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学者姓名：张宏伟
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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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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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Membrane separator that is highly ionic conductive and alkaline stable is essential for the efficient, scalable electrocatalytic oxidation of HMF to FDCA, a key process for sustainable development. Drawing inspiration from the microstructural design of Nafion, we developed a series of side-chain imidazolium-functionalized anion exchange membranes (AEMs), employing the chemically stable polyethersulfone (PES) as the base polymer. Functionalization of PES side chains with chloromethyl groups, followed by C2-substituted imidazolium modification, enabled precise tuning of the membrane's physicochemical properties and structural characteristics. This tailored approach yielded an optimized DIM-PES-1.0 AEM exhibiting complete HMF conversion, with 94.0 % selectivity for FDCA and 94.1 % Faradaic efficiency, outperforming the commercial Fumasep FAA-3-PK-130 AEM, which achieved only 85.5 % FDCA selectivity under similar conditions. Notably, the DIM-PES1.0 AEM demonstrated high alkaline stability, substantially retaining its electrocatalytic activity across 15 cycles, in contrast to the rapid degradation observed in FAA-3-PK-130 AEM after only three cycles. Our findings showcase a scalable, efficient strategy for producing high-performance AEMs under mild conditions, highlighting their potential for advancing sustainable electrocatalytic processes.
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| GB/T 7714 | Ge, Xuehui , Qian, Jun , Zhu, Zhen et al. Toward tailored anion exchange membranes for high-performance electrocatalytic oxidation of HMF to FDCA [J]. | JOURNAL OF MEMBRANE SCIENCE , 2025 , 721 . |
| MLA | Ge, Xuehui et al. "Toward tailored anion exchange membranes for high-performance electrocatalytic oxidation of HMF to FDCA" . | JOURNAL OF MEMBRANE SCIENCE 721 (2025) . |
| APA | Ge, Xuehui , Qian, Jun , Zhu, Zhen , Cheng, Yafei , Yuan, Lei , Jia, Jinjie et al. Toward tailored anion exchange membranes for high-performance electrocatalytic oxidation of HMF to FDCA . | JOURNAL OF MEMBRANE SCIENCE , 2025 , 721 . |
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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 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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Electrocatalytic nitrate reduction reaction (NO3RR) has been capturing immense interest in the industrial application of ammonia synthesis, and it involves complex reaction routes accompanied by multi-electron transfer, thus causing a challenge to achieve high efficiency for catalysts. Herein, we customized the Cu-O-Ti-Ov (oxygen vacancy) structure on the Cu/TiO2 catalyst, identified through density functional theory (DFT) calculations as the synergic active site for NO3RR. It is found that Cu-O-Ti-Ov site facilitates the adsorption/association of NOx- and promotes the hydrogenation of NO3- to NH3 via adsorbed *H species. This effectively suppresses the competing hydrogen evolution reaction (HER) and exhibits a lower reaction energy barrier for NO3RR, with the reaction pathways: NO3* -> NO2* -> HONO* -> NO* -> *NOH -> *N -> *NH -> *NH2 -> *NH3 -> NH3. The optimized Cu/TiO2 catalyst with rich Cu-O-Ti-Ov sites achieves an NH3 yield rate of 3046.5 mu g h-1 mgcat-1 at -1.0 V vs. RHE, outperforming most of the reported activities. Furthermore, the construction of Cu-O-Ti-Ov sites significantly mitigates the leaching of Cu species, enhancing the stability of the Cu/TiO2 catalyst. Additionally, a mechanistic study, using in situ characterizations and various comparative experiments, further confirms the strong synergy between Cu, Ti, and Ov sites, which is consistent with previous DFT calculations. This study provides a new strategy for designing efficient and stable electrocatalysts in the field of ammonia synthesis. Published by Elsevier B.V. All rights reserved.
