High-frequency AC electrospray ionization source for mass spectrometry of biomolecules

A novel high-frequency alternating current (AC) electrospray ionization (ESI) source has been developed for applications in mass spectrometry. The AC ESI source operates in a conical meniscus mode, analogous to the cone-jet mode of direct current (DC) electrosprays but with significant physical and mechanistic differences. In this stable conical-meniscus mode at frequencies greater than 50 kHz, the low mobility ions, which can either be cations or anions, are entrained within the liquid cone and ejected as droplets that eventually form molecular ions, thus making AC ESI a viable tool for both negative and positive mode mass spectrometry. The performance of the AC ESI source is qualitatively shown to be frequency-dependent and, for larger bio-molecules, the AC ESI source produced an ion signal intensity that is an order of magnitude higher than its DC counterpart.     

Numerical analysis of a rapid magnetic microfluidic mixer

This paper presents a detailed numerical investigation of the novel active microfluidic mixer proposed by Wen et al. (Electrophoresis 2009, 30, 4179-4186). This mixer uses an electromagnet driven by DC or AC power to induce transient interactive flows between a water-based ferrofluid and DI water. Experimental results clearly demonstrate the mixing mechanism. In the presence of the electromagnet's magnetic field, the magnetic nanoparticles create a body force vector that acts on the mixed fluid. Numerical simulations show that this magnetic body force causes the ferrofluid to expand significantly and uniformly toward miscible water. The magnetic force also produces many extremely fine finger structures along the direction of local magnetic field lines at the interface in both upstream and downstream regions of the microchannel when the external steady magnetic strength (DC power actuation) exceeds 30 Oe (critical magnetic Peclet number Pe(m),cr = 2870). This study is the first to analyze these pronounced finger patterns numerically, and the results are in good agreement with the experimental visualization of Wen et al. (Electrophoresis 2009, 30, 4179-4186). The large interfacial area that accompanies these fine finger structures and the dominant diffusion effects occurring around the circumferential regions of fingers significantly enhance the mixing performance. The mixing ratio can be as high as 95% within 2.0 s. at a distance of 3.0 mm from the mixing channel inlet when the applied peak magnetic field supplied by the DC power source exceeds 60 Oe. This study also presents a sample implementation of AC power actuation in a numerical simulation, an experimental benchmark, and a simulation of DC power actuation with the same peak magnetic strength. The simulated flow structures of the AC power actuation agree well with the experimental visualization, and are similar to those produced by DC power. The AC and DC power actuated flow fields exhibited no significant differences. This numerical study suggests approaches to maximize the performance of the proposed rapid magnetic microfluidic mixer, and confirms its exciting potential for use in lab-on-a-chip systems.     

Rapid concentration of deoxyribonucleic acid via Joule heating induced temperature gradient focusing in poly-dimethylsiloxane microfluidic channel

This paper reports rapid microfluidic electrokinetic concentration of deoxyribonucleic acid (DNA) with the Joule heating induced temperature gradient focusing (TGF) by using our proposed combined AC and DC electric field technique. A peak of 480-fold concentration enhancement of DNA sample is achieved within 40 s in a simple poly-dimethylsiloxane (PDMS) microfluidic channel of a sudden expansion in cross-section. Compared to a sole DC field, the introduction of an AC field can reduce DC field induced back-pressure and produce sufficient Joule heating effects, resulting in higher concentration enhancement. Within such microfluidic channel structure, negative charged DNA analytes can be concentrated at a location where the DNA electrophoretic motion is balanced with the bulk flow driven by DC electroosmosis under an appropriate temperature gradient field. A numerical model accounting for a combined AC and DC field and back-pressure driven flow effects is developed to describe the complex Joule heating induced TGF processes. The experimental observation of DNA concentration phenomena can be explained by the numerical model.     

Bi-directional flow induced by an AC electroosmotic micropump with DC voltage bias

This paper discusses the principle of biased alternating current electroosmosis (ACEO) and its application to move the bulk fluid in a microchannel, as an alternative to mechanical pumping methods. Previous EO-driven flow research has looked at the effect of electrode asymmetry and transverse traveling wave forms on the performance of electroosmotic pumps. This paper presents an analysis that was conducted to assess the effect of combining an AC signal with a DC (direct current) bias when generating the electric field needed to impart electroosmosis (EO) within a microchannel. The results presented here are numerical and experimental. The numerical results were generated through simulations performed using COMSOL 3.5a. Currently available theoretical models for EO flows were embedded in the software and solved numerically to evaluate the effects of channel geometry, frequency of excitation, electrode array geometry, and AC signal with a DC bias on the flow imparted on an electrically conducting fluid. Simulations of the ACEO flow driven by a constant magnitude of AC voltage over symmetric electrodes did not indicate relevant net flows. However, superimposing a DC signal over the AC signal on the same symmetric electrode array leads to a noticeable net forward flow. Moreover, changing the polarity of electrical signal creates a bi-directional flow on symmetrical electrode array. Experimental flow measurements were performed on several electrode array configurations. The mismatch between the numerical and experimental results revealed the limitations of the currently available models for the biased EO. However, they confirm that using a symmetric electrode array excited by an AC signal with a DC bias leads to a significant improvement in flow rates in comparison to the flow rates obtained in an asymmetric electrode array configuration excited just with an AC signal.     

