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Broadband NIR photon upconversion generates NIR persistent luminescence for bioimaging

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arXiv

arXiv 2024年

作者： Yang, Shuting Qi, Bing Sun, Mingzi Dai, Wenjing Miao, Ziyun Zheng, Wei Huang, Bolong Wang, Jie The Key Lab of Health Chemistry & Molecular Diagnosis of Suzhou College of Chemistry Chemical Engineering & Materials Science Soochow University Suzhou215123 China Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic University Hung Hom Kowloon Hong Kong 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 the Structure of Matter Chinese Academy of Sciences Fujian Fuzhou350002 China

Upconversion persistent luminescence (UCPL) phosphors that can be directly charged by near-infrared (NIR) light have gained considerable attention due to their promising applications ranging from photonics to biomedicine. However, current lanthanide-based UCPL phosphors show small absorption cross-sections and low upconversion charging efficiency. The development of UCPL phosphors faces challenges of lacking flexible upconversion charging pathways and poor design flexibility. Herein, we discovered a new lattice defect-mediated broadband photon upconversion process and the accompanied NIR-to-NIR UCPL in Cr-doped zinc gallate nanoparticles. The zinc gallate nanoparticles can be directly activated by broadband NIR light in the 700-1000 nm range to produce persistent luminescence at about 700 nm, which is also readily enhanced by rationally tailoring the lattice defects in the phosphors. This proposed UCPL phosphors achieved a signal-to-background ratio of over 200 in bioimaging by efficiently avoiding interference from autofluorescence and light scattering. Our findings reported the lattice defect-mediated photon upconversion for the first time, which significantly expanded the horizons for the flexible design of NIR-to-NIR UCPL phosphors toward broad applications. Copyright © 2024, The Authors. All rights reserved.

关键词： Bioimaging

F-containing cations improve the performance of perovskite solar cells

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Journal of Semiconductors 2022年第1期43卷 4-8页

作者： Qin Zhou Chuantian Zuo Zilong Zhang Peng Gao Liming Ding Key Laboratory of Design and Assembly of Functional Nanostructures(CAS) Fujian Institute of Research on the Structure of Matter(CAS)Fuzhou 350002China Center for Excellence in Nanoscience(CAS) Key Laboratory of Nanosystem and Hierarchical Fabrication(CAS)National Center for Nanoscience and TechnologyBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China Laboratory for Advanced Functional Materials Xiamen Institute of Rare Earth MaterialsHaixi Institute(CAS)Xiamen 361021China

Organic–inorganic halide perovskite solar cells(PSCs)have delivered power conversion efficiency(PCE)on par with that of crystalline silicon solar cells,due to the considerable effort on the optimization of perovskite materials and devices[1].The three-dimensional(3D)perovskite-based PSCs with the standard n–i–p architecture gave a certified PCE of25.5%[2].However,the poor device stability under operating conditions remains an obstacle to *** 3D hybrid perovskite materials are susceptible to oxygen,UV light,humidity,heat,and electric fields[3].To improve device stability,two main strategies are applied:(1)improving the intrinsic stability[4];(2)providing sufficient protection.

关键词： perovskite stability inorganic

Microporous and Grain-Sized design of High-Yield Porous Carbon Materials by Using Potassium Acetate and P-Phenylenediamine

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SSRN 2023年

作者： Shen, Zhongrong Cheng, Lin Zhang, Kai Nie, Qiaojun Wang, Gang Cai, Xiaokang Zhang, Ming Liu, Chao College of Chemistry Fuzhou University Fuzhou350108 China CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of Nanomaterials Fujian Institute of Research The Structure of Matter Chinese Academy of Sciences Fuzhou350002 China Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials Xiamen Institute of Rare Earth Materials Haixi Institute Chinese Academy of Sciences Xiamen361021 China Xiamen Tungsten Co. Ltd Xiamen361009 China

