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Tetraphenylethylene-Based Hydrogen-Bonded Organic Frameworks (HOFs) with Brilliant Fluorescence

Angewandte Chemie 2023年第52期135卷

作者： Dr. Shi-Cheng Wang Dr. Qiang-Sheng Zhang Dr. Zheng Wang Shao-Qi Guan Xiao-Dong Zhang Dr. Xiao-Hong Xiong Prof. Mei Pan MOE Laboratory of Bioinorganic and Synthetic Chemistry Lehn Institute of Functional Materials IGCME GBRCE for Functional Molecular Engineering School of Chemistry Sun Yat-Sen University Guangzhou 510006 China Key Laboratory of Advanced Materials of Tropical Island Resources Ministry of Education School of Chemistry and Chemical Engineering Hainan University Haikou 570228 China Hainan Provincial Key Laboratory of Fine Chem School of Chemistry and Chemical Engineering Hainan University Haikou 570228 China College of Chemistry and Chemical Engineering Key Laboratory of Chemical Additives for China National Light Industry Shaanxi University of Science and Technology Xi'an 710021 China

By synergistically employing four key strategies: (I) introducing tetraphenylethylene groups as the central core unit with aggregation-induced emission (AIE) properties, (II) optimizing the π-conjugated length by extending the building block branches, (III) incorporating flexible groups containing ethylenic bonds, and (IV) applying crystal engineering to attain dense stacking mode and highly twisty conformation, we successfully synthesized a series of hydrogen-bonded organic frameworks (HOFs) exhibiting exceptional one/two-photon excited fluorescence. Notably, when utilizing the fluorescently superior building block L2, HOF-LIFM-7 and HOF-LIFM-8 exhibiting high quantum yields (QY) of 82.1 % and 77.1 %, and ultrahigh two-photon absorption (TPA) cross-sections of 148959.5 GM and 123901.1 GM were achieved. These materials were successfully employed in one and two-photon excited lysosome-targeting cellular imaging. It is believed that this strategy, combining building block optimization and crystal engineering, holds significant potential for guiding the development of outstanding fluorescent HOF materials.

关键词： Crystal Engineering Hydrogen-Bonded Organic Frameworks Tetraphenylethylene Two-Photon Excited Fluorescence

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Liquid Marbles Based on Magnetic Upconversion Nanoparticles as Magnetically and Optically Responsive Miniature Reactors for Photocatalysis and Photodynamic Therapy

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Angewandte Chemie 2016年第36期128卷

作者： Dan Wang Lin Zhu Jian‐Feng Chen Liming Dai Research Centre of the Ministry of Education for High Gravity Engineering and Technology State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical Technology Beijing 100029 China Center of Advanced Science and Engineering for Carbon (Case4Carbon) Department of Macromolecular Science and Engineering Case School of Engineering Case Western Reserve University Cleveland OH 44106 USA Institute of Advanced Materials for Nano-bio Applications School of Ophthalmology and Optometry Wenzhou Medical University 270 Xueyuan Xi Road Wenzhou Zhejiang China

Magnetic liquid marbles have recently attracted extensive attention for various potential applications. However, conventional liquid marbles based on iron oxide nanoparticles are opaque and inadequate for photo‐related applications. Herein, we report the first development of liquid marbles coated with magnetic lanthanide‐doped upconversion nanoparticles (UCNPs) that can convert near‐infrared light into visible light. Apart from their excellent magnetic and mechanical properties, which are attractive for repeatable tip opening and magnetically directed movements, the resultant UCNP‐based liquid marbles can act as ideal miniature reactors for photodynamic therapy of cancer cells. This work opens new ways for the development of liquid marbles, and shows great promise for liquid marbles based on UCNPs to be used in a large variety of potential applications, such as photodynamic therapy for accelerated drug screening, magnetically guided controlled drug delivery and release, and multifunctional actuation.

