Query：
学者姓名：王秀云
Refining：
Year
Type
Indexed by
Source
Complex
Co-
Language
Clean All
Abstract ：
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.
Cite：
Copy from the list or Export to your reference management。
| 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 . |
| Export to | NoteExpress RIS BibTex |
Version ：
Abstract ：
To date, NH3 synthesis under mild conditions is largely confined to precious Ru catalysts, while nonprecious metal (NPM) catalysts are confronted with the challenge of low catalytic activity due to the inverse relationship between the N2 dissociation barrier and NHx (x = 1-3) desorption energy. Herein, we demonstrate NPM (Co, Ni, and Re)-mediated Mo2CTx MXene (where Tx denotes the OH group) to achieve efficient NH3 synthesis under mild conditions. In particular, the NH3 synthesis rate over Re/Mo2CTx and Ni/Mo2CTx can reach 22.4 and 21.5 mmol g-1 h-1 at 400 °C and 1 MPa, respectively, higher than that of NPM-based catalysts and Cs-Ru/MgO ever reported. Experimental and theoretical studies reveal that Mo4+ over Mo2CTx has a strong ability for N2 activation; thus, the rate-determining step is shifted from conventional N2 dissociation to NH2* formation. NPM is mainly responsible for H2 activation, and the high reactivity of spillover hydrogen and electron transfer from NPM to the N-rich Mo2CTx surface can efficiently facilitate nitrogen hydrogenation and the subsequent desorption of NH3. With the synergistic effect of the dual active sites bridged by H-spillover, the NPM-mediated Mo2CTx catalysts circumvent the major obstacle, making NH3 synthesis under mild conditions efficient. © 2024 The Authors. Published by American Chemical Society.
Cite：
Copy from the list or Export to your reference management。
| GB/T 7714 | Zhou, Y. , Liang, L. , Wang, C. et al. Precious-Metal-Free Mo-MXene Catalyst Enabling Facile Ammonia Synthesis Via Dual Sites Bridged by H-Spillover [J]. | Journal of the American Chemical Society , 2024 , 146 (33) : 23054-23066 . |
| MLA | Zhou, Y. et al. "Precious-Metal-Free Mo-MXene Catalyst Enabling Facile Ammonia Synthesis Via Dual Sites Bridged by H-Spillover" . | Journal of the American Chemical Society 146 . 33 (2024) : 23054-23066 . |
| APA | Zhou, Y. , Liang, L. , Wang, C. , Sun, F. , Zheng, L. , Qi, H. et al. Precious-Metal-Free Mo-MXene Catalyst Enabling Facile Ammonia Synthesis Via Dual Sites Bridged by H-Spillover . | Journal of the American Chemical Society , 2024 , 146 (33) , 23054-23066 . |
| Export to | NoteExpress RIS BibTex |
Version ：
Abstract ：
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
Cite：
Copy from the list or Export to your reference management。
| 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 . |
| Export to | NoteExpress RIS BibTex |
Version ：
Abstract ：
Ammonia (NH3) is an excellent candidate for hydrogen storage and transport. However, producing NH3 under mild conditions is a long-term, arduous task. Atomic cluster catalysts (ACCs) have been shown to be effective for catalytic N2-to-NH3 conversion, opening the door to the development of efficient catalysts under mild conditions. Still, ACC formation with thermally stable catalytic sites remains a challenge because of their high surface free energy. Herein, we report anchoring Ba and/or Ce onto Ru ACCs (2 wt% Ru atomic clusters supported on N-doped carbon) to form so-called clusters–metal oxide promoters electronic interaction (CMEI) to stabilize the Ru atomic clusters. The resulting Ba/Ce/Ru ACCs significantly boost the NH3 synthesis rate to 56.2 mmolNH3 gcat−1 h−1 at 400 °C and 1 MPa, which is 7.5-fold higher than that of Ru ACC. The strengthened CMEI between the Ba/Ce and Ru atomic clusters across the Ba/Ce/Ru ACC enables electron transfer from Ba and/or Ce to Ru atomic clusters. As such, the electron-enriched Ru atom could facilitate electron transfer to N≡N bond π* orbitals, which would weaken the N≡N bond and drive the eventual conversion of N2 to NH3. This study offers insight into the role of CMEI in Ru ACCs and provides an effective approach for designing stable atomic cluster catalysts for NH3 synthesis. © 2024 Dalian Institute of Chemical Physics, Chinese Academy of Sciences.
