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学者姓名：林建新
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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
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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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Abstract ：
The development of a bimetallic catalyst for ammonia synthesis using nonprecious metals such as Co, Fe, and Mo has attracted wide attention. In this work, because of the enhancement of the exposed Co species on the surface of the Co-Fe bimetallic catalyst through the introduction of Co into Fe-CeO2 by the impregnation method, the amount of hydrogen adsorbed on the metal surface would enhance, and the hydrogen spillover could strengthen. As a result, the as-prepared sample shows much higher ammonia synthesis activity than other Co-Fe bimetallic catalysts or monometallic samples. This finding not only provides a way for the development of bimetallic catalysts using nonprecious metals for ammonia synthesis but also helps design other bimetallic catalysts for hydrogen-involving reactions.
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| GB/T 7714 | Zhong, Guoqing , Liu, Yang , Yu, Shitong et al. Strengthening Hydrogen Spillover in Ceria-Supported Co-Fe Bimetallic Catalysts for Boosting Ammonia Synthesis [J]. | INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH , 2024 , 63 (12) : 5089-5096 . |
| MLA | Zhong, Guoqing et al. "Strengthening Hydrogen Spillover in Ceria-Supported Co-Fe Bimetallic Catalysts for Boosting Ammonia Synthesis" . | INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH 63 . 12 (2024) : 5089-5096 . |
| APA | Zhong, Guoqing , Liu, Yang , Yu, Shitong , Zhang, Chuanfeng , Ni, Jun , Lin, Jianxin et al. Strengthening Hydrogen Spillover in Ceria-Supported Co-Fe Bimetallic Catalysts for Boosting Ammonia Synthesis . | INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH , 2024 , 63 (12) , 5089-5096 . |
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The effects of promoters on Ru nanoparticles (>= 2 nm) catalysts for NH3 synthesis have been extensively elaborated, but their roles on ultrasmall Ru nanoclusters (NCs, 1-2 nm) remain largely unknown and need to be further uncovered. Herein, a series of K-promoted MgO supported Ru NCs were synthesized and investigated for NH3 synthesis. The addition of 5wt.%K onto Ru/MgO NCs leads to a significantly high NH3 synthesis rate of 21.7 mmol(NH3) g(cat)(-1)h(-1) at 400 degrees C and 0.2 MPa, close to the thermodynamic equilibrium. Out studies reveal that anchoring K onto Ru NCs can increase the electron density and cause an upshift of the d-band center of Ru entities. Moreover, the addition of K regulates the hydrogen affinity and accelerates the migration of hydrogen from the Ru NCs surface to MgO support, which is crucial in avoiding the hydrogen poisoning effect on Ru NCs. With the synergistic effect of the Ru NCs sites bridged by H-spillover, makes the K-mediated Ru/MgO NCs catalysts efficient for NH3 synthesis at mild conditions.