关键词： Aufwärtskonversion Flüssigkeitskügelchen Magnetische Eigenschaften Nanopartikel Photodynamische Therapie

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Adaptive Structured Pickering Emulsions and Porous Materials Based on Cellulose Nanocrystal Surfactants

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Angewandte Chemie 2018年第41期130卷

作者： Yanan Li Xubo Liu Zhen Zhang Shaojie Zhao Guifang Tian Jinkai Zheng Dong Wang Shaowei Shi Thomas P. Russell Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical Technology Beijing 100029 China Department of Chemical Engineering Waterloo Institute for Nanotechnology University of Waterloo Waterloo Ontario Canada Institute of Food Science and Technology Chinese Academy of Agricultural Sciences Beijing 100193 China State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical Technology Beijing 100029 China Polymer Science and Engineering Department University of Massachusetts Amherst MA 01003 USA Materials Sciences Division Lawrence Berkeley National Laboratory 1 Cyclotron Road Berkeley CA 94720 USA

Taking advantage of the formation and assembly of cellulose nanocrystal surfactants (CNCSs) at the water–oil interface, where polar cellulose nanocrystals (CNCs) and end‐functionalized polymer chains interact, the preparation and stability of emulsions prepared with CNCSs were investigated. The packing density of CNCSs at the interface can be adjusted by tuning parameters such as pH, ionic strength, and concentration/molecular weight of the end‐functionalized polymer ligands. Stable non‐spherical emulsions are obtained during homogenization, as a result of the interfacial jamming of CNCSs, with pH‐triggered reconfigurability. Porous materials are prepared by freeze‐drying creamed, CNCS‐stabilized emulsions. The cells of the porous materials have a controlled pore size and shape that are commensurate with the droplets in the emulsion and are responsive to pH. The behavior of the adaptive, reconfigurable supracolloidal system is coupled to its internal and surrounding environment.

关键词： Cellulosenanokristalltenside Pickering-Emulsionen Poröse Materialien Strukturierte Flüssigkeiten

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Sabatier Relations in Electrocatalysts Based on High-entropy Alloys with Wide-distributed d-band Centers for Li-O2Batteries

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Angewandte Chemie 2023年第44期135卷

作者： Jiaming Tian Yuan Rao Wenhui Shi Jiawei Yang Wenjie Ning Haoyu Li Yonggang Yao Haoshen Zhou Shaohua Guo College of Engineering and Applied Sciences Jiangsu Key Laboratory of Artificial Functional Materials National Laboratory of Solid State Microstructures Collaborative Innovation Centre of Advanced Microstructures Frontiers Science Center for Critical Earth Material Cycling Nanjing University Nanjing 210093 P. R. China Lab of Power and Energy Storage Batteries Shenzhen Research Institute of Nanjing University Shenzhen 518057 P. R. China State Key Laboratory of Materials Processing and Die & Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan 430074 China

Li-O 2 battery (LOB) is a promising “beyond Li-ion” technology with ultrahigh theoretical energy density (3457 Wh kg −1 ), while currently impeded by the sluggish cathodic kinetics of the reversible gas-solid reaction between O 2 and Li 2 O 2 . Despite many catalysts are developed for accelerating the conversion process, the lack of design guidance for achieving high performance makes catalysts exploring aleatory. The Sabatier principle is an acknowledged theory connecting the scaling relationship with heterogeneous catalytic activity, providing a tradeoff strategy for the topmost performance. Herein, a series of catalysts with wide-distributed d-band centers (i.e., wide range of adsorption strength) are elaborately constructed via high-entropy strategy, enabling an in-depth study of the Sabatier relations in electrocatalysts for LOBs. A volcano-type correlation of d-band center and catalytic activity emerges. Both theoretical and experimental results indicate that a moderate d-band center with appropriate adsorption strength propels the catalysts up to the top. As a demonstration of concept, the LOB using FeCoNiMnPtIr as catalyst provides an exceptional energy conversion efficiency of over 80 %, and works steadily for 2000 h with a high fixed specific capacity of 4000 mAh g −1 . This work certifies the applicability of Sabatier principle as a guidance for designing advanced heterogeneous catalysts assembled in LOBs.

