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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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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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A strategy for accurate detection of glucose in human serum and whole blood based on an upconversion nanoparticles-polydopamine nanosystem

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Nano Research 2018年第6期11卷 3164-3174页

作者： Yan Liu Datao Tu Wei Zheng Lianyu Lu Wenwu You Shanyong Zhou Ping Huang Renfu Li Xueyuan Chen 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 100049 China

The accurate detection of blood glucose is of critical importance in the diagnosis and management of diabetes and its complications. Herein, we report a novel strategy based on an upconversion nanoparticles-polydopamine （UCNPs-PDA） nanosystem for the accurate detection of glucose in human serum and whole blood through a simple blending of test samples with ligand-free UCNPs, dopamine, and glucose oxidase （GOx）. Owing to the high affinity of lanthanide ions exposed on the surface of ligand-free UCNPs, dopamine monomers could spontaneously attach to the UCNPs and further polymerize to form a PDA shell resulting in a remarkable upconversion luminescence （UCL） quenching （97.4%） of UCNPs under 980-nm excitation. Such UCL quenching can be effectively inhibited by H2O2 produced from the GOx/glucose enzymatic reaction, thus enabling the detection of H2O2 or glucose based on the UCL quenching/inhibition bioassay. Owing to the highly sensitive UCL response and background-free interference of the UCNPs-PDA nanosystem, we achieved a sensitive, selective, and high-throughput bioassay for glucose in human serum and whole blood, thereby revealing the great potential of the UCNPs-PDA nanosystem for the accurate detection of blood glucose or other HRO2-generated biomolecules in clinical bioassays.

关键词： upconversion nanoparficles polydopamine F6rster resonance energy transfer blood glucose bioassay

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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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Molten-Salt-Assisted Synthesis of Bismuth Nanosheets for Long-term Continuous Electrocatalytic Conversion of CO2 to Formate

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Angewandte Chemie 2020年第45期132卷

作者： Yi L. Chen J. Shao P. Huang J. Peng X. Li J. Wang G. Zhang C. Wen Z. 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 Fuzhou 350002 China University of Chinese Academy of Science Beijing 100049 China

Two-dimensional (2D) monometallic pnictogens (antimony or Sb, and bismuth or Bi) nanosheets demonstrate potential in a variety of fields, including quantum devices, catalysis, biomedicine and energy, because of their unique physical, chemical, electronic and optical properties. However, the development of general and high-efficiency preparative routes toward high-quality pnictogen nanosheets is challenging. A general method involving a molten-salt-assisted aluminothermic reduction process is reported for the synthesis of Sb and Bi nanosheets in high yields (>90 %). Electrocatalytic CO2 reduction was investigated on the Bi nanosheets, and high catalytic selectively to formate was demonstrated with a considerable current density at a low overpotential and an impressive stability. Bi nanosheets continuously convert CO2 into formate in a flow cell operating for one month, with a yield rate of 787.5 mmol cm−2 h−1. Theoretical results suggest that the edge sites of Bi are far more active than the terrace sites. © 2020 Wiley-VCH GmbH

关键词： bismuth nanosheets electrocatalysis formate long-term operation selectivity

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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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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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Ultrasensitive detection of cancer biomarker microRNA by amplification of fluorescence of lanthanide nanoprobes

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Nano Research 2018年第1期11卷 264-273页

作者： Lianyu Lu Datao Tu Yan Liu Shanyong Zhou Wei Zheng Xueyuan Chen College of Chemistry Fuzhou University Fuzhou 350116 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 350002 China

