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

Angewandte Chemie 2020年第3期133卷

作者： Dr. Xiaorong Song Wei Zhu Xiaoguang Ge Renfu Li Dr. Shihua Li Dr. Xian Chen Prof. Jibin Song Prof. Jianping Xie Prof. Xueyuan Chen Prof. 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： cyclodextrin gold nanoclusters NIR-II imaging protein labelling tumor imaging

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Safe, Low‐Cost, Fast‐Kinetics and Low‐Strain Inorganic‐Open‐Framework Anode for Potassium‐Ion Batteries

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Angewandte Chemie 2019年第46期131卷

作者： Ruding Zhang Jiajia Huang Wenzhuo Deng Jingze Bao Yilong Pan Shuping Huang Chuan‐Fu Sun 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 P. R. China College of Chemistry Fuzhou University Fuzhou Fujian 350108 P. R. China

A key challenge for potassium‐ion batteries is to explore low‐cost electrode materials that allow fast and reversible insertion of large‐ionic‐size K + . Here, we report an inorganic‐open‐framework anode (KTiOPO 4 ), which achieves a reversible capacity of up to 102 mAh g −1 (307 mAh cm −3 ), flat voltage plateaus at a safe average potential of 0.82 V (vs. K/K + ), a long lifespan of over 200 cycles, and K + ‐transport kinetics ≈10 times faster than those of Na‐superionic conductors. Combined experimental analysis and first‐principles calculations reveal a charge storage mechanism involving biphasic and solid solution reactions and a cell volume change (9.5 %) even smaller than that for Li + ‐insertion into graphite (≈10 %). KTiOPO 4 exhibits quasi‐3D lattice expansion on K + intercalation, enabling the disintegration of small lattice strain and thus high structural stability. The inorganic open‐frameworks may open a new avenue for exploring low‐cost, stable and fast‐kinetic battery chemistry.

关键词： Elektrochemie Schnelle Kinetik Anorganische offene Netzwerke Geringe Deformation Kalium-Ionen-Batterien

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Graphene‐Oxide‐Modified Lanthanide Nanoprobes for Tumor‐Targeted Visible/NIR‐II Luminescence Imaging

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Angewandte Chemie 2019年第52期131卷

作者： Xiaorong Song Shihua Li Hanhan Guo Wenwu You Xiaoying Shang Renfu Li Datao Tu Wei Zheng Zhuo Chen Huanghao Yang 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 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

The synthesis of hydrophilic lanthanide‐doped nanocrystals (Ln 3+ ‐NCs) with molecular recognition ability for bioimaging currently remains a challenge. Herein, we present an effective strategy to circumvent this bottleneck by encapsulating Ln 3+ ‐NCs in graphene oxide (NCs@GO). Monodisperse NCs@GO was prepared by optimizing GO size and core–shell structure of NaYF 4 :Yb,Er@NaYF 4 , thus combining the intense visible/near‐infrared II (NIR‐II) luminescence of NCs and the unique surface properties and biomedical functions of GO. Such nanostructures not only feature broad solvent dispersibility, efficient cell uptake, and excellent biocompatibility but also enable further modifications with various agents such as DNA, proteins, or nanoparticles without tedious procedures. Moreover, we demonstrate in proof‐of‐concept experiments that NCs@GO can realize simultaneous intracellular tracking and microRNA‐21 visualization, as well as highly sensitive in vivo tumor‐targeted NIR‐II imaging at 1525 nm.

关键词： Graphenoxid Lanthanoide Lumineszierende Nanosonden NIR-II-Bioimaging Tumoradressierung

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Correction: Tumor acidity-responsive carrier-free nanodrugs based on targeting activation via ICG-templated assembly for NIR-II imaging-guided photothermal-chemotherapy

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Biomaterials science 2021年第3期9卷 1047页

作者： Kaihang Xue Feng Wei Jinyan Lin Haina Tian Fukai Zhu Yang Li Zhenqing Hou Department of Biomaterials College of Materials Research Center of Biomedical Engineering of Xiamen & Key Laboratory of Biomedical Engineering of Fujian Province Xiamen University Xiamen 361005 P. R. China. linjinyan1988@***. Neurosurgical Department of Affiliated Zhongshan Hospital Xiamen University Xiamen 361004 P. R. China. Department of Biomaterials College of Materials Research Center of Biomedical Engineering of Xiamen & Key Laboratory of Biomedical Engineering of Fujian Province Xiamen University Xiamen 361005 P. R. China. linjinyan1988@*** and The United Innovation of Mengchao Hepatobiliary Technology Key Laboratory of Fujian Province Mengchao Hepatobiliary Hospital of Fujian Medical University Fuzhou 350025 P. R. 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 P. R. China. liyang@*** and Department of Translational Medicine Xiamen Institute of Rare Earth Materials Chinese Academy of Sciences Xiamen 361024 P. R. China.