Keyword ：
Ammonia synthesis Ammonia synthesis Cu-O-Ti-O v site Cu-O-Ti-O v site Cu/TiO 2 catalyst Cu/TiO 2 catalyst Electrocatalytic nitrate reduction Electrocatalytic nitrate reduction Synergic catalytic effect Synergic catalytic effect
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| GB/T 7714 | Nie, Yifei , Yan, Hongping , Lu, Suwei et al. Theory-guided construction of Cu-O-Ti-Ov active sites on Cu/TiO2 catalysts for efficient electrocatalytic nitrate reduction [J]. | CHINESE JOURNAL OF CATALYSIS , 2024 , 59 : 293-302 . |
| MLA | Nie, Yifei et al. "Theory-guided construction of Cu-O-Ti-Ov active sites on Cu/TiO2 catalysts for efficient electrocatalytic nitrate reduction" . | CHINESE JOURNAL OF CATALYSIS 59 (2024) : 293-302 . |
| APA | Nie, Yifei , Yan, Hongping , Lu, Suwei , Zhang, Hongwei , Qi, Tingting , Liang, Shijing et al. Theory-guided construction of Cu-O-Ti-Ov active sites on Cu/TiO2 catalysts for efficient electrocatalytic nitrate reduction . | CHINESE JOURNAL OF CATALYSIS , 2024 , 59 , 293-302 . |
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A series of mesoporous polymers functionalized with different kinds and contents of Br & oslash; nsted acidic sites were designed and synthesized for NH 3 capture. The textural properties, morphologies and chemical structures of synthesized mesoporous polymers were characterized in details, and the NH 3 capture performance was evaluated systematically. It is found that the mesoporous polymers functionalized with phosphoric sites exhibit much better NH 3 capture performance at low pressures than those with carboxylic and sulfonic sites. Specifically, the NH 3 adsorption capacities of P(DVB-VPA)-4.0 can reach 4.82 mmol/g at 298.2 K and 0.033 bar. The excellent ability of P(DVB-VPA)-4.0 for selectively adsorbing low -content NH 3 from NH 3 /N 2 /H 2 and NH 3 /N 2 /CO 2 mixed gases was demonstrated by breakthrough experiments, and the adsorption of NH 3 by P(DVB-VPA)-4.0 is found to be mostly reversible. The thermodynamic properties and mechanism of NH 3 adsorption were also examined in depth, disclosing the important role of Br & oslash; nsted acidic sites in enhanced capture of low -content NH 3 by P(DVBVPA)-4.0.
Keyword ：
Acid -base interaction Acid -base interaction Br & oslash;nsted acidic site Br & oslash;nsted acidic site Low content Low content Mesoporous polymer Mesoporous polymer NH 3 capture NH 3 capture
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| GB/T 7714 | Zheng, Lu , Shi, Leilian , Li, Qiuke et al. Designing Brønsted acidic sites on mesoporous polymers for enhanced capture of low-content ammonia [J]. | CHEMICAL ENGINEERING SCIENCE , 2024 , 292 . |
| MLA | Zheng, Lu et al. "Designing Brønsted acidic sites on mesoporous polymers for enhanced capture of low-content ammonia" . | CHEMICAL ENGINEERING SCIENCE 292 (2024) . |
| APA | Zheng, Lu , Shi, Leilian , Li, Qiuke , Zhang, Hongwei , Cai, Zhenping , Huang, Kuan et al. Designing Brønsted acidic sites on mesoporous polymers for enhanced capture of low-content ammonia . | CHEMICAL ENGINEERING SCIENCE , 2024 , 292 . |
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The efficient separation and collection of ammonia (NH3) during NH3 synthesis process is essential to improve the economic efficiency and protect the environment. In this work, ethanolammonium hydrochloride (EtOHACl) and phenol (PhOH) were used to prepare a novel class of deep eutectic solvents (DESs) with multiple active sites and low viscosities. The NH3 separation performance of EtOHACl + PhOH DESs was analyzed completely. It is figured out that the NH3 absorption rates in EtOHACl + PhOH DESs are very fast. The NH3 absorption capacities are very high and reach up to 5.52 and 10.74 mol$kg-1 at 11.2 and 100.4 kPa under 298.2 K, respectively. In addition, the EtOHACl + PhOH DESs present highly selective absorption of NH3 over N2 and H2 and good regenerative properties after seven cycles of absorption/desorption. The intrinsic separation mechanism of NH3 by EtOHACl + PhOH DESs was further revealed by spectroscopic analysis and quantum chemistry calculations. (c) 2023 The Chemical Industry and Engineering Society of China, and Chemical Industry Press Co., Ltd. All rights reserved.
