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1.
Molecular Structure and Dynamics of Water at the Water–Air Interface Studied with Surface‐Specific Vibrational Spectroscopy 下载免费PDF全文
Mischa Bonn Yuki Nagata Ellen H. G. Backus 《Angewandte Chemie (International ed. in English)》2015,54(19):5560-5576
Water interfaces provide the platform for many important biological, chemical, and physical processes. The water–air interface is the most common and simple aqueous interface and serves as a model system for water at a hydrophobic surface. Unveiling the microscopic (<1 nm) structure and dynamics of interfacial water at the water–vapor interface is essential for understanding the processes occurring on the water surface. At the water interface the network of very strong intermolecular interactions, hydrogen‐bonds, is interrupted and the density of water is reduced. A central question regarding water at interfaces is the extent to which the structure and dynamics of water molecules are influenced by the interruption of the hydrogen‐bonded network and thus differ from those of bulk water. Herein, we discuss recent advances in the study of interfacial water at the water–air interface using laser‐based surface‐specific vibrational spectroscopy. 相似文献
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Majid JAFARIAN Mehdi RASHVAND AVEI Iman DANAEE Fereydoon GOBAL Mohammad G.MAHJANI 《催化学报》2010,31(11):1351-1357
A stable copper (hydr)oxide-modified electrode was prepared in 0.5 mol/L NaOH solution by cyclic voltammetry in the range of -250 to 1 000 mV. It can be used for electrochemical studies in the range of -250 to 1 000 mV without interfering peaks because there is no oxidation of copper. During an anodic potential sweep, the electro-oxidation of saccharose on Cu occurred by the formation of CuIII and this reaction also occurred in the early stages of the reversed cycle until it is stopped by the negative potentials. A mechanism based on the electro-chemical generation of CuIII active sites and their subsequent consumption by saccharose was proposed, and the rate law and kinetic parameters were obtained. The charge transfer resistance from theoretical and impedance studies was used to verify the mechanism. Under chronoamperometry regimes, the reaction followed Cottrellian behavior. The transfer of up to 21 electrons was observed in further investigations of the electro-oxidation of saccharose on a (hydr)oxide Cu rotating disk electrode. 相似文献
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Dr. Kumudu Mudiyanselage Dr. Sanjaya D. Senanayake Dr. Leticia Feria Dr. Shankhamala Kundu Dr. Ashleigh E. Baber Dr. Jesús Graciani Dr. Alba B. Vidal Dr. Stefano Agnoli Prof. Jaime Evans Dr. Rui Chang Dr. Stephanus Axnanda Dr. Zhi Liu Prof. Javier F. Sanz Dr. Ping Liu Dr. José A. Rodriguez Dr. Darío J. Stacchiola 《Angewandte Chemie (International ed. in English)》2013,52(19):5101-5105
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采用熔融共混法制备了玻璃纤维增强聚对苯二甲酸乙二酯(PET-GF)/十溴二苯醚(DBDPO)/苯基膦酸铈(CeHPP)复合材料, 通过锥型量热仪(Cone)对复合材料的燃烧行为进行综合分析, 采用热失重-红外联用(TG-FTIR)分析了复合材料热降解过程中气体的释放量和主要成分, 并使用扫描电子显微镜(SEM)、 能量色散X射线光谱仪(EDX)和X射线光电子能谱(XPS)对复合材料燃烧后的残炭形貌、 残炭所含元素及含量等进行表征. 实验结果表明, 当CeHPP与DBDPO两者复配使用时, PET-GF/DBDPO/CeHPP复合材料的热解过程受到抑制, 凝聚相的燃烧减缓, 材料总的热分解量降低, 烟气释放量明显减小. 这主要是由于CeHPP在燃烧过程中形成了连续致密的残炭, 分布于基材和玻璃纤维表面, 将部分DBDPO及其分解产物滞留于凝聚相, 从而实现了气相-凝聚相双重阻燃作用, 有效阻隔了挥发性气体产物的释放. 相似文献
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Kasinath Ojha Nakkiran Arulmozhi Diana Aranzales Marc T. M. Koper 《Angewandte Chemie (International ed. in English)》2020,59(2):711-715