Correction for 'Tumor acidity-responsive carrier-free nanodrugs based on targeting activation via ICG-templated assembly for NIR-II imaging-guided photothermal-chemotherapy' by Kaihang Xue et al., Biomater. Sc...

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Manipulating Energy Transfer in Lanthanide-Doped Single Nanoparticle for Highly Enhanced Upconverting Luminescence

Manipulating Energy Transfer in Lanthanide-Doped Single Nano...

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中国稀土学会2017学术年会

作者： Yongsheng Liu Zhuo Zhu Maochun Hong CAS Key Laboratory of Optoelectronic Materials Chemistry and Physics CAS Key Laboratory of Design and Assembly of Functional Nanostructuresand State Key Laboratory of Structural ChemistryFujian Institute of Research on the Structure of MatterCAS

Energy transfer（ET） is of fundamental importance in tuning the optical performance for lanthanide-doped upconversion（UC） nanoparticles（UCNPs） that have currently attracted tremendous interest for their application in diverse fields such as biodetection,bioimaging,multiplexed encoding and 3D full-color ***,fine control and manipulation of the ETs particularly for deleterious cross-relaxation type ETs（CR-ETs） that are ubiquitous in lanthanide-doped UCNPs remains a formidable *** this work,we demonstrate for the first time a general and novel strategy to manipulate the deleterious CR-ETs in UCNPs,by fine-tuning the distances at an extremely large length scale（>20 nm,a distance hard to be tuned by traditional core-shell strategy） among multiple lanthanide emitters that are simultaneously embedded in one single nanoparticle with specially designed multilayer *** successful inhibition of the CR-ETs leads to significantly enhanced UC emission with an intensity 0 times higher than conventional UCNPs,along with a much higher absolute UC quantum yield（3.9 %）.Such improved UC properties coupled with the design flexibility of the multilayer structure thereby enable us to fabricate a series of highly photostable UCNPs with well-identified UC color and lifetime outputs that function well as promising single-nanocrystal-based UC barcodes for advanced anti-counterfeiting,which had not been realized *** findings may open up a new avenue for better control of the CR-ETs at the nanoscale within one single nanocrystal,and present a substantial advance as compared to previous work and thus could be a breakthrough in the development of single-nanocrystal-based UC barcodes for advanced anti-counterfeiting or biosensing.

关键词： Upconversion Lanthanide Ions Energy Transfer Luminescent Nanoparticle Multilayer Structures

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A 3-D Selected Solvent Large Aperture MOF

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Chinese Journal of Structural Chemistry 2016年第10期35卷 1568-1573页

作者：火苗杨文斌吴小园卢灿忠林琅 Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of MatterChinese Academy of Sciences

The metal-organic framework（MOF）{[Cu（L1）_（0.5）（CN）]·4H_2O·3DMSO}_n（1） was assembled by 1,4-bis（3？,5？-dicyano-2？,6？-di（pyrid-4-yl）-1？,4？-dihydropyridyl）benzene（L1） together with copper cyanide at room temperature. In 1,the Cu~＋ ions are linked by CN-anions into a 1D helical chain,which is further fused together by tetradentate L1 ligands to build an extended 3D porous framework with two different types of functionalized channels. 1 crystallizes in the monoclinic,space group P21/c with a = 17.8729（6）,b = 8.7298（3）,c = 22.7524（9）？,β = 96.072（4）o,V = 3530.1（2）？~3,μ = 0.845 mm-1,Dc = 1.352 Mg/m^3,Z = 4,Mr = 718.35,F（000） = 1500,S = 1.081,the final R = 0.0877 and wR = 0.2275 for 6975 observed reflections with I 〉 2σ（I）.