Keyword ：
Absorption Absorption Deep eutectic solvent Deep eutectic solvent Ionic liquid Ionic liquid Low viscosity Low viscosity Multiple active site Multiple active site Separation Separation
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| GB/T 7714 | Zhang, Jiayin , Zheng, Lu , Fang, Siqi et al. Efficient and reversible separation of NH3 by deep eutectic solvents with multiple active sites and low viscosities [J]. | CHINESE JOURNAL OF CHEMICAL ENGINEERING , 2024 , 67 : 97-105 . |
| MLA | Zhang, Jiayin et al. "Efficient and reversible separation of NH3 by deep eutectic solvents with multiple active sites and low viscosities" . | CHINESE JOURNAL OF CHEMICAL ENGINEERING 67 (2024) : 97-105 . |
| APA | Zhang, Jiayin , Zheng, Lu , Fang, Siqi , Zhang, Hongwei , Cai, Zhenping , Huang, Kuan et al. Efficient and reversible separation of NH3 by deep eutectic solvents with multiple active sites and low viscosities . | CHINESE JOURNAL OF CHEMICAL ENGINEERING , 2024 , 67 , 97-105 . |
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The hydrogenation of unsaturated bonds and elimination of sulfur impurities in C9 petroleum resin (C9PR) are crucial for improving its quality and performance. In this study, we prepared a nanoflower-like Ni2P/Al2O3 catalyst using an in-situ synthesis combined with liquid-phase phosphidation strategy and applied for the production of value-added hydrogenated C9PR. In-situ synthesis of Ni-Al hydrotalcite anchors and disperses Ni nanoparticles, while liquid-phase phosphidation introduces high-content Ni delta+ and P delta- active sites and prevents the formation of inactive AlPO4, synergistically enhancing both hydrogenation and desulfurization activities. The synthesized Ni2P/Al2O3 catalyst achieves a 99.6 % hydrogenation degree and reduces sulfur content from 137 ppm to 0 ppm, much better than the catalysts prepared by conventional impregnation and metal phosphate reduction methods. These results give valuable insights for designing efficient catalysts and advancing single-step hydrorefining processes to generate high-quality, value-added hydrogenated petroleum resins.
Keyword ：
C 9 petroleum resin C 9 petroleum resin Desulfurization Desulfurization Hydrogenation Hydrogenation Ni 2 P/Al 2 O 3 catalyst Ni 2 P/Al 2 O 3 catalyst
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| GB/T 7714 | Yang, Wenfei , Wu, Shuzheng , Hu, Cejun et al. In-situ synthesis of Ni2P/Al2O3 catalyst with liquid-phase phosphidation for enhancing hydrogenation and desulfurization performance in C9 petroleum resin [J]. | CHEMICAL ENGINEERING SCIENCE , 2024 , 286 . |
| MLA | Yang, Wenfei et al. "In-situ synthesis of Ni2P/Al2O3 catalyst with liquid-phase phosphidation for enhancing hydrogenation and desulfurization performance in C9 petroleum resin" . | CHEMICAL ENGINEERING SCIENCE 286 (2024) . |
| APA | Yang, Wenfei , Wu, Shuzheng , Hu, Cejun , Zhang, Hongwei , Cui, Qingyan , Bao, Xiaojun et al. In-situ synthesis of Ni2P/Al2O3 catalyst with liquid-phase phosphidation for enhancing hydrogenation and desulfurization performance in C9 petroleum resin . | CHEMICAL ENGINEERING SCIENCE , 2024 , 286 . |
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