关键词： High Entropy Li-O2 Batteries Oxygen Conversion Sabatier Principle d-Band Center

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Robust, Ultrafast and Reversible Photoswitching in Bulk Polymers Enabled by Octupolar Molecule Design

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Angewandte Chemie 2024年第16期136卷

作者： Long Fang Ziwei Lin Yang Zhang Bin Ye Jing Li Qishan Ran Xiaotong Wang Meijia Yang Prof. Zhongke Yuan Prof. Xiaofeng Lin Prof. Dingshan Yu Prof. Xudong Chen Prof. Quan Li Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education Key Laboratory of High Performance Polymer-based Composites of Guangdong Province GBRCE for Functional Molecular Engineering School of Chemistry Sun Yat-sen University Guangzhou 510006 China School of Computer Science and Engineering Sun Yat-sen University Guangzhou 510275 China Institute of Applied Physics and Materials Engineering University of Macau Taipa Macao SAR 999078 China School of Chemical Engineering and Light Industry Guangdong University of Technology Guangzhou 510006 China Guangdong Laboratory of Chemistry and Fine Chemical Industry Jieyang Center Jieyang 515200 China Institute of Advanced Materials and School of Chemistry and Chemical Engineering Southeast University Nanjing 211189 China Materials Science Graduate Program Kent State University Kent OH 44242 USA

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Exploiting Reusable Edge-functionalized Metal-Free Polyphthalocyanine Networks for Efficient Polymer Synthesis at Near Infrared Wavelengths

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Angewandte Chemie 2023年第24期135卷

作者： Wen Fang Wei Xue Li Kaiyue Jiang Dr. Bin Zhang Prof. Xiaodong Zhuang Prof. Tao Cai Key Laboratory of Biomedical Polymers of Ministry of Education College of Chemistry and Molecular Science Wuhan University Wuhan Hubei 430072 China The Soft2D Lab State Key Laboratory of Metal Matrix Composites & Shanghai Key Laboratory of Electrical Insulation and Thermal Ageing School of Chemistry and Chemical Engineering Shanghai Jiao Tong University Shanghai 200240 China College of Chemistry Zhengzhou University Zhengzhou Henan 450001 China Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering School of Chemistry and Molecular Engineering East China University of Science and Technology Shanghai 200237 China Frontiers Science Center for Transformative Molecules Zhang Jiang Institute for Advanced Study Shanghai Jiao Tong University Shanghai 201203 China

Heterogeneous catalysts are highly advantageous for industrial applications owing to their distinctive merits including easy separation and effective recovery. However, utilizing heterogeneous photocatalysts to harness longer wavelength light remains a critical area of research. This contribution explores the use of edge-functionalized metal-free polyphthalocyanine networks (PPc-x) to promote efficient polymer synthesis under near infrared (NIR) light irradiation. Our screening process revealed that both phenyl-edged PPc-x (PPc-p) and naphthyl-edged PPc-x (PPc-n) offer promising performance for photopolymerization. With the assistance of ppm-level PPc-n catalyst, well-defined polymers were synthesized within a few hours under the regulation of three NIR lights, regardless of shielded by synthetic and biological barriers. An excellent control over the molecular weight and molecular weight distribution was achieved. Furthermore, PPc-x can be easily recovered and reused for multiple cycles, with negligible leaching and maintenance of the catalytic performance. This study expands a new avenue in developing versatile photocatalysts for the modern synthetic toolkits and offer benefits in diverse applications.

关键词： Edge-functionalized Polyphthalocyanine High Penetration Capability Near Infrared Irradiation Photo-RDRP Reusability

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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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Thermal Management: Electrostatic Actuating Double-Unit Electrocaloric Cooling Device with High Efficiency (Adv. Energy Mater. 13/2021)

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advanced Energy Materials 2021年第13期11卷

作者： Yiwen Bo Quan Zhang Heng Cui Mengyan Wang Chunyang Zhang Wen He Xiangqian Fan Yiwen Lv Xiang Fu Jiajie Liang Yi Huang Rujun Ma Yongsheng Chen School of Materials Science and Engineering National Institute for Advanced Materials Tianjin Key Lab for Rare Earth Materials and Applications Nankai University Tongyan Road 38 Tianjin 300350 P. R. China State Key Laboratory and Institute of Elemento-Organic Chemistry Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer Materials College of Chemistry Nankai University Tianjin 300071 P. R. China

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The Crucial Role of Charge Accumulation and Spin Polarization in Activating Carbon‐Based Catalysts for Electrocatalytic Nitrogen Reduction

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Angewandte Chemie 2020年第11期132卷

