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991.
Dr. Weihui Ou Dr. Binbin Zhou Junda Shen Dr. Tsz Wing Lo Prof. Dangyuan Lei Dr. Shengliang Li Jing Zhong Prof. Yang Yang Li Prof. Jian Lu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(17):6856-6859
Hot carriers (HCs) and thermal effects, stemming from plasmon decays, are crucial for most plasmonic applications. However, quantifying these two effects remains extremely challenging due to the experimental difficulty in accurately measuring the temperature at reaction sites. Herein, we provide a novel strategy to disentangle HCs from photothermal effects based on the different traits of heat dissipation (long range) and HCs transport (short range), and quantitatively uncover the dominant and potential-dependent role of photothermal effect by investigating the rapid- and slow-response currents in plasmon-mediated electrochemistry at nanostructured Ag electrode. Furthermore, the plasmoelectric surface potential is found to contribute to the rapid-response currents, which is absent in the previous studies. 相似文献
992.
Dr. Lu Jin Fangyuan Cheng Hao Li Prof. Dr. Kui Xie 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(23):8976-8980
Porous tantalum nitride (Ta3N5) single crystals, combining structural coherence and porous microstructure, would substantially improve the photoelectrochemical performance. The structural coherence would reduce the recombination of charge carriers and maintain excellent transport properties while the porous microstructure would not only reduce photon scattering but also facilitate surface reactions. Here, we grow bulk-porous Ta3N5 single crystals on a two-centimeter scale with (002), (023), and (041) facets, respectively, and show significantly enhanced photoelectrochemical performance. We show the preferential facet growth of porous crystals in a lattice reconstruction strategy in relation to lattice match and lattice channel. We present the facet engineering to enhance light absorption, exciton lifetime and transport properties. The porous Ta3N5 single crystal boosts photoelectrochemical oxidation of alcohols with the (002) facet showing the highest performance of >99 % alcohol conversion and >99 % aldehyde/ketone selectivity. 相似文献
993.
Dr. Song Jin Youxuan Ni Zhimeng Hao Prof. Kai Zhang Dr. Yong Lu Dr. Zhenhua Yan Dr. Yajuan Wei Dr. Ying-Rui Lu Dr. Ting-Shan Chan Prof. Jun Chen 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(49):22069-22073
A general graphene quantum dot-tethering design strategy to synthesize single-atom catalysts (SACs) is presented. The strategy is applicable to different metals (Cr, Mn, Fe, Co, Ni, Cu, and Zn) and supports (0D carbon nanosphere, 1D carbon nanotube, 2D graphene nanosheet, and 3D graphite foam) with the metal loading of 3.0–4.5 wt %. The direct transmission electron microscopy imaging and X-ray absorption spectra analyses confirm the atomic dispersed metal in carbon supports. Our study reveals that the abundant oxygenated groups for complexing metal ions and the rich defective sites for incorporating nitrogen are essential to realize the synthesis of SACs. Furthermore, the carbon nanotube supported Ni SACs exhibits high electrocatalytic activity for CO2 reduction with nearly 100 % CO selectivity. This universal strategy is expected to open up new research avenues to produce SACs for diverse electrocatalytic applications. 相似文献
994.
Dr. Pengfei Cheng Lu Feng Prof. Dr. Yuefeng Liu Dr. Daoyuan Zheng Youbao Sang Wenyuan Zhao Dr. Yang Yang Dr. Songqiu Yang Prof. Dr. Donghui Wei Prof. Dr. Guoxiong Wang Prof. Dr. Keli Han 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(48):21598-21602
All-inorganic zero-dimensional (0D) metal halides have recently received increasing attention due to their excellent photoluminescence (PL) performance and high stability. Herein, we present the successful doping of copper(I) into 0D Cs2ZnBr4. The incorporating of Cu+ cations enables the originally weakly luminescent Cs2ZnBr4 to exhibit an efficient blue emission centered at around 465 nm, with a high photoluminescence quantum yield (PLQY) of 65.3 %. Detailed spectral characterizations, including ultrafast transient absorption (TA) techniques, were carried out to investigate the effect of Cu+ dopants and the origin of blue emission in Cs2ZnBr4:Cu. To further study the role of the A-site cation and halogen, A2ZnCl4:Cu (A=Cs, Rb) were also synthesized and found to generate intense sky-blue emission (PLQY≈73.1 %). This work represents an effective strategy for the development of environmentally friendly, low-cost and high-efficiency blue-emitting 0D all-inorganic metal halides. 相似文献
995.
