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学者姓名：袁珮
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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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C9石油树脂(C9PR)是由乙烯裂解副产物C9馏分聚合而成的热塑性树脂,经加氢改性后可以制得色度浅、抗氧化稳定性高、相容性好的高附加值氢化石油树脂(HC9PR).但C9PR分子量大、空间位阻高且原料中含有硫化物等杂质易使催化剂中毒失活,因此加氢难度极大.为了同时实现C9PR的加氢和脱杂,采用化学还原法结合球磨法制备了非晶态NiP@γ-Al2O3催化剂.表征结果显示,该催化剂具有较大的比表面积、富含Niδ+活性物种、较多的活性位数量,并对C＝C键具有较强的吸附能力.对其进行C9PR加氢性能评价,结果显示非晶态NiP@γ-Al2O3催化剂表现出优异的加氢活性(加氢度98.35％)和脱硫活性(硫含量从122.80 μg/g降低至8.00 μg/g),明显优于利用程序升温还原法结合球磨法制备的不同晶型磷化镍催化剂.此外,经过连续100 h的反应,该催化剂仍能保持较高的加氢度,表明其具有良好的稳定性.
Keyword ：
加氢 加氢 球磨法 球磨法 石油树脂 石油树脂 脱硫 脱硫 非晶态磷化镍 非晶态磷化镍
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| GB/T 7714 | 胡德政 , 王榕 , 王世栋 et al. 兼具加氢和脱硫活性的富含Niδ+非晶态NiP@γ-Al2O3催化剂的构筑及其用于石油树脂加氢的性能研究 [J]. | 化工学报 , 2024 , 75 (9) : 3152-3162 . |
| MLA | 胡德政 et al. "兼具加氢和脱硫活性的富含Niδ+非晶态NiP@γ-Al2O3催化剂的构筑及其用于石油树脂加氢的性能研究" . | 化工学报 75 . 9 (2024) : 3152-3162 . |
| APA | 胡德政 , 王榕 , 王世栋 , 杨文菲 , 张宏伟 , 袁珮 . 兼具加氢和脱硫活性的富含Niδ+非晶态NiP@γ-Al2O3催化剂的构筑及其用于石油树脂加氢的性能研究 . | 化工学报 , 2024 , 75 (9) , 3152-3162 . |
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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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Lignin is continuously investigated by various techniques for valorization due to its high content of oxygencontaining functional groups. Catalytic systems employing hydrolysis-hydrogenolysis, leveraging the synergistic effect of redox metal sites and acid sites, exhibit efficient degradation of lignin. The predominance of either hydrolysis or hydrogenolysis reactions hinges upon the relative activity of acid and metal sites, as well as the intensity of the reductive atmosphere. In this study, the Pd-MoOx/TiO2 catalyst was found to primarily catalyze hydrolysis in the lignin depolymerization process, attributed to the abundance of moderate acidic sites on Pd and the redox-assisted catalysis of MoOx under inert conditions. After subjecting the reaction to 240 degrees C for 30 h, a yield of 48.22 wt% of total phenolic monomers, with 5.90 wt% consisting of diphenols, was achieved. Investigation into the conversion of 4-propylguaiacol (4-PG), a major depolymerized monomer of corncob lignin, revealed the production of ketone intermediates, a phenomenon closely linked to the unique properties of MoOx. Dehydrogenation of the propyl is a key step in initiating the reaction, and 4-PG could be almost completely transformed, accompanied by an over 97 % of 4-propylcatechol selectivity. This distinctive system lays a new theoretical groundwork for the eco-friendly valorization of lignin.
