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学者姓名:袁珮

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Electron Accumulation Induced by Electron Injection-Incomplete Discharge on NiFe LDH for Enhanced Oxygen Evolution Reaction SCIE
期刊论文 | 2024 , 20 (34) | SMALL
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Abstract :

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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Argon Plasma Bombardment Induces Surface-Rich Sn Vacancy Defects to Enhance the Thermoelectric Performance of Polycrystalline SnSe SCIE
期刊论文 | 2024 , 34 (37) | ADVANCED FUNCTIONAL MATERIALS
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Abstract :

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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Argon Plasma Bombardment Induces Surface-Rich Sn Vacancy Defects to Enhance the Thermoelectric Performance of Polycrystalline SnSe EI
期刊论文 | 2024 , 34 (37) | Advanced Functional Materials
Argon Plasma Bombardment Induces Surface-Rich Sn Vacancy Defects to Enhance the Thermoelectric Performance of Polycrystalline SnSe Scopus
期刊论文 | 2024 , 34 (37) | Advanced Functional Materials
Strengthening the Synergy between Oxygen Vacancies in Electrocatalysts for Efficient Glycerol Electrooxidation SCIE
期刊论文 | 2024 , 36 (26) | ADVANCED MATERIALS
WoS CC Cited Count: 2
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Abstract :

Defect-engineered bimetallic oxides exhibit high potential for the electrolysis of small organic molecules. However, the ambiguity in the relationship between the defect density and electrocatalytic performance makes it challenging to control the final products of multi-step multi-electron reactions in such electrocatalytic systems. In this study, controllable kinetics reduction is used to maximize the oxygen vacancy density of a CuCo oxide nanosheet (CuCo2O4 NS), which is used to catalyze the glycerol electrooxidation reaction (GOR). The CuCo2O4-x NS with the highest oxygen-vacancy density (CuCo2O4-x-2) oxidizes C3 molecules to C1 molecules with selectivity of almost 100% and a Faradaic efficiency of approximate to 99%, showing the best oxidation performance among all the modified catalysts. Systems with multiple oxygen vacancies in close proximity to each other synergistically facilitate the cleavage of CC bonds. Density functional theory calculations confirm the ability of closely spaced oxygen vacancies to facilitate charge transfer between the catalyst and several key glycolic-acid (GCA) intermediates of the GOR process, thereby facilitating the decomposition of C2 intermediates to C1 molecules. This study reveals qualitatively in tuning the density of oxygen vacancies for altering the reaction pathway of GOR by the synergistic effects of spatial proximity of high-density oxygen vacancies. In this work, the qualitative tuning of oxygen-vacancy density on the reaction pathway of glycerol electrooxidation (GOR) is investigated, demonstrating that the synergistic effect induced by neighboring oxygen vacancies effectively promotes the CC bond cleavage of C2 intermediates to formate. This work offers insights for designing high-performance GOR electrocatalysts, facilitating the development of cost-effective and energy-saving chemical production technologies. image

Keyword :

defect density defect density glycerol oxidation reaction glycerol oxidation reaction nitrobenzene reduction reaction nitrobenzene reduction reaction oxygen vacancy oxygen vacancy synergistic effect synergistic effect

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GB/T 7714 Wu, Liyun , Wu, Qilong , Han, Yun et al. Strengthening the Synergy between Oxygen Vacancies in Electrocatalysts for Efficient Glycerol Electrooxidation [J]. | ADVANCED MATERIALS , 2024 , 36 (26) .
MLA Wu, Liyun et al. "Strengthening the Synergy between Oxygen Vacancies in Electrocatalysts for Efficient Glycerol Electrooxidation" . | ADVANCED MATERIALS 36 . 26 (2024) .
APA Wu, Liyun , Wu, Qilong , Han, Yun , Zhang, Dongdong , Zhang, Rongrong , Song, Nan et al. Strengthening the Synergy between Oxygen Vacancies in Electrocatalysts for Efficient Glycerol Electrooxidation . | ADVANCED MATERIALS , 2024 , 36 (26) .
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Strengthening the Synergy between Oxygen Vacancies in Electrocatalysts for Efficient Glycerol Electrooxidation
期刊论文 | 2024 , 36 (26) , n/a-n/a | Advanced Materials
Strengthening the Synergy between Oxygen Vacancies in Electrocatalysts for Efficient Glycerol Electrooxidation EI
期刊论文 | 2024 , 36 (26) | Advanced Materials
Strengthening the Synergy between Oxygen Vacancies in Electrocatalysts for Efficient Glycerol Electrooxidation Scopus
期刊论文 | 2024 , 36 (26) | Advanced Materials
Bifunctional Cu-incorporated carbon nanospheres via in-situ complexation strategy as efficient toluene adsorbents and antibacterial agents EI
期刊论文 | 2024 , 349 | Chemosphere
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Abstract :

