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Hybrid Acid/alkali All Covalent Organic Frameworks Battery

Angewandte Chemie 2023年第18期135卷

作者： Yunpeng Xu Pingwei Cai Kai Chen Qingsong Chen Prof. Dr. Zhenhai Wen Prof. Long Chen Department of Chemistry Tianjin Key Laboratory of Molecular Optoelectronic Science Tianjin University Tianjin 300072 P. R. China CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of Materials and Techniques toward Hydrogen Energy Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 China

Covalent organic frameworks (COFs), thanks to their adjustable porous structure and abundant build-in functional motifs, have been recently regarded as promising electrode materials for a variety of batteries. There still remain grand opportunities to further utilizing their merits for developing advanced COFs-based batteries. In this paper, we propose a hybrid acid/alkali all-COFs battery by coupling pyrene-4,5,9,10-tetraone based COF cathode with anthraquinone based COF anode. In such a hybrid acid/alkali all-COFs battery, the cathodic COF favorably works in acid with a relatively positive potential, while the anodic COF preferably runs in alkali with a relatively negative potential. It thus can deliver a decently high discharge capacity of 92.97 mAh g −1 with a wide voltage window of 2.0 V, and exhibit high energy density of 74.2 Wh kg −1 along with a considerable cyclic stability over 300 cycles. The development of the proof-of-concept all-COFs battery may drive forward the improvement of newly cost-effective and performance-reliable energy storage devices.

关键词： All COFs batteries Anode Cathode Hybrid Acid/alkali Device

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Construction of Cu 2 O/Ni-MOF-74 S-scheme heterojunction for enhanced photocatalytic hydrogen evolution

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Journal of Alloys and Compounds 2025年 1036卷

作者： Yanke Yang Youlin Wu Chaoyue Zheng Qingyang Pang Yachong Wang Jihuai Wu Jia Liu Canzhong Lu Yiming Xie Engineering Research Center of Environment-Friendly Functional Materials Ministry of Education Institute of Materials Physical Chemistry Huaqiao University Xiamen 361021 PR China CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 PR China Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials Center of Rare-earth Materials Haixi Institutes Chinese Academy of Sciences Xiamen 361021 PR China University of Chinese Academy of Sciences Beijing 100049 PR China

Metal-organic frameworks (MOFs) have attracted considerable interest in photocatalytic applications owing to their exceptionally large specific surface areas and structurally customizable architectures. However, their potential is constrained by challenges including structural instability and rapid recombination of photogenerated carriers. Strategies such as heterojunction construction, elemental doping, and defect engineering have proven effective in enhancing MOF photocatalytic performance. This study developed an NMC S-scheme heterojunction photocatalytic system through precise loading of Cu 2 O onto a layered Ni-MOF-74 substrate using combined physical mixing and hydrothermal treatment. The Fermi level difference between Cu 2 O and Ni-MOF-74 induced band bending and formed a built-in electric field, facilitating efficient recombination of electrons from Cu 2 O with holes from Ni-MOF-74, thereby enhancing the composite catalyst's redox capability. Under 10 W white light illumination, the NMC-20 % sample demonstrated exceptional hydrogen evolution activity of 116.44 μmol, representing 2.88 times and 4.89 times improvements over pristine Ni-MOF-74 and Cu 2 O. Comprehensive photophysical characterizations revealed superior light absorption and suppressed carrier recombination in the NMC system. Electrochemical analyses confirmed its enhanced charge transfer efficiency and electrochemical properties. Through synergistic validation via density functional theory (DFT) calculations and experimental characterization, the photogenerated charge transfer mechanism within this system was elucidated. This study offers groundbreaking perspectives on the utilization of S-scheme heterojunctions for enhanced photocatalytic hydrogen production.

