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991.
Direct Detection of the Superoxide Anion as a Stable Intermediate in the Electroreduction of Oxygen in a Non‐Aqueous Electrolyte Containing Phenol as a Proton Source
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Prof. Zhangquan Peng Dr. Yuhui Chen Prof. Peter G. Bruce Prof. Ye Xu 《Angewandte Chemie (International ed. in English)》2015,54(28):8165-8168
The non‐aqueous Li–air (O2) battery has attracted intensive interest because it can potentially store far more energy than today′s batteries. Presently Li–O2 batteries suffer from parasitic reactions owing to impurities, found in almost all non‐aqueous electrolytes. Impurities include residual protons and protic compounds that can react with oxygen species, such as the superoxide (O2?), a reactive, one‐electron reduction product of oxygen. To avoid the parasitic reactions, it is crucial to have a fundamental understanding of the conditions under which reactive oxygen species are generated in non‐aqueous electrolytes. Herein we report an in situ spectroscopic study of oxygen reduction on gold in a dimethyl sulfoxide electrolyte containing phenol as a proton source. It is shown directly that O2?, not HO2, is the first stable intermediate during the oxygen reduction process to hydrogen peroxide. The unusual stability of O2? is explained using density functional theory (DFT) calculations. 相似文献
992.
Monitoring of Endogenous Hydrogen Sulfide in Living Cells Using Surface‐Enhanced Raman Scattering
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Dr. Da‐Wei Li Lu‐Lu Qu Kai Hu Prof. Dr. Yi‐Tao Long Prof. Dr. He Tian 《Angewandte Chemie (International ed. in English)》2015,54(43):12758-12761
Hydrogen sulfide (H2S) has emerged as an important gasotransmitter in diverse physiological processes, although many aspects of its roles remain unclear, partly owing to a lack of robust analytical methods. Herein we report a novel surface‐enhanced Raman scattering (SERS) nanosensor, 4‐acetamidobenzenesulfonyl azide‐functionalized gold nanoparticles (AuNPs/4‐AA), for detecting the endogenous H2S in living cells. The detection is accomplished with SERS spectrum changes of AuNPs/4‐AA resulting from the reaction of H2S with 4‐AA on AuNPs. The SERS nanosensor exhibits high selectivity toward H2S. Furthermore, AuNPs/4‐AA responds to H2S within 1 min with a 0.1 μM level of sensitivity. In particular, our SERS method can be utilized to monitor the endogenous H2S generated in living glioma cells, demonstrating its great promise in studies of pathophysiological pathways involving H2S. 相似文献
993.
Spectroscopic Observation of the Hydroxy Position in Butanol Hydrates and Its Effect on Hydrate Stability
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In this study, we investigate the crystal structures and phase equilibria of butanols+CH4+H2O systems to reveal the hydroxy group positioning and its effects on hydrate stability. Four clathrate hydrates formed by structural butanol isomers are identified with powder X‐ray diffraction (PXRD). In addition, Raman spectroscopy is used to analyze the guest distributions and inclusion behaviors of large alcohol molecules in these hydrate systems. The existence of a free OH indicates that guest molecules can be captured in the large cages of structure II hydrates without any hydrogen‐bonding interactions between the hydroxy group of the guests and the water‐host framework. However, Raman spectra of the binary (1‐butanol+CH4) hydrate do not show the free OH signal, indicating that there could be possible hydrogen‐bonding interactions between the guests and hosts. We also measure the four‐phase equilibrium conditions of the butanols+CH4+H2O systems. 相似文献
994.