关键词： four-coordinate Cu（Ⅰ） complex crystal structure selected solvent

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Activating Lattice Oxygen at the Twisted Surface in a Mesoporous CeO2Single Crystal for Efficient and Durable Catalytic CO Oxidation

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Angewandte Chemie 2020年第10期133卷

作者： Yongchun Xiao Hao Li Prof. Dr. Kui Xie Key Laboratory of Optoelectronic Materials Chemistry and Physics Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 China Key Laboratory of Design & Assembly of Functional Nanostructures 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 Dalian National Laboratory For Clean Energy Dalian Institute of Chemical Physics Chinese Academy of Sciences 457 Zhongshan Road Dalian 116023 China Advanced Energy Science and Technology Guangdong Laboratory 29 Sanxin North Road Huizhou 116023 China

Activating lattice oxygen linked to active sites at surface remains a fundamental challenge in many catalytic reactions. Here we create well-defined surface by directly growing porous CeO 2 single crystals at 2 cm scale and confining Pt in lattice to construct isolated Pt 1 /CeO 2 sites at a continuously twisted surface in a monolith. We demonstrate significantly enhanced activation of lattice oxygen linked to Pt ions in contrast to Ce ions in local structures. We show complete CO oxidation with air at 67 °C without degradation being observed after operation of 300 hours. The isolated Pt 1 /CeO 2 sites at twisted surfaces not only contribute to the chemisorption of CO but also effectively activate the lattice oxygen linked to Pt ion for CO oxidation. The current work would open a new route to activate lattice oxygen by incorporating well-defined active structures confined at the surfaces.

关键词： CeO2 lattice oxygen porous single crystal surface structure twisted surface

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Carbon‐Based Electrocatalysts: Atomic Modulation and Structure design of Carbons for Bifunctional Electrocatalysis in Metal–Air Batteries (Adv. Mater. 13/2019)

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Advanced Materials 2019年第13期31卷

作者： Yiyin Huang Yueqing Wang Cheng Tang Jun Wang Qiang Zhang Yaobing Wang Jintao Zhang 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 Fujian 350002 China Key Laboratory for Colloid and Interface Chemistry (Ministry of Education) School of Chemistry and Chemical Engineering and Key Laboratory for Liquid‐Solid Structural Evolution and Processing of Materials (Ministry of Education) Shandong University Jinan 250100 China Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical Engineering Tsinghua University Beijing 100084 China

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Photocatalytic Oxidation of Low Molecular Weight Hydrocarbon Gases over Pt-TiO2 Nanotubes

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Chinese Journal of Structural Chemistry 2016年第9期35卷 1328-1338页

作者：蔡元珠潘晓阳李云鹏易志国 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 University of Chinese Academy of Sciences

Pt-TiO2 nanotubes with tube diameter of -120 nm and uniformly dispersed Pt particles（size of -2 nm） were successfully synthesized via a carbon nanotube（CNT） templating method followed by a photo-deposition processing of Pt nanoparticles. The as-obtained Pt-TiO2 NTs possess both enhanced visible light absorption and reduced recombination of photogenerated electrons and holes. These merits boost the Pt-TiO2 NTs an excellent photocatalytic material toward photooxidation of a variety of low molecular hydrocarbons under atmospheric environment.

关键词： small molecular hydrocarbons Pt-supported TiO2 nanotubes photocatalysis

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Synthesis and Characterization of a Water-stable Metal-organic Framework Based on Mixed Ligands

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Chinese Journal of Structural Chemistry 2016年第12期35卷 1929-1935页

作者：张磊吴小园卢灿忠陈文哲 College of Materials Science and Engineering Fuzhou University Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of MatterChinese Academy of Sciences

A new water-stable metal-organic framework,[Cu_2（bdc）_2（tpt）_3]·2H_2O（1,H_2 bdc = terephthalic acid,tpt = 2,4,6-tri（4-pyridinyl）-1,3,5-triazine）,has been synthesized and characterized by elemental analysis,infrared（IR） spectrum,thermogravimetric analysis（TGA）,powder X-ray diffraction（PXRD） and single-crystal X-ray diffraction. Compund 1 crystalizes in monoclinic,space group C2/c with a = 30.147（5）,b = 11.0548（17）,c = 20.867（4）？,β = 115.035（2）o,C_（70）H_（48）Cu_2N_（18）O_（10）,Mr = 1428.34,V = 6301.0（18）？~3,Z = 8,D_c = 1.506 g/cm^3,μ = 0.754 mm^（–1）,F（000） = 2928,GOOF = 1.058,λ（MoK α） = 0.71073 ？,the final R = 0.0387 and wR = 0.1091 for 6230 observed reflections with I 〉 2σ（I）. In compound 1,the half metallacycles [Cu_2（tpt）_3] are linked by the bdc2-ligands to form a 1D bent ladder-like chain featured with a nano-sized channel,and these chains link each other via intermolecular hydrogen bonds and π-π stacking interactions to form a 3D supramolecular architecture with the voids filled with free water molecules. In addition,the water stability of 1 was investigated by PXRD patterns,which indicate that compound 1 keeps its structural integrity in boiling water for at least three days.

关键词： crystal structure metal-organic framework mixed ligands water-stable

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