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学者姓名：胡策军
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Abstract ：
Electrochemical biomass upgrading is a promising substitute for oxygen evolution reaction (OER) to generate valuable chemicals in conjunction with hydrogen generation. Pursuing highly efficient and durable electrocatalysts for significant concentration levels (≥ 50 mM) of biomass electrooxidation remains an enduring challenge. Herein, we introduce a robust Cu-supported CoFe Prussian blue analogue (CoFe PBA/CF) electrocatalyst, adept at facilitating high-concentration (50 mM) 5-hydroxymethylfurfural (HMF) oxidation into 2,5-furandicarboxylic acid (FDCA), achieving an exceptional HMF conversion (100%) with a notable FDCA yield of 98.4%. The influence of copper substrate and adsorption energy are therefore discussed. Impressively, the CoFe PBA/CF electrode sustains considerable durability in a continuous-flow electrochemical reactor designed for consecutive FDCA production, showcasing FDCA yields of 100/94% at flow rates of 0.4/0.8 mL·min-1 over 60 h’ uninterrupted electrolysis. This work provides a promising strategy to develop highly efficient and robust electrocatalysts for the consecutive production of high-value products coupled with green H2 production. © The Author(s) 2025.
Keyword ：
5-hydroxymethylfurfural oxidation 5-hydroxymethylfurfural oxidation CoFe Prussian blue analogues CoFe Prussian blue analogues electrochemical conversion electrochemical conversion high concentration high concentration structural reconstruction structural reconstruction
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| GB/T 7714 | Zhang, B. , Xiao, T. , Hu, C. et al. Continuous-flow electrooxidation for scalable biomass upgrading over copper-supported CoFe Prussian blue analogues [J]. | Chemical Synthesis , 2025 , 5 (1) . |
| MLA | Zhang, B. et al. "Continuous-flow electrooxidation for scalable biomass upgrading over copper-supported CoFe Prussian blue analogues" . | Chemical Synthesis 5 . 1 (2025) . |
| APA | Zhang, B. , Xiao, T. , Hu, C. , Liu, Z. , Chen, P. , Zhao, Z. et al. Continuous-flow electrooxidation for scalable biomass upgrading over copper-supported CoFe Prussian blue analogues . | Chemical Synthesis , 2025 , 5 (1) . |
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The electrocatalytic coupling of methanol and CO to produce dimethyl carbonate (DMC) is an attractive strategy for converting C1 resources into value-added products, while the controlled adsorption and coupling of two key intermediates, *CO and *OCH3, have not been demonstrated yet. Herein, a heterointerface engineering strategy is developed to modulate intermediate adsorption and facilitate the C & horbar;O bond formation. By constructing a Pd and PdO heterostructure catalyst with abundant interfaces (designated as Pd/PdO-r), the Pd0 sites serve to stabilize *CO and the electrophilic Pd2+ sites can promote the *OCH3 adsorption, thereby optimizing their spatial proximity and reactivity. In addition, the heterointerfaces allow to lower the coupling reaction barrier, enabling an efficient electrocatalytic pathway for the DMC synthesis. Consequently, the Pd/PdO-r heterostructure catalyst exhibited a high Faradaic efficiency of 86% with a DMC yield rate of 252 mu mol h-1 mgcat-1 in flow cells. The work suggests an effective approach to design heterointerfaces for enhanced intermediate adsorption and coupling, thus promoting the formation of valuable multicarbon products from C1 resources.