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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Bifunctional Cu-incorporated carbon nanospheres via in-situ complexation strategy as efficient toluene adsorbents and antibacterial agents Scopus
期刊论文 | 2024 , 349 | Chemosphere
Construction of Highly Active Pd-Ti3+ Sites in Defective Pd/TiO2 Catalysts for Efficient Hydrogenation of Styrene-Butadiene-Styrene SCIE
期刊论文 | 2024 , 14 (3) , 1432-1442 | ACS CATALYSIS
WoS CC Cited Count: 2
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Abstract :

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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Construction of Highly Active Pd-Ti3+ Sites in Defective Pd/TiO2 Catalysts for Efficient Hydrogenation of Styrene-Butadiene-Styrene Scopus
期刊论文 | 2024 , 14 (3) , 1432-1442 | ACS Catalysis
Construction of Highly Active Pd-Ti3+ Sites in Defective Pd/TiO2 Catalysts for Efficient Hydrogenation of Styrene-Butadiene-Styrene EI
期刊论文 | 2024 , 14 (3) , 1432-1442 | ACS Catalysis
On the Activity and Selectivity of 5-Hydroxymethylfurfural Electrocatalytic Oxidation over Cation-Defective Nickel Hydroxides SCIE
期刊论文 | 2024 , 14 (12) , 9565-9574 | ACS CATALYSIS
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Abstract :

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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On the Activity and Selectivity of 5-Hydroxymethylfurfural Electrocatalytic Oxidation over Cation-Defective Nickel Hydroxides EI
期刊论文 | 2024 , 14 (12) , 9565-9574 | ACS Catalysis
On the Activity and Selectivity of 5-Hydroxymethylfurfural Electrocatalytic Oxidation over Cation-Defective Nickel Hydroxides Scopus
期刊论文 | 2024 , 14 (12) , 9565-9574 | ACS Catalysis
Advanced Catalyst Design Strategies and In-Situ Characterization Techniques for Enhancing Electrocatalytic Activity and Stability of Oxygen Evolution Reaction SCIE
期刊论文 | 2024 , 7 (1) | ELECTROCHEMICAL ENERGY REVIEWS
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Abstract :

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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Advanced Catalyst Design Strategies and In-Situ Characterization Techniques for Enhancing Electrocatalytic Activity and Stability of Oxygen Evolution Reaction EI CSCD
期刊论文 | 2024 , 7 (1) | Electrochemical Energy Reviews
Advanced Catalyst Design Strategies and In-Situ Characterization Techniques for Enhancing Electrocatalytic Activity and Stability of Oxygen Evolution Reaction Scopus CSCD
期刊论文 | 2024 , 7 (1) | Electrochemical Energy Reviews
Hydrolysis-dominated catalytic system: Hydrogen-free hydrogenolysis of lignin from Pd-MoO x /TiO 2 SCIE
期刊论文 | 2024 , 267 | INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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Abstract :

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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Hydrolysis-dominated catalytic system: Hydrogen-free hydrogenolysis of lignin from Pd-MoOx/TiO2 EI
期刊论文 | 2024 , 267 | International Journal of Biological Macromolecules
Hydrolysis-dominated catalytic system: Hydrogen-free hydrogenolysis of lignin from Pd-MoOx/TiO2 Scopus
期刊论文 | 2024 , 267 | International Journal of Biological Macromolecules
Advances in enhancing hydrodeoxygenation selectivity of lignin-derived oxygenates: From synthetic strategies to fundamental techniques Scopus CSCD
期刊论文 | 2024 | Green Energy and Environment
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Abstract :

In recent years, studies focusing on the conversion of renewable lignin-derived oxygenates (LDOs) have emphasized their potential as alternatives to fossil-based products. However, LDOs, existing as complex aromatic mixtures with diverse oxygen-containing functional groups, pose a challenge as they cannot be easily separated via distillation for direct utilization. A promising solution to this challenge lies in the efficient removal of oxygen-containing functional groups from LDOs through hydrodeoxygenation (HDO), aiming to yield biomass products with singular components. However, the high dissociation energy of the carbon–oxygen bond, coupled with its similarity to the hydrogenation energy of the benzene ring, creates a competition between deoxygenation and benzene ring hydrogenation. Considering hydrogen consumption and lignin properties, the preference is directed towards generating aromatic hydrocarbons rather than saturated components. Thus, the goal is to selectively remove oxygen-containing functional groups while preserving the benzene ring structure. Studies on LDOs conversion have indicated that the design of active components and optimization of reaction conditions play pivotal roles in achieving selective deoxygenation, but a summary of the correlation between these factors and the reaction mechanism is lacking. This review addresses this gap in knowledge by firstly summarizing the various reaction pathways for HDO of LDOs. It explores the impact of catalyst design strategies, including morphology modulation, elemental doping, and surface modification, on the adsorption–desorption dynamics between reactants and catalysts. Secondly, we delve into the application of advanced techniques such as spectroscopic techniques and computational modeling, aiding in uncovering the true active sites in HDO reactions and understanding the interaction of reactive reactants with catalyst surface-interfaces. Additionally, fundamental insights into selective deoxygenation obtained through these techniques are highlighted. Finally, we outline the challenges that lie ahead in the design of highly active and selective HDO catalysts. These challenges include the development of detection tools for reactive species with high activity at low concentrations, the study of reaction medium–catalyst interactions, and the development of theoretical models that more closely approximate real reaction situations. Addressing these challenges will pave the way for the development of efficient and selective HDO catalysts, thus advancing the field of renewable LDOs conversion. © 2024 Institute of Process Engineering, Chinese Academy of Sciences