The Quest for Polysulfides in Lithium–Sulfur Battery Electrolytes: An Operando Confocal Raman Spectroscopy Study
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Dr. Julien Hannauer Dr. Johan Scheers Julien Fullenwarth Dr. Bernard Fraisse Prof. Dr. Lorenzo Stievano Prof. Dr. Patrik Johansson 《Chemphyschem》2015,16(13):2755-2759
Confocal Raman spectra of a lithium–sulfur battery electrolyte are recorded operando in a depth‐of‐discharge resolved manner for an electrochemical cell with a realistic electrolyte/sulfur loading ratio. The evolution of various possible polysulfides is unambiguously identified by combining Raman spectroscopy data with DFT simulations. 相似文献
995.
Susana Chatzipapadopoulos Tobias Zentel Prof. Dr. Ralf Ludwig Matthias Lütgens Prof. Dr. Stefan Lochbrunner Prof. Dr. Oliver Kühn 《Chemphyschem》2015,16(12):2519-2523
Understanding both structure and dynamics is crucial for producing tailor‐made ionic liquids (ILs). We studied the vibrational and structural dynamics of medium versus weakly hydrogen‐bonded C?H groups of the imidazolium ring in ILs of the type [1‐alkyl‐3‐methylimidazolium][bis(trifluoromethanesulfonyl)imide] ([Cnmim][NTf2]), with n=1, 2, and 8, by time‐resolved coherent anti‐Stokes Raman scattering (CARS) and quantum‐classical hybrid (QCH) simulations. From the time series of the CARS spectra, dephasing times were extracted by modeling the full nonlinear response. From the QCH calculations, pure dephasing times were obtained by analyzing the distribution of transition frequencies. Experiments and calculations reveal larger dephasing rates for the vibrational stretching modes of C(2)?H compared with the more weakly hydrogen‐bonded C(4,5)?H. This finding can be understood in terms of different H‐bonding motifs and the fast interconversion between them. Differences in population relaxation rates are attributed to Fermi resonance interactions. 相似文献
996.
997.
Cover Picture: The Quest for Polysulfides in Lithium–Sulfur Battery Electrolytes: An Operando Confocal Raman Spectroscopy Study (ChemPhysChem 13/2015)
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998.
Surface‐Enhanced Raman Scattering Based on Controllable‐Layer Graphene Shells Directly Synthesized on Cu Nanoparticles for Molecular Detection
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Hengwei Qiu Dr. Yanyan Huo Zhen Li Dr. Chao Zhang Peixi Chen Prof. Shouzhen Jiang Dr. Shicai Xu Prof. Yong Ma Prof. Shuyun Wang Hongsheng Li 《Chemphyschem》2015,16(14):2953-2960
Graphene shells with a controllable number of layers were directly synthesized on Cu nanoparticles (CuNPs) by chemical vapor deposition (CVD) to fabricate a graphene‐encapsulated CuNPs (G/CuNPs) hybrid system for surface‐enhanced Raman scattering (SERS). The enhanced Raman spectra of adenosine and rhodamine 6G (R6G) showed that the G/CuNPs hybrid system can strongly suppress background fluorescence and increase signal‐to‐noise ratio. In four different types of SERS systems, the G/CuNPs hybrid system exhibits more efficient SERS than a transferred graphene/CuNPs hybrid system and pure CuNPs and graphene substrates. The minimum detectable concentrations of adenosine and R6G by the G/CuNPs hybrid system can be as low as 10?8 and 10?10 M , respectively. The excellent linear relationship between Raman intensity and analyte concentration can be used for molecular detection. The graphene shell can also effectively prevent surface oxidation of Cu nanoparticles after exposure to ambient air and thus endow the hybrid system with a long lifetime. This work provides a basis for the fabrication of novel SERS substrates. 相似文献
999.
Inside Cover: Surface‐Enhanced Raman Scattering Based on Controllable‐Layer Graphene Shells Directly Synthesized on Cu Nanoparticles for Molecular Detection (ChemPhysChem 14/2015)
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1000.
Inside Back Cover: On the Resolution Limit of Femtosecond Stimulated Raman Spectroscopy: Modelling Fifth‐Order Signals with Overlapping Pulses (ChemPhysChem 16/2015)
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