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Perovskite Sr0.9Fe0.9Zr0.1O3-δ:Redox-stable Structure,Oxygen Vacancy,Electrical Properties and Steam Electrolysis Performance

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Chinese Journal of Structural Chemistry 2018年第1期37卷 65-74页

作者：李哲叶灵婷谢奎 CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of Sciences

Many researchers have studied on perovskite oxide for its unique *** oxides,ABO3-δ,with different A and B metals have shown wide applications in many fields,in particular solid oxide ***3-δ,typical perovskite oxides,in which iron is the mixed-valence cation with the capacity to change the chemical valence,have a wide range of oxygen *** this study,Sr（0.9）Fe（0.9）Zr（0.1）O3-δ（SFZO） is synthesized and then treated in 5%H2/Ar and air at high temperature,exhibiting excellent redox ***-stable structure,oxygen vacancy and electrical properties of SFZO are *** electrolysis is then performed with SFZO cathode under 5%H2O/5%H2/Ar and 5%H2O/Ar atmospheres,*** present results indicate that the SFZO is a novel promising cathode material for solid oxide steam electrolyser.

关键词： phase structure solid oxide electrolyser Sr0.9Fe0.9Zr0.1O3-δ cathode steam electrolysis

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Disorder Over Pore Size: Boosting Supercapacitor Efficiency

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Angewandte Chemie 2024年第49期136卷

作者： Dr. Hao Zhang Yu Zhang Prof. Zhenhai Wen Department of Chemical Engineering Massachusetts Institute of Technology Cambridge MA 02139 USA Department of Chemistry University of Oxford Oxford OX1 3TA UK CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of Materials and Techniques toward Hydrogen Energy Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou 350002 China

The urgent need for efficient energy storage systems has spotlighted supercapacitors and nanostructured porous carbon materials. These materials require structural optimization to enhance their performance and lifespan, necessitating advanced design and synthesis techniques. In a recent publication, Forse and co-workers reveal that structural disorder in nanoporous carbon materials significantly enhances their capacitance performance, suggesting that optimizing structural disorder is key to developing high-energy-density supercapacitors. This study innovatively shows that structural disorder in nanoporous carbon materials significantly enhances capacitance performance, surpassing traditional factors like pore size and surface area. The investigation of multiple nanoporous carbons from a range of different suppliers showcases the generalizability of the findings. Annealing treatment further confirms that the capacitance enhancement is due to structural disorder. This discovery guides the design and synthesis of new efficient electrode materials, providing a new direction for the future development of supercapacitors.

关键词： nanoporous carbon structural disorder capacitance performance thermal annealing supercapacitors

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Coupling effects of Zn single atom and high curvature supports for improved performance of CO_(2) reduction

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Science Bulletin 2021年第16期66卷 1649-1658,M0004页

作者： Zhongjing Hao Junxiang Chen Dafeng Zhang Lirong Zheng Yueming Li Zi Yin Gang He Lei Jiao Zhenhai Wen Xiao-Jun Lv State Key Laboratory of Alternate Electrical Power System with Renewable Energy Sources School of New EnergyNorth China Electric Power UniversityBeijing 102206China State Key Laboratory of Metastable Materials Science and Technology College of Materials Science and EngineeringYanshan UniversityQinhuangdao 066004China CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Province Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China Key Laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190China Department of Energy and Chemical Engineering College of Chemistry and Chemical EngineeringHenan Key Laboratory of Coal Green ConversionHenan Polytechnic UniversityJiaozuo 454003China Key Laboratory of Cryogenics Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China

Single-atom catalysts(SACs)have emerged as one of the most competitive catalysts toward a variety of important electrochemical reactions,thanks to their maximum atom economy,unique electronic and geometric ***,the role of SACs supports on the catalytic performance does not receive enough research ***,we report an efficient route for synthesis of single atom Zn loading on the N-doped carbon nano-onions(ZnN/CNO).ZnN/CNO catalysts show an excellent high selectivity for CO_(2) electro-reduction to CO with a Faradaic efficiency of CO(FECO)up to 97%at -0.47 V(*** hydrogen electrode,RHE)and remarkable durability without activity *** our knowledge,ZnN/CNO is the best activity for the Zn based catalysts up to now,and superior to single atom Zn loading on the two-dimensional planar and porous structure of graphene substrate,although the graphene with larger surface *** exact role of such carbon nano-onions(CNO)support is studied systematically by coupling characterizations and electrochemistry with density functional theory(DFT)calculations,which have attributed such good performance to the increased *** increased curvature modifies the surface charge,which then changes the adsorption energies of key intermediates,and improves the selectivity for CO generation accordingly.

