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学者姓名：江莉龙
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Abstract ：
The electrochemical nitrogen reduction reaction (eNRR) has emerged as a promising strategy for green ammonia synthesis. However, it suffers unsatisfactory reaction performance owing to the low aqueous solubility of N-2 in aqueous solution, the high dissociation energy of N equivalent to N, and the unavoidable competing hydrogen evolution reaction (HER). Herein, a MIL-53(Fe)@TiO2 catalyst is designed and synthesized for highly efficient eNRR. Relative to simple MIL-53(Fe), MIL-53(Fe)@TiO(2 )achieves a 2-fold enhancement in the Faradaic efficiency (FE) with an improved ammonia yield rate by 76.5% at -0.1 V versus reversible hydrogen electrode (RHE). After four cycles of electrocatalysis, MIL-53(Fe)@TiO2 can maintain a good catalytic activity, while MIL-53(Fe) exhibits a significant decrease in the NH3 yield rate and FE by 79.8 and 82.3%, respectively. Benefiting from the synergetic effect between TiO2 and MIL-53(Fe) in the composites, Fe3+ ions can be greatly stabilized in MIL-53(Fe) during the eNRR process, which greatly hinders the catalyst deactivation caused by the electrochemical reduction of Fe3+ ions. Further, the charge transfer ability in the interface of composites can be improved, and thus, the eNRR activity is significantly boosted. These findings provide a promising insight into the preparation of efficient composite electrocatalysts.
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| GB/T 7714 | Sun, Zhuangzhi , Lin, Jiawei , Lu, Suwei et al. Interfacial Engineering Boosting the Activity and Stability of MIL-53(Fe) toward Electrocatalytic Nitrogen Reduction [J]. | LANGMUIR , 2024 , 40 (10) : 5469-5478 . |
| MLA | Sun, Zhuangzhi et al. "Interfacial Engineering Boosting the Activity and Stability of MIL-53(Fe) toward Electrocatalytic Nitrogen Reduction" . | LANGMUIR 40 . 10 (2024) : 5469-5478 . |
| APA | Sun, Zhuangzhi , Lin, Jiawei , Lu, Suwei , Li, Yuhang , Qi, Tingting , Peng, Xiaobo et al. Interfacial Engineering Boosting the Activity and Stability of MIL-53(Fe) toward Electrocatalytic Nitrogen Reduction . | LANGMUIR , 2024 , 40 (10) , 5469-5478 . |
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碳中和背景下,氨-氢混合无碳燃料备受关注,但合成氨与氨分解制氢过程也存在着氨-氢混合燃爆的风险.目前对氨-氢燃烧爆炸详细机理的研究不够充分,传统的详细机理十分复杂,计算耗时过长.为了研究高压下氨-氢混合气体的燃烧爆炸特性,使用零维均质模型(即不考虑空间分布且物理和化学性质均为均匀的简化模型),采用带有误差传播的有向关系图(DRGEP)法简化现有的氨-氢燃烧爆炸详细机理,再通过敏感性分析得到基元反应较少的氨-氢燃烧爆炸简化机理.将简化机理与计算流体动力学(CFD)模型耦合,开展管道内氨-氢燃烧数值模拟.结果表明,简化机理在验证层流火焰速度和点火延迟时间等方面表现出良好的性能.在爆破压力为 59.61 atm 和 69.97 atm下,平均激波速度的相对误差低于 1.4%,精度较高;且与简化机理耦合的CFD模型节约了计算资源.研究成果有助于推动氨-氢燃烧CFD模拟技术的发展,可为氨-氢混合无碳燃料的燃烧过程及爆炸防控提供理论指导.
Keyword ：
化学动力学 化学动力学 反应机理 反应机理 数值模拟 数值模拟 氨氢燃烧 氨氢燃烧 爆炸 爆炸 简化机理 简化机理
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| GB/T 7714 | 滕霖 , 单志伟 , 李西贵 et al. 基于化学反应动力学的氨-氢混合无碳燃料燃烧爆炸机理研究 [J]. | 油气与新能源 , 2024 , 36 (1) : 72-81 . |
| MLA | 滕霖 et al. "基于化学反应动力学的氨-氢混合无碳燃料燃烧爆炸机理研究" . | 油气与新能源 36 . 1 (2024) : 72-81 . |
| APA | 滕霖 , 单志伟 , 李西贵 , 李卫东 , 罗宇 , 江莉龙 . 基于化学反应动力学的氨-氢混合无碳燃料燃烧爆炸机理研究 . | 油气与新能源 , 2024 , 36 (1) , 72-81 . |
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Electrocatalytic depolymerization of lignin into value-added chemicals offers a promising technique to make biorefining sustainable.Herein,we report a robust trimetallic PdNiBi electrocatalyst for reductive C-O bond cleavage of different lignin model dimers and oxidized lignin under mild conditions.The reduction reaction proceeds with complete substrate conversion and excellent yields toward monomers of phenols(80％-99％)and acetophenones(75％-96％)in the presence of an ionic liquid electrolyte with operational stability.Systematic experimental investigations together with density functional theory(DFT)calculations reveal that the outstanding performance of the catalyst results from the synergistic effect of the metal elements,which facilitates the easier formation of a key Cα radical intermediate and the facile desorption of the as-formed products at the electrode.The results open up new opportunities for lignin valorization through the green electrocatalytic approach.
