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designing of covalent organic framework/2D g-C 3 N 4 heterostructure using a simple method for enhanced photocatalytic hydrogen production

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Journal of Colloid and Interface Science 2024年 653卷 1650-1661页

作者： Ahmed E. Hassan Ahmed M. Elewa Mai S.A. Hussien Ahmed F.M. EL-Mahdy Islam M.A. Mekhemer Ibrahim S. Yahia Tarek A. Mohamed Ho-Hsiu Chou Zhenhai Wen 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 China University of Chinese Academy of Sciences Beijing 100049 China Department of Chemistry Faculty of Science Al-Azhar University Nasr City 11884 Cairo Egypt Department of Chemical Engineering National Tsing Hua University Hsinchu 300044 Taiwan Nuclear Chemistry Department Hot Laboratories Center Atomic Energy Authority Cairo 13759 Egypt Nanoscience Laboratory for Environmental and Biomedical Applications (NLEBA) Semiconductor Lab Department of Physics Faculty of Education Ain Shams University Roxy Cairo 11757 Egypt Department of Chemistry Faculty of Education Ain Shams University Roxy Cairo 11757 Egypt Department of Materials and Optoelectronic Science National Sun Yat-Sen University Kaohsiung 80424 Taiwan Laboratory of Nano-Smart Materials for Science and Technology (LNSMST) Department of Physics Faculty of Science King Khalid University P.O. Box 9004 Abha Saudi Arabia Research Center for Advanced Materials Science (RCAMS) King Khalid University Abha 61413 P.O. Box 9004 Saudi Arabia Center of Medical and Bio-Allied Health Sciences Research (CMBHSR) Ajman University Ajman P.O. Box 346 United Arab Emirates

designing heterostructure photocatalysts is a promising approach for developing highly efficient photocatalysts for hydrogen energy production. In this work, we synthesized a series of a covalent organic framework (COF)/g-C 3 N 4 (CN) heterojunction photocatalysts, denoted as x % COF/CN (in which x indicates the weight % of COF and x = 5, 10, 20, 30, 40, 50, 90, 95, 100), for hydrogen production . The COF, which is a key component of the photocatalyst, was prepared by assembling benzothiadiazole (BT) and pyrene (Py) derivatives as building blocks. Integrating COF rods into the two-dimensional (2D) layered g-C 3 N 4 structure significantly improved photocatalytic H 2 production. The hybrid system (30 % COF/CN) displayed an outstanding hydrogen evolution rate (HER) of 27540 ± 805 μmol g −1 h −1 , outperforming most known COFs and g-C 3 N 4 -based photocatalysts, besides exhibiting stable photocatalytic performance. Moreover, the apparent quantum yield (AQY) was 15.5 ± 0.8 % at 420 nm. Experimental techniques and density functional theory (DFT) calculations demonstrated that the 30 % COF/CN heterostructure has broad visible-light absorption, adequate band energy levels, and the best chemical reactivity descriptors compared to the individual components, resulting in effective carrier separation and excellent performance. Our findings offer a valuable strategy for developing highly efficient and stable heterojunction photocatalysts for visible-light‐driven H 2 evolution.

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A New Class of NIR-II Gold Nanocluster-Based Protein Biolabels for In Vivo Tumor-Targeted Imaging

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Angewandte Chemie (International ed. in English) 2021年第3期60卷 1306-1312页

作者： Xiaorong Song Wei Zhu Xiaoguang Ge Renfu Li Shihua Li Xian Chen Jibin Song Jianping Xie Xueyuan Chen Huanghao Yang MOE Key Laboratory for Analytical Science of Food Safety and Biology & State Key Laboratory of Photocatalysis on Energy and Environment College of Chemistry Fuzhou University Fuzhou Fujian 350116 China. Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou Fujian 350108 China. CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 China. Department of Chemical and Biomolecular Engineering National University of Singapore 4 Engineering Drive 4 Singapore 117585 Singapore. Joint School of National University of Singapore and Tianjin University International Campus of Tianjin University Binhai New City Fuzhou Fujian 350207 China.

