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Coupling Electron Transfer and Redox Site in Boranil Covalent Organic Framework Toward Boosting Photocatalytic Water Oxidation

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Angewandte Chemie 2024年第13期136卷

作者： Rahul Anil Borse Yan-Xi Tan Jing Lin Enbo Zhou Yangdan Hui Prof. Daqiang Yuan 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 350002 Fuzhou Fujian P. R. China Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China 350108 Fuzhou Fujian P. R. China University of Chinese Academy of Sciences 100049 Beijing P. R. China Institute of Molecular Engineering Plus Fuzhou University 350108 Fuzhou Fujian P. R. China

The efficient polymeric semiconducting photocatalyst for solar-driven sluggish kinetics with multielectron transfer oxygen evolution has spurred scientific interest. However, existing photocatalysts limited by π-conjugations, visible-light harvest, and charge transfer often compromise the O 2 production rate. Herein, we introduced an alternative strategy involving a boranil functionalized-based fully π-conjugated ordered donor and acceptor (D–A) covalent organic frameworks ( Ni-TAPP-COF-BF 2 ) photocatalyst. The co-catalyst-free Ni-TAPP-COF-BF 2 exhibits an excellent ~11-fold photocatalytic water oxidation rate, reaching 1404 μmol g −1 h −1 under visible light irradiation compared to pristine Ni-TAPP-COF (123 μmol g −1 h −1 ) alone and surpasses to reported organic frameworks counterpart. Both experimental and theoretical results demonstrate that the push/pull mechanism (metalloporphyrin/BF 2 ) is responsible for the appropriate light-harvesting properties and extending π-conjugation through chelating BF 2 moieties. This strategy benefits in narrowing band structure, improving photo-induced charge separation, and prolonged charge recombination. Further, the lower spin magnetic moment of M-TAPP-COF-BF 2 and the closer d-band center of metal sites toward the Fermi level lead to a lower energy barrier for *O intermediate. Reveal the potential of the functionalization strategy and opens up an alternative approach for engineering future photocatalysts in energy conversion applications.

关键词： covalent organic frameworks boranil-metalloporphyrin oxygen evolution reaction donor-acceptor-photocatalysts density functional theory

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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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Fluorinated Polyimide Tunneling Layer for Efficient and Stable Perovskite Photovoltaics

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Angewandte Chemie 2024年第21期136卷

作者： Chunming Liu Wei Yu Yuheng Li Can Wang Zilong Zhang Chi Li Lusheng Liang Kangcheng Chen Lin Liu Tinghao Li Xuteng Yu Yao Wang Prof. Peng Gao Institution 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 Laboratory for Advanced Functional Materials Xiamen Institute of Rare Earth Materials Haixi Institute Chinese Academy of Sciences Xiamen 361021 China Fujian College University of Chinese Academy of Sciences Fuzhou 350002 China University of Chinese Academy of Sciences Beijing 100049 China College of Materials Science and Engineering Beijing Institute of Technology Beijing 100081 China Instrumentation and Service Center for Physical Sciences Westlake University Hangzhou 310024 China

Despite the remarkable progress of perovskite solar cells (PSCs), challenges remain in terms of finding effective and viable strategies to enhance their long-term stability while maintaining high efficiency. In this study, a new insulating and hydrophobic fluorinated polyimide (FPI: 6FDA-6FAPB) was used as the interface layer between the perovskite layer and the hole transport layer (HTL) in PSCs. The functional groups of FPI play a pivotal role in passivating interface defects within the device. Due to its high work function, FPI demonstrates field-effect passivation (FEP) capabilities as an interface layer, effectively mitigating non-radiative recombination at the interface. Notably, the FPI insulating interface layer does not impede carrier transmission at the interface, which is attributed to the presence of hole tunneling effects. The optimized PSCs achieve an outstanding power conversion efficiency (PCE) of 24.61 % and demonstrate excellent stability, showcasing the efficacy of FPI in enhancing device performance and reliability.