Yue Sun Dr. Tiandu Dong Dr. Chunxin Lu Weiwen Xin Linsen Yang Pei Liu Yongchao Qian Yuanyuan Zhao Dr. Xiang-Yu Kong Prof. Liping Wen Prof. Lei Jiang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(40):17576-17581
Osmotic energy, obtained through different concentrations of salt solutions, is recognized as a form of a sustainable energy source. In the past years, membranes derived from asymmetric aromatic compounds have attracted attention because of their low cost and high performance in osmotic energy conversion. The membrane formation process, charging state, functional groups, membrane thickness, and the ion-exchange capacity of the membrane could affect the power generation performance. Among asymmetric membranes, a bipolar membrane could largely promote the ion transport. Here, two polymers with the same poly(ether sulfone) main chain but opposite charges were synthesized to prepare bipolar membranes by a nonsolvent-induced phase separation (NIPS) and spin-coating (SC) method. The maximum power density of the bipolar membrane reaches about 6.2 W m−2 under a 50-fold salinity gradient, and this result can serve as a reference for the design of bipolar membranes for osmotic energy conversion systems. 相似文献
996.
Dr. Yuanyuan Li Dr. Shunjie Liu Huwei Ni Haoke Zhang Dr. Hequn Zhang Clarence Chuah Chao Ma Prof. Kam Sing Wong Prof. Jacky W. Y. Lam Prof. Ryan T. K. Kwok Prof. Jun Qian Prof. Xuefeng Lu Prof. Ben Zhong Tang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(31):12922-12926
The traditional design strategies for highly bright solid-state luminescent materials rely on weakening the intermolecular π–π interactions, which may limit diversity when developing new materials. Herein, we propose a strategy of tuning the molecular packing mode by regioisomerization to regulate the solid-state fluorescence. TBP-e-TPA with a molecular rotor in the end position of a planar core adopts a long-range cofacial packing mode, which in the solid state is almost non-emissive. By shifting molecular rotors to the bay position, the resultant TBP-b-TPA possesses a discrete cross packing mode, giving a quantum yield of 15.6±0.2 %. These results demonstrate the relationship between the solid-state fluorescence efficiency and the molecule's packing mode. Thanks to the good photophysical properties, TBP-b-TPA nanoparticles were used for two-photon deep brain imaging. This molecular design philosophy provides a new way of designing highly bright solid-state fluorophores. 相似文献
997.
Yanan Jiang Wenjie Ma Yujuan Qiao Yifei Xue Jiahao Lu Jun Gao Nannan Liu Fei Wu Prof. Ping Yu Prof. Lei Jiang Prof. Lanqun Mao 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(31):12895-12899
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
998.
Dr. Ding Yi Fei Lu Fengchu Zhang Dr. Shoujie Liu Dr. Bo Zhou Denglei Gao Prof. Xi Wang Prof. Jiannian Yao 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(37):15989-15993
Single-atom catalysts have attracted much attention. Reported herein is that regulating charge transfer of lattice oxygen atoms in serial single-atom-doped titania enables tunable hydrogen evolution reaction (HER) activity. First-principles calculations disclose that the activity of lattice oxygen for the HER can be regularly promoted by substituting its nearest metal atom, and doping-induced charge transfer plays an essential role. Besides, the realm of the charge transfer of the active site can be enlarged to the second nearest atom by creating oxygen vacancies, resulting in further optimization for the HER. Various single-atom-doped titania nanosheets were fabricated to validate the proposed model. Taking advantage of the localized charge transfer to the lattice atom is demonstrated to be feasible for realizing precise regulation of the electronic structures and thus catalytic activity of the nanosheets. 相似文献
999.
Qun-Liang Zhang Qin Xiong Miao-Miao Li Wei Xiong Bin Shi Prof. Yu Lan Prof. Liang-Qiu Lu Prof. Wen-Jing Xiao 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(33):14200-14204
Higher-order cycloadditions, particularly [8+2] cycloadditions, are a straightforward and efficient strategy for constructing significant medium-sized architectures. Typically, configuration-restrained conjugated systems are utilized as 8π-components for higher-order concerted cycloadditions. However, for this reason, 10-membered monocyclic skeletons have never been constructed via catalytic asymmetric [8+2] cycloaddition with high peri- and stereoselectivity. Here, we accomplished an enantioselective [8+2] dipolar cycloaddition via the merger of visible-light activation and asymmetric palladium catalysis. This protocol provides a new route to 10-membered monocyclic architectures bearing chiral quaternary stereocenters with high chemo-, peri-, and enantioselectivity. The success of this strategy relied on the facile in situ generation of Pd-containing 1,8-dipoles and their enantioselective trapping by ketene dipolarophiles, which were formed in situ via a photo-Wolff rearrangement. 相似文献
1000.