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Ultra-Small Air-Stable Triplet-Triplet Annihilation Upconversion Nanoparticles for Anti-Stokes Time-Resolved Imaging

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Angewandte Chemie 2023年第47期135卷

作者： Dr. Bolong Zhang Dr. Kieran D. Richards Beatrice E. Jones Abigail R. Collins Rosie Sanders Dr. Sarah R. Needham Dr. Pu Qian Amoghavarsha Mahadevegowda Prof. Caterina Ducati Prof. Stanley W. Botchway Prof. Rachel C. Evans Department of Materials Science and Metallurgy University of Cambridge 27 Charles Babbage Road Cambridge CB3 0FS UK 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 Diamond Light Source Didcot Oxfordshire OX11 0QX UK Central Laser Facility Science and Technology Facilities Council Rutherford Appleton Laboratory Harwell Science and Innovation Campus Oxfordshire OX11 0QX UK Materials and Structural Analysis Thermo Fisher Scientific Achtseweg Noord 5 5651 GG Eindhoven The Netherlands The Faraday Institution Quad One Harwell Science and Innovation Campus Didcot UK

Image contrast is often limited by background autofluorescence in steady-state bioimaging microscopy. Upconversion bioimaging can overcome this by shifting the emission lifetime and wavelength beyond the autofluorescence window. Here we demonstrate the first example of triplet-triplet annihilation upconversion (TTA-UC) based lifetime imaging microscopy. A new class of ultra-small nanoparticle (NP) probes based on TTA-UC chromophores encapsulated in an organic–inorganic host has been synthesised. The NPs exhibit bright UC emission (400–500 nm) in aerated aqueous media with a UC lifetime of ≈1 μs, excellent colloidal stability and little cytotoxicity. Proof-of-concept demonstration of TTA-UC lifetime imaging using these NPs shows that the long-lived anti-Stokes emission is easily discriminable from typical autofluorescence. Moreover, fluctuations in the UC lifetime can be used to map local oxygen diffusion across the subcellular structure. Our TTA-UC NPs are highly promising stains for lifetime imaging microscopy, affording excellent image contrast and potential for oxygen mapping that is ripe for further exploitation.

关键词： Fluorescence Lifetime Imaging Microscopy Nanoparticles Triplet-Triplet Annihilation Upconversion

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N-doped defective carbon with trace Co for efficient rechargeable liquid electrolyte-/all-solid-state Zn-air batteries

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Science Bulletin 2018年第9期63卷 548-555页

作者： Zhiyan Chen Qichen Wang Xiaobin Zhang Yongpeng Lei Wei Hu Yao Luo Yaobing Wang College of Materials Science and Engineering Central South University of Forestry and Technology State Key Laboratory for Modification of Chemical Fibers and Polymer Materials Donghua University Center for Nano Materials and Technology Japan Advanced Institute of Science and Technology School of Aeronautics and Astronautics & Science and Technology on High Strength Structural Materials Laboratory Central South University College of Basic Education National University of Defense Technology 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

Simple synthesis of multifunctional electrocatalysts with plentiful active sites from earth-abundant materials is especially fascinating. Here, N-doped defective carbon with trace Co （1.5 wt%） was prepared via a scalable one pot solid pyrolysis process. The sample exhibits efficient bifunctional OER/ORR activiW in alkaline, mainly ascribed to the unique micro-mesoporous structure （1-3 nm）, high population of graphitic-N doping （up to 49.0%）, abundant defects and the encapsulated Co nanoparticles with graphitized carbon. The according rechargeahle liquid Zn-air batteries showed excellent performance （maximum power density of 154.0 mWcm-2： energy density of 773Wh kg -1 at 5 mAcm 2 and charging-discharging cycling stability over 100 cycles）. As a proof-of-concept, the flexible, rechargeable all-solid-state Zn-air batteries were constructed, and displayed a maximum power density as high as 45.9 mW cm 2 among the top level of those reported previously.

关键词： Defect Oxygen electrocatalysts Rechargeable all-solid-state batteries

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Simple Preparation of LaPO4:Ce, Tb Phosphors by an Ionic--Liquid--Driven Supported Liquid Membrane System

Simple Preparation of LaPO4:Ce, Tb Phosphors by an Ionic--Li...

