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学者姓名：鲍晓军
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Abstract ：
Palladium-based catalysts have been intensively investigated for the hydrogenation of nitroarenes due to their high activity. However, it remains a challenge to achieve high selectivity when reducing or halo groups are present. Herein, we propose a facet engineering strategy to regulate the activity and selectivity of Pd/TiO2 and a series of Pd/TiO2 catalysts with adjustable proportions of (101) and (001) facet of TiO2 were synthesized for the selective hydrogenation of nitroarenes. With increased percentage of (101) facet, better dispersed Pd species and more oxygen vacancies (OV) can be generated on the Pd/TiO2 catalyst, thereby providing increasing hydrogenation reaction centers with strongly adsorbed nitro groups. As a result, the Pd/TiO2 with dominant (101) facet and 0.1 wt% of Pd loading (Pd/TiO2-c) delivers an outstanding conversion (100 %) of m-chloronitrobenzene, high selectivity (96.8 %) toward m-chloroaniline, and excellent reusability. In situ characterizations and density functional theory (DFT) simulation reveal that the Pd/TiO2-c exhibits much stronger adsorption toward nitro groups than chlorine group, while the catalyst with more (001) facet shows similar adsorption capability toward these two groups. Thereby, nitro group is more preferentially adsorbed and hydrogenated during the reaction on Pd/TiO2-c, which explains the excellent selectivity. Remarkably, Pd/TiO2-c can also realize excellent conversion (100 %) and selectivity (> 96 %) toward other functional nitroarenes containing −F, –OH, –CHO, –COCH2- groups. This work highlights the facet engineering of supports to tune the physicochemical properties of loaded active metal and the adsorption behavior of reactants, and provides an effective strategy for the further development of efficient Pd-based catalysts for selective nitroarenes hydrogenation. © 2024
Keyword ：
Catalyst selectivity Catalyst selectivity Hydrogenation Hydrogenation Palladium Palladium Reusability Reusability Silicon compounds Silicon compounds Sustainable development Sustainable development
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| GB/T 7714 | Liu, Zhichen , Yang, Zongxuan , Zhang, Hongwei et al. Crystal facet engineering of Pd/TiO2 to boost the activity and selectivity for nitroarenes hydrogenation [J]. | Chemical Engineering Journal , 2025 , 503 . |
| MLA | Liu, Zhichen et al. "Crystal facet engineering of Pd/TiO2 to boost the activity and selectivity for nitroarenes hydrogenation" . | Chemical Engineering Journal 503 (2025) . |
| APA | Liu, Zhichen , Yang, Zongxuan , Zhang, Hongwei , Wang, Shidong , Liu, Qunhong , Zhao, Zhengyu et al. Crystal facet engineering of Pd/TiO2 to boost the activity and selectivity for nitroarenes hydrogenation . | Chemical Engineering Journal , 2025 , 503 . |
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Water electrolysis for hydrogen production holds great promise as an energy conversion technology. The electrolysis process contains two necessary electrocatalytic reactions, one is the hydrogen evolution reaction (HER) at the cathode, and the other is the oxygen evolution reaction (OER) at the anode. In general, the kinetics of OER is much slower than that of HER, dominating the overall of performance electrolysis. As identified, the slow kinetics of catalytic OER is mainly resulted from multiple electron transfer steps, and the catalysts often undergo compositional, structural, and electronic changes during operation, leading to complicated dynamic reaction mechanisms which have not been fully understood. Obviously, this challenge presents formidable obstacles to the development of highly efficient OER electrocatalysts. To address the issue, it is crucial to unravel the origins of intrinsic OER activity and stability and elucidate the catalytic mechanisms across diverse catalyst materials. In this context, in-situ/operando characterization techniques would play a pivotal role in understanding the catalytic reaction mechanisms by enabling real-time monitoring of catalyst structures under operational conditions. These techniques can facilitate the identification of active sites for OER and provide essential insights into the types and quantities of key reaction intermediates. This comprehensive review explores various catalyst design and synthesis strategies aimed at enhancing the intrinsic OER activity and stability of catalysts and examines the application of advanced in-situ/operando techniques for probing catalyst mechanisms during the OER process. Furthermore, the imperative need for developing innovative in-situ/operando techniques, theoretical artificial intelligence and machine learning and conducting theoretical research to better understand catalyst structural evolution under conditions closely resembling practical OER working states is also deeply discussed. Those efforts should be able to lay the foundation for the improved fabrication of practical OER catalysts.