Porous carbon with large specific surface area (SSA) and high porosity is an ideal electrode material for supercapacitors. However, the traditional KOH activation remains several barriers, such as low yield, high corrosion, and pollution. In this paper, nitrogen-doped (1.68% N content) porous carbon (C-PKAC1.5) with high yield (26.3%), large SSA (2820.65 m2/g) and uniform size was prepared from p-phenylenediamine (PDA) in one-pot by using potassium acetate (KAc) instead of KOH. Throughout the process, KAc played the vital roles: 1) KAc could form hydrogen bonding network with PDA and mixed homogeneously, while PDA providing nitrogen dopant and carbon source. 2) After polymerization, the KAc lamellae reconstituted and achieved geometric partition of polymer matrix, left diffusion micro-tunnels and provided homogenized size of carbon particles at the following stage. 3) During activation, KAc melt and diffused into polymer matrix through micro-tunnels and converted to K2CO3 to activate from inside to outside, while avoiding the low yield for conventional activation from outside to inside. The supercapacitor assembled for C-PKAC1.5 exhibits high specific capacitance of 25.17 F/g and 82.77% of capacitance retention after 30,000 cycles, and achieves a high energy density of 8.29 Wh/L at a power density of 199.25 W/L. © 2023, The Authors. All rights reserved.

关键词： Supercapacitor

Metal-Organic Framework-Derived Heterostructural Bi-Sm2o3 as a Novel Sulfur Immobilizer for High-Performance Lithium-Sulfur Batteries

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SSRN 2023年

作者： Lai, Xiaoxu Chen, Qiujie Wang, Haodong Chen, Chengwei Chen, Zifang Chen, Chi Sun, Dan 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 College of Chemistry and Materials Fujian Normal University Fujian Fuzhou350007 China Xiamen Institute of Rare Earth Materials Haixi Institutes Chinese Academy of Sciences Xiamen361021 China Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials Xiamen361021 China

Owing to their high theoretical energy density, low cost, and eco-friendliness, lithium-sulfur (Li-S) batteries are one of the most promising alternatives to Li-ion batteries. However, the commercialization of Li-S batteries has been hampered by their rapid capacity fading and poor cycling lifetime due to the shuttling and sluggish redox kinetics of polysulfides (LiPSs). To address these issues, functionalizing a commercial separator is a simple and effective strategy. In this study, we developed a novel modified polypropylene separator coated with samarium-based metal-organic framework-derived heterostructural bi-phased Sm2O3 (Bi-Sm2O3), which contains cubic Sm2O3 (C-Sm2O3) and monoclinic Sm2O3 (M-Sm2O3) phase in a single polycrystalline particle. The alleviated "shuttle effect" of LiPSs can be achieved by synergistic effect at the Bi-Sm2O3 surface through strong adsorption of LiPSs on M-Sm2O3 surface followed by catalytic conversion over C-Sm2O3. An optimized Bi-Sm2O3-modified separator with a thickness of 150 µm can enable the Li-S battery to deliver an improved cycling and rate performance with a high specific capacity of 860.1 mAh g−1 at 2 C and a low decay rate of 0.11% per cycle over 500 cycles at 1 C. © 2023, The Authors. All rights reserved.

关键词： Separators

Controllable Preparation of Cu2o/Cu-Cutcpp Mof Heterojunction for Enhanced Electrocatalytic Co2 Reduction to C2h4

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SSRN 2024年

作者： Sun, Miao Xu, Xiao Min, Shihao He, Jiaxin Li, Kun Kang, Longtian Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Provincial Key Laboratory of Nanomaterials Fujian Institute of Research The Structure of Matter Chinese Academy of Sciences Fujian Fuzhou350002 China College of Chemistry and Materials Science Fujian Normal University Fuzhou350007 China Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China Fujian Fuzhou350108 China University Chinese Academy of Science Fujian College Fuzhou350002 China