The design of bright NIR-II luminescent nanomaterials that enable efficient labelling of proteins without disturbing their physiological properties in vivo is challenging. We developed an efficient strategy to synthesize bright NIR-II gold nanoclusters (Au NCs) protected by biocompatible cyclodextrin (CD). Leveraging the ultrasmall size of Au NCs (<2 nm) and strong macrocycle-based host-guest chemistry, the as-synthesized CD-Au NCs can readily label proteins/antibodies. Moreover, the labelled proteins/antibodies enable highly efficient in vivo tracking during blood circulation, without disturbing their biodistribution and tumor targeting ability, thus leading to a sensitive tumor-targeted imaging. CD-Au NCs are stable in the harsh biological environment and show good biocompatibility and high renal clearance efficiency. Therefore, the NIR-II biolabels developed in this study provide a promising platform to monitor the physiological behavior of biomolecules in living organisms.

关键词： NIR-II imaging cyclodextrin gold nanoclusters protein labelling tumor imaging

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Correction: Self-powered integrated system of a strain sensor and flexible all-solid-state supercapacitor by using a high performance ionic organohydrogel

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Materials Horizons 2020年第10期7卷 2768-2769页

作者： Jianren Huang Shuijiao Peng Jianfeng Gu Guoqi Chen Jianhong Gao Jin Zhang Linxi Hou Xiaoxiang Yang Xiancai Jiang Lunhui Guan College of Chemical Engineering Fuzhou University Fuzhou 350108 China 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 350108 China School of Mechanical Engineering and Automation Fuzhou University Fuzhou 350108 China

Correction for ‘Self-powered integrated system of a strain sensor and flexible all-solid-state supercapacitor by using a high performance ionic organohydrogel’ by Jianren Huang et al., Mater. Horiz., 2020, 7, 2085–...

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Synthesis,Crystal Structure and Photophysical Property of 2-(9H-carbazol-9-yl)-3-(2-(2,4,5-tri-(9H-carbazol-9-yl)-3,6-dicyanophenoxy)phenoxy)dibenzo[b,e]dioxine-1,4-dicarbonitrile

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Chinese Journal of Structural Chemistry 2018年第9期37卷 1433-1439页

作者：董亚芳余荣民卢灿忠 College of Chemistry Fuzhou University 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

A purely organic compound 2-（9 H-carbazol-9-yl）-3-（2-（2,4,5-tri-（9 H-carbazol-9-yl）-3,6-dicyanophenoxy）phenoxy）dibenzo[b,e][1,4]dioxine-1,4-dicarbonitrile, C76 H40 N8 O4, was synthesized and characterized by NMR, UV-Vis, photoluminescenceand X-ray single-crystal structure analysis. The compound crystallizes in monoclinic system, space group P21/n with a = 11.6537（3）, b = 34.9738（8）, c = 15.5053（3）？, β =101.992（2）°, V = 6181.6（2）？3, Z = 4, Mr= 1129.18 g/mol, Dc =1.396 g/cm3, F（000） =2672, μ = 2.239 mm–1, GOOF = 1.019, the final R = 0.0577 and wR= 0.1559 for 11925 observed reflections with I 〉2σ（I）. The UV-vis absorption and fluorescence of the compound were discussed. The compound exhibitsyellow-green luminescence with maximum emission peak at 538 nm, and quantum yields of ф = 0.25 and 0.48 in air-equilibrated and degassed toluene at room temperature. Transient decay spectral studies show that compound 1 displays two component decay fashions with a short decay lifetime of 23 ns for the prompt fluoresce anda long decay lifetime of 3.8ms for thermally activated delayed fluorescence. In air-equilibrated toluene, only a short decay lifetime of 17 ns was *** experimental and computational results show thatthe emission of the compound originates from the CT excited states.

关键词： purely organic compound synthesis crystal structure luminescence DFT calculation

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Quantized auger recombination of polaronic self-trapped excitons in bulk iron oxide

arXiv

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arXiv 2020年

作者： Liao, Hongyan Fan, Yunyan Lin, Yumei Wang, Kang Li, Renfu Chen, Xueyuan Zhang, Kelvin H.L. Yang, Ye State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical Engineering Xiamen University Xiamen361005 China 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 Fuzhou350002 China

The Auger recombination in bulk semiconductors can depopulate the charge carriers in a non-radiative way, which, fortunately, only has detrimental impact on optoelectronic device performance under the condition of high carrier density because the restriction arising from concurrent momentum and energy conservation limits the Auger rate. Here, we surprisingly found that the Auger recombination in bulk a-Fe2O3 films was more efficient than narrow-bandgap high-mobility semiconductors that were supposed to have much higher Auger rate constants than metal oxides. The Auger process in a-Fe2O3 was ascribed to the Coulombically coupled self-trapped excitons (STEs), which was enhanced by the relaxation of momentum conservation because of the strong spatial localization of these STEs. Furthermore, due to this localization effect the kinetic traces of the STE annihilation for different STE densities exhibited characteristics of quantized Auger recombination, and we demonstrated that these traces could be simultaneously modeled by taking into account the quantized Auger rates. Copyright © 2020, The Authors. All rights reserved.