关键词： fluorinated polyimide perovskite solar cells tunneling layer field-effect passivation

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A Perimidin Derivative with Multiple Redox Centers as an Anode for Lithium-ion Batteries①

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结构化学 2020年第2期

作者： FUYu-Ru LIUQin SUNChuan-Fu 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 350002，China University of Chinese Academy of Sciences，Beijing 100039，China

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Dual-Band-Tunable White-Light Emission from Bi3+/Te4+Emitters in Perovskite-Derivative Cs2SnCl6Microcrystals

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Angewandte Chemie 2022年第9期134卷

作者： Wei Zhang Prof. Wei Zheng Dr. Lingyun Li Prof. Ping Huang Dr. Zhongliang Gong Ziwei Zhou Jinyue Sun Prof. Yan Yu Prof. Xueyuan Chen 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 Fuzhou Fujian 350002 China Key Laboratory of Advanced Materials Technologies College of Materials Science and Engineering Fuzhou University Fuzhou Fujian 350108 China Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou Fujian 350108 China

Luminescent metal halides have attracted considerable attention in next-generation solid-state lighting because of their superior optical properties and easy solution processibility. Herein, we report a new class of highly efficient and dual-band-tunable white-light emitters based on Bi 3+ /Te 4+ co-doped perovskite derivative Cs 2 SnCl 6 microcrystals. Owing to the strong electron-phonon coupling and efficient energy transfer from Bi 3+ to Te 4+ , the microcrystals exhibited broad dual-band white-light emission originating from the inter-configurational 3 P 0,1 → 1 S 0 transitions of Bi 3+ and Te 4+ , with good stability and a high photoluminescence (PL) quantum yield of up to 68.3 %. Specifically, a remarkable transition in Bi 3+ -PL lifetime from milliseconds at 10 K to microseconds at 300 K was observed, as solid evidence for the isolated Bi 3+ emission. These findings provide not only new insights into the excited-state dynamics of Bi 3+ and Te 4+ in Cs 2 SnCl 6 , but also a general approach to achieve single-composition white-light emitters based on lead-free metal halides through ns 2 -metal ion co-doping.

关键词： Bismuth Cs2SnCl6 Excited-State Dynamics Tellurium White-Light Emission

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Self-assembled Nanohybrid from Opposite Charged Sheets:Alternate Stacking of CoAl LDH and MoS2

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Chinese Journal of Structural Chemistry 2018年第7期37卷 1093-1101页

作者：魏艳华李广社王江浩薛程淋方绍帆李莉萍 State Key Laboratory of Inorganic Synthesis & Preparative Chemistry College of 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

Hybrid materials are attracting intensive attention for their applications in electronics, photoelectronics, LEDs, field-effect transistors, etc. Engineering new hybrid materials and further exploiting their new functions will be significant for future science and technique development. In this work, alternatively stacked self-assembled CoAl LDH/MoS2 nanohybrid has been successfully synthesized by an exfoliation-flocculation method from positively charged CoAl LDH nanosheets（CoAl-NS） with negatively charged MoS2 nanosheets（MoS2-NS）. The CoAl LDH/MoS2 hybrid material exhibits an enhanced catalytic performance for oxygen evolution reaction（OER） compared with original constituents of CoAl LDH nanosheets and MoS2 nanosheets. The enhanced OER catalytic performance of CoAl LDH/MoS2 is demonstrated to be due to the improved electron transfer, more exposed catalytic active sites, and accelerated oxygen evolution reaction kinetics.

关键词： CoAl LDH/MoS2 nanohybrid exfoliation-flocculation method self-assembly electrocatalytic oxygen evolution reaction

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Efficient CO_2 Electrolysis with Fluorite Structure Nanoparticles Modified Perovskite Structure La_(0.75)Sr_(0.25)Cr_(0.5)Mn_(0.5)O_(3-δ) Cathode

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Chinese Journal of Structural Chemistry 2018年第10期37卷 1596-1602页

作者： WANG Wen-Yuan HOU Shi-Sheng HU Xiu-Lia XIE Kui 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 SciencesFuzhou 350002China College of Chemistry and Materials Science Fujian Normal UniversityFuzhou 350007China

Perovskite structure La_（0.75）Sr_（0.25）Cr_（0.5）Mn_（0.5）O_（3-δ）（LSCM） cathode with unique structure can electrolyze CO_2 to CO in solid oxide electrolysers（SOEs）.However,the cell performance is restricted by its electro-catalysis *** this work,fluorite structure nanoparticles（CeO_（2-δ）） are impregnated on LSCM cathode to improve the electro-catalysis activity.X-ray diffraction（XRD）,scanning electron microscope（SEM） and X-ray photoelectron spectroscopy（XPS） together approve that the fluorite structure nanoparticles are uniformly distributed on the perovskite structure LSCM *** measurements illustrate that direct CO_2 electrolysis with 10%mol CeO_（2-δ） impregnated LSCM cathode exhibits excellent performance for current density（0.5 A×cm^（-2）） and current efficiency（～95%） at 800 ℃ under 1.6 *** is believed that the enhanced performance of directed CO_2 electrolysis may be due to the synergetic effect of fluorite structure CeO_（2-δ） nanoparticles and perovskite structure LSCM ceramic electrode.