Rapid Transformation of Hexagonal to Cubic Silicon Carbide (SiC) by Electric Discharge Assisted Mechanical Milling

Silicon carbide powder was successfully transformed from hexagonal SiC into cubic SiC using the electric discharge assisted mechanical milling (EDAMM) method. The milling process was conducted in nitrogen plasma at atmospheric pressure. The effects of pulsed alternating current (AC) and direct current (DC) discharge on product formation were investigated. Products were characterized by X-ray diffractometry, scanning electron microscopy, transmission electron microscopy and nanohardness. It was found that hexagonal SiC can be transformed into cubic SiC under EDAMM processing, near complete transformation occurring within 5 min when applying AC mode electrical pulses, and within 10 min when applying DC mode discharges.     

Electrowetting without electrolysis on self-healing dielectrics

An electrowetting system with protection against dielectric breakdown is presented. It comprises an electrolyte and a Parylene-C film deposited on an aluminum electrode. The system demonstrates virtually instantaneous self-healing (within 100 ms) after dielectric breakdown under both DC and certain AC electrowetting conditions. DC current response during electrowetting on intentionally damaged Parylene-C is presented. Also presented is a characterization of DC offset voltages and duty cycle percentages required for electrolysis free AC electrowetting between 10 Hz and 4 kHz.     

聚苯胺类电流变体的稳态剪切流动分析

对聚苯胺、及聚苯胺/聚丙烯酸盐复合粒子的稳态剪切流动行为进行了综合考察.结果表明, 在交流电场下,电流变体的剪切应力和剪切速率的关系符合Bingham流体形为.并对此现象进行了分析,提出用非理想塑性体的新模型来描述交流电场下聚苯胺类电流变体的稳态剪切流动.     

Effect of solution acidity on cytochrome c conformations of alternating current electrospray ionization mass spectrometry

This paper reports notable observations regarding the ion charge states of thermally stable cytochrome c, generated using an alternating current (AC) electrospray ionization (ESI) device. An AC ESI sprayer entrains low-mobility ions to accumulate at the meniscus cone tip prior to the ejection of detached aerosols to produce analyte ions. Therefore, as the solvent acidity varies, protein ions entrained in the AC cone tip are found to change conformation less significantly compared with those in the direct current (DC) cone. We acquired the AC ESI mass spectra of cytochrome c at pH range from 2 to 4. Unlike the DC ESI mass spectra showing clear conformation changes due to denaturing, the AC spectra indicated that only partial denaturing occurs even at extremely acidic pH 2. More native cytochrome c in lower charge states therefore remained. Moreover, with a solvent mixture of aqueous buffer and acetonitrile (70:30), partially denatured cytochrome c was still preserved at pH 2 by using AC ESI. Completely denatured proteins are observed at pH 2 by using DC ESI.     

A Comparison of Alternating Current and Direct Current Electrospray Ionization for Mass Spectrometry

A series of studies comparing the performance of alternating current electrospray ionization (AC ESI) mass spectrometry (MS) and direct current electrospray ionization (DC ESI) MS have been conducted, exploring the absolute signal intensity and signal-to-background ratios produced by both methods using caffeine and a model peptide as targets. Because the high-voltage AC signal was more susceptible to generating gas discharges, the operating voltage range of AC ESI was significantly smaller than that for DC ESI, such that the absolute signal intensities produced by DC ESI at peak voltages were one to two orders of magnitude greater than those for AC ESI. Using an electronegative nebulizing gas, sulfur hexafluoride (SF₆), instead of nitrogen (N₂) increased the operating range of AC ESI by ~50 %, but did not appreciably improve signal intensities. While DC ESI generated far greater signal intensities, both ionization methods produced comparable signal-to-background noise, with AC ESI spectra appearing qualitatively cleaner. A quantitative calibration analysis was performed for two analytes, caffeine and the peptide MRFA. AC ESI utilizing SF₆ outperforms all other techniques for the detection of MRFA, producing chromatographic limits of detection nearly one order of magnitude lower than that of DC ESI utilizing N₂, and one-half that of DC ESI utilizing SF₆. However, DC ESI outperforms AC ESI for the analysis of caffeine, indicating that improvements in spectral quality may benefit certain compounds or classes of compounds, on an individual basis.