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稀土元素镧铈钇应用研究研讨会暨广东省稀土产业技术联盟成立大会

作者： Jianguo Li Hongying Dong Fan Yang Liangcheng Sun Zhigang Zhao Ruixi Bai Hao Zhang School of Chemical Engineering Inner Mongolia University of Technology Xiamen Institute of Rare Earth Materials Chinese Academy of Sciences 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 Baotou Research Institute of Rare Earths

In this work, LaPO:Ce, Tb phosphors were prepared by firing a LaPO:Ce, Tb precipitate using an ionic-liquid-driven supported liquid membrane system. The entire system consisted of three parts: a mixed rare earth ion supply phase, a phosphate supply phase, and an ionic-liquid-driven supporting liquid membrane phase. This method showed the advantages of a high flux, high efficiency, and more controllable reaction process. The release rate of POfrom the liquid film under different types of ionic liquid, the ratio of the rare earth ions in the precursor mixture, and the structure, morphology, and photoluminescence properties of LaPO:Ce, Tb were investigated by inductively coupled plasma-atomic emission spectroscopy, X-ray diffraction, Raman spectra, scanning electron microscopy, and photoluminescence emission spectra methods. The results showed that a pure phase of lanthanum orthophosphate with a monoclinic structure can be formed. Due to differences in the anions in the rare earth supply phase, the prepared phosphors showed micro-spherical（when using rare earth sulfate as the raw material） and nanoscale stone-shape（when using rare earth nitrate as the raw material） morphologies. Moreover, the phosphors prepared by this method had good luminescent properties, reaching a maximum emission intensity under 277 nm excitation with a predominant green emission at 543 nm which corresponded to the 5 D4-7 F5 transition of Tb.

关键词： Simple Preparation of LaPO4:Ce Tb Phosphors by an Ionic Driven Supported Liquid Membrane System Liquid

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Facile preparation of Ce enhanced vinyl-functionalized silica aerogel-like monoliths for selective separation of radioactive thorium from monazite

Facile preparation of Ce enhanced vinyl-functionalized silic...

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稀土元素镧铈钇应用研究研讨会暨广东省稀土产业技术联盟成立大会

作者： Hao Zhang Fan Yang Ruixi Bai Zhigang Zhao Chunqing Cai Jianguo Li Ying Ma 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 Xiamen Institute of Rare Earth Materials Haixi Institute Chinese Academy of Sciences University of Chinese Academy of Sciences Baotou Research Institute of Rare Earths

Thorium(Th) is an associated ore of rare earth metals that is radioactive and harmful to the environment, but it is also a potential nuclear fuel replacement for uranium. The separation of Th from rare earth elements(REEs) is of great importance in environmental governance and clean-energy development. In this work, a monolithic cerium(Ce) doped silica aerogel-like with flexibility was synthesized using a low consumption and rapid technique, and it was used in a continuous solid-phase extraction as an adsorbent for the selective separation of Th/REEs. The batch adsorption experiments showed that the adsorption efficiency of Th(IV) can be up to 96% when abnormally high levels of metal ions(20 ppm) exist. Under the same conditions, the adsorption efficiency of REEs is at a near-zero level, which demonstrates the great selective separation of Th/REEs for the aerogel-like. The results also indicated that Th(IV) could desorb from the adsorbent in weak acidic media, which is friendly to the environment. Therefore, the material has application prospects for the separation of Th/REEs and removal of radioactive contamination from the environment.