Keyword ：
dimethyl carbonate (DMC) dimethyl carbonate (DMC) electrocatalytic carbonylation electrocatalytic carbonylation heterointerfaces heterointerfaces interface engineering interface engineering Pd catalysts Pd catalysts
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| GB/T 7714 | Mi, Yuying , Xue, Yuanyuan , Yan, Yaqin et al. Promoting Intermediate Stabilization and Coupling for Dimethyl Carbonate Electrosynthesis [J]. | SMALL , 2025 , 21 (19) . |
| MLA | Mi, Yuying et al. "Promoting Intermediate Stabilization and Coupling for Dimethyl Carbonate Electrosynthesis" . | SMALL 21 . 19 (2025) . |
| APA | Mi, Yuying , Xue, Yuanyuan , Yan, Yaqin , Hao, Shuya , Hu, Cejun , Zhang, Lijuan et al. Promoting Intermediate Stabilization and Coupling for Dimethyl Carbonate Electrosynthesis . | SMALL , 2025 , 21 (19) . |
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Deep hydrogenation of dicyclopentadiene resin (DCPD resin) plays an important role in enhancing its performance and broadening its applications. However, designing suitable catalysts for promoting DCPD resin deep hydrogenation remains a challenge due to the high steric hindrance and abundant unsaturated bonds in DCPD resin, requiring strong binding to C=C double bonds. We herein propose a strategy for simultaneously constructing highly-dispersed Ni particles for hydrogen dissociation and interfacial Ni0/Ni(OH)+ sites for C=C adsorption by controlled reduction of Ni phyllosilicate (Ni PS). The catalyst, after reduction at 400 degrees C, demonstrated balanced ratio between Ni0 and interfacial Ni0/Ni(OH)+ sites, and achieved a hydrogenation degree of 99.8% (TOF: 68.8 h-1) while maintaining 99.3% efficiency after seven consecutive cycles. Through in-situ DRIFTS analysis and density functional theory (DFT) calculations, it is confirmed that the introduction of Ni0/Ni(OH)+ interfacial sites results in superior activity compared to pure Ni0 or unreduced PS due to optimized charge transfer and electronic configuration. This work not only establishes a simple and environmentally-friendly approach to design efficient catalysts for polymer hydrogenation, but also provides insights into the mechanism of unsaturated bond hydrogenation through the synergistic effects of Ni0 and Ni0/Ni(OH)+ interfacial sites.
Keyword ：
DCPD resin DCPD resin Hydrogenation Hydrogenation Ni(OH) plus Ni(OH) plus Ni phyllosilicate Ni phyllosilicate
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| GB/T 7714 | Liu, Qunhong , Liu, Zhen , Yang, Zongxuan et al. Deciphering Ni0/Ni(OH)+ interfacial sites for deep hydrogenation of dicyclopentadiene resin [J]. | CHEMICAL ENGINEERING JOURNAL , 2025 , 512 . |
| MLA | Liu, Qunhong et al. "Deciphering Ni0/Ni(OH)+ interfacial sites for deep hydrogenation of dicyclopentadiene resin" . | CHEMICAL ENGINEERING JOURNAL 512 (2025) . |
| APA | Liu, Qunhong , Liu, Zhen , Yang, Zongxuan , Wu, Qingchen , Li, Zimeng , Liu, Zhichen et al. Deciphering Ni0/Ni(OH)+ interfacial sites for deep hydrogenation of dicyclopentadiene resin . | CHEMICAL ENGINEERING JOURNAL , 2025 , 512 . |
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Diffusion behavior of catalyst pores plays a crucial influence in polymer heterogeneous hydrogenation reactions. However, experimental methods on how to accurately measure the diffusion coefficient of polymer molecules are still lacking. Herein, we develop an in-situ infrared-based method combined with mathematical models to accurately obtain the diffusion coefficients of polymers and investigate the effect of pore size on the diffusion and hydrogenation performance. Taking dicyclopentadiene resin as the model polymer, the results show that the selected Pd/Al2O3 catalyst with a pore size of 14.7 nm possesses an apparent diffusion coefficient of 3.83 x 10-15 m2/s and exhibits the best catalytic hydrogenation activity with a hydrogenation degree of 98.4%. This study provides a universal method for measuring the diffusion coefficients of polymer molecules, which holds significant guiding importance for the further development of more efficient polymer hydrogenation catalysts.