作者： Yuanyuan Yang Lifu Zhang Zhenpeng Hu Yao Zheng Cheng Tang Ping Chen Ruguang Wang Kangwen Qiu Jing Mao Tao Ling Shi‐Zhang Qiao Key Laboratory for Advanced Ceramics and Machining Technology of Ministry of Education Tianjin Key Laboratory of Composite and Functional Materials School of Materials Science and Engineering Tianjin University Tianjin 300072 China School of Physics Nankai University Tianjin 300071 China School of Chemical Engineering The University of Adelaide Adelaide SA 5005 Australia School of Chemistry and Chemical Engineering Anhui University Hefei 230000 China

Cost‐effective carbon‐based catalysts are promising for catalyzing the electrochemical N 2 reduction reaction (NRR). However, the activity origin of carbon‐based catalysts towards NRR remains unclear, and regularities and rules for the rational design of carbon‐based NRR electrocatalysts are still lacking. Based on a combination of theoretical calculations and experimental observations, chalcogen/oxygen group element (O, S, Se, Te) doped carbon materials were systematically evaluated as potential NRR catalysts. Heteroatom‐doping‐induced charge accumulation facilitates N 2 adsorption on carbon atoms and spin polarization boosts the potential‐determining step of the first protonation to form *NNH. Te‐doped and Se‐doped C catalysts exhibited high intrinsic NRR activity that is superior to most metal‐based catalysts. Establishing the correlation between the electronic structure and NRR performance for carbon‐based materials paves the pathway for their NRR application.

关键词： Kohlenstoffmaterialien Chalkogene Elektrokatalyse Stickstoffreduktionsreaktion

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Combining advanced photoelectron spectroscopy approaches to analyse deeply buried GaP(As)/Si(100) interfaces: Interfacial chemical states and complete band energy diagrams

arXiv

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arXiv 2022年

作者： Romanyuk, Oleksandr Paszuk, A. Gordeev, I. Wilks, R.G. Ueda, S. Hartmann, C. Félix, R. Bär, M. Schlueter, C. Gloskovskii, A. Bartoš, I. Nandy, M. Houdková, J. Jiříček, P. Jaegermann, W. Hofmann, J.P. Hannappel, T. FZU - Institute of Physics of the Czech Academy of Sciences Prague Czech Republic Dep: Fundamentals of Energy Materials Institute of Physics Ilmenau University of Technology Ilmenau Germany Department Interface Design Helmholtz-Zentrum Berlin fur Materialien und Energie GmbH Berlin Germany Helmholtz-Zentrum Berlin fur Materialien und Energie GmbH Berlin Germany Hyogo Japan Research Center for Functional Materials NIMS Tsukuba Japan Research Center for Advanced Measurement and Characterization NIMS Tsukuba Japan Department of Chemistry and Pharmacy Friedrich-Alexander-Universitat Erlangen-Nurnberg Erlangen Germany Berlin Germany Deutsches Elektronen-Synchrotron DESY Ein Forschungszentrum der Helmholtz-Gemeinschaft Hamburg Germany Surface Science Laboratory Department of Materials and Earth Sciences Technical University of Darmstadt Darmstadt Germany

The epitaxial growth of the polar GaP(100) on the nonpolar Si(100) substrate suffers from inevitable defects at the antiphase domain boundaries, resulting from mono-atomic steps on the Si(100) surface. Stabilization of Si(100) substrate surfaces with arsenic is a promising technological step enabling the preparation of Si substrates with double atomic steps and reduced density of the APDs. In this paper, 4 - 50-nm-thick GaP epitaxial films were grown on As-terminated Si(100) substrates with different types of doping, miscuts, and As-surface termination by metalorganic vapor phase epitaxy. The GaP(As)/Si(100) heterostructures were investigated by X-ray photoelectron spectroscopy (XPS) combined with gas cluster ion beam (GCIB) sputtering and by hard X-ray photoelectron spectroscopy (HAXPES). We found residuals of arsenic atoms in the GaP lattice (∼0.2-0.3 at.%) and a localization of As atoms at the GaP(As)/Si(100) interface (∼1 at.%). Deconvolution of core level peaks revealed interface core level shifts. In As core levels, chemical shifts between 0.5-0.8 eV were measured and identified by angle-resolved XPS measurements. Similar valence band offset (VBO) values of 0.6 eV were obtained, regardless of the doping type of Si substrate, Si substrate miscut or type of As-terminated Si substrate surface. The band alignment diagram of the heterostructure was deduced. © 2022, CC BY-NC-ND.

关键词： X ray photoelectron spectroscopy

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