关键词： perovskite structure fluorite structure LSCM solid oxide electrolysers impregnation

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Correction: Efficiently increasing the radiative rate of TADF material with metal coordination

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Chemical communications (Cambridge, England) 2022年第84期58卷 11871页

作者： Xian-Bao Cai Dong Liang Mingxue Yang Xiao-Yuan Wu Can-Zhong Lu Rongmin Yu College of Chemical Engineering Fuzhou University Fuzhou 350116 P. R. China. rongminyu@***. 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. University of Chinese Academy of Sciences Beijing 100049 China.

Correction for 'Efficiently increasing the radiative rate of TADF material with metal coordination' by Xian-Bao Cai , , 2022, , 8970-8973, https://***/10.1039/D2CC02930H.

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Artificial Photosynthetic Cell with Molecular Biomimetic Thylakoid

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Angewandte Chemie 2024年第4期137卷

作者： Enbo Zhou Shichen Yan Xiang Zhang Ateeq Ur Rehman Baloch Yangdan Hui Futong Wang Lei Jiao Jiafang Xie Prof. Daqiang Yuan Prof. Yaobing Wang Fujian Agriculture and Forestry University Fuzhou 350002 Fujian P. R. China CAS Key Laboratory of Design and Assembly of Functional Nanostructures 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 Key Laboratory of Urban Pollutant Conversion Institute of Urban Environment Chinese Academy of Sciences Xiamen P. R. China Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108 Fujian P. R. China

The construction of solar-to-chemical conversion system by mimicking the photosynthetic network of the chloroplast holds great promise on efficient solar energy utilization. We developed an artificial photosynthetic cell (APC) based on molecular biomimetic thylakoid (CoTPP-FePy) to split water into hydrogen and oxygen (H 2 and O 2 ) at low driving voltage (1.1 V) and neutral condition (pH≈7). The CoTPP-FePy can emulate the light reaction in thylakoids to produce O 2 by coupling light harvesting, photocatalysis, and electron/energy storage (Fe III /Fe II −Py). Subsequently, a membrane electrode assembly (MEA) were employed to simulate the dark reaction, wherein the proton, electron and energy generated by the light reaction can drive the H 2 producing process. By a temporally and spatially coupling of the light and dark reactions, the resulting APC achieved a solar conversion efficiency of 3.1 %, exceeding that of natural photosynthetic systems and demonstrating the potential of artificial photosynthesis.

关键词： Artificial photosynthesis Photocatalytic water oxidation Water splitting Metal organic cage Biomimetic chemistry

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Synthesis and Characterization of a Novel Coordination Complex Based on Fluorescein

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Chinese Journal of Structural Chemistry 2018年第1期37卷 113-118页

作者：张冠华吴小园王洒洒蒋晓瑜卢灿忠 Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of MatterChinese Academy of Sciences Graduate University of Chinese Academy of Sciences Fujian University of Technology

A novel coordination complex,{[Cd）2（C（20）H（10）O5）2（H2O）4]·10H2O}n,has been synthesized based on fluorescein（2-（6-hydroxy-3-oxo-3 H-xanthen-9-yl） benzoic acid） and systematically characterized by elemental analysis,infrared（IR） spectrum,thermo gravimetric analysis（TGA）,powder X-ray diffraction（PXRD） and single-crystal X-ray *** 1 crystallizes in monoclinic,space group P2/n with a = 20.428（5）,b = 8.084（2）,c = 21.689（5）A,β = 96.360（5）°,Mr = 993.46,V = 3559.7（15）A^3,Z = 4,Dx = 1.845 g/cm^3,μ = 1.276 mm^-1,F（000） = 1974,GOOF = 1.044,λ（Mo Kα） = 0.71073 ？,the final R = 0.0553 and wR = 0.1720 for 7245 observed reflections with I 〉 2σ（I）.

关键词： crystal structure coordination complex fluorescein

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