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141.
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Atika Muhammad Dr. Graziano Di Carmine Luke Forster Dr. Carmine D'Agostino 《Chemphyschem》2020,21(11):1101-1106
Solvent effects in homogeneous catalysis are known to affect catalytic activity. Whilst these effects are often described using qualitative features, such as Kamlet-Taft parameters, experimental tools able to quantify and reveal in more depth such effects have remained unexplored. In this work, PFG NMR diffusion and T1 relaxation measurements have been carried out to probe solvent effects in the homogeneous catalytic reduction of propionaldehyde to 1-propanol in the presence of aluminium isopropoxide catalyst. Using data on diffusion coefficients it was possible to estimate trends in aggregation of different solvents. The results show that solvents with a high hydrogen-bond accepting ability, such as ethers, tend to form larger aggregates, which slow down the molecular dynamics of aldehyde molecules, as also suggested by T1 measurements, and preventing their access to the catalytic sites, which results in the observed decrease of catalytic activity. Conversely, weakly interacting solvents, such as alkanes, do not lead to the formation of such aggregates, hence allowing easy access of the aldehyde molecules to the catalytic sites, resulting in higher catalytic activity. The work reported here is a clear example on how combining traditional catalyst screening in homogeneous catalysis with NMR diffusion and relaxation time measurements can lead to new physico-chemical insights into such systems by providing data able to quantify aggregation phenomena and molecular dynamics. 相似文献
144.
Cover Picture: Mild and Low‐Pressure fac‐Ir(ppy)3‐Mediated Radical Aminocarbonylation of Unactivated Alkyl Iodides through Visible‐Light Photoredox Catalysis (Chem. Eur. J. 27/2016)
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145.
Sainan Luo Tao Yuan Luke Soule Jiafeng Ruan Yahui Zhao Dalin Sun Junhe Yang Meilin Liu Shiyou Zheng 《Advanced functional materials》2020,30(5)
Ion‐insertion capacitors show promise to bridge the gap between supercapacitors of high power densities and batteries of high energy densities. While research efforts have primarily focused on Li+‐based capacitors (LICs), Na+‐based capacitors (SICs) are theoretically cheaper and more sustainable. Owing to the larger size of Na+ compared to Li+, finding high‐rate anode materials for SICs has been challenging. Herein, an SIC anode architecture is reported consisting of TiO2 nanoparticles anchored on a sheared‐carbon nanotubes backbone (TiO2/SCNT). The SCNT architecture provides advantages over other carbon architectures commonly used, such as reduced graphene oxide and CNT. In a half‐cell, the TiO2/SCNT electrode shows a capacity of 267 mAh g?1 at a 1 C charge/discharge rate and a capacity of 136 mAh g?1 at 10 C while maintaining 87% of initial capacity over 1000 cycles. When combined with activated carbon (AC) in a full cell, an energy density and power density of 54.9 Wh kg?1 and 1410 W kg?1, respectively, are achieved while retaining a 90% capacity retention over 5000 cycles. The favorable rate capability, energy and power density, and durability of the electrode is attributed to the enhanced electronic and Na+ conductivity of the TiO2/SCNT architecture. 相似文献
146.
Ryan Murphy Yucun Zhou Lei Zhang Luke Soule Weilin Zhang Yu Chen Meilin Liu 《Advanced functional materials》2020,30(35)
Reversible solid oxide cells based on ceramic proton conductors have potential to be the most efficient system for large‐scale energy storage. The performance and long‐term durability of these systems, however, are often limited by the ionic conductivity or stability of the proton‐conducting electrolyte. Here new family of solid oxide electrolytes, BaHfxCe0.8?xY0.1Yb0.1O3?δ (BHCYYb), which demonstrate a superior ionic conductivity to stability trade‐off than the state‐of‐the‐art proton conductors, BaZrxCe0.8?xY0.1Yb0.1O3?δ (BZCYYb), at similar Zr/Hf concentrations, as confirmed by thermogravimetric analysis, Raman, and X‐ray diffraction analysis of samples over 500 h of testing are reported. The increase in performance is revealed through thermodynamic arguments and first‐principle calculations. In addition, lab scale full cells are fabricated, demonstrating high peak power densities of 1.1, 1.4, and 1.6 W cm?2 at 600, 650, and 700 °C, respectively. Round‐trip efficiencies for steam electrolysis at 1 A cm?2 are 78%, 72%, and 62% at 700, 650, and 600 °C, respectively. Finally, CO2? H2O electrolysis is carried out for over 700 h with no degradation. 相似文献
147.
