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学者姓名：袁珮
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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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Electrocatalytic/photocatalytic C & horbar;N coupling from small carboncontaining (such as CO2 and CH3OH) and nitrogen-containing species (such as N2, NO3-, and NH3) enables the synthesis of value-added organonitrogen compounds, including urea, amides, and amino acids. This approach, ideally driven by renewable energy, holds great promise for sustainable developments and has thus been attracting increasing research interest in recent years. To enhance the C & horbar;N coupling under mild reaction conditions, it is necessary to activate different substrate molecules effectively and balance the adsorption and desorption of various C- and N-containing intermediates and/or radicals, thereby realizing different value-added organonitrogen compounds. In this review, the recent advances in electrocatalytic/photocatalytic C & horbar;N coupling reactions targeting those three types of products, i.e., urea, amides, and amino acids is aimed to summarized. The rational designs of active sites for synergistic catalysis are discussed, including their types, compositions, spatial arrangements, crystal facets, heterostructures, and local environments. Different reactant molecules and catalytic mechanisms for the electrocatalytic/photocatalytic C & horbar;N coupling reactions, as well as the methods of C & horbar;N coupling products detection, are also described. Finally, the existing challenges in this field are summarized, and the potential research perspectives are also proposed.
Keyword ：
active sites active sites C & horbar;N coupling C & horbar;N coupling electrocatalysis electrocatalysis nitrogen-containing compounds nitrogen-containing compounds photocatalysis photocatalysis
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| GB/T 7714 | Xu, Mengqiu , Wang, Maoyin , Wang, Haozhen et al. Electrocatalytic and Photocatalytic C―N Coupling From Small Molecules [J]. | ADVANCED MATERIALS , 2025 . |
| MLA | Xu, Mengqiu et al. "Electrocatalytic and Photocatalytic C―N Coupling From Small Molecules" . | ADVANCED MATERIALS (2025) . |
| APA | Xu, Mengqiu , Wang, Maoyin , Wang, Haozhen , Yuan, Pei , Han, Qing , Zheng, Gengfeng . Electrocatalytic and Photocatalytic C―N Coupling From Small Molecules . | ADVANCED MATERIALS , 2025 . |
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The shale gas revolution has shifted propylene production from naphtha cracking to on-purpose production with propane dehydrogenation (PDH) as the dominant technology1, 2, 3, 4, 5, 6, 7, 8-9. Because PDH is endothermic and requires high temperatures that favour sintering and coking, the challenge is to develop active and stable catalysts1, 2-3 that are sufficiently stable10,11. Zeolite-supported Pt-Sn catalysts have been developed to balance activity, selectivity and stability12,13 and more recent work documented a PDH catalyst based on zeolite-anchored single rhodium atoms with exceptional performance and stability14. Here we show for silicalite-1 (S-1) that migration of encapsulated Pt-Sn2 clusters and hence agglomeration and anchoring within the zeolite versus agglomeration on the external surface can be controlled by adjusting the length of the S-1 crystals' b-axis. We find that, when this axis is longer than 2.00 mu m, migration of Pt-Sn2 monomers during PDH results in intracrystalline formation of (Pt-Sn2)2 dimers that are securely locked in the channels of S-1 and capable of converting pure propane feed to propylene at 550 degrees C for more than 6 months with 98.3% selectivity at 91% equilibrium conversion. This performance exceeds that of other Pt-based PDH catalysts and approaches that of the Rh-based catalyst. Although synthesis requirements and cost are at present prohibitive for industrial use, we anticipate that our approach to controlling the migration and lockup of metals in zeolites may enable the development of other noble-metal catalysts that offer extended service lifetimes in industrial applications15, 16-17.