Keyword ：
DCPD resin DCPD resin Diffusion coefficient Diffusion coefficient Heterogeneous hydrogenation Heterogeneous hydrogenation In-situ infrared spectroscopy In-situ infrared spectroscopy Pore size Pore size
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| GB/T 7714 | Liu, Qunhong , Song, Zhaohui , Zhang, Hongwei et al. Determination of diffusion coefficients of polymer molecules in porous Pd/ Al2O3 catalyst and their impact on the hydrogenation performance [J]. | CHEMICAL ENGINEERING SCIENCE , 2025 , 310 . |
| MLA | Liu, Qunhong et al. "Determination of diffusion coefficients of polymer molecules in porous Pd/ Al2O3 catalyst and their impact on the hydrogenation performance" . | CHEMICAL ENGINEERING SCIENCE 310 (2025) . |
| APA | Liu, Qunhong , Song, Zhaohui , Zhang, Hongwei , Hu, Dezheng , Hu, Cejun , Bao, Xiaojun et al. Determination of diffusion coefficients of polymer molecules in porous Pd/ Al2O3 catalyst and their impact on the hydrogenation performance . | CHEMICAL ENGINEERING SCIENCE , 2025 , 310 . |
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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, (c) 2024 Institute of Process Engineering, Chinese Academy of Sciences. Publishing services by Elsevier B.V. on behalf of KeAi Communications Co., Ltd. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
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, Xinru , Zhang, Hongwei , Hu, Cejun et al. Advances in enhancing hydrodeoxygenation selectivity of lignin-derived oxygenates: From synthetic strategies to fundamental techniques [J]. | GREEN ENERGY & ENVIRONMENT , 2025 , 10 (2) : 292-321 . |
| MLA | Wu, Xinru et al. "Advances in enhancing hydrodeoxygenation selectivity of lignin-derived oxygenates: From synthetic strategies to fundamental techniques" . | GREEN ENERGY & ENVIRONMENT 10 . 2 (2025) : 292-321 . |
| APA | Wu, Xinru , Zhang, Hongwei , Hu, Cejun , Bao, Xiaojun , Yuan, Pei . Advances in enhancing hydrodeoxygenation selectivity of lignin-derived oxygenates: From synthetic strategies to fundamental techniques . | GREEN ENERGY & ENVIRONMENT , 2025 , 10 (2) , 292-321 . |
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2,5-Furandicarboxylic acid (FDCA), a crucial precursor for synthesizing biodegradable polymers as a sustainable alternative to petroleum-derived plastics, has garnered significant interest for its production via electrolysis. However, this approach remains hindered by the inherent weak reactant-catalyst adsorption and sluggish interfacial kinetics. Herein, we report Cu-incorporated NiFe Prussian blue analogues (PBA) that enable rapid electrooxidation of 5-hydroxymethylfurfural (HMF) to FDCA with nearly 100 % conversion, selectivity, and Faradaic efficiency, even at an industrial-scale concentration of 100 mM. In situ Raman and electrochemical characterizations reveal that Cu-incorporation elongates Ni-N bonds and accelerates their reconstruction into defect-rich Ni2+-OH species, which undergo deprotonation to form highly active Ni3+-O species. X-ray technology and theoretical calculations show that the electronegative Cu2+ prompts a shift of the d-band center of neighboring Ni atoms toward the Fermi level, thereby enhancing the adsorption of both hydroxyl (-OH) and aldehyde (-CHO) groups in HMF and thus accelerating electrooxidation of HMF to FDCA. Practical applicability using a continuous flow electrolyzer demonstrates the potential for industrial application, achieving a kilogramscale FDCA production with 99 % purity and a yield exceeding 90 % over 1200 h. This work realizes the valence regulation of active sites in PBA through a cation engineering approach and verifies its feasibility in sustainable biomass electro-oxidation upgrading.
Keyword ：
2,5-furandicarboxylic acid 2,5-furandicarboxylic acid Cu-induced reconstruction Cu-induced reconstruction Ni3+-O active sites Ni3+-O active sites Prussian blue analogues Prussian blue analogues Selective electrooxidation Selective electrooxidation
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| GB/T 7714 | Liu, Zhichen , Xiao, Tiantian , Wu, Xinru et al. Cu-induced Ni3+ -O active sites in Prussian blue analogues enable nearly 100 % selective electrooxidation of 5-hydroxymethylfurfural to produce kilogram-scale 2,5-furandicarboxylic acid [J]. | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2025 , 378 . |
| MLA | Liu, Zhichen et al. "Cu-induced Ni3+ -O active sites in Prussian blue analogues enable nearly 100 % selective electrooxidation of 5-hydroxymethylfurfural to produce kilogram-scale 2,5-furandicarboxylic acid" . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY 378 (2025) . |
| APA | Liu, Zhichen , Xiao, Tiantian , Wu, Xinru , Hu, Cejun , Lu, Xue Feng , Zhang, Hongwei et al. Cu-induced Ni3+ -O active sites in Prussian blue analogues enable nearly 100 % selective electrooxidation of 5-hydroxymethylfurfural to produce kilogram-scale 2,5-furandicarboxylic acid . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2025 , 378 . |