Keyword ：
Ammonia synthesis Ammonia synthesis Electronic structure Electronic structure Hydrogen spillover Hydrogen spillover Oxygen vacancies Oxygen vacancies Ultrasmall Ru nanoclusters Ultrasmall Ru nanoclusters
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| GB/T 7714 | Peng, Xuanbei , Luo, Yongjin , Zhang, Tianhua et al. Potassium promoter regulates electronic structure and hydrogen spillover of ultrasmall Ru nanoclusters catalyst for ammonia synthesis [J]. | CHEMICAL ENGINEERING SCIENCE , 2024 , 292 . |
| MLA | Peng, Xuanbei et al. "Potassium promoter regulates electronic structure and hydrogen spillover of ultrasmall Ru nanoclusters catalyst for ammonia synthesis" . | CHEMICAL ENGINEERING SCIENCE 292 (2024) . |
| APA | Peng, Xuanbei , Luo, Yongjin , Zhang, Tianhua , Deng, Jinxiu , Zhou, Yanliang , Li, Jiaxin et al. Potassium promoter regulates electronic structure and hydrogen spillover of ultrasmall Ru nanoclusters catalyst for ammonia synthesis . | CHEMICAL ENGINEERING SCIENCE , 2024 , 292 . |
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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
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| 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 . |
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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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Catalytic reactions involving hydrogen over reducible oxide-supported metal catalysts are inseparable from the hydrogen storage capacity and hydrogen migration, which are mainly dependent on the interaction between reducible oxides and active metals. In this work, we report that the hydrogen migration rate of Ru/CeO2 could be tuned by changing cerium nitrate solvents for the preparation of ceria. There are more kinds of oxygen species and a large amount of Ce3+ concentration, defects and Ru-O-Ce interfacial sites for Ru catalyst supported on ceria obtained by ethanol-precipitated synthesis, resulting in a reduction in the amount of the exposed Ru species and proportion of Ru metal. In such a case, the migration and desorption of hydrogen species as well as nitrogen activation would be inhibited. Conversely, there are a higher ratio of Ru metal and a great deal of the Ru exposure for Ru catalyst supported on ceria obtained by water-precipitated synthesis, facilitating the migration and desorption of hydrogen species, as well as nitrogen activation. As a result, the water-precipitated synthesized ceria-supported Ru catalyst has 4.9-fold higher in catalytic activity than Ru catalyst supported on the ethanol -precipitated synthesized ceria. This work provides insight into the design of Ru catalysts used ammonia syn-thesis by controlling hydrogen spillover and migration between Ru species and CeO2.
Keyword ：
Ammonia synthesis Ammonia synthesis Ceria Ceria Hydrogen migration Hydrogen migration Metal-support interactions Metal-support interactions Ru catalyst Ru catalyst
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| GB/T 7714 | Li, Chunyan , Li, Minghui , Zheng, Yiping et al. Revealing hydrogen migration effect on ammonia synthesis activity over ceria-supported Ru catalysts [J]. | APPLIED CATALYSIS B-ENVIRONMENTAL , 2023 , 320 . |
| MLA | Li, Chunyan et al. "Revealing hydrogen migration effect on ammonia synthesis activity over ceria-supported Ru catalysts" . | APPLIED CATALYSIS B-ENVIRONMENTAL 320 (2023) . |
| APA | Li, Chunyan , Li, Minghui , Zheng, Yiping , Fang, Biyun , Lin, Jianxin , Ni, Jun et al. Revealing hydrogen migration effect on ammonia synthesis activity over ceria-supported Ru catalysts . | APPLIED CATALYSIS B-ENVIRONMENTAL , 2023 , 320 . |
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Ruthenium-based catalysts are widely used in ammonia (NH3) synthesis because of a high affinity for N2 acti-vation, while confronting the challenge of facile deactivation due to sintering. Herein, for the first time, we develop a highly active and sintering-resistant Ru2.1-CC catalyst via colloid carbonization (CC) for NH3 syn-thesis. It exhibits a superior NH3 synthesis rate around 9.4-fold that of Ru catalyst synthesized by impregnation method, displaying extremely high stability without aggregation of Ru nanoparticle after 100 h stability test. Our studies show that Ru2.1-CC possesses the average Ru particle size of 2.1 nm with narrow size distribution and thus exposes more active sites for N2 activation. Moreover, the formation of Ru-C interaction via colloid carbonization over Ru2.1-CC can stabilize Ru particle size to realize high stability, meanwhile reduce work function and upshift the d-band center of Ru metal to accelerate its electron transfer for N2 activation and NH3 synthesis. This study provides a new strategy for simple synthesis of noble metal-based catalysts that are highly active and stable for NH3 synthesis.
