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学者姓名：倪军
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Abstract ：
Achieving green ammonia (NH3) synthesis requires developing effective catalysts under mild conditions. However, the competitive adsorption of N-2 and H-2, as well as the strong binding of N-containing intermediates on the catalyst, greatly inhibits the active sites for efficient NH3 synthesis. Here, we constructed a series of ZrH2-modified Fe catalysts with dual active sites to address these issues and realized efficient NH3 synthesis under mild conditions. Our study shows that ZrH2 can not only provide active sites for H-2 activation but also transfer electrons to Fe sites for accelerating N-2 activation. The interaction between Fe and ZrH2 over 40ZrH(2)-Fe leads to a decrease in work function and a downward shift of the d-band center, which is conducive to N-2 activation and NH3 desorption, respectively. The utilization of distinct sites for activating different reactants can avoid the competitive adsorption of N-2 and H-2, leading to excellent NH3 synthesis activity of the 40 wt.% ZrH2-mediated Fe catalyst. As a result, 40ZrH(2)-Fe exhibits a high NH3 synthesis rate of 23.3 mmol g(cat)(-1) h(-1) at 400 degrees C and 1 MPa and robust stability during 100 h time-on-stream.
Keyword ：
ammonia synthesis ammonia synthesis competitive adsorption competitive adsorption dual-site catalyst dual-site catalyst N-2 activation N-2 activation synergistic effect synergistic effect
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| GB/T 7714 | Zhang, Shiyong , Zhang, Mingyuan , Zhang, Tianhua et al. A dual-site Fe-based catalyst for efficient ammonia synthesis under mild conditions [J]. | SCIENCE CHINA-CHEMISTRY , 2025 , 68 (4) : 1576-1584 . |
| MLA | Zhang, Shiyong et al. "A dual-site Fe-based catalyst for efficient ammonia synthesis under mild conditions" . | SCIENCE CHINA-CHEMISTRY 68 . 4 (2025) : 1576-1584 . |
| APA | Zhang, Shiyong , Zhang, Mingyuan , Zhang, Tianhua , Sun, Jizhen , Li, Jiaxin , Su, Kailin et al. A dual-site Fe-based catalyst for efficient ammonia synthesis under mild conditions . | SCIENCE CHINA-CHEMISTRY , 2025 , 68 (4) , 1576-1584 . |
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Abstract ：
The development of advanced catalysts is critical to realize efficient ammonia (NH3) synthesis under mild conditions. However, the activation of an inert N equivalent to N bond in N2 molecules is the primary hindrance to NH3 synthesis, and hydrogen poisoning is another major and a serious problem, especially in Ru-based catalysts. Here, we develop an H-ZSM-5-supported Ru-based catalyst (Ce-Ru/HZ) via decorating with a CeO2 promoter to realize efficient NH3 synthesis. Our study shows that the Ce species can serve as an electron donor to enrich the electron density of Ru sites, thus accelerating N2 activation for NH3 synthesis. Meanwhile, the interaction of Ru and Ce can alleviate the effect of hydrogen poisoning on Ru sites. Consequently, the 16 wt % Ce-promoted Ru/HZ catalyst displays a superior NH3 synthesis rate and long-term stability of more than 550 h at 400 degrees C and 1 MPa.
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| GB/T 7714 | Zhang, Tianhua , Yue, Kexin , Mo, Jiangyang et al. Enhanced Ammonia Synthesis Performance over Ru-Based Catalysts via the Addition of Ce Promoter [J]. | INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH , 2025 , 64 (18) : 9070-9077 . |
| MLA | Zhang, Tianhua et al. "Enhanced Ammonia Synthesis Performance over Ru-Based Catalysts via the Addition of Ce Promoter" . | INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH 64 . 18 (2025) : 9070-9077 . |
| APA | Zhang, Tianhua , Yue, Kexin , Mo, Jiangyang , Zhang, Mingyuan , Zhu, Jie , Lin, Ruting et al. Enhanced Ammonia Synthesis Performance over Ru-Based Catalysts via the Addition of Ce Promoter . | INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH , 2025 , 64 (18) , 9070-9077 . |
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Molybdenum (Mo) serves as the key site in the nitrogenase enzyme, catalyzing the conversion of N-2 into NH(3 )under ambient conditions. However, the strong affinity of Mo sites for N-2 hinders H-2 adsorption due to the competitive nature of N-2 and H-2 on a single site, resulting in an unsatisfactory ammonia synthesis performance. Here, we propose an approach of intervening C-60 layer as a second site for H-2 adsorption on two-dimensional Mo2CTx. The C-60 layer thickness is readily tunable by varying its loading content. An optimal C-60 layer significantly enhances the electronic interaction between the C-60 layer and the Mo(2)CT(x )layer, leading to a remarkable decrease in the work function and an increase in the electron density of Mo atoms. Therefore, the separate adsorption of N-2 and H-2 on distinct sites is substantially facilitated. The present work offers insights into the correlation between structure and performance in NH(3 )synthesis catalysts.