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The copper-based electrocatalysts feature attractive potentials of converting CO2 into multi-carbon (C2+) products, while the instability of Cu–O often induces the reduction of Cu+/Cu0 catalytic sites at the cathode and refrains the capability of stable electrolysis especially at high powers. In this work, we developed an Erbium (Er) oxide-modified Cu (Er–O–Cu) catalyst with enhanced covalency of Cu–O and more stable active sites. The f-p-d coupling strengthens the covalency of Cu–O, and the stability of Cu+ sites under electroreduction condition is critical for promoting the C–C coupling and improving the C2+ product selectivity. As a result, the Er–O–Cu sites exhibited a high Faradaic efficiency of C2+ products (FEC2+) of 86 % at 2200 mA cm−2, and a peak partial current density of |jC2+| of 1900 mA cm−2, comparable to the best reported values for the CO2-to-C2+ electroreduction. The CO2 electrolysis by the Er–O–Cu sites was further scaled up to 100 cm2 to achieve high-power (∼200 W) electrolysis with ethylene production rate of 16 mL min−1. © 2025 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Keyword ：
Bonding Bonding Electrolysis Electrolysis Electrolytic reduction Electrolytic reduction
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| GB/T 7714 | Wang, Maoyin , Huang, Yuhang , Song, Lu et al. f-p-d coupling-induced bonding covalency boosts C–C coupling in electrocatalytic CO2 reduction over Er–O–Cu sites [J]. | Journal of Energy Chemistry , 2025 , 108 : 239-245 . |
| MLA | Wang, Maoyin et al. "f-p-d coupling-induced bonding covalency boosts C–C coupling in electrocatalytic CO2 reduction over Er–O–Cu sites" . | Journal of Energy Chemistry 108 (2025) : 239-245 . |
| APA | Wang, Maoyin , Huang, Yuhang , Song, Lu , Wei, Ruilin , Hao, Shuya , Liu, Zhengzheng et al. f-p-d coupling-induced bonding covalency boosts C–C coupling in electrocatalytic CO2 reduction over Er–O–Cu sites . | Journal of Energy Chemistry , 2025 , 108 , 239-245 . |
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The single-atom Fe-N-C electrocatalyst is considered one of the most promising alternatives to the expensive and scarce Pt-based catalysts for promoting oxygen reduction reaction in fuel cells. Regulating the coordination environment of the Fe center is a feasible strategy to improve its stability and catalytic activity. Recently, the introduction of axial ligands to Fe-N-C has attracted extensive research interest, providing a new dimension for coordination environment regulation compared with the common approaches of in-plane doping or defect construction. This review focuses on discussing the contribution of axial ligand decoration to the activity and stability of the Fe-N-C catalyst, evaluating different types of axial ligands that have been introduced in the recent literature. Through summarizing the progress in decorating axial ligands to the Fe-N-C system, this review provides profound insights into the design and preparation of axially coordinated Fe-N-C catalysts.
Keyword ：
axially coordinated ligands axially coordinated ligands electronic structures electronic structures Fe-N-C Fe-N-C oxygen reduction reactions oxygen reduction reactions single-atom catalysts single-atom catalysts
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| GB/T 7714 | Yang, Zongxuan , Wu, Qingchen , Zhang, Hongwei et al. Strategic Engineering of Axially Coordinated Ligands in Fe-N-C Catalysts for Enhanced Oxygen Reduction Electrocatalysis [J]. | CHEMSUSCHEM , 2025 , 18 (15) . |
| MLA | Yang, Zongxuan et al. "Strategic Engineering of Axially Coordinated Ligands in Fe-N-C Catalysts for Enhanced Oxygen Reduction Electrocatalysis" . | CHEMSUSCHEM 18 . 15 (2025) . |
| APA | Yang, Zongxuan , Wu, Qingchen , Zhang, Hongwei , Hu, Cejun , Bao, Xiaojun , Yuan, Pei . Strategic Engineering of Axially Coordinated Ligands in Fe-N-C Catalysts for Enhanced Oxygen Reduction Electrocatalysis . | CHEMSUSCHEM , 2025 , 18 (15) . |
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Heterogeneous hydrogenation of nitrile butadiene rubber (NBR) is a pivotal technology for producing highvalue-added hydrogenated NBR, yet the complex macromolecular configuration poses critical challenges to catalyst activity and stability. Herein, metal-doped M-TiO2 (M = Mo, V, Mn species) nanosheet supports featuring aerobic-stable oxygen vacancies (Vo) and Ti3+ sites were engineered, and loaded with Pd for NBR hydrogenation. Among the dopants, Mn species exhibits optimal charge compensation effect, achieving the lowest Vo formation energy (1.73 eV) and highest Vo-Ti3+ density (25.8% Vo, 27.1% Ti3+), outperforming V (3.38 eV; 18.1% Vo, 17.2% Ti3+) and Mo (4.03 eV; 15.5% Vo, 12.7% Ti3+). These Vo-Ti3+ sites enhance the dispersion and stability of Pd, endowing Pd with electron-rich characteristics which synergistically strengthen C--C and H2 adsorption-activation process while reducing the activation energy barrier. As a result, Pd/Mn-TiO2 exhibits excellent catalytic activity (97%) and TOF value (306 h- 1) for NBR hydrogenation, surpassing Pd/VTiO2 (94%, 268 h- 1), Pd/Mo-TiO2 (86%, 245 h- 1), and Pd/TiO2 (75%, 204 h- 1). This work elucidates the role of high-valence metal doping on TiO2 defect engineering, establishing a universal design principle for durable macromolecular hydrogenation catalysts.