We report, for the first time, the observation of a Gouy–Chapman capacitance minimum at the potential of zero charge of the Pt(111)‐aqueous perchlorate electrolyte interface. The potential of zero charge of 0.3 V vs. NHE agrees very well with earlier values obtained by different methods. The observation of the potential of zero charge of this interface requires a specific pH (pH 4) and anomalously low electrolyte concentrations (<10?3 m ). By comparison to gold and mercury double‐layer data, we conclude that the diffuse double layer structure at the Pt(111)‐electrolyte interface deviates significantly from the Gouy–Chapman theory in the sense that the electrostatic screening is much better than predicted by purely electrostatic mean‐field Poisson–Boltzmann theory. 相似文献
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研究了在低温、近中性条件下,在微量Fe(II)离子存在下Ferrihydrite(又称为水合氧化铁hydrousironoxide)的相转化过程.结果表明,微量Fe(II)离子的存在不仅可以加速Ferrihydrite的相转化过程,而且其相转化产物的组成也与没有Fe(II)离子存在时产物的组成有所不同,即除了α-FeOOH和α-Fe2O3外,还形成了γ-FeOOH;相转化过程既与阴离子的种类、反应温度、反应时间等因素有关,也与Fe(II)离子存在状态有关;Fe(II)离子通过催化Ferrihydrite的溶解过程,从而加速整个相转化过程.对该过程的深入研究将对认识和了解自然条件下铁氧化物的形成与相互转化具有重要意义. 相似文献
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Luminescentmaterialshavinglongdecayperi0dhaveat-IIactedmuchinterestduetotheirpotentialwidespreadaPplicati0ns.Recently,alongdecayluminescentp0wderhavingthecomPositionofSrAl2O4activatedwithEu' wasreportedandregardedasthebestcandidateforpracticalaPPlicationbecauseofitsuniqueadVantages0veritsprecursors.l'2Inthispaper,wereportthesynthesisofthelongdecayluminescentpowderandtheinnuence0fthemolarratioofAlt0sr0ntheethessioncolor.Toproducethelundnescentp0wder,amixtureofSrCO3,Al2O3,Eu2O3andsomesol… 相似文献
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Femtosecond Hydrogen Bond Dynamics of Bulk‐like and Bound Water at Positively and Negatively Charged Lipid Interfaces Revealed by 2D HD‐VSFG Spectroscopy 下载免费PDF全文
Dr. Prashant Chandra Singh Dr. Ken‐ichi Inoue Dr. Satoshi Nihonyanagi Prof. Dr. Shoichi Yamaguchi Prof.Dr. Tahei Tahara 《Angewandte Chemie (International ed. in English)》2016,55(36):10621-10625
Interfacial water in the vicinity of lipids plays an important role in many biological processes, such as drug delivery, ion transportation, and lipid fusion. Hence, molecular‐level elucidation of the properties of water at lipid interfaces is of the utmost importance. We report the two‐dimensional heterodyne‐detected vibrational sum frequency generation (2D HD‐VSFG) study of the OH stretch of HOD at charged lipid interfaces, which shows that the hydrogen bond dynamics of interfacial water differ drastically, depending on the lipids. The data indicate that the spectral diffusion of the OH stretch at a positively charged lipid interface is dominated by the ultrafast (<~100 fs) component, followed by the minor sub‐picosecond slow dynamics, while the dynamics at a negatively charged lipid interface exhibit sub‐picosecond dynamics almost exclusively, implying that fast hydrogen bond fluctuation is prohibited. These results reveal that the ultrafast hydrogen bond dynamics at the positively charged lipid–water interface are attributable to the bulk‐like property of interfacial water, whereas the slow dynamics at the negatively charged lipid interface are due to bound water, which is hydrogen‐bonded to the hydrophilic head group. 相似文献
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测量了钌镧氧化物涂层的电化学阻抗谱(EIS), 结合循环伏安(CV)及扫描电子显微镜形貌分析, 研究了钌镧氧化物涂层阳极在3.5% NaCl 溶液中电化学表面结构及电化学行为. 在非析氯反应区间, 该涂层EIS 数据的最佳拟合等效电路是Rs(RctQdl), 在析氯反应区间, 其等效电路为Rs(RfQf)(RctWQdl). 高频段阻抗行为对应涂层的物理阻抗, 低频段对应涂层与溶液界面的电化学反应阻抗. 实验结果表明, 随着La 浓度增加, 氧化膜及双电层的伪电容增大, 且在La 含量30mol%时达到最大值, 与CV实验结果一致, 证明了加入La 能提高RuO2涂层的电催化活性. 但在析氯反应区间, 涂层氧化膜的导电性在含La 大于30 mol%之后迅速下降, 在低频段产生Warburg 阻抗, 与其表面钝化和特性吸附现象有关,这是导致含La 70 mol%时电催化活性急剧下降的原因. 相似文献
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J. -J. Point 《Journal of inclusion phenomena and macrocyclic chemistry》1988,6(3):253-262
The far infrared spectra of various poly(ethylene oxide)-para-disubstituted benzene intercalates are reported. From a detailed discussion, it is strongly suggested that the formula of these intercalates is either [(p-C6H4XY)3(CH2CH2O–)10]