关键词： silica aerogel-like monoliths selective adsorption rare earth thorium monazite

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Synthesis of 3D Porous and Interconnected Hollow Carbon Nanospheres Array and Its Applications in Lithium-sulfur Batteries

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Chinese Journal of Structural Chemistry 2017年第10期36卷 1647-1655页

作者：徐金剑吴王亮官轮辉 College of Chemistry Fuzhou University Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences

Lithium-sulfur（Li–S） batteries are receiving much attention due to their high theoretical lithium storage capacity and energy density. However, the commercialization of Li–S batteries is mainly impeded by the inherent poor electrical conductivity of sulfur, the side shuttle behavior of polysulfides, and the volumetric change of sulfur during cycles. To solve these problems, here we report a unique 3D porous and interconnected hollow carbon nanospheres array（3D-HCNA） as sulfur host for lithium-sulfur batteries. This 3D-HCNA was synthesized through a nanocasting approach with sucrose as carbon precursors and mesoporous silica nanospheres as hard-templates. The silica nanospheres with special nanostructure were obtained by a biphase stratification approach. Owing to its unique architecture, as-prepared 3D-HCNA/S cathode with a high sulfur loading of 76 wt% exhibited excellent electrochemical performance. It showed highinitial capacity of 1318 m Ah/g at 0.05 C and good rate capability of 760 m Ah/g at 1 C. Moreover, excellent cycling performance was also observed with a capacity of 757 m Ah/g maintained after 200 cycles at 0.5 C.

关键词： lithium-sulfur batteries nanostructure cathode hollow nanosphere

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Dry Reforming of CH4/CO2by Stable Ni Nanocrystals on Porous Single-Crystalline MgO Monoliths at Reduced Temperature

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Angewandte Chemie 2021年第34期133卷

作者： Fangyuan Cheng Xiuyun Duan Prof. 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 University of Chinese Academy of Sciences Beijing 100049 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

Dry reforming of CH 4 /CO 2 provides a promising and economically feasible route for the large-scale carbon fixation; however, the coking and sintering of catalysts remain a fundamental challenge. Here we stabilize single-crystalline Ni nanoparticles at the surface of porous single-crystalline MgO monoliths and show the quantitative production of syngas from dry reforming of CH 4 /CO 2 . We show the complete conversion of CH 4 /CO 2 even only at 700 °C with excellent performance durability after a continuous operation of 500 hours. The well-defined and catalytically active Ni-MgO interfaces facilitate the reforming reaction and enhance the coking resistance. Our findings would enable an industrially and economically viable path for carbon reclamation, and the “Nanocrystal On Porous Single-crystalline Monoliths” technique could lead to stable catalyst designs for many challenging reactions.

关键词： basic site interface monolith porous single crystal reforming reaction

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Corrigendum to Dissolving the high-cost with acidity: A happy encounter between fluidized struvite crystallization and wastewater from activated carbon manufacture [Water Research, 188 (2021) 116521]

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Water research 2021年 198卷 117218页

作者： Xin Ye Minquan Chen Wei Wang Junhuang Shen Junbin Wu Wei Huang Lishan Xiao Xiangyu Lin Zhi-Long Ye Shaohua Chen Key Laboratory of Urban Environment and Health Institute of Urban Environment Chinese Academy of Sciences Xiamen 361021 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 Xiamen Institute of Rare Earth Materials Haixi Institute Chinese Academy of Science Xiamen 361021 China. School of Environmental and Geographical Sciences Shanghai Normal University Shanghai 200234 China.

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Boosting Electroreduction Kinetics of Nitrogen to Ammonia via Tuning Electron Distribution of Single-Atomic Iron Sites

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Angewandte Chemie 2021年第16期133卷

作者： Yan Li Junwei Li Dr. Junheng Huang Dr. Junxiang Chen Yan Kong Dr. Bin Yang Dr. Zhongjian Li Prof. Dr. Lecheng Lei Dr. Guoliang Chai Prof. Dr. Zhenhai Wen Prof. Dr. Liming Dai Prof. Dr. Yang Hou Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological Engineering Zhejiang University Hangzhou 310027 China 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 Fujian 350002 China Australian Carbon Materials Centre (A-CMC) School of Chemical Engineering University of New South Wales Sydney NSW 2052 Australia Institute of Zhejiang University–Quzhou Quzhou 324000 China