关键词： Single-atom catalysts Highly curved substrate Electrocatalytic CO_(2) reductions High activity and selectivity Coupling effect

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Redox-Mediated TEMPO-Based Donor-Acceptor Covalent Organic Framework for Efficient Photo-Induced Hydrogen Peroxide Generation

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Angewandte Chemie 2025年

作者： Junlan Chen Dr. Shichen Yan Futong Wang Fuwen Lin Dr. Jing Lin Dr. Rahul Anil Borse Prof. Yaobing Wang CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of Nanomaterials State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou 350002 Fujian P. R. China University of Chinese Academy of Sciences Beijing 100049 P. R. China Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108 Fujian P. R. China

Molecular engineering of covalent organic frameworks (COFs) offers an alternative approach to conventional anthraquinone oxidation via photo-induced H 2 O 2 production from O 2 reduction. Despite their potential, reported photocatalysts suffer limited proton mobility, low selectivity, and insufficient charge separation and utilization. Herein, we report a nitroxyl radical (TEMPO) decorated two-dimensional (2D) donor-acceptor (D-A)-COF photocatalyst via a one-pot strategy. Under visible light irradiation, highly crystalline TAPP-TPDA-TEMPO-COF ( TT-T-COF ) exhibits a remarkable photocatalytic H 2 O 2 yield of 10066 μmol g −1 h −1 in two-phase water-benzyl alcohol (10 % BA) system through direct two-electron (2 e − ) pathway. The mechanistic study by DFT calculations and in situ DRIFT spectra suggests Yeager-type adsorption of *O 2 ⋅ − intermediate on the nitroxyl radical site (N−O⋅). The efficient photocatalytic performance and stability of TT-T-COF are attributed to the involvement of the nitroxyl radical, which enhances selective O 2 adsorption, establishes a distinct electron density distribution, and facilitates photogenerated charge separation compared to TT-HT-COF and TT-COF counterparts. This study uncovers a new perspective for constructing metal-free, redox-mediated radical-based COFs for sustainable energy conversion, storage, and biomedical applications.

关键词： radical covalent organic frameworks oxygen reduction reaction TEMPO-based photocatalyst density functional theory

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Recent advances and strategies in vat photopolymerization of high-performance engineering elastomers for specialized applications

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Chemical Engineering Journal 2025年 519卷

作者： Xianmei Huang Haoran Zhai Shuqiang Peng Weiqiang Chen Longhui Zheng Zixiang Weng Lixin Wu CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 PR China University of Chinese Academy of Sciences Beijing 100049 PR China Key Laboratory of Polymer Materials and Products College of Materials Science and Engineering Fujian University of Technology Fuzhou 350118 PR China. Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou Fujian 350108 PR China.

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Mn^(2+)-activated calcium fluoride nanoprobes for time-resolved photoluminescence biosensing

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Science China Materials 2019年第1期62卷 130-137页

作者： Jiaojiao Wei Wei Zheng Xiaoying Shang Renfu Li Ping Huang Yan Liu Zhongliang Gong Shanyong Zhou Zhuo Chen Xueyuan Chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures State Key Laboratory of Structural Chemistry and Fujian Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences College of Materials Science and Engineering Fujian Normal University

Time-resolved (TR)photoluminescence (PL) technique has shown great promise in ultrasensitive biodetection and high-resolution ***,almost all the TRPL bioprobes are based on the parity-forbidden f→f transition of lanthanide ***,we report TRPL biosensing by taking advantage of the d→d transition of transition metal (TM)Mn^2+ *** demonstrate that the Forster resonance energy transfer (FRET)signal can be distinguished from that of radiative reabsorption process through measuring the PL lifetime of Mn^2+,thus establishing a reliable method for Mn^2+ in homogeneous TR-FRET *** also demonstrate the biotin receptor-targeted cancer cell imaging by utilizing biotinylated CaF2:Ce,Mn ***,we show in a proof-of-concept experiment the appli- cation of the long-lived PL of Mn^2+ for TRPL bioimaging through the burst shot with a cell *** findings provide a general approach for exploiting the long-lived PL of TM ions for TRPL biosensing,thereby opening up a new avenue for the exploration of novel and versatile applications of TM ions.