关键词： Excitons

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Anchoring Cs+Ions on Carbon Vacancies for Selective CO2Electroreduction to CO at High Current Densities in Membrane Electrode assembly Electrolyzers

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Angewandte Chemie 2024年第40期136卷

作者： Yanhui Sun Prof. Junxiang Chen XueMei Du Jiwei Cui Xin Chen Chenhe Wu Xinmin Yang Lequan Liu Prof. Jinhua Ye Advanced Catalytic Materials Research Center School of Materials Science and Engineering Tianjin University Tianjin 300072 China CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou 350002 China International Center for Materials Nanoarchitectonics (WPI-MANA) National Institute for Materials Science (NIMS) Tsukuba 305-0047 Japan

Electrolyte cations have been demonstrated to effectively enhance the rate and selectivity of the electrochemical CO 2 reduction reaction (CO 2 RR), yet their implementation in electrolyte-free membrane electrode assembly (MEA) electrolyzer presents significant challenges. Herein, an anchored cation strategy that immobilizes Cs + on carbon vacancies was designed and innovatively implemented in MEA electrolyzer, enabling highly efficient CO 2 electroreduction over commercial silver catalyst. Our approach achieves a CO partial current density of approximately 500 mA cm −2 in the MEA electrolyzer, three-fold enhancement compared to pure Ag. In situ Raman and theoretical analyses, combined with machine learning potentials, reveal anchored Cs induces an electric field that significantly promotes the adsorption of *CO 2 − intermediates through performing muti-point energy calculations on each structure. Furthermore, reduced adsorption of *OH intermediates effectively hampers competing hydrogen evolution reaction, as clarified by disk electrode experiments and density functional theory studies. Additionally, coupling our system with commercial polysilicon solar cells yields a notable solar-to-CO energy conversion efficiency of 8.3 %. This study opens a new avenue for developing effective cation-promoting strategy in MEA reactors for efficient CO 2 RR.

关键词： anchored Cs CO2 electrolysis high current density CO electric field

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Synthesis,Crystal Structure and Photoluminescence of a TADF Cuprous Complex

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Chinese Journal of Structural Chemistry 2018年第11期37卷 1749-1755页

作者：甘学敏吴小园余荣民卢灿忠 CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Provincial Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of MatterChinese Academy of Sciences Graduate University of Chinese Academy of Sciences

A four-coordinate mononuclear cuprous complex oCBP-Cu-Pym(1, oCBP =1,2-bis(diphenylphosphine)-nido-carborane, Pym = 2-methyl-6-(1 H-pyrazol-1-yl)pyridine) was synthe-sized and characterized by elemental analysis, NMR, UV-Vis and X-ray single-crystal structure analysis. It crystallizes in monoclinic space group C2/c with a = 28.4182(8), b =16.2994(4), c = 22.2708(5) ?, β = 127.219(2)°, V = 8214.8(3) ?3, Z = 8, Mr = 766.92, ρcalc = 1.24 g/cm3, F(000) = 3160, μ = 2.30 mm–1, GOOF = 1.063, the final R = 0.0700 and wR = 0.1903 for7158 observed reflections with I > 2σ(I). The Cu(I) ion adopts a highly distorted tetrahedral geometry defined by two nitrogen and two phosphorous atoms. Under UV 365 nm at room temperature, this complex exhibits green emission with maximum emission peak at 516 nm,lifetime 32.4 μs and quantum yield(ф = 0.461) in the solid state. Photophysical investigation suggests that the emission of complex 1 at room temperature was attributed to TADF, which is strongly supported by theoretic calculation.