Tuning the Molecular Weight of the Electron Accepting Polymer in All‐Polymer Solar Cells: Impact on Morphology and Charge Generation
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Rukiya Matsidik Shyamal K. K. Prasad Luke A. Connal Amelia C. Y. Liu Lars Thomsen Justin M. Hodgkiss Christopher R. McNeill 《Advanced functional materials》2018,28(18)
Molecular weight is an important factor determining the morphology and performance of all‐polymer solar cells. Through the application of direct arylation polycondention, a series of batches of a fluorinated naphthalene diimide‐based acceptor polymer are prepared with molecular weight varying from Mn = 20 to 167 kDa. Used in conjunction with a common low bandgap donor polymer, the effect of acceptor molecular weight on solar cell performance, morphology, charge generation, and transport is explored. Increasing the molecular weight of the acceptor from Mn = 20 to 87 kDa is found to increase cell efficiency from 2.3% to 5.4% due to improved charge separation and transport. Further increasing the molecular weight to Mn = 167 kDa however is found to produce a drop in performance to 3% due to liquid–liquid phase separation which produces coarse domains, poor charge generation, and collection. In addition to device studies, a systematic investigation of the microstructure and photophysics of this system is presented using a combination of transmission electron microscopy, grazing‐incidence wide‐angle X‐ray scattering, near‐edge X‐ray absorption fine‐structure spectroscopy, photoluminescence quenching, and transient absorption spectroscopy to provide a comprehensive understanding of the interplay between morphology, photophysics, and photovoltaic performance. 相似文献
148.
Gene delivery by electroporation after dielectrophoretic positioning of cells in a non-uniform electric field 总被引:1,自引:0,他引:1
MacQueen LA Buschmann MD Wertheimer MR 《Bioelectrochemistry (Amsterdam, Netherlands)》2008,72(2):141-148
We report the use of dielectrophoresis (DEP) to position U-937 monocytes within a non-uniform electric field, prior to electroporation (EP) for gene delivery. DEP positioning and EP pulsing were both accomplished using a common set of inert planar electrodes, micro-fabricated on a glass substrate. A single-shell model of the cell's dielectric properties and finite-element modeling of the electric field distribution permitted us to predict the major features of cell positioning. The extent to which electric pulses increased the permeability of the cell membranes to fluorescent molecules and to pEGFPLuc DNA plasmids were found to depend on prior positioning. For a given set of pulse parameters, EP was either irreversible (resulting in cytolysis), reversible (leading to gene delivery), or not detectable, depending on where cells were positioned. Our results clearly demonstrate that position-dependent EP of cells in a non-uniform electric field can be controlled by DEP. 相似文献
149.
150.
Xie F Li D Tyree L Li L Sovkov VB Ivanov VS Magnier S Marjatta Lyyra A 《The Journal of chemical physics》2008,128(20):204313
The Cs(2) 2 (3)Delta(1g) and b (3)Pi(0u) states have been observed by infrared-infrared double resonance spectroscopy for the first time. 221 2 (3)Delta(1g)<--A (1)Sigma(u) (+)<--X (1)Sigma(g) (+) double resonance lines have been assigned to transitions into the 2 (3)Delta(1g) v=6-13 vibrational levels. Resolved fluorescence into the b (3)Pi(0u) v(')=0-48 levels has been recorded. Molecular constants and potential energy curves are determined by the global fit of the entire set of the experimental data. Theoretical potential energy curves of the 2 (3)Delta(g) and b (3)Pi(u) states have been determined in the framework of the pseudopotential method and are compared with the experimental results. 相似文献