Keyword ：
4-Propylguaiacol 4-Propylguaiacol Hydrogen-free Hydrogen-free Hydrogenolysis Hydrogenolysis Hydrolysis Hydrolysis Ketone Ketone Lignin Lignin
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| GB/T 7714 | Tang, Daobin , Lin, Xuebin , Zhang, Qi et al. Hydrolysis-dominated catalytic system: Hydrogen-free hydrogenolysis of lignin from Pd-MoO x /TiO 2 [J]. | INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES , 2024 , 267 . |
| MLA | Tang, Daobin et al. "Hydrolysis-dominated catalytic system: Hydrogen-free hydrogenolysis of lignin from Pd-MoO x /TiO 2" . | INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES 267 (2024) . |
| APA | Tang, Daobin , Lin, Xuebin , Zhang, Qi , Wang, Zhenni , Liu, Yuhang , Jin, Yanqiao et al. Hydrolysis-dominated catalytic system: Hydrogen-free hydrogenolysis of lignin from Pd-MoO x /TiO 2 . | INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES , 2024 , 267 . |
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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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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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Nanoscale defects can induce the effective modulation of carrier concentration, mobility, and phonon scattering to secure high thermoelectric performance in semiconductors. However, it is still limited to effectively controlling nanoscale defects in thermoelectric materials. Here, argon plasma bombardment is employed to introduce a large number of point defects and dislocations in microcrystalline SnSe powders, synthesized by a solvothermal method. After sintering these powders into polycrystalline bulk materials, bulk SnSe shows the ZT increasing by up to 66.7% (from 0.36 to 0.6 at 773 K). Through detailed micro/nanostructure characterizations and first-principles calculations, the underlying mechanism is elucidated for the evaluation of thermoelectric performance. This work provides a deep understanding of the mechanism of nanoscale defects in modulating thermoelectric performance and presents experimental evidence and experience for the design and synthesis of efficient thermoelectric materials, making significant contributions to future green energy technologies. Argon plasma is utilized to induce Sn vacancy defects in SnSe powders, enhancing ZT by 66.7% after sintering into bulk materials. Micro/nanostructure analyses and first-principles calculations elucidate the mechanism, advancing thermoelectric understanding. The findings offer insight into defect modulation for efficient thermoelectric materials, vital for future green energy technologies. image
Keyword ：
Ar plasma bombardment Ar plasma bombardment polycrystal polycrystal SnSe SnSe thermoelectric thermoelectric vacancy vacancy
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| GB/T 7714 | Wu, Chunlu , Shi, Xiao-Lei , Li, Meng et al. Argon Plasma Bombardment Induces Surface-Rich Sn Vacancy Defects to Enhance the Thermoelectric Performance of Polycrystalline SnSe [J]. | ADVANCED FUNCTIONAL MATERIALS , 2024 , 34 (37) . |
| MLA | Wu, Chunlu et al. "Argon Plasma Bombardment Induces Surface-Rich Sn Vacancy Defects to Enhance the Thermoelectric Performance of Polycrystalline SnSe" . | ADVANCED FUNCTIONAL MATERIALS 34 . 37 (2024) . |
| APA | Wu, Chunlu , Shi, Xiao-Lei , Li, Meng , Zheng, Zhuanghao , Zhu, Liangkui , Huang, Keke et al. Argon Plasma Bombardment Induces Surface-Rich Sn Vacancy Defects to Enhance the Thermoelectric Performance of Polycrystalline SnSe . | ADVANCED FUNCTIONAL MATERIALS , 2024 , 34 (37) . |
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Electrocatalytic oxidation as a promising route to produce value-added products from biomass-derived organics has received increasing attention in recent years. However, the efficient conversion of concentrated feedstock solutions with high selectivity and Faradaic efficiency (FE) remains challenging. Herein, we report a cation-defective Ni-based electrocatalyst derived from the surface reconstruction of the NiCo Prussian blue analogue (NiCo PBA) in alkaline media for the efficient oxidation of biomass-derived organics in a high concentration solution. Taking 5-hydroxymethylfurfural (HMF) as an example, the NiCo PBA can deliver a satisfactory catalytic performance in terms of high HMF conversion (97%), selectivity to 2,5-furandicarboxylic acid (98%), and FE (100%), even at a concentration as high as 100 mM. Theoretical calculations suggest that the cation defects not only promote the fast conversion of Ni(OH)(2) to electrochemically active NiOOH under anodic potential but also enhance the adsorption of HMF onto the active sites and accelerate the spontaneous chemical oxidation. This study provides deep insights into the structural evolution of PBA-based catalysts and reveals the pivotal factor that affects the performance of electrocatalytic oxidation, paving the way to further develop advanced electrocatalysts for efficient oxidation reactions with a high concentration.