Copper-based metal-organic framework (Cu-MOF) materials with multiple active sites have attracted increasing attention to the electrocatalytic CO2 reduction reaction (ECR), however, face the huge challenge owing to the poor stability and low C2 selectivity. Here, the Cu2O/Cu-CuTCPP heterojunction (Cu2O/CPFs) with three Cu active sites are firstly constructed through in-situ electrodeposition method. The effect of CuSO4 concentration and electrodeposition conditions on ECR is systematically investigated. The optimized Cu2O/CPFs composite achieves the ethylene Faraday efficiency (FEC2H4) of 61.8% at –1.3 V vs. RHE, which is 1.9 and 3.42 times higher than those of CPFs and Cu2O, respectively. Meanwhile, the C2H4 partial current density (jC2H4) of –7.96 mA·cm-2 is 2.91 and 4.68 times higher than those of CPFs and Cu2O. Further experiments reveals that the formation of Cu2+-O–Cu+–O bond between Cu2O and Cu–O4 sites in Cu2O/CPF heterojunction is crucial. Consequently, the hydrogen (H2), formic acid (HCOOH) and methane (CH4) evolution reactions are restricted, the C–C coupling reaction of *CHO and *CO intermediates is significantly enhanced, and the Cu–O4 sites in CPFs are protected. This work provides an effective strategy to stabilize MOF structure and obtain high value-added C2+ products. © 2024, The Authors. All rights reserved.

关键词： Heterojunctions

Multiple Strategies from Apparatus to Synthetic Process Toward High-Performance Spherical Manganese Hexacyanoferrate for Sodium-Ion Batteries

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SSRN 2024年

作者： Zheng, Jun Wang, Gang Zhang, Kai Zheng, Jiafan Fu, Wenwu Zhang, Chengyu Liu, Jiayi Wang, Jieyuan Li, Junwei Cai, Fu Huang, Wenbo Zhang, Ming Shen, Zhongrong 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 Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials Xiamen Institute of Rare Earth Materials Haixi Institutes Chinese Academy of Sciences Xiamen361021 China College of Chemistry and Materials Science Fujian Normal University Fuzhou350007 China University of Chinese Academy of Sciences Beijing101408 China Xiamen 3-circles Battery Co. Ltd Xiamen361023 China

Traditional cube Prussian blue analogs with limited processability and low density are not suitable for the fabrication of high energy density sodium-ion batteries. Here, we present a novel reactor called the dual-vortexed coprecipitation chamber (DVCC) and a corresponding click reaction mechanism for producing high-density, size-controllable, spherical and low-deficiency manganese-based Prussian blue analogs. Through the optimized controlled crystallization precipitation technique, we are able to precisely regulate the nucleation, crystallization and spherical agglomeration process. In comparison to cubic crystals, our unique spherical particles exhibited superior performance with a controllable size distribution of 0 ~ 40 μm, compacted density of 1.60 g cm-3, an initial capacity of 132.5 mAh g-1 and notably retention rates of 99.5% for coin cell and 86.7% for pouch cell respectively after 500 cycles at 1 C rate. Benefit by the low H2O content (less than 300 ppm) in the electrodes, the pouch cell avoided gas expansion and also demonstrated excellent fast discharge capability with a retention of 78.7% at a maximum rate of 40C compared to 1C rate. © 2024, The Authors. All rights reserved.

关键词： Metal ions

"Chameleon-like" optical behavior of lanthanide-doped fluoride nanoplates for multilevel anti-counterfeiting applications

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Nano Research 2019年第6期12卷 1417-1422页

作者： Wenwu You Datao Tu Renfu Li Wei Zheng Xueyuan Chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China

Lanthanide-based luminescent anti-counterfeiting materials are widely used in various kinds of ***,the emission color of traditional lanthanide-based luminescent materials usually remains nearly unaltered upon different excitation lights,which may only work for single-level ***,the NaYbF4∶2%Er@NaYF4 core/shell nanoplates (NPs) with "chameleon-like" optical behavior are *** NPs display single-band red or green downshifting (DS) emission upon excitation at 377 or 490 nm,*** 980 nm excitation,the color of upconversion (UC) emission can be finely tuned from green to yellow,and to red with increasing the excitation power density from 0.1 to 4.0 W/cm^*** proposed materials readily integrate the advantages of excitation wavelength-dependent DS single-band emissions and sensitive excitation power-dependent UC multicolor emissions in one and the same material,which has never been reported ***,the proposed NPs exhibit excellent performance as security labels on trademark tag and security ink on painting,thus revealing the great potential of these lanthanide-doped fluoride NPs in multilevel anti-counterfeiting applications.

