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941.
Zhong Wei Jiang Yang Chun Zou Ting Ting Zhao Shu Jun Zhen Yuan Fang Li Cheng Zhi Huang 《Angewandte Chemie (International ed. in English)》2020,59(8):3300-3306
Synthesizing 2D metal–organic frameworks (2D MOFs) in high yields and rational tailoring of the properties in a predictable manner for specific applications is extremely challenging. Now, a series of porphyrin‐based 2D lanthanide MOFs (Ln‐TCPP, Ln=Ce, Sm, Eu, Tb, Yb, TCPP=tetrakis(4‐carboxyphenyl) porphyrin) with different thickness were successfully prepared in a household microwave oven. The as‐prepared 2D Ln‐TCPP nanosheets showed thickness‐dependent photocatalytic performances towards photooxidation of 1,5‐dihydroxynaphthalene (1,5‐DHN) to synthesize juglone. Particularly, the Yb‐TCPP displayed outstanding photodynamic activity to generate O2? and 1O2. This work not only provides fundamental insights into structure designing and property tailoring of 2D MOFs nanosheets, but also pave a new way to improve the photocatalytic performance. 相似文献
942.
Christoph Gbel Christian Hils Markus Drechsler Dirk Baabe Andreas Greiner Holger Schmalz Birgit Weber 《Angewandte Chemie (International ed. in English)》2020,59(14):5765-5770
Nanoparticles of the spin‐crossover coordination polymer [FeL(bipy)]n were synthesized by confined crystallization within the core of polystyrene‐block‐poly(4‐vinylpyridine) (PS‐b‐P4VP) diblock copolymer micelles. The 4VP units in the micellar core act as coordination sites for the Fe complex. In the bulk material, the spin‐crossover nanoparticles in the core are well isolated from each other allowing thermal treatment without disintegration of their structure. During annealing above the glass transition temperature of the PS block, the transition temperature is shifted gradually to higher temperatures from the as‐synthesized product (T1/2↓=163 K and T1/2↑=170 K) to the annealed product (T1/2↓=203 K and T1/2↑=217 K) along with an increase in hysteresis width from 6 K to 14 K. Thus, the spin‐crossover properties can be shifted towards the properties of the related bulk material. The stability of the nanocomposite allows further processing, such as electrospinning from solution. 相似文献
943.
Ruben Canton‐Vitoria Tobias Scharl Anastasios Stergiou Alejandro Cadranel Raul Arenal Dirk M. Guldi Nikos Tagmatarchis 《Angewandte Chemie (International ed. in English)》2020,59(10):3976-3981
Molybdenum disulfide nanosheets covalently modified with porphyrin were prepared and fully characterized. Neither the porphyrin absorption nor its fluorescence was notably affected by covalent linkage to MoS2. The use of transient absorption spectroscopy showed that a complex ping‐pong energy‐transfer mechanism, namely from the porphyrin to MoS2 and back to the porphyrin, operated. This study reveals the potential of transition‐metal dichalcogenides in photosensitization processes. 相似文献
944.
Jun‐Chao Liu Wei‐Qiang Liao Peng‐Fei Li Yuan‐Yuan Tang Xiao‐Gang Chen Xian‐Jiang Song Han‐Yue Zhang Yi Zhang Yu‐Meng You Ren‐Gen Xiong 《Angewandte Chemie (International ed. in English)》2020,59(9):3495-3499
Molecular ferroelectrics have attracted considerable interests because of their easy and environmentally friendly processing, low acoustical impedance and mechanical flexibility. Herein, a molecular thermochromic ferroelectric, N,N′‐dimethyl‐1,4‐diazoniabicyclo[2.2.2]octonium tetrachlorocuprate(II) ([DMe‐DABCO]CuCl4) is reported, which shows both excellent ferroelectricity and intriguing thermochromism. [DMe‐DABCO]CuCl4 undergoes a ferroelectric phase transition from Pca21 to Pbcm at a significantly high Curie temperature of 413 K, accompanied by a color change from yellow to red that is due to the remarkable deformation of [CuCl4]2? tetrahedron, where the ferroelectric and paraelectric phases correspond to yellow and red, respectively. Combined with multiple bistable physical properties, [DMe‐DABCO]CuCl4 would be a promising candidate for next‐generation smart devices, and should inspire further exploration of multifunctional molecular ferroelectrics. 相似文献
945.
Yulin Jie Xiaojing Liu Zhanwu Lei Shiyang Wang Yawei Chen Fanyang Huang Ruiguo Cao Genqiang Zhang Shuhong Jiao 《Angewandte Chemie (International ed. in English)》2020,59(9):3505-3510
Lithium metal is an ideal electrode material for future rechargeable lithium metal batteries. However, the widespread deployment of metallic lithium anode is significantly hindered by its dendritic growth and low Coulombic efficiency, especially in ester solvents. Herein, by rationally manipulating the electrolyte solvation structure with a high donor number solvent, enhancement of the solubility of lithium nitrate in an ester‐based electrolyte is successfully demonstrated, which enables high‐voltage lithium metal batteries. Remarkably, the electrolyte with a high concentration of LiNO3 additive presents an excellent Coulombic efficiency up to 98.8 % during stable galvanostatic lithium plating/stripping cycles. A full‐cell lithium metal battery with a lithium nickel manganese cobalt oxide cathode exhibits a stable cycling performance showing limited capacity decay. This approach provides an effective electrolyte manipulation strategy to develop high‐voltage lithium metal batteries. 相似文献
946.
