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81.
Yuebin Lian Wenjuan Yang Chufeng Zhang Hao Sun Zhao Deng Wenjie Xu Li Song Zhongwen Ouyang Zhenxing Wang Jun Guo Yang Peng 《Angewandte Chemie (International ed. in English)》2020,59(1):286-294
Reversible oxygen conversion is important for various green energy technologies. Herein we synthesize a series of bimetallic coordination polymers by varying the Ni/Co ratio and using HITP (HITP=2,3,6,7,10,11‐hexaiminotriphenylene) as the ligand, to interrogate the role of metal centres in modulating the activity of the oxygen reduction reaction (ORR). Co3HITP2 and Ni3HITP2 are compared. Unpaired 3d electrons in Co3HITP2 result in less coplanarity but more radical character. Thus, despite of a reduced crystallinity and conductivity, the best ORR activity, comparable to 20 % Pt/C, is obtained for Co3HITP2, showing the 3d orbital configuration of the metal centre promotes ORR. Experimental and DFT studies show a transition of ORR pathway from four‐electron for Co3HITP2 to two‐electron for Ni3HITP2. Rechargeable zinc–air batteries using Co3HITP2 as the air cathode catalyst demonstrate excellent energy efficiency and stability. 相似文献
82.
Zhennan Wu Qiaofeng Yao Osburg Jin Huang Chai Nan Ding Wen Xu Shuangquan Zang Jianping Xie 《Angewandte Chemie (International ed. in English)》2020,59(25):9934-9939
Aggregation‐induced emission (AIE) provides an efficient strategy to synthesize highly luminescent metal nanoclusters (NCs), however, rational control of emission energy and intensity of metal NCs is still challenging. This communication reveals the impact of surface AuI‐thiolate motifs on the AIE properties of Au NCs, by employing a series of water‐soluble glutathione (GSH)‐coordinated Au complexes and NCs as a model ([Au10SR10], [Au15SR13], [Au18SR14], and [Au25SR18]?, SR=thiolate ligand). Spectroscopic investigations show that the emission wavelength of Au NCs is adjustable from visible to the near‐infrared II (NIR‐II) region by controlling the length of the AuI‐SR motifs on the NC surface. Decreasing the length of AuI‐SR motifs also changes the origin of cluster luminescence from AIE‐type phosphorescence to Au0‐core‐dictated fluorescence. This effect becomes more prominent when the degree of aggregation of Au NCs increases in solution. 相似文献
83.
Qi‐Zhi Zhong Joseph J. Richardson Shiyao Li Wenjie Zhang Yi Ju Jianhua Li Shuaijun Pan Jingqu Chen Frank Caruso 《Angewandte Chemie (International ed. in English)》2020,59(4):1711-1717
Functional coatings are of considerable interest because of their fundamental implications for interfacial assembly and promise for numerous applications. Universally adherent materials have recently emerged as versatile functional coatings; however, such coatings are generally limited to catechol, (ortho‐diphenol)‐containing molecules, as building blocks. Here, we report a facile, biofriendly enzyme‐mediated strategy for assembling a wide range of molecules (e.g., 14 representative molecules in this study) that do not natively have catechol moieties, including small molecules, peptides, and proteins, on various surfaces, while preserving the molecule's inherent function, such as catalysis (≈80 % retention of enzymatic activity for trypsin). Assembly is achieved by in situ conversion of monophenols into catechols via tyrosinase, where films form on surfaces via covalent and coordination cross‐linking. The resulting coatings are robust, functional (e.g., in protective coatings, biological imaging, and enzymatic catalysis), and versatile for diverse secondary surface‐confined reactions (e.g., biomineralization, metal ion chelation, and N‐hydroxysuccinimide conjugation). 相似文献
84.
Zhang Jiaqing Zhang Bosi Li Wenjie Ouyang Benhong Fan Minghao Wang Haoming 《Journal of Thermal Analysis and Calorimetry》2020,140(6):2749-2756
Journal of Thermal Analysis and Calorimetry - The burning process and typical fire parameters of power-cable silicon ointment were explored experimentally using a cone calorimeter, and the effects... 相似文献
85.
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
86.