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(for XY=ClCl, BrBr, BrCl, ICl, ClF and CH3Br) or [(p-C6H4XY)2(CH2CH2O)7]
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(for XY=BrF and IF). In both cases the conformation of the polymer molecule is nearly TTG. In addition the previously described relative disposition of the host and guest molecules is confirmed. 相似文献
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Iron–Carbonyl Aqueous Vesicles (MCsomes) by Hydration of [Fe(CO){CO(CH2)5CH3}(Cp)(PPh3)] (FpC6): Highly Integrated Colloids with Aggregation‐Induced Self‐Enhanced IR Absorption (AI‐SEIRA) 下载免费PDF全文
Nimer Murshid Prof. Xiaosong Wang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(52):19223-19230
Self‐assembly of hydrophobic molecules into aqueous colloids contradicts common chemical intuition, but has been achieved through hydration of [Fe(CO){CO(CH2)5CH3}(Cp)(PPh3)] (FpC6). FpC6 has no surface activity, no NMR signals in D2O and no critical aggregation concentration (CAC) in H2O. The molecule, however, contains both acyl and terminal CO groups that are prone to being hydrated. By adding water to a solution in THF, self‐assembly of FpC6 can be initiated through water–carbonyl interactions (WCIs) with the highly polarized acyl CO groups. This aggregation subsequently enhances the hydration of the acyl CO groups and also induces the WCI of otherwise unhydrated terminal CO groups. The resultant metal–carbonyl aggregates have been proved to be bilayer vesicles with iron complexes exposed towards water and alkyl chains forming inner walls (MCsomes). These MCsomes show high structure integration upon dilution due to the hydrophobic nature of the building blocks. The highly polarized CO groups on the surface of the MCsomes result in a negative zeta potential (?65 mV) and create a local electric field, which significantly enhances the IR absorption of CO groups by more than 100‐fold. This is the first discovery of aggregation‐induced self‐enhanced IR absorption (AI‐SRIRA) without the assistant of external dielectric substrates. Highly integrated MCsomes are, therefore, promising as a novel group of materials, for example, for IR‐based sensing and imaging. 相似文献
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Nanosized surface-enhanced Raman scattering (SERS) substrates fabricated by the controlled growth of metal nanostructures on water-dispersed two-dimensional nanomaterials can open a new avenue for SERS analysis of liquid samples in biological fields. In this work, regular and uniform Ag nanostructures were grown on the surface of graphene oxide (GO) through a microwave-assisted hydrothermal method. Polyamidoamine (PAMAM) dendrimers were assembled on the surface of GO to form GO/PAMAM templates for growing Ag nanostructures, which are primarily comprised of Ag dimers and trimers. The prepared Ag/GO nanocomposites are highly dispersed and stable in aqueous solution and may be used as substrates for enhanced Raman detection of rhodamine 6?G (R6G) in aqueous solution. This special substrate provides high-performance SERS and suppresses R6G fluorescence in aqueous solution and is promising as a nanosized material for the enhanced Raman detection of liquid samples in biological diagnostics. 相似文献
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《Angewandte Chemie (International ed. in English)》2017,56(50):15846-15851
The surface tension of the air—water interface increases upon addition of inorganic salts, implying a negative surface excess of ionic species. Most acids, however, induce a decrease in surface tension, indicating a positive surface excess of hydrated protons. In combination with the apparent negative charge at pure air–water interfaces derived from electrokinetic experiments, this experimental observation has been a source of intense debate since the mid‐19th century. Herein, we calculate surface tensions and ionic surface propensities at air–water interfaces from classical, thermodynamically consistent molecular dynamics simulations. The surface tensions of NaOH, HCl, and NaCl solutions show outstanding quantitative agreement with experiment. Of the studied ions, only H3O+ adsorbs to the air–water interface. The adsorption is explained by the deep potential well caused by the orientation of the H3O+ dipole in the interfacial electric field, which is confirmed by ab initio simulations. 相似文献