Keyword ：
Electrocatalysts Electrocatalysts In-situ techniques In-situ techniques Oxygen evolution reaction Oxygen evolution reaction Reaction mechanism Reaction mechanism
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| GB/T 7714 | Hu, Cejun , Hu, Yanfang , Zhang, Bowen et al. Advanced Catalyst Design Strategies and In-Situ Characterization Techniques for Enhancing Electrocatalytic Activity and Stability of Oxygen Evolution Reaction [J]. | ELECTROCHEMICAL ENERGY REVIEWS , 2024 , 7 (1) . |
| MLA | Hu, Cejun et al. "Advanced Catalyst Design Strategies and In-Situ Characterization Techniques for Enhancing Electrocatalytic Activity and Stability of Oxygen Evolution Reaction" . | ELECTROCHEMICAL ENERGY REVIEWS 7 . 1 (2024) . |
| APA | Hu, Cejun , Hu, Yanfang , Zhang, Bowen , Zhang, Hongwei , Bao, Xiaojun , Zhang, Jiujun et al. Advanced Catalyst Design Strategies and In-Situ Characterization Techniques for Enhancing Electrocatalytic Activity and Stability of Oxygen Evolution Reaction . | ELECTROCHEMICAL ENERGY REVIEWS , 2024 , 7 (1) . |
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Heterogeneous hydrogenation is an effective way to improve the performance of unsaturated polymers, but the preparation of supported catalysts with high metal dispersion and stability remains challenging. Herein, we synthesize a SiO2-based support wrapping with carbon nitride on the surface (CNx@SiO2) via the thermal polycondensation of melamine, on which Pd nanoclusters with highly exposed active sites are formed and stably anchored via the strong interaction between N and Pd. The thermal temperature affects the properties of CNx, which further modulates the electronic and structural state of Pd nanoclusters. The Pd/CNx @SiO2-500 catalyst, prepared at 500 degrees C with an optimal CNx structure (g-C3N4) and high nitrogen content, features highly dispersed and electron-rich Pd nanoclusters (1.3 nm). This catalyst exhibits a hydrogenation activity of 98.0% for nitrile rubber, with a selectivity of 100% for C=C bonds. This work provides a facile method to prepare Pd catalysts with high activity and stability, paving the way for the upgrading of unsaturated polymers via hydrogenation.
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| GB/T 7714 | Zhang, Kewen , Fan, Benwei , Wang, Shidong et al. Highly dispersed Pd nanoclusters anchored on CNx-modified SiO2 for selective hydrogenation of nitrile-butadiene rubber [J]. | JOURNAL OF MATERIALS SCIENCE , 2024 , 59 (46) : 21265-21276 . |
| MLA | Zhang, Kewen et al. "Highly dispersed Pd nanoclusters anchored on CNx-modified SiO2 for selective hydrogenation of nitrile-butadiene rubber" . | JOURNAL OF MATERIALS SCIENCE 59 . 46 (2024) : 21265-21276 . |
| APA | Zhang, Kewen , Fan, Benwei , Wang, Shidong , Zhang, Hongwei , Liu, Qunhong , Bao, Xiaojun et al. Highly dispersed Pd nanoclusters anchored on CNx-modified SiO2 for selective hydrogenation of nitrile-butadiene rubber . | JOURNAL OF MATERIALS SCIENCE , 2024 , 59 (46) , 21265-21276 . |
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Controllable synthesis of hierarchical zeolites from natural aluminosilicate minerals is considered an efficient and eco-friendly approach for the production of high-performance zeolites, but its synthesis mechanism is still obscure. Herein, we take the synthesis of a single-crystalline hierarchical NaA zeolite using submolten salt depolymerized kaolin (SMS-K) as the sole source of silicon and aluminum via a mesoscale reorganization strategy as an example to elucidate the reorganization process. Comprehensive morphological and structural analyses reveal that sodium-rich voids in SMS-K facilitate concurrent assembly both within the interior and at the interface of the amorphous gel, leading to the formation of numerous nanoparticles with short-range order which assemble into single-crystal nanocube NaA zeolites with intracrystalline mesopores. By harnessing confinement effects, SMS-K modulates the growth of nanoparticle sizes and enhances the intimate interconnection of nanocubes, thereby yielding NaA zeolite aggregates that exhibit hierarchical porosity, encompassing micro-, meso-, and macropores. This study offers the potential for designing and precisely controlling the fabrication of hierarchical zeolites derived from natural minerals.