Sensitive detection of cancer biomarker microRNAs （miRNAs） is of vital importance for cancer diagnosis and treatment. Nonetheless, the detection sensitivity in the existing miRNA bioassays is severely limited by the structural characteristics of miRNA （including small length and high sequence homology） because most of these methods are based on target amplification. Herein, we report a novel approach to sensitive and specific detection of low-abundance miRNA via a unique strategy of nanoprobe dissolution-enhanced fluorescence amplification, in which a capture probe featuring molecular beacon structure is designed. By means of this strategy, miRNA-21 was detected in a linear range from 10 fM to 100 pM with a detection limit as low as 1.38 fM. High selectivity of the newly developed biosensor was demonstrated by the good discrimination against a target with a single-base mismatch. Furthermore, this assay was used for the detection of miRNA-21 added into fetal bovine serum samples with the recovery in the range of 90.2%--108% and coefficients of variation below 10.1%, indicating its promising applications to RNA immunoassays and early cancer diagnosis.

关键词： microRNA lanthanide nanoparticles fluorescence amplification cancer biomarker molecular beacon

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Effective reduction of matrix thermal conductivity through composite softening

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Newton 2025年第1期1卷

作者： Jiajing Huang James Patrick Male Yandong Sun Ramya Gurunathan Pochung Huang Gerald Jeffrey Snyder Yue Lin CAS Key Laboratory of Design and Assembly of Functional Nanostructures and State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 China Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou Fujian 350108 China University of Chinese Academy of Sciences Beijing 100049 China Department of Materials Science and Engineering Northwestern University Evanston IL 60208 USA Materials Science and Engineering Division National Institute of Standards and Technology Gaithersburg 20899 MD USA

Conventional wisdom suggests that incorporating high-thermal-conductivity nanomaterials, such as graphene and carbon nanotubes, can enhance the thermal conductivity of composite matrices. However, our study on graphene nanoplatelets (GNPs) within a lead telluride (PbTe) matrix, along with an extensive review of 18 composites, reveals that such additions can lead to a significant decrease in thermal conductivity. This reduction is attributed to a decrease in phonon velocity, as seen by measuring the sound velocity v s , which strongly impacts lattice thermal conductivity ( κ L ). For instance, a volume fraction of just 1.47% GNPs results in an 11.1% reduction in PbTe’s v s , cutting κ L by 29.7%. We introduce a dimensionless parameter, χ , derived from the contrasts in Young’s modulus and density between the composite constituents. This parameter allows for the prediction of the degree to which v s and, consequently, κ L are reduced, based on the mechanical properties of the composite components. Alongside interfacial phonon scattering, this research pivots the focus toward composite softening as a critical factor in manipulating thermal conductivity.

关键词： structure-properties relationship composites phenomenological model thermal conductivity graphene thermoelectrics

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Synthesis,Crystal Structure and Photoluminescence of a Dinulear Copper Complex

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Chinese Journal of Structural Chemistry 2018年第10期37卷 1645-1650页

作者： LI Xiao-Ning WU Xiao-Yuan ZHAO Wan-Wan YANG Ming-Xue YU Rong-Min LU Can-Zhong 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 College of Chemistry and Materials Science Fujian Normal University

A binuclear cuprous complex [Cu（μ-I）（NPPh）]2（1,NPPh = 1-（2-（diphenylphosphanyl）phenyl）-3-phenyl-4,5-dihydro-1 H-pyrazole） was synthesized and characterized by elemental analysis,NMR and X-ray single-crystal structure *** crystallizes in triclinic space group P2_1/n with a = 10.7520（3）,b = 18.1860（5）,c = 11.8487（3）？,β = 91.864（2）,V = 2315.61（11）？~3,Z = 4,Mr = 594.87,Dc = 1.706 g/cm^3,F（000） = 1176.0,μ = 12.582 mm（-1）,GOOF = 1.048,the final R = 0.0289 and wR = 0.0670 for 3787 observed reflections with I 〉 2σ（I）.The Cu atoms in the complex are four-coordinated and adopt distorted tetrahedral coordination *** the solid state,the complex exhibits greenish yellow photoluminescence with a peak maximum of 533 nm,a decay time of 34 μs,and a photoluminescence quantum yield of 63.6% at room temperature,respectively.

关键词： cuprous complex crystal structure emissive property

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