AC conductance of transmembrane protein channels. The number of ionized residue mobile counterions at infinite dilution

Simultaneous measurements of the AC and DC conductances of alpha-hemolysin (alphaHL) ion channels and outer membrane protein F (OmpF) porins in dilute ionic solutions is described. AC conductance measurements were performed by applying a 10 mV rms AC voltage across a suspended planar bilayer of 1-palmitoyl-2-oleoyl-sn-glycero-3-phosphocholine in the absence and presence of the protein and detecting the AC current response using phase-sensitive lock-in techniques. The conductances of individual alphaHL channels and OmpF porins were measured in symmetric KCl solutions containing between 5 and 1000 mM KCl. The AC and DC conductances of each protein were in agreement for all solution conditions, demonstrating the reliability of the AC method in single-channel recordings. Linear plots of conductance versus bulk KCl concentration for both proteins extrapolate to significant nonzero conductances (0.150 +/- 0.050 nS and 0.028 +/- 0.008 nS for OmpF and alphaHL, respectively) at infinite KCl dilution. The infinite dilution conductances are ascribed to mobile counterions of the ionizable residues within the protein lumens. A method of analyzing the plots of conductance vs KCl concentration is introduced that allows the determination of the concentration of mobile counterions associated with ionizable groups without knowledge of either the protein geometry or the ion mobilities. At neutral pH, an equivalent of 3 mobile counterions (K+ or Cl-) is estimated to contribute to the conductivity of the alphaHL channel.     

Alternating current electrophoretic deposition (EPD) of TiO2 nanoparticles in aqueous suspensions

TiO(2)-nanostructured coatings from aqueous suspensions have been successfully prepared by the application of alternating current (AC) instead of direct current (DC) during electrophoretic deposition (EPD). No organic additives in suspension were required for successful EPD. The quality of the AC-EPD TiO(2) coatings in terms of homogeneity and extent of microcracking, upon drying, observed by SEM, was superior to that of DC-EPD coatings made from the same type of suspensions. The main difference between AC- and DC-EPD was the suppression of bubble formation. The absence of water electrolysis at the electrodes can be explained by the particular distribution of the electric field during AC mode, which prevents the nucleation of bubbles. The preparation of TiO(2) coatings from aqueous suspension and without the aid of organic stabilizers opens the possibility for co-deposition of sensitive materials such as biomolecules and even cells for biomedical applications, given the high biocompatibility of TiO(2). The deposition of TiO(2) coatings from aqueous suspensions is also attractive from environmental and economical points of view.     

Role of electric field on surface wetting of polystyrene surface

The role of surface charge in fluid flow in micro/nanofluidics systems as well as the role of electric field to create switchable hydrophobic surfaces is of interest. In this work, the contact angle (CA) and contact angle hysteresis (CAH) of a droplet of deionized (DI) water were measured with applied direct current (DC) and alternating current (AC) electric fields. The droplet was deposited on a polystyrene (PS) surface, commonly used in various nanotechnology applications, coated on a doped silicon (Si) wafer. With the DC field, CA decreased with an increase in voltage. Because of the presence of a silicon oxide layer and a space charge layer, the change of the CA was found to be lower than with a metal substrate. The CAH had no obvious change with a DC field. An AC field with a positive value was applied to the droplet to study its effect on CA and CAH. At low frequency (lower than 10 Hz), the droplet was visibly oscillating. The CA was found to increase when the frequency of the applied AC field increased from 1 Hz to 10 kHz. On the other hand, the CA decreased with an increasing peak-peak voltage at or lower than 10 kHz. The CAH in the AC field was found to be lower than in the DC field and had a similar trend to static CA with increasing frequency. A model is presented to explain the data.     