Keyword ：
depolymerized kaolin depolymerized kaolin hierarchical NaA zeolite hierarchical NaA zeolite mesoscale reorganization mechanism mesoscale reorganization mechanism role of sodium and hydroxide ions role of sodium and hydroxide ions single-crystalline single-crystalline
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| GB/T 7714 | Chen, Xiaoling , Li, Tiesen , Cui, Qingyan et al. Mesoscale Reorganization of the Depolymerized Aluminosilicate into Single-Crystalline Hierarchical Zeolite [J]. | ACS APPLIED MATERIALS & INTERFACES , 2024 , 16 (44) : 61371-61380 . |
| MLA | Chen, Xiaoling et al. "Mesoscale Reorganization of the Depolymerized Aluminosilicate into Single-Crystalline Hierarchical Zeolite" . | ACS APPLIED MATERIALS & INTERFACES 16 . 44 (2024) : 61371-61380 . |
| APA | Chen, Xiaoling , Li, Tiesen , Cui, Qingyan , Shi, Jie , Tan, Yisheng , Bao, Xiaojun et al. Mesoscale Reorganization of the Depolymerized Aluminosilicate into Single-Crystalline Hierarchical Zeolite . | ACS APPLIED MATERIALS & INTERFACES , 2024 , 16 (44) , 61371-61380 . |
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Propylene is the second most important chemicals in the petrochemical industry. Propane dehydrogenation as the on -purpose propylene production route, has attracted much attentions due to great success in the exploitation of shale gas. Recently, Pt@zeolite is proven to the most promising catalyst for propane dehydrogenation, because Pt clusters encapsulated in zeolite channel show high resistance to Pt particles sintering. However, the micropore of zeolite imposes severe diffusion limitation of propylene, and thus the coke formation easily takes place which leads to a fast deactivation. Herein, we report efficient Pt/Zn-MFIhierarchical catalysts for PDH with auxiliary mesopore for accelerating mass transfer, and these Pt/Zn-MFIhierarchical exhibit not only high thermal stability but also excellent resistance to coking. The Pt/Zn-MFIhierarchical catalyst is obtained by an introduction of Pt species into the hierarchically porous Zn-MFI that is prepared from one-step hydrothermal synthesis. The formed Pt-Zn clusters are exclusively located in the micropore of MFIhierarchical, and the migrating of Pt-Zn clusters is largely prevented under the harsh reaction conditions. Mesopores in MFIhierarchical greatly enhances the diffusion rate of propylene, which significantly alleviates the coke formation arising from polymerization of propylene. The most efficient Pt/Zn-MFI-120hierarchical catalyst delivers propane conversion of around 46 % and propylene selectivity of above 98 %. This catalyst undergoes a slow loss of activity with a deactivation rate kd of as low as 0.005 h-1, and its catalytic performance can be fully restored via a simple calcination.