Keyword :

Catalyst design Catalyst design Hydrodeoxygenation Hydrodeoxygenation Lignin-derived oxygenates Lignin-derived oxygenates Targeted deoxidation Targeted deoxidation Techniques and theoretical calculation Techniques and theoretical calculation

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GB/T 7714 Wu, X. , Zhang, H. , Hu, C. et al. Advances in enhancing hydrodeoxygenation selectivity of lignin-derived oxygenates: From synthetic strategies to fundamental techniques [J]. | Green Energy and Environment , 2024 .
MLA Wu, X. et al. "Advances in enhancing hydrodeoxygenation selectivity of lignin-derived oxygenates: From synthetic strategies to fundamental techniques" . | Green Energy and Environment (2024) .
APA Wu, X. , Zhang, H. , Hu, C. , Bao, X. , Yuan, P. . Advances in enhancing hydrodeoxygenation selectivity of lignin-derived oxygenates: From synthetic strategies to fundamental techniques . | Green Energy and Environment , 2024 .
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氮化碳负载钯催化剂的制备及对SBS选择性催化加氢性能的研究 CSCD PKU
期刊论文 | 2023 , 74 (2) , 766-775 | 化工学报
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Abstract :

苯乙烯-丁二烯-苯乙烯嵌段共聚物(SBS)选择性催化加氢是保留链段中苯环不被加氢而C=C双键选择性加氢,从而得到具有更优异性能的高附加值氢化产物SEBS.为了消除反应物大分子孔内扩散限制问题,采用胶体SiO2亚微米球为模板,通过氰胺热缩合成功合成了三维有序超大孔氮化碳(3DOM g-C3N4),以其为载体采用化学还原负载法得到了具有超大孔结构的Pd/3DOM g-C3N4催化剂,并将其用于SBS的选择性催化加氢反应.结果表明,Pd/3DOM g-C3N4催化剂具有超大孔-大孔-介孔多级孔三维贯穿结构且Pd颗粒尺寸小、分散均匀,该催化剂在较为温和的反应条件下,即表现出极为优异的加氢活性和选择性.根据红外表征计算得到其对SBS的1,2-C=C和1,4-C=C总加氢度达到98%,而对苯环没有加氢,选择性为100%.其优异的催化性能主要归功于载体独特的超大孔-大孔-介孔多级孔三维贯穿结构可以有效消除大分子在孔隙中的扩散限制,从而提高了对活性位点的可接近性;Pd和载体氮化碳中的吡啶N之间存在强相互作用,有利于Pd的锚定,进而获得颗粒尺寸小且分散度和稳定性高的Pd纳米颗粒.

Keyword :

g-C3N4 g-C3N4 SBS SBS 加氢 加氢 负载型Pd基催化剂 负载型Pd基催化剂 超大孔载体 超大孔载体

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GB/T 7714 梁梦欣 , 郭艳 , 王世栋 et al. 氮化碳负载钯催化剂的制备及对SBS选择性催化加氢性能的研究 [J]. | 化工学报 , 2023 , 74 (2) : 766-775 .
MLA 梁梦欣 et al. "氮化碳负载钯催化剂的制备及对SBS选择性催化加氢性能的研究" . | 化工学报 74 . 2 (2023) : 766-775 .
APA 梁梦欣 , 郭艳 , 王世栋 , 张宏伟 , 袁珮 , 鲍晓军 . 氮化碳负载钯催化剂的制备及对SBS选择性催化加氢性能的研究 . | 化工学报 , 2023 , 74 (2) , 766-775 .
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氮化碳负载钯催化剂的制备及对SBS选择性催化加氢性能的研究 CSCD PKU
期刊论文 | 2023 , 74 (02) , 766-775 | 化工学报
氮化碳负载钯催化剂的制备及对SBS选择性催化加氢性能的研究 CSCD PKU
期刊论文 | 2023 , 74 (02) , 766-775 | 化工学报
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