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Charge Polarization at a Au–TiC Interface and the Generation of Highly Active and Selective Catalysts for the Low‐Temperature Water–Gas Shift Reaction 下载免费PDF全文
Dr. José A. Rodriguez Dr. Pedro J. Ramírez Gian Giacomo Asara Dr. Francesc Viñes Prof. Jaime Evans Dr. Ping Liu Prof. Josep M. Ricart Prof. Francesc Illas 《Angewandte Chemie (International ed. in English)》2014,53(42):11270-11274
Au atoms in contact with TiC(001) undergo significant charge polarization. Strong metal–support interactions make Au/TiC(001) an excellent catalyst for the low‐temperature water–gas shift (WGS), with turnover frequencies orders of magnitude larger than those observed for conventional metal/oxide catalysts. DFT calculations indicate that the WGS reaction follows an associative mechanism with HOCO as a key intermediate. 相似文献
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A platinum-lined, flowing autoclave facility was used to investigate the solubility behavior of cobalt(II) oxide (CoO) in deoxygenated ammonium and sodium hydroxide solutions between 22 and 288°C. Co(II) ion activity in aqueous solution was controlled by a hydrous Co(II) oxide when nitrogen was used for deoxygenation and by metallic cobalt when hydrogen was used. Measured cobalt solubilities are interpreted using a Co(II) ion hydroxo- and amminocomplexing model and thermodynamic functions for these equilibria were obtained from a least-squares analysis of the data. A common set of thermodynamic properties for the species Co(OH)+, Co(OH)2(aq) and Co(OH)(NH3)+ is provided to permit accurate cobalt oxide solubility calculations over broad ranges of temperature and alkalinity. 相似文献
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Kuz'mina R. I. Ivanova Yu. V. Sevost'yanov V. P. 《Theoretical and Experimental Chemistry》2003,39(4):259-262
We have studied the reaction of NO and CO on aluminum/nickel/copper catalysts obtained under short high-voltage discharge conditions. We have established that electrohydraulic shock affects formation of heterogeneous catalytic systems and increases the activity of catalysts during simultaneous removal of nitrogen and carbon oxides from gaseous exhausts. 相似文献
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Wen‐Chao Geng Dongmei Zhang Chu Gong Zhihao Li Kevin M. Barraza Jesse L. Beauchamp Dong‐Sheng Guo Xinxing Zhang 《Angewandte Chemie (International ed. in English)》2020,59(31):12684-12688
The oxidation of antioxidants by oxidizers imposes great challenges to both living organisms and the food industry. Here we show that the host–guest complexation of the carefully designed, positively charged, amphiphilic guanidinocalix[5]arene pentadodecyl ether (GC5A‐12C) and negatively charged oleic acid (OA), a well‐known cell membrane antioxidant, prevents the oxidation of the complex monolayers at the air–water interface from two potent oxidizers hydroxyl radicals (OH) and singlet delta oxygen (SDO). OH is generated from the gas phase and attacks from the top of the monolayer, while SDO is generated inside the monolayer and attacks amphiphiles from a lateral direction. Field‐induced droplet ionization mass spectrometry results have demonstrated that the host–guest complexation achieves steric shielding and prevents both types of oxidation as a result of the tight and “sleeved in” physical arrangement, rather than the chemical reactivity, of the complexes. 相似文献