Zhu Mao Yutong Ye Haiming Lv Xiao Xia Han Yeonju Park Libin Zang Bing Zhao Young Mee Jung 《Angewandte Chemie (International ed. in English)》2020,59(27):10780-10784
Interfaces play an important role in enhancing the energy conversion performance of dye‐sensitized solar cells (DSCs). The interface effects have been studied by many techniques, but most of the studies only focused on one part of a DSC, rather than on a complete solar cell. Hence, monitoring the interface evolution of a DSC is still very challenging. Here, in situ/operando resonance Raman (RR) spectroscopic analyses were carried out to monitor the dynamics of the photovoltaic conversion processes in a DSC. We observed the creation of new species (i.e., polyiodide and iodine aggregates) in the photosensitization process. We also obtained molecular‐scale dynamic evidence that the bands from the C=C and C=N bonds of 2,2′‐bipyridyl (bpy), the S=C=N bonds of the NCS ligand, and photochemical products undergo reasonably strong intensity and frequency changes, which clearly demonstrates that they are involved in charge separation. Furthermore, RR spectroscopy can also be used to quickly evaluate the performance of DSCs. 相似文献
87.
Yanan Jiang Wenjie Ma Yujuan Qiao Yifei Xue Jiahao Lu Jun Gao Nannan Liu Fei Wu Ping Yu Lei Jiang Lanqun Mao 《Angewandte Chemie (International ed. in English)》2020,59(31):12795-12799
Biological ion channels and ion pumps with sub‐nanometer sizes modulate ion transport in response to external stimuli. Realizing such functions with sub‐nanometer solid‐state nanopores has been an important topic with wide practical applications. Herein, we demonstrate a biomimetic photoresponsive ion channel and photodriven ion pump using a porphyrin‐based metal–organic framework membrane with pore sizes comparable to hydrated ions. We show that the molecular‐size pores enable precise and robust optoelectronic ion transport modulation in a broad range of concentrations, unparalleled with conventional solid‐state nanopores. Upon decoration with platinum nanoparticles to form a Schottky barrier photodiode, photovoltage across the membrane is generated with “uphill” ion transport from low concentration to high concentration. These results may spark applications in energy conversion, ion sieving, and artificial photosynthesis. 相似文献
88.
The dielectric elastomer (DE) has attracted significant attention due to its desired features, including large deformation, fast response, and high energy density. However, for a DE actuator (DEA) utilizing a snap-through deformation mode, most existing theoretical models fail to predict its deformation path. This paper develops a new finite element method (FEM) based on the three-parameter Gent-Gent model suitable for capturing strain-stiffening behaviors. The simulation results are verified by experiments, indicating that the FEM can accurately characterize the snap-through path of a DE. The method proposed in this paper provides theoretical guidance and inspiration for designing and applying DEs and bistable electroactive actuators. 相似文献
89.
电缆沿桥跨海铺设是海缆铺设的一种新的形式, 针对由汽车和列车交通载荷诱发的沿跨海桥梁敷设电缆的振动问题, 建立了桥梁-电缆的整体组合结构分析模型, 将汽车和列车的作用载荷简化为移动的随机集中载荷序列, 发展虚拟激励法(pseudo-excitation method, PEM)用于分析移动随机载荷作用下电缆位移和应力响应的标准差及演变功率谱 (power spectral density, PSD), 并研究了汽车和列车运行速度对电缆动力响应标准差的影响. PEM将移动随机载荷问题转化为特定频率简谐移动载荷作用下的动力响应分析, 能够计算得到与Monte Carlo (MC) 方法非常吻合的电缆动力响应标准差, 但所需的时域响应分析次数远少于MC方法. 数值结果表明, 随着汽车和列车运行速度的提升, 电缆位移和应力标准差呈现增大的趋势; 在汽车和列车交通载荷作用下, 铝护套的位移标准差和功率谱的值比缆芯要大, 这可能会使得电缆的疲劳破坏首先发生在铝护套层, 本文工作对电缆沿桥跨海铺设实际工程具有一定的借鉴意义. 相似文献
90.
Nonlinear Dynamics - During the process of spacecraft launch, the extreme vibration environment is the major influence factor that induces the failure of the mission. Inspired by the smooth motions... 相似文献