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| GB/T 7714 | Guangyong Liu , Yumiao Lu , JunFeng Lu et al. Ionic liquid-trimetallic electrocatalytic system for C-O bond cleavage in lignin model compounds and lignin under ambient conditions [J]. | 纳米研究（英文版） , 2024 , 17 (4) : 2420-2428 . |
| MLA | Guangyong Liu et al. "Ionic liquid-trimetallic electrocatalytic system for C-O bond cleavage in lignin model compounds and lignin under ambient conditions" . | 纳米研究（英文版） 17 . 4 (2024) : 2420-2428 . |
| APA | Guangyong Liu , Yumiao Lu , JunFeng Lu , Yanlei Wang , Shijing Liang , Hongyan He et al. Ionic liquid-trimetallic electrocatalytic system for C-O bond cleavage in lignin model compounds and lignin under ambient conditions . | 纳米研究（英文版） , 2024 , 17 (4) , 2420-2428 . |
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Electrocatalytic nitrate reduction reaction (NO3RR) has been capturing immense interest in the industrial application of ammonia synthesis, and it involves complex reaction routes accompanied by multi-electron transfer, thus causing a challenge to achieve high efficiency for catalysts. Herein, we customized the Cu-O-Ti-Ov (oxygen vacancy) structure on the Cu/TiO2 catalyst, identified through density functional theory (DFT) calculations as the synergic active site for NO3RR. It is found that Cu-O-Ti-Ov site facilitates the adsorption/association of NOx– and promotes the hydrogenation of NO3– to NH3 via adsorbed *H species. This effectively suppresses the competing hydrogen evolution reaction (HER) and exhibits a lower reaction energy barrier for NO3RR, with the reaction pathways: NO3* → NO2* → HONO* → NO* → *NOH → *N → *NH → *NH2 → *NH3 → NH3. The optimized Cu/TiO2 catalyst with rich Cu-O-Ti-Ov sites achieves an NH3 yield rate of 3046.5 μg h–1 mgcat–1 at –1.0 V vs. RHE, outperforming most of the reported activities. Furthermore, the construction of Cu-O-Ti-Ov sites significantly mitigates the leaching of Cu species, enhancing the stability of the Cu/TiO2 catalyst. Additionally, a mechanistic study, using in situ characterizations and various comparative experiments, further confirms the strong synergy between Cu, Ti, and Ov sites, which is consistent with previous DFT calculations. This study provides a new strategy for designing efficient and stable electrocatalysts in the field of ammonia synthesis. © 2024 Dalian Institute of Chemical Physics, the Chinese Academy of Sciences
Keyword ：
Ammonia Ammonia Catalyst activity Catalyst activity Copper compounds Copper compounds Density functional theory Density functional theory Electrocatalysts Electrocatalysts Kinetic theory Kinetic theory Nitrates Nitrates Nitrogen oxides Nitrogen oxides Selective catalytic reduction Selective catalytic reduction Titanium compounds Titanium compounds
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| GB/T 7714 | Nie, Yifei , Yan, Hongping , Lu, Suwei et al. Theory-guided construction of Cu-O-Ti-Ov active sites on Cu/TiO2 catalysts for efficient electrocatalytic nitrate reduction [J]. | Chinese Journal of Catalysis , 2024 , 59 : 293-302 . |
| MLA | Nie, Yifei et al. "Theory-guided construction of Cu-O-Ti-Ov active sites on Cu/TiO2 catalysts for efficient electrocatalytic nitrate reduction" . | Chinese Journal of Catalysis 59 (2024) : 293-302 . |
| APA | Nie, Yifei , Yan, Hongping , Lu, Suwei , Zhang, Hongwei , Qi, Tingting , Liang, Shijing et al. Theory-guided construction of Cu-O-Ti-Ov active sites on Cu/TiO2 catalysts for efficient electrocatalytic nitrate reduction . | Chinese Journal of Catalysis , 2024 , 59 , 293-302 . |
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The ammonia decomposition for the production of carbon-free hydrogen has triggered great attention yet still remains challenging due to its sluggish kinetics, posting the importance of precise design of efficient catalysts for ammonia decomposition under low temperatures. Constructing the metal-support interaction and interface is one of the most important strategies for promoting catalysts. In this work, by coating ceria onto the Ni nanoparticles (NPs), we discover that the Ni-CeO2 interfaces create an exceptional effect to enhance the catalytic decomposition of ammonia by over 10 folds, compared with the pristine Ni. The kinetic analysis demonstrates that the recombinative N2 desorption is the rate-determining step (RDS) and the Ni-CeO2 interface greatly increases the RDS. Based on these understandings, a strategy to fabricate the Ni/CeO2 catalyst with abundant Ni-Ce-O interfaces via one-pot sol-gel method was employed (hereafter denoted to s-Ni/CeO2). The s-Ni/CeO2 catalyst shows a high activity for ammonia decomposition, achieving a H2 formation rate of 10.5 mmol gcat-1 min-1 at 550 degrees C. Combined with a series of characterizations, the relationship between the catalyst structure and the performance was investigated for further understanding the effect of metal-oxide interfaces.
