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981.
Xingtao Wang Dr. Yong Wang Dr. Taiyang Zhang Xiaomin Liu Prof. Yixin Zhao 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(4):1485-1489
The reduced dimension perovskite including 2D perovskites are one of the most promising strategies to stabilize lead halide perovskite. A mixed-cation 2D perovskite based on a steric phenyltrimethylammonium (PTA) cation is presented. The PTA-MA mixed-cation 2D perovskite of PTAMAPbI4 can be formed on the surface of MAPbI3 (PTAI-MAPbI3) by controllable PTAI intercalation by either spin coating or soaking. The PTAMAPbI4 capping layer can not only passivate PTAI-MAPbI3 perovskite but also act as MA+ locker to inhibit MAI extraction and significantly enhance the stability. The highly stable PTAI-MAPbI3 based perovskite solar cells exhibit a reproducible photovoltaic performance with a champion PCE of 21.16 %. Such unencapsulated devices retain 93 % of initial efficiency after 500 h continuous illumination. This steric mixed-cation 2D perovskite as MA+ locker to stabilize the MAPbI3 is a promising strategy to design stable and high-performance hybrid lead halide perovskites. 相似文献
982.
Zheng Li Liang Zhang Yong Liu Chenyi Shao Yuying Gao Prof. Fengtao Fan Prof. Junxi Wang Prof. Jinmin Li Prof. Janchang Yan Prof. Rengui Li Prof. Can Li 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(2):945-952
Photocatalytic overall water splitting has been recognized as a promising approach to convert solar energy into hydrogen. However, most of the photocatalysts suffer from low efficiencies mainly because of poor charge separation. Herein, taking a model semiconductor gallium nitride (GaN) as an example, we uncovered that photogenerated electrons and holes can be spatially separated to the nonpolar and polar surfaces of GaN nanorod arrays, which is presumably ascribed to the different surface band bending induced by the surface polarity. The photogenerated charge separation efficiency of GaN can be enhanced significantly from about 8 % to more than 80 % via co-exposing polar and nonpolar surfaces. Furthermore, spatially assembling reduction and oxidation cocatalysts on the nonpolar and polar surfaces remarkably boosts photocatalytic overall water splitting, with the quantum efficiency increased from 0.9 % for the film photocatalyst to 6.9 % for the nanorod arrays photocatalyst. 相似文献
983.
Dr. Yong Wang Yajun Zhao Shuaishuai Zhu Prof. Dr. Xingping Zhou Prof. Dr. Jing Xu Prof. Dr. Xiaolin Xie Prof. Dr. Rinaldo Poli 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(15):6044-6050
A strategy that uses carbon monoxide (CO) as a molecular trigger to switch the polymerization mechanism of a cobalt Salen complex [salen=(R,R)-N,N′-bis(3,5-di-tert-butylsalicylidene)-1,2-cyclohexanediamine] from ring-opening copolymerization (ROCOP) of epoxides/anhydrides to organometallic mediated controlled radical polymerization (OMRP) of acrylates is described. The key phenomenon is a rapid and quantitative insertion of CO into the Co−O bond, allowing for in situ transformation of the ROCOP active species (Salen)CoIII-OR into the OMRP photoinitiator (Salen)CoIII-CO2R. The proposed mechanism, which involves CO coordination to (Salen)CoIII-OR and subsequent intramolecular rearrangement via migratory insertion has been rationalized by DFT calculations. Regulated by both CO and visible light, on-demand sequence control can be achieved for the one-pot synthesis of polyester-b-polyacrylate diblock copolymers (Đ<1.15). 相似文献
984.
Dr. Zheng Yi Song Jiang Dr. Jie Tian Yong Qian Prof. Shimou Chen Prof. Shiqiang Wei Dr. Ning Lin Prof. Yitai Qian 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(16):6521-6527
An amidation-dominated re-assembly strategy is developed to prepare uniform single atom Ni/S/C nanotubes. In this re-assembly process, a single-atom design and nano-structured engineering are realized simultaneously. Both the NiO5 single-atom active centers and nanotube framework endow the Ni/S/C ternary composite with accelerated reaction kinetics for potassium-ion storage. Theoretical calculations and electrochemical studies prove that the atomically dispersed Ni could enhance the convention kinetics and decrease the decomposition energy barrier of the chemically-absorbed small-molecule sulfur in Ni/S/C nanotubes, thus lowering the electrode reaction overpotential and resistance remarkably. The mechanically stable nanotube framework could well accommodate the volume variation during potassiation/depotassiation process. As a result, a high K-storage capacity of 608 mAh g−1 at 100 mA g−1 and stable cycling capacity of 330.6 mAh g−1 at 1000 mA g−1 after 500 cycles are achieved. 相似文献
985.
986.
