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91.
Tho Duc Khanh Nguyen Stefania Rabasco Alicia A. Lork Andre Du Toit Prof. Andrew G. Ewing 《Angewandte Chemie (International ed. in English)》2023,62(28):e202304098
We used correlative transmission electron microscopy (TEM) and nanoscale secondary ion mass spectrometry (NanoSIMS) imaging to quantify the contents of subvesicular compartments, and to measure the partial release fraction of 13C-dopamine in cellular nanovesicles as a function of size. Three modes of exocytosis comprise full release, kiss-and-run, and partial release. The latter has been subject to scientific debate, despite a growing amount of supporting literature. We tailored culturing procedures to alter vesicle size and definitively show no size correlation with the fraction of partial release. In NanoSIMS images, vesicle content was indicated by the presence of isotopic dopamine, while vesicles which underwent partial release were identified by the presence of an 127I-labelled drug, to which they were exposed during exocytosis allowing entry into the open vesicle prior to its closing again. Demonstration of similar partial release fractions indicates that this mode of exocytosis is predominant across a wide range of vesicle sizes. 相似文献
92.
Hongting Du Haoran Guo Kaike Wang Xiangning Du Bayu Admasu Beshiwork Shengjun Sun Yongsong Luo Dr. Qian Liu Prof. Tingshuai Li Prof. Xuping Sun 《Angewandte Chemie (International ed. in English)》2023,62(5):e202215782
We propose the pseudobrookite Fe2TiO5 nanofiber with abundant oxygen vacancies as a new electrocatalyst to ambiently reduce nitrate to ammonia. Such catalyst achieves a large NH3 yield of 0.73 mmol h−1 mg−1cat. and a high Faradaic Efficiency (FE) of 87.6 % in phosphate buffer saline solution with 0.1 M NaNO3, which is lifted to 1.36 mmol h−1 mg−1cat. and 96.06 % at −0.9 V vs. RHE for nitrite conversion to ammonia in 0.1 M NaNO2. It also shows excellent electrochemical durability and structural stability. Theoretical calculation reveals the enhanced conductivity of this catalyst and an extremely low free energy of −0.28 eV for nitrate adsorption at the presence of vacant oxygen. 相似文献
93.
Dr. Dao-Sheng Liu Zhaoyu Zhang Dr. Yufei Zhang Dr. Minghui Ye Song Huang Shunzhang You Zijian Du Jiangfeng He Dr. Zhipeng Wen Dr. Yongchao Tang Prof. Xiaoqing Liu Prof. Cheng Chao Li 《Angewandte Chemie (International ed. in English)》2023,62(5):e202215385
The anode-cathode interplay is an important but rarely considered factor that initiates the degradation of aqueous zinc ion batteries (AZIBs). Herein, to address the limited cyclability issue of V-based AZIBs, Al2(SO4)3 is proposed as decent electrolyte additive to manipulate OH−-mediated cross-communication between Zn anode and NaV3O8 ⋅ 1.5H2O (NVO) cathode. The hydrolysis of Al3+ creates a pH≈0.9 strong acidic environment, which unexpectedly prolongs the anode lifespan from 200 to 1000 h. Such impressive improvement is assigned to the alleviation of interfacial OH− accumulation by Al3+ adsorption and solid electrolyte interphase formation. Accordingly, the strongly acidified electrolyte, associated with the sedated crossover of anodic OH− toward NVO, remarkably mitigate its undesired dissolution and phase transition. The interrupted OH−-mediated communication between the two electrodes endows Zn||NVO batteries with superb cycling stability, at both low and high scan rates. 相似文献
94.