Keyword ：
Metal-doped Metal-doped NBR Hydrogenation NBR Hydrogenation Oxygen vacancies Oxygen vacancies Ti 3+sites Ti 3+sites
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| GB/T 7714 | Wang, Shidong , Yang, Zongxuan , Li, Runzhi et al. Engineering aerobic-stable oxygen vacancies-Ti3+defects of Pd/Mn-TiO2 for boosting nitrile butadiene rubber hydrogenation [J]. | CHEMICAL ENGINEERING JOURNAL , 2025 , 522 . |
| MLA | Wang, Shidong et al. "Engineering aerobic-stable oxygen vacancies-Ti3+defects of Pd/Mn-TiO2 for boosting nitrile butadiene rubber hydrogenation" . | CHEMICAL ENGINEERING JOURNAL 522 (2025) . |
| APA | Wang, Shidong , Yang, Zongxuan , Li, Runzhi , Zhang, Kewen , Zhao, Zhenyu , Zhang, Hongwei et al. Engineering aerobic-stable oxygen vacancies-Ti3+defects of Pd/Mn-TiO2 for boosting nitrile butadiene rubber hydrogenation . | CHEMICAL ENGINEERING JOURNAL , 2025 , 522 . |
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Acetaldehyde is an essential commodity chemical with high demand, while its conventional production by homogeneous Wacker oxidation suffers from high corrosivity, high chlorine by-products, and separation difficulties. In this work, a Pd nanoparticle-loaded ZnO (Pd-ZnO) photocatalyst is developed for the selective oxidation of ethylene to acetaldehyde. The ZnO substrate provides hydroxyl radicals (center dot OH) from water oxidation, and the Pd active sites allow to promote the dehydrogenation of adsorbed symmetrical ethylene to form asymmetrical vinyl specie (*CH2 & boxH;CH) with negatively charged carbon, which can be further attacked by center dot OH to vinyl alcohol (*C2H3OH) and finally undergo isomerization to produce acetaldehyde products. The Pd-ZnO photocatalyst exhibits a high C2H4-to-acetaldehyde yield of >3500 mu mol g(-1) h(-1) with 60% selectivity at ambient temperature and pressure under illumination without the use of sacrificial agents, featuring one of the highest performances in both photocatalytic and electrocatalytic conversion. This work suggests an attractive opportunity for the photocatalytic production of acetaldehyde from ethylene.
Keyword ：
acetaldehyde acetaldehyde dehydrogenation dehydrogenation ethylene ethylene palladium palladium photocatalytic oxidation photocatalytic oxidation
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| GB/T 7714 | Yan, Yaqin , Yang, Chao , Wang, Huining et al. Efficient Photocatalytic Ethylene Oxidation to Acetaldehyde by Asymmetrical Dehydrogenation [J]. | SMALL , 2025 , 21 (30) . |
| MLA | Yan, Yaqin et al. "Efficient Photocatalytic Ethylene Oxidation to Acetaldehyde by Asymmetrical Dehydrogenation" . | SMALL 21 . 30 (2025) . |
| APA | Yan, Yaqin , Yang, Chao , Wang, Huining , Hu, Cejun , Yuan, Pei , Zhang, Lijuan et al. Efficient Photocatalytic Ethylene Oxidation to Acetaldehyde by Asymmetrical Dehydrogenation . | SMALL , 2025 , 21 (30) . |
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