关键词： Cu(Ⅰ) complex crystal structure TADF DFT calculation

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Pseudo-2D Layered Organic-Inorganic Manganese Bromide with a Near-Unity Photoluminescence Quantum Yield for White Light-Emitting Diode and X-Ray Scintillator

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Angewandte Chemie 2023年第45期135卷

作者： Wei Zhang Ping Sui Prof. Wei Zheng Prof. Lingyun Li Prof. Shuaihua Wang Prof. Ping Huang Wen Zhang Qi Zhang Prof. Yan Yu Prof. Xueyuan Chen Key Laboratory of Advanced Materials Technologies and International (Hongkong Macao and Taiwan) Joint Laboratory on Advanced Materials Technologies College of Materials Science and Engineering Fuzhou University 350108 Fuzhou Fujian China CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of Nanomaterials State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences 350002 Fuzhou Fujian China Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China 350108 Fuzhou Fujian China

Eco-friendly lead-free organic–inorganic manganese halides (OIMHs) have attracted considerable attention in various optoelectronic applications because of their superior optical properties and flexible solution processibility. Herein, we report a novel pseudo-2D layered OIMH (MTP) 2 MnBr 4 (MTP: methyltriphenylphosphonium), which exhibits intense green emission under UV/blue or X-ray excitation, with a near-unity photoluminescence quantum yield, high resistance to thermal quenching (I 150 °C =84.1 %) and good photochemical stability. These features enable (MTP) 2 MnBr 4 as an efficient green phosphor for blue-converted white light-emitting diodes, demonstrating a commercial-level luminous efficiency of 101 lm W −1 and a wide color gamut of 116 % NTSC. Moreover, these (MTP) 2 MnBr 4 crystals showcase outstanding X-ray scintillation properties, delivering a light yield of 67000 photon MeV −1 , a detection limit of 82.4 nGy s −1 , and a competitive spatial resolution of 6.2 lp mm −1 for X-ray imaging. This work presents a new avenue for the exploration of eco-friendly luminescent OIMHs towards multifunctional light-emitting applications.

关键词： Manganese Halide Photoluminescence Scintillator WLED X-Ray Imaging

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Direct Z-Scheme Heterostructure of In-Situ Planted Zno Nanorods on G-C3n4 Thin Sheets Sprayed on Tio2 Layer: A Strategy for Ternary-Photoanode Engineering Towards Enhanced Photoelectrochemical Water Splitting

SSRN

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SSRN 2023年

作者： Hung, Chen-Hsiung Aboubakr, Ahmed Esmail A. Hussien, Mahmoud Kamal Sabbah, Amr Hassan, Ahmed E. Elsayed, Mohamed Hammad Wen, Zhenhai Chen, Kuei-Hsien Sustainable Chemical Science and Technology Taiwan International Graduate Program Taiwan Department of Applied Chemistry National Yang Ming Chiao Tung University Hsinchu30010 Taiwan Institute of Chemistry Academia Sinica 128 Sec 2 Academia Rd. Nankang Taipei11529 Taiwan Department of Chemistry Faculty of Science Assiut University Assiut71516 Egypt Institute of Atomic and Molecular Sciences Academia Sinica Taipei10617 Taiwan Center for Condensed Matter Sciences National Taiwan University Taipei10617 Taiwan 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 Fujian Fuzhou350002 China University of Chinese Academy of Sciences Beijing100049 China Department of Chemistry Faculty of Science Al-Azhar University Nasr City Cairo11884 Egypt

A novel approach to enhance the separation and transfer of charge carriers of photoanode for photoelectrochemical water splitting has developed. We improved the procedures for in-situ implantation of ZnO on g-C3N4, resulting in strong chemical adhesion between the interface of ZnO and g-C3N4. Our airbrushing procedure for fabricating the g-C3N4/ZnO composite on TiO2 also enhanced the charge collection efficiency, enabling us to construct a high performance photoanode. The Z-scheme type charge migration route was verified by EPR spectroscopy through trapping the radicals generated by charges and holes. PEC-WS measurements showed that TiO2/g-C3N4/ZnO heterostructure improved the produced photocurrent by about 160-, 40-, 20-, 8-, 2-, and 2-fold, relative to pristine g-C3N4, pristine ZnO nanorods, ZnO/g-C3N4 composite, pristine TiO2, TiO2/ZnO, and TiO2/g-C3N4, respectively, versus reversible hydrogen electrode (RHE) at 1.23 V. © 2023, The Authors. All rights reserved.

关键词： Zinc oxide

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Corrigendum to ’Ultrafast-Kinetics, Ultralong-Cycle-Life, Bifunctional Inorganic Open-Framework for Potassium-Ion Batteries’

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Energy Storage Materials 2022年 45卷 1238-1238页

作者： Jingze Bao Wenzhuo Deng Jiandongyong Liu Chuan-Fu Sun CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 P.R. China University of Chinese Academy of Sciences Beijing 100039 P.R. China

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