关键词： lanthanide-doped chameleon-like upconversion downshifting multilevel anti-counterfeiting

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 toward Enhanced Photoelectrochemical Water Splitting

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ACS Applied Energy Materials 2024年第3期7卷 906-918页

作者： Aboubakr, Ahmed Esmail A. Hussien, Mahmoud Kamal Sabbah, Amr Hassan, Ahmed E. Elsayed, Mohamed Hammad Wen, Zhenhai Chen, Kuei-Hsien Hung, Chen-Hsiung Sustainable Chemical Science and Technology Taiwan International Graduate Program Academia Sinica Taipei11529 Taiwan Department of Applied Chemistry National Yang Ming Chiao Tung University Hsinchu30010 Taiwan Institute of Chemistry Academia Sinica 128 Sec 2 Academia Rd. Taipei11529 Taiwan Department of Chemistry Faculty of Science Assiut University Assiut71516 Egypt Center for Condensed Matter Sciences National Taiwan University Taipei10617 Taiwan Tabbin Institute for Metallurgical Studies Tabbin Helwan 109 Cairo11421 Egypt 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 Fujian Fuzhou350002 China University of Chinese Academy of Sciences Beijing100049 China Institute of Atomic and Molecular Sciences Academia Sinica Taipei10617 Taiwan Department of Chemistry Faculty of Science Al-Azhar University Cairo11884 Egypt

In this study, we developed an approach to enhance the separation and transfer of charge carriers for photoelectrochemical water splitting in solar-driven hydrogen production. We achieved this by designing a highly efficient Z-scheme TiO2/g-C3N4/ZnO photoanode. The process involved electrodepositing a thin TiO2 layer on FTO and optimizing the in situ ZnO implantation onto g-C3N4. These composites were confirmed by XRD, SEM, EDX, and TEM measurements. The growth of ZnO on g-C3N4 resulted in strong chemical adhesion between the interface of ZnO and g-C3N4, as supported by XPS data, and increased active surface area, as demonstrated by BET. The composition of ZnO and g-C3N4 facilitated rapid charge separation and retarded change recombination through directional charge migration and decreased charge resistance, as evidenced by PEIS and TRPL measurements. 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 by 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. The charge carriers’ separation and injection measurements showed that the fabrication of this ternary photoanode remarkably improved the PEC-WS performance. DFT results contributed to a deeper understanding of the mechanism of the photocatalytic process and confirmed that the as-fabricated ternary heterojunction promoted the separation/transfer efficiency of the photogenerated charge carriers, thereby promoting the activity of the photocatalytic process. This work could pave the way for bette

关键词： Zinc oxide

Synthesis, Structure, and Magnetism of a Rhombic Metallocycle

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SSRN 2023年

作者： Wu, Zhi-Yan Chen, Ting Huang, Min Nan, Zi-Ang Liao, Jin-Sheng Zhuo, Zhu Huang, You-Gui School of Material and Chemistry Engineering Jiangxi University of Science and Technology Jiangxi Ganzhou341000 China CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Provincial Key Laboratory of Nanomaterials Fujian Institute of Research The Structure of Matter Chinese Academy of Sciences China Xiamen Institute of Rare Earth Materials Haixi Institutes Chinese Academy of Sciences Xiamen361021 China

A rhombic metallocycle [CoII6Cl6(L‒H+)2(L‒2H+)2]·6DMF·6H2O (1) (L = tris(2-naphthimidazolylmethyl) amine) composed of two CoIICl(L‒H+) moieties and two CoIICl(L‒2H+) moieties alternately bridged by two μ3-CoII ions has been synthesized under solvothermal condition. Each metallocycle associate with its six neighbors through intermolecular π···π interactions between naphthimidazolylmethyl arms forming a supramolecular framework with a distorted pcu network. Magnetic measurements on the metallocycle reveal dominant antiferromagnetic couplings between CoII centers. © 2023, The Authors. All rights reserved.

关键词： Supramolecular chemistry