Keyword ：
Ammonia Ammonia Atoms Atoms Catalyst supports Catalyst supports Cerium Cerium Doping (additives) Doping (additives) Electron transitions Electron transitions Free energy Free energy Hydrogen storage Hydrogen storage Kinetic theory Kinetic theory Ruthenium Ruthenium
Cite：
Copy from the list or Export to your reference management。
| GB/T 7714 | Zhang, Tianhua , Hu, Haihui , Li, Jiaxin et al. Tuning clusters-metal oxide promoters electronic interaction of Ru-based catalyst for ammonia synthesis under mild conditions [J]. | Chinese Journal of Catalysis , 2024 , 60 : 209-218 . |
| MLA | Zhang, Tianhua et al. "Tuning clusters-metal oxide promoters electronic interaction of Ru-based catalyst for ammonia synthesis under mild conditions" . | Chinese Journal of Catalysis 60 (2024) : 209-218 . |
| APA | Zhang, Tianhua , Hu, Haihui , Li, Jiaxin , Gao, Yinglong , Li, Lingling , Zhang, Mingyuan et al. Tuning clusters-metal oxide promoters electronic interaction of Ru-based catalyst for ammonia synthesis under mild conditions . | Chinese Journal of Catalysis , 2024 , 60 , 209-218 . |
| Export to | NoteExpress RIS BibTex |
Version ：
Abstract ：
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
Cite：
Copy from the list or Export to your reference management。
| 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) . |
| Export to | NoteExpress RIS BibTex |
Version ：
Abstract ：
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.
Cite：
Copy from the list or Export to your reference management。
| 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 . |
| Export to | NoteExpress RIS BibTex |
Version ：
Abstract ：
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.
Cite：
Copy from the list or Export to your reference management。
| 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 . |
| Export to | NoteExpress RIS BibTex |
Version ：
Abstract ：
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.
Cite：
Copy from the list or Export to your reference management。
| 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 . |
| Export to | NoteExpress RIS BibTex |
Version ：
Abstract ：
Harnessing the selectivity in catalytic hydrogenation of CO2 is important for producing valuable chemicals. Herein, the shape dependency of the CO2 hydrogenation on singly dispersed Ru/CeO2 catalysts is investigated. CeO2 of three shapes, including nanocube, nanooctahedron and nanorod, are prepared as the catalyst supports and assigned to the surface of (100), (111) and (110) crystal plane, respectively. The Ru/CeO2 (nanorod) exhibits the highest selectivity to CO (97.6 %) at 350 degrees C, while the Ru/CeO2 (nanocube) exhibits a mediocre selectivity to CO (41.4 %) but the highest CO2 conversion. The shape of the CeO2 support determines the electronic state of supported Ru atoms through the electronic metal-support interaction. The low CO affinity on cationic Ru-beta sites leads to the higher selectivity to CO on the Ru/CeO2 (nanorod) and Ru/CeO2 (nanooctahedron) catalysts, while the strong dissociation ability of H-2 on low valence Ru-alpha sites results in the high activity on the Ru/CeO2 (nanocube) catalyst.
Keyword ：
Ceria Ceria CO2 hydrogenation CO2 hydrogenation Electronic metal-support interaction Electronic metal-support interaction Ruthenium Ruthenium Shape effect Shape effect
Cite：
Copy from the list or Export to your reference management。
| GB/T 7714 | An, Zemin , Ma, Nan , Xu, Yuanjie et al. Shape dependency of CO2 hydrogenation on ceria supported singly dispersed Ru catalysts [J]. | JOURNAL OF CATALYSIS , 2023 , 429 . |
| MLA | An, Zemin et al. "Shape dependency of CO2 hydrogenation on ceria supported singly dispersed Ru catalysts" . | JOURNAL OF CATALYSIS 429 (2023) . |
| APA | An, Zemin , Ma, Nan , Xu, Yuanjie , Yang, Hua , Zhao, Huibo , Wu, Lizhi et al. Shape dependency of CO2 hydrogenation on ceria supported singly dispersed Ru catalysts . | JOURNAL OF CATALYSIS , 2023 , 429 . |
| Export to | NoteExpress RIS BibTex |
Version ：
Abstract ：
本发明公开一种尺寸稳定Ru基催化剂的制备方法及其在氨合成中的应用。所述制备方法包括以下步骤：(1)将钌前驱体、无机碱和溶剂混合，在惰性氛围下加热搅拌，制备得到钌胶体颗粒；(2)采用胶体碳化法，将步骤(1)中制备的钌胶体颗粒负载到GC载体上，经高温碳化后制备得到Ru/GC‑CD催化剂。本发明的催化剂在400℃和1MPa下的氨合成性能达到了11.1mmol g‑1h‑1，其约为Ru/GC‑IM催化剂的11倍；通过碳化锚定方式使催化剂在100h稳定性测试中催化活性及Ru尺寸基本不改变；而普通浸渍法制备的Ru/GC‑IM催化剂在10h反应后催化活性开始下降，30h后催化剂几乎完全失活。
Cite：
Copy from the list or Export to your reference management。
| GB/T 7714 | 江莉龙 , 周岩良 , 王秀云 . 一种尺寸稳定Ru基催化剂的制备方法及其在氨合成中的应用 : CN202210648059.6[P]. | 2022-06-08 00:00:00 . |
| MLA | 江莉龙 et al. "一种尺寸稳定Ru基催化剂的制备方法及其在氨合成中的应用" : CN202210648059.6. | 2022-06-08 00:00:00 . |
| APA | 江莉龙 , 周岩良 , 王秀云 . 一种尺寸稳定Ru基催化剂的制备方法及其在氨合成中的应用 : CN202210648059.6. | 2022-06-08 00:00:00 . |
| Export to | NoteExpress RIS BibTex |
Version ：
Export
| Results： |
Selected to |
| Format： |