Keyword ：
ammonia synthesis ammonia synthesis carbon clusters carbon clusters electronic interaction electronic interaction Mo catalysts Mo catalysts N-2 activation N-2 activation
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| GB/T 7714 | Zhang, Yangyu , Zhou, Yanliang , Peng, Xuanbei et al. Enhanced layer-layer interaction via a tunable C60 layer in Mo2CTx-based catalyst for ammonia synthesis [J]. | AICHE JOURNAL , 2025 , 71 (6) . |
| MLA | Zhang, Yangyu et al. "Enhanced layer-layer interaction via a tunable C60 layer in Mo2CTx-based catalyst for ammonia synthesis" . | AICHE JOURNAL 71 . 6 (2025) . |
| APA | Zhang, Yangyu , Zhou, Yanliang , Peng, Xuanbei , Chen, Ming , Li, Jiaxin , Zhang, Mingyuan et al. Enhanced layer-layer interaction via a tunable C60 layer in Mo2CTx-based catalyst for ammonia synthesis . | AICHE JOURNAL , 2025 , 71 (6) . |
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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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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 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 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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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 degrees 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 equivalent to N bond pi* orbitals, which would weaken the N equivalent to 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.
Keyword ：
Ammonia synthesis Ammonia synthesis Atomic cluster Atomic cluster Electronic interaction Electronic interaction N 2 activation N 2 activation Promoter Promoter
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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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Ammonia (NH3) plays an important role in the development and evolution of Earth's life system. The extremely high bond energy (941 kJ mol(-1)) of N-2 hinder the conversion of N-2 to NH3 under mild conditions. Meanwhile, clearly identifying the distribution of intermediates for NH3 synthesis remains a huge challenge in the experiment. Herein, we anchored carbon clusters (C-60 or C-70) onto Ru catalysts supported on rare earth oxides, forming a class of Ru-carbon cluster co-catalysts that exhibit strong electronic metal-carbon cluster interaction (EMCI). Carbon clusters function as an electron buffer that induced electron uptake from metallic Ru sites and concurrently provides electron feedback to Ru delta+ in a reversible manner, achieving a flexible balance of electron density at the Ru active sites. Moreover, H-affinitive carbon clusters serve as the site for the adsorption, activation and migration of hydrogen. With Ru and carbon clusters synergistically bridged by hydrogen spillover, the Ru-C-60 co-catalyst exhibits an exceptionally high NH3 synthesis rate and remarkable stability. Experimental provides direct evidence of the distribution and evolution of *N2Hx (x = 1 similar to 3) intermediates, with the hydrogenation of *NH2 to form *NH3 identified as the rate-determining step. This work paves the way for utilizing carbon clusters in important chemical reactions.
Keyword ：
ammonia synthesis ammonia synthesis carbon clusters carbon clusters electron buffer electron buffer N-2 activation N-2 activation reaction mechanism reaction mechanism
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| GB/T 7714 | Zhang, Mingyuan , Luo, Yongjin , Peng, Xuanbei et al. Contribution of Carbon Clusters to Ammonia Synthesis Over Ru-Based Catalysts [J]. | ADVANCED FUNCTIONAL MATERIALS , 2024 , 35 (8) . |
| MLA | Zhang, Mingyuan et al. "Contribution of Carbon Clusters to Ammonia Synthesis Over Ru-Based Catalysts" . | ADVANCED FUNCTIONAL MATERIALS 35 . 8 (2024) . |
| APA | Zhang, Mingyuan , Luo, Yongjin , Peng, Xuanbei , Zhang, Shiyong , Zhang, Lei , Xu, Cong-Qiao et al. Contribution of Carbon Clusters to Ammonia Synthesis Over Ru-Based Catalysts . | ADVANCED FUNCTIONAL MATERIALS , 2024 , 35 (8) . |
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The amount of dopant used in conventional cases for improving catalytic performance is higher than 5%. In this work, a strategy to enhance the ammonia synthesis performance of a Ru/CeO2 catalyst by using trace Pr (0.1 mol%) is reported. Owing to the improvement of oxygen defects, Ce3+ concentration and interfaced Ru species, the hydrogen adsorption was enhanced, and the desorption of hydrogen species would be promoted. As a result, Ru/CeO2 with 0.1 mol% Pr shows 1.4 times higher ammonia synthesis rate and excellent stability compared to Ru/CeO2 or the sample with high Pr loading (50 mol% Pr). This study provides a new idea for the design of high-efficiency ammonia synthesis catalysts. The amount of dopant used in conventional cases for improving catalytic performance is higher than 5%.
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| GB/T 7714 | Li, Chunyan , Zhang, Zecheng , Zhou, Lingyun et al. Boosting the ammonia synthesis activity of ceria-supported Ru catalysts achieved through trace Pr addition [J]. | CHEMICAL COMMUNICATIONS , 2023 , 59 (77) : 11552-11555 . |
| MLA | Li, Chunyan et al. "Boosting the ammonia synthesis activity of ceria-supported Ru catalysts achieved through trace Pr addition" . | CHEMICAL COMMUNICATIONS 59 . 77 (2023) : 11552-11555 . |
| APA | Li, Chunyan , Zhang, Zecheng , Zhou, Lingyun , Fang, Biyun , Ni, Jun , Lin, Jianxin et al. Boosting the ammonia synthesis activity of ceria-supported Ru catalysts achieved through trace Pr addition . | CHEMICAL COMMUNICATIONS , 2023 , 59 (77) , 11552-11555 . |
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