Keyword ：
biomass upgrade biomass upgrade cation defects cation defects electrooxidation electrooxidation operandoRaman spectroscopies operandoRaman spectroscopies Prussian blue analogues catalysts Prussian blue analogues catalysts
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| GB/T 7714 | Zhang, Hongwei , Yang, Qin , Luo, Shuting et al. On the Activity and Selectivity of 5-Hydroxymethylfurfural Electrocatalytic Oxidation over Cation-Defective Nickel Hydroxides [J]. | ACS CATALYSIS , 2024 , 14 (12) : 9565-9574 . |
| MLA | Zhang, Hongwei et al. "On the Activity and Selectivity of 5-Hydroxymethylfurfural Electrocatalytic Oxidation over Cation-Defective Nickel Hydroxides" . | ACS CATALYSIS 14 . 12 (2024) : 9565-9574 . |
| APA | Zhang, Hongwei , Yang, Qin , Luo, Shuting , Liu, Zhichen , Huang, Jinming , Zheng, Yun et al. On the Activity and Selectivity of 5-Hydroxymethylfurfural Electrocatalytic Oxidation over Cation-Defective Nickel Hydroxides . | ACS CATALYSIS , 2024 , 14 (12) , 9565-9574 . |
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Optimizing the local electronic structure of electrocatalysts can effectively lower the energy barrier of electrochemical reactions, thus enhancing the electrocatalytic activity. However, the intrinsic contribution of the electronic effect is still experimentally unclear. In this work, the electron injection-incomplete discharge approach to achieve the electron accumulation (EA) degree on the nickel-iron layered double hydroxide (NiFe LDH) is proposed, to reveal the intrinsic contribution of EA toward oxygen evolution reaction (OER). Such NiFe LDH with EA effect results in only 262 mV overpotential to reach 50 mA cm-2, which is 51 mV-lower compared with pristine NiFe LDH (313 mV), and reduced Tafel slope of 54.8 mV dec-1 than NiFe LDH (107.5 mV dec-1). Spectroscopy characterizations combined with theoretical calculations confirm that the EA near concomitant Vo can induce a narrower energy gap and lower thermodynamic barrier to enhance OER performance. This study clarifies the mechanism of the EA effect on OER activity, providing a direct electronic structure modulation guideline for effective electrocatalyst design. The electron accumulation (EA) on the NiFe LDH can modulate the electronic structure directly to enhance the OER performance. Spectroscopy and theoretical calculations confirm EA near concomitant Vo narrows the energy gap and reduces the thermodynamic barrier. This study clarifies the effect of EA on OER activity and provides an electron injection-incomplete discharging approach for effective electrocatalyst design. image
Keyword ：
electron accumulation (EA) electron accumulation (EA) electronic effect electronic effect oxygen evolution reaction oxygen evolution reaction oxygen vacancies oxygen vacancies
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| GB/T 7714 | Zhang, Rongrong , Han, Yun , Wu, Qilong et al. Electron Accumulation Induced by Electron Injection-Incomplete Discharge on NiFe LDH for Enhanced Oxygen Evolution Reaction [J]. | SMALL , 2024 , 20 (34) . |
| MLA | Zhang, Rongrong et al. "Electron Accumulation Induced by Electron Injection-Incomplete Discharge on NiFe LDH for Enhanced Oxygen Evolution Reaction" . | SMALL 20 . 34 (2024) . |
| APA | Zhang, Rongrong , Han, Yun , Wu, Qilong , Lu, Min , Liu, Guangsheng , Guo, Zhangtao et al. Electron Accumulation Induced by Electron Injection-Incomplete Discharge on NiFe LDH for Enhanced Oxygen Evolution Reaction . | SMALL , 2024 , 20 (34) . |
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