Here we described the design and synthesis of a discrete 3D amphiphilic metallacage 4,in which the tetragonal prismatic frameworks act as the hydrophobic cores and the poly(ethylene glycol)(PEG)chains as the hydrophilic tails.The structure of 4 was characterized by 1H NMR,31P NMR and electrospray ionization time-of-flight mass spectrometry(ESI-TOF-MS).Notably,4 with its Iong PEG tails was subsequently ordered into micelles at a low concentration(1.20×10^-6 mol/L)in water.As the concentration and cultivation time increased,the micelles can further self-assembly into nanofibers and nanoribbons.Considering the dynamic property of the coordination bond,these structures show reversible transformation under external stimuli. 相似文献
987.
We apply the first-principles approach to study the structural stability, Vickers hardness, and elastic modulus of ReB12 and RuB12. In particular, we further investigate the influence of high pressure on the structural stability and mechanical properties of ReB12 and RuB12. The calculated results show that ReB12 and RuB12 are thermodynamic stability under high pressure. Here, ReB12 is more thermodynamic stability than that of the RuB12. The calculated Vickers hardness of ReB12 and RuB12 is 16.25 and 16.55 GPa, respectively. It is found that the calculated elastic constants and elastic modulus of ReB12 and RuB12 increase with increasing pressure. In particular, the calculated elastic constants and elastic modulus of ReB12 are larger than that of the RuB12. The calculated electronic structure shows that the high hardness and elastic modulus of ReB12 and RuB12 are attributed to the 3D network B-B covalent bonds. 相似文献
988.
Xingtao Wang Yong Wang Taiyang Zhang Xiaomin Liu Yixin Zhao 《Angewandte Chemie (International ed. in English)》2020,59(4):1469-1473
The reduced dimension perovskite including 2D perovskites are one of the most promising strategies to stabilize lead halide perovskite. A mixed‐cation 2D perovskite based on a steric phenyltrimethylammonium (PTA) cation is presented. The PTA‐MA mixed‐cation 2D perovskite of PTAMAPbI4 can be formed on the surface of MAPbI3 (PTAI‐MAPbI3) by controllable PTAI intercalation by either spin coating or soaking. The PTAMAPbI4 capping layer can not only passivate PTAI‐MAPbI3 perovskite but also act as MA+ locker to inhibit MAI extraction and significantly enhance the stability. The highly stable PTAI‐MAPbI3 based perovskite solar cells exhibit a reproducible photovoltaic performance with a champion PCE of 21.16 %. Such unencapsulated devices retain 93 % of initial efficiency after 500 h continuous illumination. This steric mixed‐cation 2D perovskite as MA+ locker to stabilize the MAPbI3 is a promising strategy to design stable and high‐performance hybrid lead halide perovskites. 相似文献
989.
Yao Xiao Yan‐Fang Zhu Wei Xiang Zhen‐Guo Wu Yong‐Chun Li Jing Lai Shi Li Enhui Wang Zu‐Guang Yang Chun‐Liu Xu Ben‐He Zhong Xiao‐Dong Guo 《Angewandte Chemie (International ed. in English)》2020,59(4):1491-1495
Demands for large‐scale energy storage systems have driven the development of layered transition‐metal oxide cathodes for room‐temperature rechargeable sodium ion batteries (SIBs). Now, an abnormal layered‐tunnel heterostructure Na0.44Co0.1Mn0.9O2 cathode material induced by chemical element substitution is reported. By virtue of beneficial synergistic effects, this layered‐tunnel electrode shows outstanding electrochemical performance in sodium half‐cell system and excellent compatibility with hard carbon anode in sodium full‐cell system. The underlying formation process, charge compensation mechanism, phase transition, and sodium‐ion storage electrochemistry are clearly articulated and confirmed through combined analyses of in situ high‐energy X‐ray diffraction and ex situ X‐ray absorption spectroscopy as well as operando X‐ray diffraction. This crystal structure engineering regulation strategy offers a future outlook into advanced cathode materials for SIBs. 相似文献
990.
Jing Guo Yan‐Zhong Fan Yu‐Lin Lu Shao‐Ping Zheng Cheng‐Yong Su 《Angewandte Chemie (International ed. in English)》2020,59(22):8661-8669
Although the photodimerization of acenaphthylene (ACE) has been known for 100 years, the asymmetric cycloaddition of its 1‐substituted derivatives is unknown. Herein, we report a supramolecular photochirogenic approach in which a homochiral and photoactive Δ/Λ‐[Pd6(RuL3)8]28+ metal–organic cage (Δ/Λ‐MOC‐16) is used as a supramolecular reactor for the enantioselective exited‐state photocatalysis of 1‐Br‐ACE. Owing to preorganization of the substrates by the supramolecular cage, stereochemical control of the triplet state, and nanospace transfer of energy and chirality, the cycloaddition of ACE proceeded with high selectivity for the formation of anti over syn stereoisomers, whereas the regio‐, stereo‐, and enantioselective cycloaddition of unsymmetrical 1‐Br‐ACE showed effective enantiodifferentiation of a pair of anti head‐to‐head stereoisomers. The enzyme‐mimicking photocatalysis was verified by catalytic turnover, rate enhancement, and competing‐guest inhibition experiments. 相似文献