Xingxing Zhang Qingmei Su Gaohui Du Bingshe Xu Shun Wang Zhuo Chen Liming Wang Wenhuan Huang Huan Pang 《Angewandte Chemie (International ed. in English)》2023,62(39):e202304947
Pursuing high power density lithium metal battery with high safety is essential for developing next-generation energy-storage devices, but uncontrollable electrolyte degradation and the consequence formed unstable solid-electrolyte interface (SEI) make the task really challenging. Herein, an ionic liquid (IL) confined MOF/Polymer 3D-porous membrane was constructed for boosting in situ electrochemical transformations of Janus-heterarchical LiF/Li3N-rich SEI films on the nanofibers. Such a 3D-Janus SEI-incorporated into the separator offers fast Li+ transport routes, showing superior room-temperature ionic conductivity of 8.17×10−4 S cm−1 and Li+ transfer number of 0.82. The cryo-TEM was employed to visually monitor the in situ formed LiF and Li3N nanocrystals in SEI and the deposition of Li dendrites, which is greatly benefit to the theoretical simulation and kinetic analysis of the structural evolution during the battery charge and discharge process. In particular, this membrane with high thermal stability and mechanical strength used in solid-state Li||LiFePO4 and Li||NCM-811 full cells and even in pouch cells showed enhanced rate-performance and ultra-long life spans. 相似文献
95.
Xiangyu Li Ailing Tang Helin Wang Zongtao Wang Mengzhen Du Qiang Guo Qing Guo Erjun Zhou 《Angewandte Chemie (International ed. in English)》2023,62(39):e202306847
A third component featuring a planar backbone structure similar to the binary host molecule has been the preferred ingredient for improving the photovoltaic performance of ternary organic solar cells (OSCs). In this work, we explored a new avenue that introduces 3D-structured molecules as guest acceptors. Spirobifluorene (SF) is chosen as the core to combine with three different terminal-modified (rhodanine, thiazolidinedione, and dicyano-substituted rhodanine) benzotriazole (BTA) units, affording three four-arm molecules, SF-BTA1, SF-BTA2, and SF-BTA3, respectively. After adding these three materials to the classical system PM6 : Y6, the resulting ternary devices obtained ultra-high power-conversion efficiencies (PCEs) of 19.1 %, 18.7 %, and 18.8 %, respectively, compared with the binary OSCs (PCE=17.4 %). SF-BTA1-3 can work as energy donors to increase charge generation via energy transfer. In addition, the charge transfer between PM6 and SF-BTA1-3 also acts to enhance charge generation. Introducing SF-BTA1-3 could form acceptor alloys to modify the molecular energy level and inhibit the self-aggregation of Y6, thereby reducing energy loss and balancing charge transport. Our success in 3D multi-arm materials as the third component shows good universality and brings a new perspective. The further functional development of multi-arm materials could make OSCs more stable and efficient. 相似文献
96.
Chuanshen Du Paul Gregory Dhanush U. Jamadgni Alana M. Pauls Julia J. Chang Rick W. Dorn Andrew Martin E. Johan Foster Aaron J. Rossini Martin Thuo 《Angewandte Chemie (International ed. in English)》2023,62(44):e202308822
Combustion is often difficult to spatially direct or tune associated kinetics—hence a run-away reaction. Coupling pyrolytic chemical transformation to mass transport and reaction rates (Damköhler number), however, we spatially directed ignition with concomitant switch from combustion to pyrolysis (low oxidant). A ‘surface-then-core’ order in ignition, with concomitant change in burning rate,is therefore established. Herein, alkysilanes grafted onto cellulose fibers are pyrolyzed into non-flammable SiO2 terminating surface ignition propagation, hence stalling flame propagating. Sustaining high temperatures, however, triggers ignition in the bulk of the fibers but under restricted gas flow (oxidant and/or waste) hence significantly low rate of ignition propagation and pyrolysis compared to open flame (Liñán's equation). This leads to inside-out thermal degradation and, with felicitous choice of conditions, formation of graphitic tubes. Given the temperature dependence, imbibing fibers with an exothermically oxidizing synthon (MnCl2) or a heat sink (KCl) abets or inhibits pyrolysis leading to tuneable wall thickness. We apply this approach to create magnetic, paramagnetic, or oxide containing carbon fibers. Given the surface sensitivity, we illustrate fabrication of nm- and μm-diameter tubes from appropriately sized fibers. 相似文献
97.