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| GB/T 7714 | Xu, Zhikang , Gao, Mingbin , Wei, Yao et al. Pt migration-lockup in zeolite for stable propane dehydrogenation catalyst [J]. | NATURE , 2025 , 643 (8072) . |
| MLA | Xu, Zhikang et al. "Pt migration-lockup in zeolite for stable propane dehydrogenation catalyst" . | NATURE 643 . 8072 (2025) . |
| APA | Xu, Zhikang , Gao, Mingbin , Wei, Yao , Yue, Yuanyuan , Bai, Zhengshuai , Yuan, Pei et al. Pt migration-lockup in zeolite for stable propane dehydrogenation catalyst . | NATURE , 2025 , 643 (8072) . |
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The design of bifunctional and high-performance electrocatalysts that can be used as both cathodes and anodes for the two-electron oxygen reduction reaction (2e- ORR) and biomass valorization is attracting increasing attention. Herein, a conserved ligand replacement strategy is developed for the synthesis of highly ordered conductive metal-organic frameworks (Ni-HITP, HITP = 2, 3, 6, 7, 10, 11-hexaiminotriphenylene) with chemically confined phosphotungstic acid (PW12) nanoclusters in the nanopores. The newly formed Ni-O-W bonds in the resultant Ni-HITP/PW12 electrocatalysts modulate the electronic structures of both Ni and W sites, which are favorable for cathodic 2e- ORR to H2O2 production and anodic 5-hydroxymethylfurfural oxidation reaction (HMFOR) to 2, 5-furandicarboxylic acid (FDCA), respectively. In combination with the deliberately retained conductive frameworks and ordered pores, the dual-functional Ni-HITP/PW12 composites enable a H2O2 production rate of 9.51 mol gcat-1 h-1 and an FDCA yield of 96.8% at a current density of 100 mA cm-2/cell voltage of 1.38 V in an integrated 2e- ORR/HMFOR system, significantly improved than the traditional 2e- ORR/oxygen evolution reaction system. This work has provided new insights into the rational design of advanced electrocatalysts and electrocatalytic systems for the green synthesis of valuable chemicals.
Keyword ：
biomass valorization biomass valorization conductive metal-organic frameworks conductive metal-organic frameworks electrocatalysis electrocatalysis polyoxometalates polyoxometalates two-electron reduction reaction two-electron reduction reaction
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| GB/T 7714 | Bao, Tong , Wu, Yunuo , Tang, Chencheng et al. Highly Ordered Conductive Metal-Organic Frameworks with Chemically Confined Polyoxometalate Clusters: A Dual-Functional Electrocatalyst for Efficient H2O2 Synthesis and Biomass Valorization [J]. | ADVANCED MATERIALS , 2025 , 37 (17) . |
| MLA | Bao, Tong et al. "Highly Ordered Conductive Metal-Organic Frameworks with Chemically Confined Polyoxometalate Clusters: A Dual-Functional Electrocatalyst for Efficient H2O2 Synthesis and Biomass Valorization" . | ADVANCED MATERIALS 37 . 17 (2025) . |
| APA | Bao, Tong , Wu, Yunuo , Tang, Chencheng , Xi, Yamin , Zou, Yingying , Shan, Pengyue et al. Highly Ordered Conductive Metal-Organic Frameworks with Chemically Confined Polyoxometalate Clusters: A Dual-Functional Electrocatalyst for Efficient H2O2 Synthesis and Biomass Valorization . | ADVANCED MATERIALS , 2025 , 37 (17) . |
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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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High-active nonplatinum group metal oxygen reduction reaction (ORR) catalysts have great potential to improve fuel cell and metal-air battery performance due to their efficiency and cost-effectiveness. However, a fundamental understanding of their size-dependent structure-performance relationships remain elusive. Here a mesoporous-dominant carbon nanoreactor with dimensions in the range of 15-43 nm with edge-rich defective atomic Zn sites is designed. The crystal size and pore diameter of this carbon nanoreactors can be precisely adjusted to enable tunable mass diffusion pathways and porosities. Importantly, the hydrophobic nature of 25 nm nanoreactors maximizes the nonkinetic advantages of active site exposure and rapid O2 mass transfer at the triple-phase interface. The developed Zn-N-P/NPC catalysts delivers outstanding alkaline and acidic ORR performance with half-wave potentials of 0.92 and 0.80 V, respectively, as well as excellent zinc-air battery performance with charge/discharge over 400 h under 20 mA cm-2. X-ray absorption spectroscopy and theoretical calculations indicate that the enhanced ORR catalytic activity of Zn-N-P/NPC stems from the introduction of P atoms and edge carbon defects effectively exciting the localized electronic asymmetric distribution of Zn species. The findings provide new perspectives on the size effect of porous carbon supports for the development of efficient cathodes catalysts with multifunctionality.