Keyword ：
Ammonia synthesis Ammonia synthesis Colloid carbonization Colloid carbonization Particle size Particle size Ru catalyst Ru catalyst Sintering-resistant Sintering-resistant
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| GB/T 7714 | Peng, Xuanbei , Su, Kailin , Fang, Hongpeng et al. Colloid carbonization-stabilized Ru nanoparticle catalyst for efficient ammonia synthesis at mild conditions [J]. | CHEMICAL ENGINEERING SCIENCE , 2023 , 278 . |
| MLA | Peng, Xuanbei et al. "Colloid carbonization-stabilized Ru nanoparticle catalyst for efficient ammonia synthesis at mild conditions" . | CHEMICAL ENGINEERING SCIENCE 278 (2023) . |
| APA | Peng, Xuanbei , Su, Kailin , Fang, Hongpeng , Sai, Qianjin , Ni, Jun , Qi, Haifeng et al. Colloid carbonization-stabilized Ru nanoparticle catalyst for efficient ammonia synthesis at mild conditions . | CHEMICAL ENGINEERING SCIENCE , 2023 , 278 . |
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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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Development of the cost-effective catalysts with excellent catalytic performance is highly demanded for ammonia synthesis, and the strong adsorption of ammonia greatly hinders the design of cost-effective and high-performance ammonia synthesis catalysts. Herein, we report that the addition of a small amount of Co species (0.1 wt%) into Mo2C catalyst, which can provide electrons to Mo2C, not only leads to improvement of the adsorption and migration of hydrogen, but also facilitates the adsorption and desorption of ammonia. Consequently, Mo2C catalyst with 0.1 wt%Co offers a 40% higher ammonia synthesis activity and a lower negative reaction order with respect to NH3 in comparison to Mo2C. This work stresses the importance of the minor components in improving the ammonia synthesis activity by accelerating the migration of reactants over the catalyst surface and the escape of products from the catalyst.
Keyword ：
ammonia desorption ammonia desorption ammonia synthesis ammonia synthesis cobalt cobalt molybdenum carbide molybdenum carbide
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| GB/T 7714 | Fang, Biyun , Zhang, Chuanfeng , Yang, Miaodi et al. Introducing trace Co to molybdenum carbide catalyst for efficient ammonia synthesis [J]. | AICHE JOURNAL , 2023 , 69 (10) . |
| MLA | Fang, Biyun et al. "Introducing trace Co to molybdenum carbide catalyst for efficient ammonia synthesis" . | AICHE JOURNAL 69 . 10 (2023) . |
| APA | Fang, Biyun , Zhang, Chuanfeng , Yang, Miaodi , Li, Jiahui , Li, Chunyan , Ni, Jun et al. Introducing trace Co to molybdenum carbide catalyst for efficient ammonia synthesis . | AICHE JOURNAL , 2023 , 69 (10) . |
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The development of a Ru catalyst with excellent ammonia synthesis performance plays a key role in the application of ammonia in the upcoming renewable energy era. Herein, a ceria-supported Ru catalyst was prepared by oxygen-induced activation, resulting in enhancement of the amount of the exposed Ru species, active oxygen species, and Ru-O-Ce bond. As a result, the amount of Ru species surrounded by active oxygen species would be enhanced, facilitating the exchange and reaction of the hydrogen species adsorbed on the Ru catalyst with the gaseous reactants. Oxygen-induced activation of the ceria-supported Ru catalyst leads to enhancement of the ammonia synthesis activity by more than 63%; moreover, the as-obtained catalyst has a smaller negative reaction order of H2 than its Ru/CeO2 counterpart.
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| GB/T 7714 | Zhou, Jian , Xia, Fei , Zhang, Chuanfeng et al. Oxygen-Induced Activation of a Ceria-Supported Ru Catalyst for Enhancing Ammonia Synthesis Activity [J]. | INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH , 2023 , 62 (15) : 6142-6148 . |
| MLA | Zhou, Jian et al. "Oxygen-Induced Activation of a Ceria-Supported Ru Catalyst for Enhancing Ammonia Synthesis Activity" . | INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH 62 . 15 (2023) : 6142-6148 . |
| APA | Zhou, Jian , Xia, Fei , Zhang, Chuanfeng , Ni, Jun , Lin, Jianxin , Lin, Bingyu et al. Oxygen-Induced Activation of a Ceria-Supported Ru Catalyst for Enhancing Ammonia Synthesis Activity . | INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH , 2023 , 62 (15) , 6142-6148 . |
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