Keyword ：
Coking-resistance Coking-resistance Hierarchical zeolite Hierarchical zeolite Propane dehydrogenation Propane dehydrogenation Propylene production Propylene production Pt-Zn clusters Pt-Zn clusters Sintering-resistance Sintering-resistance
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| GB/T 7714 | Lu, Jinyang , Xu, Zhikang , Yue, Yuanyuan et al. Pt-Zn clusters encapsulated in hierarchical MFI zeolite for efficient propane dehydrogenation [J]. | CHEMICAL ENGINEERING JOURNAL , 2024 , 484 . |
| MLA | Lu, Jinyang et al. "Pt-Zn clusters encapsulated in hierarchical MFI zeolite for efficient propane dehydrogenation" . | CHEMICAL ENGINEERING JOURNAL 484 (2024) . |
| APA | Lu, Jinyang , Xu, Zhikang , Yue, Yuanyuan , Bao, Xiaojun , Lin, Minggui , Zhu, Haibo . Pt-Zn clusters encapsulated in hierarchical MFI zeolite for efficient propane dehydrogenation . | CHEMICAL ENGINEERING JOURNAL , 2024 , 484 . |
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热催化CO2加氢制甲醇具有显著的减碳效应,能够有效储存可再生能源,具有广阔的工业应用前景.介绍了 CO2加氢制甲醇的反应网络及其热力学挑战,并概述了其工艺流程、国内外工业应用情况,系统综述了近年来不同活性组分催化剂的研究进展,从催化剂的制备方式、活性位点、反应机理及动力学等方面阐述Cu基催化剂、贵金属催化剂、氧化物催化剂以及其他新型催化剂存在的问题和优势.重点阐述Cu基催化剂的构效关系,包括其活性组分结构、载体性质和助剂对催化活性和甲醇选择性的影响,并展望CO2加氢制甲醇催化剂的未来发展方向.
Keyword ：
CO2 CO2 催化剂 催化剂 加氢 加氢 反应动力学 反应动力学 反应机理 反应机理 甲醇 甲醇
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| GB/T 7714 | 王佳静 , 王建文 , 李茂帅 et al. CO2催化加氢合成甲醇研究进展 [J]. | 石油炼制与化工 , 2024 , 55 (2) : 75-83 . |
| MLA | 王佳静 et al. "CO2催化加氢合成甲醇研究进展" . | 石油炼制与化工 55 . 2 (2024) : 75-83 . |
| APA | 王佳静 , 王建文 , 李茂帅 , 宋奕慧 , 王石维 , 吕静 et al. CO2催化加氢合成甲醇研究进展 . | 石油炼制与化工 , 2024 , 55 (2) , 75-83 . |
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We report a facile yet effective strategy to prepare hierarchical Beta zeolite with high molecular transport effectivity in catalysis. Alkaline etching involves preferential desilication from Beta framework and collapse of microporosity. The preferential desilication from outer rim of Beta stacking faults enlarged intercrystallite mesopores, while the collapse of microporosity created cylindroid-like intracrystalline mesopore. Part of Altet with lower stability was removed during alkaline etching, leading to a decrease in acid sites density. Alkaline etching of Beta zeolite with 0.2 mol/L NaOH solution greatly improved n -hexane isomerization activity over Ptbased catalysts. The maximum yield of isohexane and dibranched isomers increased by 6.2 % and 38.6 %, respectively. The enlargement of intercrystallite mesopores and the generation of intracrystalline mesopores of Beta zeolite lowered apparent activation energy of reaction. The apparent diffusivities measurements further revealed that Pt/Beta-0.2 M showed much lower transport limitation than Pt/Beta-parent. Our findings provide a promising catalyst for industrial alkane isomerization.