Shuo Tao Xiaolei Li Xiaoge Wang Ying Wei Yunling Jia Jing Ju Yuanhui Cheng Huaisheng Wang Shuwen Gong Xingjun Yao Haixu Gao Cunyin Zhang Qiqi Zang Zhijian Tian 《Angewandte Chemie (International ed. in English)》2020,59(9):3455-3459
The synthesis of hierarchical nanosized zeolite materials without growth modifiers and mesoporogens remains a substantial challenge. Herein, we report a general synthetic approach to produce hierarchical nanosized single‐crystal aluminophosphate molecular sieves by preparing highly homogeneous and concentrated precursors and heating at elevated temperatures. Accordingly, aluminophosphate zeotypes of LTA (8‐rings), AEL (10‐rings), AFI (12‐rings), and ‐CLO (20‐rings) topologies, ranging from small to extra‐large pores, were synthesized. These materials show exceptional properties, including small crystallites (30–150 nm), good monodispersity, abundant mesopores, and excellent thermal stability. A time‐dependent study revealed a non‐classical crystallization pathway by particle attachment. This work opens a new avenue for the development of hierarchical nanosized zeolite materials and understanding their crystallization mechanism. 相似文献
947.
Gerardo Salinas Alice L. Dauphin Camille Colin Elena Villani Stphane Arbault Laurent Bouffier Alexander Kuhn 《Angewandte Chemie (International ed. in English)》2020,59(19):7508-7513
Miniaturized autonomous chemo‐electronic swimmers, based on the coupling of spontaneous oxidation and reduction reactions at the two poles of light‐emitting diodes (LEDs), are presented as chemotactic and magnetotactic devices. In homogeneous aqueous media, random motion caused by a bubble‐induced propulsion mechanism is observed. However, in an inhomogeneous environment, the self‐propelled devices exhibit positive chemotactic behavior, propelling themselves along a pH or ionic strength gradient (?pH and ?I, respectively) in order to reach a thermodynamically higher active state. In addition, the intrinsic permanent magnetic moment of the LED allows self‐orientation in the terrestrial magnetic field or following other external magnetic perturbations, which enables a directional motion control coupled with light emission. The interplay between chemotaxis and magnetotaxis allows fine‐tuning of the dynamic behavior of these swimmers. 相似文献
948.
Julien Es Sayed Cdric Lorthioir Philippe Banet Patrick Perrin Nicolas Sanson 《Angewandte Chemie (International ed. in English)》2020,59(18):7042-7048
The combination of supramolecular chemistry and soft colloids as microgels represents an ambitious way to develop multi‐versatile colloidal assemblies. Hereafter, terpyridine‐functionalized poly(N‐isopropylacrylamide) (PNiPAM) microgel building blocks are shown to undergo an assemble–freeze–disassemble process. The microgel assemblies, which are controlled by monitoring the attractive and repulsive potentials between the soft colloidal particles, are then frozen by forming inter‐particle metal–terpyridine bis‐complexes upon addition of the metallic cation (such as FeII, CoII). By oxidation of the metal–terpyridine bis‐complex links, the aggregates open up, which is due to the complex dissociation releasing the connected particles in the form of single microgels. We extended our work to the development of 1D filaments and 2D membranes materials made of soft particles connected via supramolecular chemistry. 相似文献
949.
Pengfei Xia Shaowen Cao Bicheng Zhu Mingjin Liu Miusi Shi Jiaguo Yu Yufeng Zhang 《Angewandte Chemie (International ed. in English)》2020,59(13):5218-5225
Constructing heterojunctions between two semiconductors with matched band structure is an effective strategy to acquire high‐efficiency photocatalysts. The S‐scheme heterojunction system has shown great potential in facilitating separation and transfer of photogenerated carriers, as well as acquiring strong photoredox ability. Herein, a 0D/2D S‐Scheme heterojunction material involving CeO2 quantum dots and polymeric carbon nitride (CeO2/PCN) is designed and constructed by in situ wet chemistry with subsequent heat treatment. This S‐scheme heterojunction material shows high‐efficiency photocatalytic sterilization rate (88.1 %) towards Staphylococcus aureus (S. aureus) under visible‐light irradiation (λ≥420 nm), which is 2.7 and 8.2 times that of pure CeO2 (32.2 %) and PCN (10.7 %), respectively. Strong evidence of S‐scheme charge transfer path is verified by theoretical calculations, in situ irradiated X‐ray photoelectron spectroscopy, and electron paramagnetic resonance. 相似文献
950.
Fast, mass, and low‐cost production of high‐quality graphene, which is alluring, remains a great challenge, even though some approaches have shown potential for mass synthesis of graphene. Very recently a great breakthrough was made by Tour and co‐workers (Nature 2020, 577, 647–651): in just a second, easily exfoliated and highly crystalline graphene was produced from abundant carbon‐containing species by cost‐effective flash Joule heating with a low energy input of 7.2 kJ per gram graphene. Such an ultrafast, economic, and scalable process for high‐quality graphene production can be considered as a milestone in the graphene field and is highlighted in this article. 相似文献