Keyword ：
carbon nanoreactors carbon nanoreactors coordination structure regulation coordination structure regulation nanosize adjustment nanosize adjustment oxygen reduction reaction oxygen reduction reaction single atom catalysts single atom catalysts Zn-air batteries Zn-air batteries
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| GB/T 7714 | Tan, Yangyang , Zhang, Zeyi , Guo, Fei et al. Highly Defective Ultrafine Carbon Nanoreactors Enriched with Edge-Type Zn-N3P1 Moiety Boosting Oxygen Electrocatalysis [J]. | ADVANCED MATERIALS , 2025 , 37 (26) . |
| MLA | Tan, Yangyang et al. "Highly Defective Ultrafine Carbon Nanoreactors Enriched with Edge-Type Zn-N3P1 Moiety Boosting Oxygen Electrocatalysis" . | ADVANCED MATERIALS 37 . 26 (2025) . |
| APA | Tan, Yangyang , Zhang, Zeyi , Guo, Fei , Chen, Suhao , Jiang, Haoran , Chen, Runzhe et al. Highly Defective Ultrafine Carbon Nanoreactors Enriched with Edge-Type Zn-N3P1 Moiety Boosting Oxygen Electrocatalysis . | ADVANCED MATERIALS , 2025 , 37 (26) . |
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The selective oxidation of methane (CH4) has attractive potentials for mitigating global warming and producing value-added chemicals, whereas the efficient generation of multicarbon products such as ethanol remains challenging, due to the short lifetimes and high unpaired concentrations of reactive intermediates (like center dot OH, center dot CH3, center dot OCH3, and center dot CH2OH). Herein, we developed a medium-spin Zn-O-Fe(MS) catalyst with tunable Fe(III) spin states, which can efficiently photo-oxidize CH4 to ethanol at ambient conditions. The unpaired electrons in d orbitals of Fe sites allow for efficient adsorption of center dot OH, and the e(g) orbital occupancy enables stabilizing different key carbon-containing intermediates (center dot OCH3 versus center dot CH2OH). By balancing those two descriptors, the medium-spin Zn-O-Fe(MS) catalyst allows to achieve selective generation of center dot CH2OH intermediates with a moderate *OH coverage and subsequent coupling of center dot CH3 and center dot CH2OH to ethanol. With a light intensity of 100 mWcm(-2) and water as a weak oxidant, the Zn-O-Fe(MS) catalyst exhibited a peak photocatalytic CH4-to-ethanol yield of 372 mu molg(-1)h(-1) without the use of photosensitizers or sacrificial reagents, which is similar to 3 times higher than the previously best reported photocatalytic CH4 oxidation to ethanol under similar conditions. Our study suggests an attractive potential of converting CH4 to multicarbon products by modulating spin states of the catalytic sites.
Keyword ：
CH4 oxidation CH4 oxidation C & horbar;C coupling C & horbar;C coupling Intermediates Intermediates Photocatalysis Photocatalysis Spin state Spin state
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| GB/T 7714 | Hao, Shuya , Wang, Maoyin , Zhang, Leshen et al. Switching Photocatalytic Methane Oxidation Toward Ethanol by Tuning Spin States [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 . |
| MLA | Hao, Shuya et al. "Switching Photocatalytic Methane Oxidation Toward Ethanol by Tuning Spin States" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2025) . |
| APA | Hao, Shuya , Wang, Maoyin , Zhang, Leshen , Lv, Ximeng , Peng, Chen , Huang, Yuhang et al. Switching Photocatalytic Methane Oxidation Toward Ethanol by Tuning Spin States . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 . |
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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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