Electrocatalytic nitrogen reduction reaction (NRR) plays a vital role for next-generation electrochemical energy conversion technologies. However, the NRR kinetics is still limited by the sluggish hydrogenation process on noble-metal-free electrocatalyst. Herein, we report the rational design and synthesis of a hybrid catalyst with atomic iron sites anchored on a N,O-doped porous carbon (Fe SA -NO-C) matrix of an inverse opal structure, leading to a remarkably high NH 3 yield rate of 31.9 μg h −1 mg −1 cat. and Faradaic efficiency of 11.8 % at −0.4 V for NRR electrocatalysis, outperformed almost all previously reported atomically dispersed metal-nitrogen-carbon catalysts. Theoretical calculations revealed that the observed high NRR catalytic activity for the Fe SA -NO-C catalyst stemmed mainly from the optimized charge-transfer between the adjacent O and Fe atoms homogenously distributed on the porous carbon support, which could not only significantly facilitate the transportation of N 2 and ions but also effectively decrease the binding energy between the isolated Fe atom and *N 2 intermediate and the thermodynamic Gibbs free energy of the rate-determining step (*N 2 → *NNH).

关键词： Fe-N2O4 inverse opal structure kinetic enhanced catalysis N2 electroreduction single atom catalyst

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High-Density Lewis Acid Sites in Porous Single-Crystalline Monoliths to Enhance Propane Dehydrogenation at Reduced Temperatures

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Angewandte Chemie 2021年第17期133卷

作者： Dr. Guoming Lin Yunqi Su Xiuyun Duan 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 Advanced Energy Science and Technology Guangdong Laboratory 29 Sanxin North Road Huizhou Guangdong 116023 China

The non-oxidative dehydrogenation of propane to propylene plays an important role in the light-olefin chemical industry. However, the conversion and selectivity remain a fundamental challenge at low temperatures. Here we create and engineer high-density Lewis acid sites at well-defined surfaces in porous single-crystalline Mo 2 N and MoN monoliths to enhance the non-oxidative dehydrogenation of propane to propylene. The top-layer Mo ions with unsaturated Mo-N 1/6 and Mo-N 1/3 coordination structures provide high-density Lewis acid sites at the surface, leading to the effective activation of C−H bonds without the overcracking of C−C bonds during the non-oxidative dehydrogenation of propane. We demonstrate a propane conversion of ≈11 % and a propylene selectivity of ≈95 % with porous single-crystalline Mo 2 N and MoN monoliths at 500 °C.

关键词： dehydrogenation Lewis acids molybdenum nitrides porous materials

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Synthesis,Crystal Structure,and Photo-and Electro-luminescence of a TADF Cu(Ⅰ)Complex

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Chinese Journal of Structural Chemistry 2017年第9期36卷 1493-1501页

作者：林玲陈旭林陈东徽吴小园余荣民卢灿忠 Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Provincial Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of Sciences Graduate University of Chinese Academy of Sciences

A four-coordinate mononuclear cuprous complex [Cu（ac1m）POP]BF4·0.5（C6H14）· 0.5（C2H5OH）（1, ac1 m = 2-（2-ethoxyphenyl）-1-phenyl-1H-imidazo[4,5-f][1,10]phenanthroline, POP = bis[2-（dipenylphosphino）phenyl]ether） was synthesized and characterized by elemental analysis, NMR, UV-vis, cyclic voltammetry and X-ray single-crystal structure analysis. It crystallizes in monoclinic space group P21/c with a = 17.0546（19）, b = 15.4650（17）, c = 23.685（2） A, β = 104.007（11）°, V = 6061.1（12）A^3, Z = 4, Mr = 1171.46, Dc = 1.284 g/cm^3, F（000） = 2432, μ = 1.50 mm^–1, GOOF = 1.070, the final R = 0.059 and wR = 0.1640 for 8952 observed reflections with I 〉 2σ（Ⅰ）. Compound 1 is composed of a BF4-anion and a [Cu（ac1m）POP]^＋ cation. The Cu（Ⅰ） ion adopts a tetrahedral coordination geometry defined by two nitrogen and two phosphorous atoms. The complex exhibits yellow luminescence with maximum emission peaks at 546 nm, lifetimes 15.1 μs and quantum yields（ф = 0.130） at room temperature. The complex displays thermally activated delayed fluorescence（TADF） at room temperature, which is proved experimentally and theoretically. And the organic light-emitting diode（OLED） with 1 as the light emitting material has the maximum current efficiency of 5.86 cd/A and the highest brightness of 3215 cd/m^2.

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

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