et al. "一种MXene基热催化合成氨催化剂及其制备和应用" : CN202210211034.X. | 2022-03-04 00:00:00 . |
| APA | 王秀云 , 王聪颖 , 周岩良 , 江莉龙 . 一种MXene基热催化合成氨催化剂及其制备和应用 : CN202210211034.X. | 2022-03-04 00:00:00 . |
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