Keyword ：
Alkaline etching Alkaline etching Alkane isomerization Alkane isomerization Dibranched isomers Dibranched isomers Diffusion barrier Diffusion barrier Mesoporous Beta zeolite Mesoporous Beta zeolite
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| GB/T 7714 | Wang, Pengzhao , Chen, Tingting , Qiu, Zihui et al. Pt-promoted mesoporous Beta zeolite catalysts for n-Hexane isomerization with enhanced selectivity to dibranched isomers [J]. | FUEL , 2024 , 368 . |
| MLA | Wang, Pengzhao et al. "Pt-promoted mesoporous Beta zeolite catalysts for n-Hexane isomerization with enhanced selectivity to dibranched isomers" . | FUEL 368 (2024) . |
| APA | Wang, Pengzhao , Chen, Tingting , Qiu, Zihui , Yao, Wenjun , Liu, Pengpeng , Zhang, Yongze et al. Pt-promoted mesoporous Beta zeolite catalysts for n-Hexane isomerization with enhanced selectivity to dibranched isomers . | FUEL , 2024 , 368 . |
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Cu/ZnO/Al2O3 catalysts have been widely applied as industrial catalysts for methanol synthesis from syngas, but suffers low activity for CO2 hydrogenation to methanol. This study establishes highly active Cu catalysts through modulation of the composite of Al2O3 and ZrO2 in Cu/ZnO-based catalysts. The composition of Al2O3 and ZrO2 impacts the Cu dispersion, exposed surface area of Cu, the Cu0/(Cu0+Cu+) ratio and surface basicity. An appropriate content of Al2O3 and ZrO2 presents the higher Cu surface area, desirable ratio of Cu0/(Cu0+Cu+) and moderate -strong basic sites for effective CO2 adsorption/activation, giving rise to higher space-time yield of methanol (up to 648 gCH3OH & sdot;kgcat - 1 & sdot;h- 1) than the commercial Cu catalyst. STY of methanol can be correlated with Cu surface area and Cu0/(Cu0+Cu+) ratio under the investigated conditions. The mechanistic analysis demonstrates that surface formate and methoxy species are the major intermediates. The methanol formation principally follows the formate-methoxy intermediate pathway.
Keyword ：
CO2 hydrogenation CO2 hydrogenation Cu Cu Methanol synthesis Methanol synthesis Oxide promoter Oxide promoter
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| GB/T 7714 | Wang, Jianwen , Song, Yihui , Li, Jing et al. Modulation of Al2O3 and ZrO2 composite in Cu/ZnO-based catalysts with enhanced performance for CO2 hydrogenation to methanol [J]. | APPLIED CATALYSIS A-GENERAL , 2024 , 674 . |
| MLA | Wang, Jianwen et al. "Modulation of Al2O3 and ZrO2 composite in Cu/ZnO-based catalysts with enhanced performance for CO2 hydrogenation to methanol" . | APPLIED CATALYSIS A-GENERAL 674 (2024) . |
| APA | Wang, Jianwen , Song, Yihui , Li, Jing , Liu, Fengdong , Wang, Jiajing , Lv, Jing et al. Modulation of Al2O3 and ZrO2 composite in Cu/ZnO-based catalysts with enhanced performance for CO2 hydrogenation to methanol . | APPLIED CATALYSIS A-GENERAL , 2024 , 674 . |
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Carbon adsorbents have been widely used to remove indoor volatile organic compounds (VOCs), however, the proliferation of bacteria on the carbon adsorbents may deteriorate the indoor air quality and thus pose a serious threat to human health. Herein, we report the synthesis of antibacterial porous carbon spheres (carbonized aminophenol-formaldehyde resin, CAF) with well-dispersed Cu species via an in situ incorporation of Cu2+ during the polymerization of 3-aminophenol-formaldehyde resin followed by a thermal carbonization and reduction process. Compared with CAF, the Cu/CAF-x nanocomposites with Cu loading show a much higher specific surface area (>700 m2 g−1 vs. 569 m2 g−1 for CAF). In addition, the pore size of Cu/CAF-x is ranging from 0.7 to 1.68 nm, which is exactly conducive to adsorb the toluene molecules. As a result, the toluene adsorption capacity is improved from 123.50 mg g−1 for CAF to >170 mg g−1 for Cu/CAF-x. More importantly, such adsorbents possess excellent antibacterial performance, the Cu/CAF-10 (10 wt% of Cu loading) with a concentration of 50 μg mL−1 can completely kill the E. coli within 30 min. Our work paves the way to the development of bifunctional adsorbents with both efficient VOCs adsorption and excellent antibacterial performance. © 2023