Taotao Wang Li Zhang Jinbao Wu Prof. Muqing Chen Prof. Shangfeng Yang Prof. Yalin Lu Prof. Pingwu Du 《Angewandte Chemie (International ed. in English)》2023,62(40):e202311352
A few-layer fullerene network possesses several advantageous characteristics, including a large surface area, abundant active sites, high charge mobility, and an appropriate band gap and band edge for solar water splitting. Herein, we report for the first time that the few-layer fullerene network shows interesting photocatalytic performance in pure water splitting into H2 and H2O2 in the absence of any sacrificial reagents. Under optimal conditions, the H2 and H2O2 evolution rates can reach 91 and 116 μmol g−1 h−1, respectively, with good stability. This work demonstrates the novel application of the few-layer fullerene network in the field of energy conversion. 相似文献
98.
Guopeng Du Pingliang Zhu Jing Wang Xinjin Li Dao-Peng Zhang Chuan-Zeng Wang Prof. Dr. Feng-Gang Sun 《European journal of organic chemistry》2023,26(6):e202201382
Herein, we report a palladium/norbornene/copper co-catalyzed single-step approach that merges selective ortho C−H bond esterification with ipso thiolation for construction of synthetically versatile 2-arylthio aryl esters under exceptionally mild conditions. Importantly, this process proceeded in a highly efficient manner, allowing alkoxycarbonyl and thio groups to be installed into one aryl iodides simultaneously by harnessing thiocarbonate as bifunctional reagent. The method has been demonstrated to accommodate good functionalities and features broad substrate scope. 相似文献
99.
Temiloluwa T. Adejumo Marianna Danopoulou Leandros P. Zorba Dr. Andrej Pevec Dr. Matija Zlatar Dr. Dušanka Radanović Milica Savić Prof. Dr. Maja Gruden Prof. Dr. Katarina K. Anđelković Prof. Dr. Iztok Turel Dr. Božidar Čobeljić Prof. Dr. Georgios C. Vougioukalakis 《欧洲无机化学杂志》2023,26(33):e202300193
Two new Zn(II) complexes bearing tridentate hydrazone-based ligands with NNO or NNS donor atoms were synthesised and characterised by elemental analysis, infrared (IR) and nuclear magnetic resonance (NMR) spectroscopies, and single crystal X-ray diffraction methods. These complexes, together with four previously synthesised analogues, having hydrazone ligands with a NNO donor set of atoms, were successfully employed as catalysts in the ketone-amine-alkyne (KA2) coupling reaction, furnishing tetrasubstituted propargylamines, compounds with unique applications in organic chemistry. DFT calculations at the CAM-B3LYP/TZP level of theory were performed to elucidate the electronic structure of the investigated Zn(II) complexes, excellently correlating the structure of the complexes to their catalytic reactivity. 相似文献
100.
The realization of ferromagnetic ordering of two-dimensional (2D) carbon material graphdiyne (GDY) has attracted great attention due to its promising application in spin semiconductor devices. However, the absence of localized spins makes the pristine GDY intrinsically nonferromagnetic. Herein, we report the realization of robust room-temperature (RT) ferromagnetism (FM) with Curie temperature (TC) up to 325 K for GDY Nanosheets (GDYNs) by supercritical CO2 (SC CO2). Experimental and theoretical calculations reveal that the new chemical bond of C−O−Si can be formed because of the unique effect of SC CO2, which help to enhance the charge transfer and generates long-range ferromagnetic order. The RT saturation magnetization (MS) reaches 1.125 emu/g, which is much higher than that of carbon-based materials reported up to now. Meanwhile, by changing the conditions of SC CO2 such as pressure, ferromagnetic responses can be manipulated, which is great for potential spintronics applications of GDY. 相似文献