关键词： manganese time-resolved photoluminescence energy transfer biodetection bioimaging

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Peptization Induced WO3@SnO2 to Enable Perovskite Solar Cell with Record Fill-Factor Approaching the Shockley–Queisser Limit

SSRN

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SSRN 2022年

作者： Gao, Peng Li, Zicheng Wang, Can Sun, Ping-Ping Zhang, Zhihao Zhou, Qin Du, Yitian Xu, Jianbin Chen, Yibo Xiong, Qiu Ding, Liming Nazeeruddin, Mohammad Khaja CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Provincial Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fujian Fuzhou350002 China Laboratory for Advanced Functional Materials Xiamen Institute of Rare Earth Materials Haixi Institute Chinese Academy of Sciences Xiamen361021 China Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials Xiamen Institute of Rare Earth Materials Haixi Institute Chinese Academy of Sciences Xiamen361021 China School of Mechanical and Aerospace Engineering Nanyang Technological University 50 Nanyang Avenue Singapore639798 Singapore Institute of Materials Physical Chemistry Huaqiao University Xiamen361021 China Xiamen Honglu Wumu Industry Limited Company Liansheng Rd Jimei District Fujian Xiamen China National Center for Nanoscience and Technology Beijing100190 China Group for Molecular Engineering of Functional Materials Institute of Chemical Sciences and Engineering École Polytechnique Fedérale de Lausanne Sion1951 Switzerland

SnO2-based electron transport layers (ETLs) offer outstanding band alignment, excellent chemical and UV stability, high transmittance, high conductivity, and processability at low temperatures. However, unfortunately, the state-of-the-art SnO2 colloid precursor suffered from agglomeration over time and structural defects such as dangling hydroxyl groups and oxygen vacancies, which deteriorate both the morphology and electronic quality of the resulting ETL. Especially, these trap states near the valence band can hinder charge extraction and transport of electrons to couple with non-radiative recombination loss. Here, we introduce a novel WO3@SnO2 nanocomposite ETL, which is synthesized by in situ peptizations of WO3 in commercial alkaline SnO2 colloid nanocrystals. The hydrated (peptized) WO3 forms H2WO4 (WO42-) to effectively stabilize the SnO2 nanocrystals in the dispersion and bind to the defect sites. Intriguingly, the H2WO4 converts back to the WO3 phase to form nano-heterostructured composite with SnO2 particles during the process of film fabrication, further promoting passivation and charge extraction. Through the novel method, we could achieve molecular level passivation of SnO2 layer by WO3, and a power conversion efficiency of 23.6% for a 0.1 cm2 PSC device with ultra-high FF of 85.8% was demonstrated. Furthermore, a modified detailed balance model was used to verify the drastically lessened surface & bulk defect-induced recombination loss in WO3@SnO2 based devices. Finally, the corresponding unencapsulated cell retained ~91% of its initial efficiency after 2000 hours of damp exposure. This work provides a promising method to access the Shockley–Queisser limit of fill factor for single-junction PSC. © 2022, The Authors. All rights reserved.

关键词： Perovskite solar cells

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Understanding De-protonation Induced Formation of Spinel Phase in Li-rich Layered Oxides for Improved Rate Performance

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Chinese Journal of Structural Chemistry 2018年第11期37卷 1723-1736页

作者：李保云李广社张丹范建明冯涛李莉萍 State Key Laboratory of Inorganic Synthesis & Preparative Chemistry Jilin University Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences

Constructing layered-spinel composites is important to improve the rate performance of lithium-rich layered ***,up to now,the effect of microstructure of composites on the rate performance has not been well *** this study,a series of samples were prepared by a simple protonation and de-protonation for the pristine layered material(LiMnNiCoO)obtained by sol-gel *** characterizations of XRD,Raman and oxidation-reduction potentials of charge-discharge curves demonstrated that these samples after de-protonation are layered-spinel *** these composites were tested as a cathode of lithium-ion batteries,the sample treated with 0.1 M of nitric acid exhibited higher discharge capacities at each current density than that of other *** outstanding rate performance is attributed to the high concentration of conduction electron resulting from the low average valence state(44.2%of Ni)as confirmed by its high conductivity(1.124×10??mat39800Hz)and ambient temperature magnetic susceptibility(8.40×10emu/Oe?mol).This work has a guiding significance for the synthesis of high rate performance of lithium battery cathode materials.

关键词： protonation and de-protonation layered-spinel composites rate performance conduction electron

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