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学者姓名：周岩良
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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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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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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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Strong metal-support interaction (SMSI) is a crucial strategy for modulating the activity. Finely tailoring the size of the support to the nanoscale still faces significant challenges. Herein, for the first time, C60 carbon cluster is utilized as a nano-support to anchor ultrafine Ru nanoclusters to create a Ru-C60 cluster-cluster co-catalyst. The unique geometric structure of the nano-support C60 enables the construction of a strong cluster-cluster interaction (SCCI), quite different from traditional SMSI. La-modified Ru-C60 presents a surprising discovery that NH3 can even be synthesized at 150 degrees C, and exhibits an unprecedentedly high NH3 synthesis rate at 400 degrees C. C60 not only acts as an electron buffer to balance the charge density of Ru sites, but also stabilizes more metallic Ru active sites with a smaller size due to its spatial and SCCI effect, thereby achieving superior catalytic performance over a wide range of temperatures and pressures.
Keyword ：
Ammonia synthesis Ammonia synthesis Cluster-cluster interaction Cluster-cluster interaction Electronic structure Electronic structure Heterogeneous catalysis Heterogeneous catalysis Nano-support Nano-support
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| GB/T 7714 | Zhang, Tianhua , Zhang, Yangyu , Chen, Zuo-Chang et al. Coupling metal and support clusters dictates the reactivity of Ru catalysts for ammonia synthesis [J]. | CHEMICAL ENGINEERING SCIENCE , 2025 , 312 . |
| MLA | Zhang, Tianhua et al. "Coupling metal and support clusters dictates the reactivity of Ru catalysts for ammonia synthesis" . | CHEMICAL ENGINEERING SCIENCE 312 (2025) . |
| APA | Zhang, Tianhua , Zhang, Yangyu , Chen, Zuo-Chang , Qiu, Yujue , Zhang, Mingyuan , Zhang, Shiyong et al. Coupling metal and support clusters dictates the reactivity of Ru catalysts for ammonia synthesis . | CHEMICAL ENGINEERING SCIENCE , 2025 , 312 . |
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The development of highly efficient catalysts that enable Haber-Bosch ammonia (NH3) synthesis under mild conditions remains critically challenging since the competitive activation of coadsorbates, particularly excessive N2 or H2 binding at active sites, is a trade-off and detrimental to NH3 synthesis. Herein, we design a novel Ru tandem catalyst that combines Ru single atom (Ru1) with nanoparticle sites (RuNP) on CeO2 nanoislands, leveraging cascade hydrogen catalysis between functionally distinct Ru sites to realize highly efficient NH3 synthesis under mild conditions. Our studies reveal that RuNP sites suffer from hydrogen poisoning, whereas Ru1 sites exclusively adsorb N2. The hydrogen spillover from RuNP to Ru1 sites reduces hydrogen coverage on RuNP sites to effectively decrease the N2 dissociation barrier and also greatly facilitates N2 hydrogenation at Ru1 sites for NH3 synthesis, thus overcoming the trade-off in the dynamic N2/H2 activation equilibrium. As a result, the Ru single atom and nanoparticle tandem catalyst achieves a remarkable NH3 synthesis rate of 59.0 mmol gcat -1 h-1 with 600 h long-term operational stability at 400 degrees C and 1 MPa, possessing an exceptionally high specific rate among reported Ru-based catalysts. This catalyst structure design paves a new path for NH3 synthesis under mild conditions.
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| GB/T 7714 | Zhou, Yanliang , Yang, Bo , Wang, Lu et al. Ru Single Atom and Nanoparticle Tandem Catalyst Unlocking High-Efficiency Ammonia Synthesis under Mild Conditions [J]. | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2025 , 147 (34) : 31136-31146 . |
| MLA | Zhou, Yanliang et al. "Ru Single Atom and Nanoparticle Tandem Catalyst Unlocking High-Efficiency Ammonia Synthesis under Mild Conditions" . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 147 . 34 (2025) : 31136-31146 . |
| APA | Zhou, Yanliang , Yang, Bo , Wang, Lu , Su, Kailin , Liu, Ben , Fang, Hongpeng et al. Ru Single Atom and Nanoparticle Tandem Catalyst Unlocking High-Efficiency Ammonia Synthesis under Mild Conditions . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2025 , 147 (34) , 31136-31146 . |
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Olefins are important building blocks that have been extensively used to produce diverse consumer products in petrochemical industry. Owing to the requirement of low-carbon-footprint processes and the increasing use of light alkanes sourced from shale gas, an environmentally friendly and economic route alternative to the state-of-the-art steam cracking of crude oil has been investigated for olefin production. The oxidative dehydrogenation (ODH) of alkanes to olefins has attracted wide attention due to the absence of thermodynamic limitations and coke formation. However, excessive oxidation of olefin is prone to occur in this process. Developing a suitable ODH catalyst with high performance, particularly with enhanced selectivity, is more and more urgent but still remains a challenge. In this Review, we talk about the representative currently developed isolation strategies to optimize the selectivity of olefins via the ODH process, particularly for the conversion of ethane to ethylene, which include the dispersion regulation of metal oxide, the isolation of metal and nonmetal sites, the construction of dual functional sites to isolate dehydrogenation and oxidation steps, and the adoption of selective oxygen species with the promotion of soft oxidants as reactants. Furthermore, the mechanistic aspects about the activation of ethane and the participation of oxygen species for tailoring the selectivity are then classified and discussed in detail. Finally, the perspectives and the emerging technologies for the ODH process are listed and evaluated.
Keyword ：
active site active site olefins olefins oxidative dehydrogenation oxidative dehydrogenation oxygen species oxygen species selectivity selectivity
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| GB/T 7714 | Chai, Yicong , Zhou, Yanliang , Lin, Sen et al. Tailoring the Olefin Selectivity in Catalytic Oxidative Dehydrogenation of Light Alkane by the Isolation Strategy [J]. | ACS CATALYSIS , 2024 , 14 (4) : 2502-2521 . |
| MLA | Chai, Yicong et al. "Tailoring the Olefin Selectivity in Catalytic Oxidative Dehydrogenation of Light Alkane by the Isolation Strategy" . | ACS CATALYSIS 14 . 4 (2024) : 2502-2521 . |
| APA | Chai, Yicong , Zhou, Yanliang , Lin, Sen , Wang, Xiaodong , Lin, Jian . Tailoring the Olefin Selectivity in Catalytic Oxidative Dehydrogenation of Light Alkane by the Isolation Strategy . | ACS CATALYSIS , 2024 , 14 (4) , 2502-2521 . |
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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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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 N-2 dissociation barrier and NHx (x = 1-3) desorption energy. Herein, we demonstrate NPM (Co, Ni, and Re)-mediated Mo2CTx MXene (where T-x 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 degrees 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 N-2 activation; thus, the rate-determining step is shifted from conventional N-2 dissociation to NH2* formation. NPM is mainly responsible for H-2 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.
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| GB/T 7714 | Zhou, Yanliang , Liang, Lili , Wang, Congying 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, Yanliang 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, Yanliang , Liang, Lili , Wang, Congying , Sun, Fuxiang , Zheng, Lirong , Qi, Haifeng 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 . |
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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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