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211.
Mithilesh Kumar Nayak Jessica Stubbe Dr. Nicolás I. Neuman Dr. Ramakirushnan Suriya Narayanan Sandipan Maji Prof. Dr. Carola Schulzke Prof. Vadapalli Chandrasekhar Prof. Dr. Biprajit Sarkar Dr. Anukul Jana 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(19):4425-4431
This work presents a stepwise reversible two-electron transfer induced hydrogen shift leading to the conversion of a bis-pyrrolinium cation to an E-diaminoalkene and vice versa. Remarkably, the forward and the reverse reaction, which are both reversible, follow two completely different reaction pathways. Establishing such unprecedented property in this type of processes was possible by developing a novel synthetic route towards the starting dication. All intermediates involved in both the forward and the backward reactions were comprehensively characterized by a combination of spectroscopic, crystallographic, electrochemical, spectroelectrochemical, and theoretical methods. The presented synthetic route opens up new possibilities for the generation of multi-pyrrolinium cation scaffold-based organic redox systems, which constitute decidedly sought-after molecules in contemporary chemistry. 相似文献
212.
Lea Kremer Elisabeth Hennes Alexandra Brause Andrei Ursu Lucas Robke Hideaki T. Matsubayashi Yuta Nihongaki Jana Flegel Ivana Mejdrov Jan Eickhoff Matthias Baumann Radim Nencka Petra Janning Susanne Kordes Hans R. Schler Jared Sterneckert Takanari Inoue Slava Ziegler Herbert Waldmann 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(46):16770-16781
213.
Frontispiece: Dative Au→Al Interactions: Crystallographic Characterization and Computational Analysis
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Hasmat Khan Malobi Seth Atanu Naskar Sunirmal Jana 《Journal of Sol-Gel Science and Technology》2018,88(2):359-370
Nano noble metal coating on surface patterned mesoporous semiconductor thin film can play an important role in enhancing visible light harvesting efficiency (LHE) towards improvement in photoelectrochemical (PEC) activity of the material. In this work, one-dimensional (1D) and two-dimensional (2D) mesoscale surface patterns have been created on sol–gel-based titanium tin oxide (TSO) nanostructured thin film on pure silica/indium tin oxide-coated glass by soft lithography. The TSO film matrix is observed to be mesoporous and semicrystalline as evidenced from the structural characterization by transmission electron microscopy and measurement of atmospheric ellipso-porosimetry, respectively. The 2D patterned film exhibits maximum LHE value in visible wavelength region. Further film surface modification has been carried out by depositing nano Au coating onto the bare patterned TSO films by a low temperature solution technique. Under visible light, a significant improvement in PEC activity is found and the gold-coated patterned 2D film shows higher visible LHE as well as >2.7 times higher photocurrent density than bare 2D film. This facile fabrication strategy can create an avenue toward improvement in LHE vis-à-vis the PEC activity of mesoporous mixed metal oxide semiconductor thin film. 相似文献
218.
Chemical Fixation of CO2 and Other Heterogeneous Catalytic Studies by Employing a Layered Cu‐Porphyrin Prepared Through Single‐Crystal to Single‐Crystal Exchange of a Zn Analogue
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A solvothermal reaction of Zn(NO3)2 ? 6 H2O, tetra‐(4‐pyridyl)porphyrin (H2TPyP), and 4,4′‐oxybis(benzoic acid) (H2OBA) resulted in a new two‐dimensional Zn‐ porphyrin metal–organic framework compound, [Zn2(C40H24N8)0.5(C14H8O5)(DMA)](DMA)(H2O)6 ( 1 ; DMA=N,N‐dimethylacetamide). The ZnII ions present in 1 could be exchanged by using a solution of Cu(NO3)2 ? 3 H2O in DMA at room temperature to give [Cu2(C40H24N8)0.5(C14H8O5)(DMA)](DMA)(H2O)3 ( Cu∈1 ). The extra‐framework solvent molecules have been shown to be reversibly removed or exchanged without collapse of the framework. Solvent‐free Cu∈1 was explored as an active heterogeneous catalyst towards three different organic reactions: 1) the chemical fixation of CO2 into cyclic carbonate at room temperature and 1 atm; 2) the nitroaldol reaction under solvent‐free conditions, and 3) the three‐component coupling of aminopyridine, benzaldehyde, and aryl alkynes followed by 5‐exo‐dig cyclization to produce the important pharmacophore imidazopyridine. 相似文献
219.
Dr. Nguyen Van Nghia Dr. Saibal Jana Surendran Sujith Ji Yeon Ryu Prof. Junseong Lee Prof. Sang Uck Lee Prof. Min Hyung Lee 《Angewandte Chemie (International ed. in English)》2018,57(38):12483-12488
An approach to the design of nido‐carborane‐based luminescent compounds that can exhibit thermally activated delayed fluorescence (TADF) is proposed. 7,8‐Dicarba‐nido‐undecaboranes (nido‐carboranes) having various 8‐R groups (R=H, Me, i‐Pr, Ph) are appended to the meta or para position of the phenyl ring of the dimesitylphenylborane (PhBMes2) acceptor, forming donor–acceptor compounds (nido‐ m1 – m4 and nido‐ p1 – p4 ). The bulky 8‐R group and meta substitution of the nido‐carborane are essential to attain a highly twisted arrangement between the donor and acceptor moieties, leading to a very small energy splitting between the singlet and triplet excited states (ΔEST <0.05 eV for nido‐ m2 , ‐ m3 , and ‐ p3 ). These compounds exhibit efficient TADF with microsecond‐range lifetimes. In particular, nido‐ m2 and ‐ m3 display aggregation‐induced emission (AIE) with TADF properties. 相似文献
220.
Soft Phonon Modes Leading to Ultralow Thermal Conductivity and High Thermoelectric Performance in AgCuTe
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Subhajit Roychowdhury Manoj K. Jana Jaysree Pan Satya N. Guin Prof. Dirtha Sanyal Prof. Umesh V. Waghmare Prof. Kanishka Biswas 《Angewandte Chemie (International ed. in English)》2018,57(15):4043-4047
Crystalline solids with intrinsically low lattice thermal conductivity (κL) are crucial to realizing high‐performance thermoelectric (TE) materials. Herein, we show an ultralow κL of 0.35 Wm?1 K?1 in AgCuTe, which has a remarkable TE figure‐of‐merit, zT of 1.6 at 670 K when alloyed with 10 mol % Se. First‐principles DFT calculation reveals several soft phonon modes in its room‐temperature hexagonal phase, which are also evident from low‐temperature heat‐capacity measurement. These phonon modes, dominated by Ag vibrations, soften further with temperature giving a dynamic cation disorder and driving the superionic transition. Intrinsic factors cause an ultralow κL in the room‐temperature hexagonal phase, while the dynamic disorder of Ag/Cu cations leads to reduced phonon frequencies and mean free paths in the high‐temperature rocksalt phase. Despite the cation disorder at elevated temperatures, the crystalline conduits of the rigid anion sublattice give a high power factor. 相似文献