Keyword ：
Ammonia decomposition Ammonia decomposition Cerium oxide Cerium oxide Metal -oxide interfaces Metal -oxide interfaces Metal-support interaction Metal-support interaction Nickel Nickel
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| GB/T 7714 | Chen, Jiangping , Ren, Hongju , Wu, Kai et al. Boosting hydrogen production of ammonia decomposition via the construction of metal-oxide interfaces [J]. | CHINESE JOURNAL OF STRUCTURAL CHEMISTRY , 2024 , 43 (2) . |
| MLA | Chen, Jiangping et al. "Boosting hydrogen production of ammonia decomposition via the construction of metal-oxide interfaces" . | CHINESE JOURNAL OF STRUCTURAL CHEMISTRY 43 . 2 (2024) . |
| APA | Chen, Jiangping , Ren, Hongju , Wu, Kai , Fang, Huihuang , Chen, Chongqi , Lin, Li et al. Boosting hydrogen production of ammonia decomposition via the construction of metal-oxide interfaces . | CHINESE JOURNAL OF STRUCTURAL CHEMISTRY , 2024 , 43 (2) . |
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【目的】绿氨作为氢能的优质载体，生产工艺无碳化的优势使其成为实现碳中和目标的备选能源之一，因此绿氨终端站的布局与建设对促进氢能产业链的快速发展具有重要作用，有利于推动社会能源结构的绿色转型。【方法】概述了氨的性质：氨作为高效的储能与储氢介质，具有高能量密度、易储运、终端站无碳排放、安全性高等特点，能够显著降低储氢、运氢、用氢的成本，并可提高能源安全性。分析了氨用于储氢与储能介质具有的能量密度高、安全、长时储能等优势，调研了全球多国的氨氢项目发展与贸易情况，论述了全球快速增长的绿氨产能及需求，总结了目前氨能的贸易现状与终端站建设情况；对比目前成熟的LNG接收站相关工艺技术，详细介绍了绿氨终端站的关键工艺及技术，包括终端站绿氨存储工艺系统、液氨蒸发气处理工艺系统、终端站加注及卸载工艺系统。【结果】提出绿氨终端站的安全性问题，深入剖析了终端站液氨泄漏导致的毒性、燃烧爆炸性等危害，并给出了预防及防护措施。【结论】从化肥行业到能源领域，绿氨终端站技术的研究与发展对促进绿色能源氢能的利用具有重要意义，未来绿氨终端站的数量与规模将持续增加以适应新时代的需求，同时可以考虑改造LNG接收站等大宗能源及化工品储运设施以降低成本。（图5，表3，参59）
Keyword ：
储氢载体 储氢载体 接收工艺 接收工艺 接收终端 接收终端 液氨泄漏 液氨泄漏 碳中和 碳中和 绿氢 绿氢 绿氨 绿氨 绿色能源 绿色能源
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| GB/T 7714 | 滕霖 , 林崴 , 尹鹏博 et al. 碳中和目标下绿氨终端站储运技术发展现状及趋势 [J]. | 油气储运 , 2024 , 43 (01) : 1-11 . |
| MLA | 滕霖 et al. "碳中和目标下绿氨终端站储运技术发展现状及趋势" . | 油气储运 43 . 01 (2024) : 1-11 . |
| APA | 滕霖 , 林崴 , 尹鹏博 , 李卫东 , 黄鑫 , 李加庆 et al. 碳中和目标下绿氨终端站储运技术发展现状及趋势 . | 油气储运 , 2024 , 43 (01) , 1-11 . |
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【目的】在“双碳”背景下，氨作为无碳富氢的能源载体，体积能量密度高、易液化存储，具有广阔的发展前景。然而复杂的储运环境增加了液氨储罐和管道腐蚀的风险，因此，研究复杂输送环境下液氨腐蚀问题是“氨-氢”能源基础设施制造和安全服役的关键。【方法】通过综述液氨腐蚀的研究进展，探讨了不同环境、不同材料的氨腐蚀行为和应力腐蚀开裂机制。同时，总结了相关氨腐蚀检测方法和具体防护措施，并展望了未来氨腐蚀研究的发展方向。【结果】氧气、碳氧化合物、硫化物及氯化物的混入对氨腐蚀有促进作用，而水杂质对氨腐蚀的影响具有两面性；应力能够引起液氨应力腐蚀开裂，不同材料的应力腐蚀敏感性从大到小依次为铜及其合金、高强钢、碳钢。【结论】基于国内对液氨腐蚀行为机理尚不明确、氨腐蚀防护措施有待完善等问题，提出以下建议：(1)采用实验研究、仿真模拟等方法，探究多杂质关联作用下不同材质的液氨腐蚀行为和内在腐蚀机理；(2)需结合液氨管道实际输送环境及材料失效特征，开展管线钢及焊材-液氨临界失效边界检验与腐蚀风险评价；(3)从液氨储罐及管道的设计、选材、制造、使用等多个角度，结合多种腐蚀防腐措施，形成完善的液氨储运系统腐蚀控制、防护及评价标准体系。（图5，表2，参77）
Keyword ：
应力腐蚀 应力腐蚀 液氨储运 液氨储运 环境腐蚀 环境腐蚀 腐蚀检测 腐蚀检测 防护技术 防护技术
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| GB/T 7714 | 李加庆 , 冯智雨 , 梁辉龙 et al. 复杂输送环境下液氨腐蚀行为及防护技术研究进展 [J]. | 油气储运 , 2024 , 43 (02) : 121-133,162 . |