Keyword ：
Adsorption Adsorption Air quality Air quality Carbonization Carbonization Copper compounds Copper compounds Escherichia coli Escherichia coli Formaldehyde Formaldehyde Health risks Health risks Indoor air pollution Indoor air pollution Pore size Pore size Porous materials Porous materials Toluene Toluene Volatile organic compounds Volatile organic compounds
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| GB/T 7714 | Zhang, Hongwei , Wu, Guanghui , Liu, Qunhong et al. Bifunctional Cu-incorporated carbon nanospheres via in-situ complexation strategy as efficient toluene adsorbents and antibacterial agents [J]. | Chemosphere , 2024 , 349 . |
| MLA | Zhang, Hongwei et al. "Bifunctional Cu-incorporated carbon nanospheres via in-situ complexation strategy as efficient toluene adsorbents and antibacterial agents" . | Chemosphere 349 (2024) . |
| APA | Zhang, Hongwei , Wu, Guanghui , Liu, Qunhong , Liu, Zhichen , Yang, Qin , Cui, Qingyan et al. Bifunctional Cu-incorporated carbon nanospheres via in-situ complexation strategy as efficient toluene adsorbents and antibacterial agents . | Chemosphere , 2024 , 349 . |
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Defect-rich Pd/TiO2 catalysts are intensively adopted in heterogeneous hydrogenation reactions; however, the complexity of the defect structure makes it difficult to precisely identify which Pd-defect combination dominates the catalytic activity. Herein, defective TiO2 nanoflakes with tunable ratios of Vo to Ti3+ defects were synthesized and used to construct Pd-Vo and Pd-Ti3+ active sites after loading Pd to investigate the role of defects in regulating the structural and catalytic properties of defective Pd/TiO2 catalysts. Combining the experimental results and theoretical calculations, we reveal that both Vo and Ti3+ defects act as the electron donors for Pd and induce the strong metal-support interaction. When compared to the Vo defect, the Ti3+ defect behaves more significantly and donates more electrons, causing the Pd species on the catalysts to be better dispersed and more rich in electrons. These unique features endow the Pd-Ti3+ active centers with enhanced adsorption-activation ability toward C & boxH;C and H-2 as well as reduced energy barrier of the rate-limiting step, thus improving the intrinsic activity. The Pd-Ti3+ site manifests a high turnover frequency of 348 h(-1) and hydrogenation degree of 97% for hydrogenation of C & boxH;C in styrene-butadiene-styrene, which significantly outperforms the Pd-Vo site (254 h(-1) and 78%) and Pd nanoparticle (217 h(-1) and 53%). This work provides deep insight into the role of defects in regulating the properties of metal active sites, which can be used to guide the development of high-performance Pd/TiO2 catalysts for versatile applications.
Keyword ：
defective TiO2 defective TiO2 electronic structure electronic structure hydrogenation hydrogenation styrene-butadiene-styrene styrene-butadiene-styrene Ti3+-Pd site Ti3+-Pd site Vo-Pd site Vo-Pd site
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| GB/T 7714 | Wang, Shidong , Ge, Bingqing , Yang, Zongxuan et al. Construction of Highly Active Pd-Ti3+ Sites in Defective Pd/TiO2 Catalysts for Efficient Hydrogenation of Styrene-Butadiene-Styrene [J]. | ACS CATALYSIS , 2024 , 14 (3) : 1432-1442 . |
| MLA | Wang, Shidong et al. "Construction of Highly Active Pd-Ti3+ Sites in Defective Pd/TiO2 Catalysts for Efficient Hydrogenation of Styrene-Butadiene-Styrene" . | ACS CATALYSIS 14 . 3 (2024) : 1432-1442 . |
| APA | Wang, Shidong , Ge, Bingqing , Yang, Zongxuan , Zhang, Hongwei , Yang, Qin , Hu, Cejun et al. Construction of Highly Active Pd-Ti3+ Sites in Defective Pd/TiO2 Catalysts for Efficient Hydrogenation of Styrene-Butadiene-Styrene . | ACS CATALYSIS , 2024 , 14 (3) , 1432-1442 . |
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