| MLA | 李加庆 et al. "复杂输送环境下液氨腐蚀行为及防护技术研究进展" . | 油气储运 43 . 02 (2024) : 121-133,162 . |
| APA | 李加庆 , 冯智雨 , 梁辉龙 , 尹鹏博 , 滕霖 , 陈崇启 et al. 复杂输送环境下液氨腐蚀行为及防护技术研究进展 . | 油气储运 , 2024 , 43 (02) , 121-133,162 . |
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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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Selective adsorption of sulfur dioxide (SO2) is an important clean technology for purification of exhaust gas from fossil fuel combustion. The widely applied zeolite-based adsorbents interact with SO2 through weakly physical adsorption, resulting in low adsorption capacity and selectivity for SO2. Herein, a facile strategy that combines improving the textural property of zeolite and optimizing adsorption sites is developed for efficient and stable SO2 adsorption. The micro-mesoporous silica sphere (MS) with high specific surface area and well-defined pore structure is obtained through a micelle expander assisted soft-template method, which can facilitate the dispersion and exposure of designed adsorption sites- methylated polyethyleneimine (mPEI). Since the Lewis basic sites of N in mPEI can strongly interact with the pi-receptor SO2, and the tertiary amine groups exhibit a weak attraction for CO2, the optimized MS supported mPEI adsorbent exhibits remarkable SO2 adsorption performance (7.5 mmol/g), exceptionally high SO2/N2 selectivity (16673) and SO2/CO2 selectivity (551). Moreover, it presents an outstanding stability in the adsorption-regeneration test. This work sheds light on the design of high-performance organic-solid composite adsorbent for selective capture of SO2.
Keyword ：
Adsorption Adsorption Micro-mesoporous silica sphere Micro-mesoporous silica sphere Polytertiary amine Polytertiary amine Selective desulfurization Selective desulfurization SO 2 capture SO 2 capture
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| GB/T 7714 | Zhang, Qiongdan , Wei, Jixiang , Gao, Changbo et al. Highly selective capture of SO2 with supported micro-mesoporous silica sphere from CO2-rich environment [J]. | JOURNAL OF CLEANER PRODUCTION , 2024 , 436 . |
| MLA | Zhang, Qiongdan et al. "Highly selective capture of SO2 with supported micro-mesoporous silica sphere from CO2-rich environment" . | JOURNAL OF CLEANER PRODUCTION 436 (2024) . |
| APA | Zhang, Qiongdan , Wei, Jixiang , Gao, Changbo , Zheng, Yong , Xiao, Yihong , Liu, Fujian et al. Highly selective capture of SO2 with supported micro-mesoporous silica sphere from CO2-rich environment . | JOURNAL OF CLEANER PRODUCTION , 2024 , 436 . |
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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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