对称电场催化增强甲烷转化合成C_2研究(英文)

利用电场作用通过交流和直流等离子体在低温、常压和低功率下催化反应将甲烷直接转化为碳二烃（乙烷、乙烯、乙炔）。考察了在对称电场作用下催化剂的催化性能。实验结果表明,在交流电场作用下,碳二烃选择性差别不大;甲烷转化率的大小顺序为： ＭｎＯ_２／Ａｌ２Ｏ３＞Ｎｉ／Ａｌ２Ｏ３＞ＭｏＯ_３／Ａｌ２Ｏ３＞Ａｌ２Ｏ３＞Ｎｉ／Ａｌ２Ｏ３＞ＭｏＯ_３／Ａｌ２Ｏ３＞Ｎｉ／ＮａＹ＞Ｐｄ／ＺＳＭ－５＞Ｎｉ／Ｈ４Ｍｇ２Ｓｉ３Ｏ４＞Ｎｉ／ＺＳＭ－５＞Ｃｏ／ＺＳＭ－５＞无催化剂：在直流电场作用下,碳二烃选择性差别也不大（除Ｎｉ／ＮａＹ外）,甲烷转化率的大小顺序为： Ｎｉ／Ａ１２Ｏ３＞Ｎｉ／Ｈ４Ｍｇ２Ｓｉ３Ｏ４＞Ｎｉ／ＺＳＭ－５＞Ｃｏ／ＺＳＭ－５＞ＭｎＯ２／Ａ１２Ｏ３＞ＭｏＯ３／Ａ１２Ｏ３＞Ｎｉ／ＮａＹ＞无催化剂＞Ｐｄ／ＺＳＭ－５。     

Droplet-based microfluidics with nonaqueous solvents and solutions

In droplet-based ("digital") microfluidics, liquid droplets in contact with dielectric surfaces are created, moved, merged and mixed by applying AC or DC potentials across electrodes patterned beneath the dielectric. We show for the first time that it is possible to manipulate droplets of organic solvents, ionic liquids, and aqueous surfactant solutions in air by these mechanisms using only modest voltages (<100 V) and frequencies (<10 kHz). The feasibility of moving any liquid can be predicted empirically from its frequency-dependent complex permittivity, epsilon*. The threshold for droplet actuation in air with our two-plate device configuration is /epsilon*/>8x10(-11). The mechanistic implications of these results are discussed, along with the greatly expanded range of applications for digital microfluidics that these results suggest are now feasible.     

Scalable activated carbon/graphene based supercapacitors with improved capacitance retention at high current densities

Scalable, highly stable supercapacitor electrodes were developed from the mixture of a tea factory waste based activated carbon (AC) and a low-cost electrochemical exfoliated graphene (EEG). The hybrid electrodes showed notably enhanced stability at high current densities. The AC sample was prepared by chemical method and exposed to a further heat treatment to enhance electrochemical performance. Graphene used in the preparation of hybrid electrodes was obtained by direct electrochemical exfoliation of graphite in an aqueous solution. Detailed structural characterization of AC, EEG, and hybrid material was performed. The original electrochemical performances of AC and EEG were examined in button size cells using an aqueous electrolyte. The hybrid materials were prepared by mixing AC and EEG at different mass percentage ratios, and tested as supercapacitor electrodes under the same conditions. Capacitance stability of the electrodes developed from AC:EEG (70:30) at high currents increased by about 45% compared to the original AC. The highest gravimetric capacitance (110 F/g) was achieved by this hybrid electrode. The hybrid electrode was scaled up to the pouch size and tested using an organic electrolyte. The organic electrolyte was preferred for scaling up due to its wider voltage ranges. The pouch cell had a gravimetric capacitance of 85 F/g and exhibited as good performance as the coin cell in the organic electrolyte.     

气体放电对SO_2和SO_3~(2-)氧化的影响

研究气体放电对SO2和亚硫酸盐氧化的影响,采用了直流电源和交直流叠加电源进行气体放电.结果表明,气体放电对于SO2氧化促进作用很少;但对溶液中的SO2-3的氧化则有明显促进作用.通过对两个反应过程的机理分析,认为亚硫酸盐溶液氧化快是因为气体放电产生的OH等自由基和液相里的亚硫酸根起作用,引发链反应,促进了溶液中四价硫被空气中的O2氧化为六价硫的过程.而气相中的SO2与OH等自由基作用不能形成链反应,所以影响不明显.实验表明,选择交直流叠加电源进行气体放电比用纯粹直流电源放电效果更好.     

A concise study on dimedone: A versatile molecule in multi-component reactions,an outlook to the green reaction media

Dimedone is an interesting and versatile motif in most organic transformations. Its white to light yellow crystals have been utilized as substrate in wide range of organic reactions including multi-component transformations. The notability of dimedone is due to the acidic property of its methylene group which is in equilibrium with its tautomeric enol form. This phenomena permit dimedone to be utilized in several kinds of organic reactions eventuated to several organic molecules with potent pharmaceutical exclusivity. The mentioned nature of dimedone in addition with its low toxicity, easily accessibility and handling, moisture stability, and low cost make it interesting for organic chemists. During the last decades, perfuming an organic transformation based on green chemistry rules, is in demand. In this review the reactions of dimedone has been focused with an outlook to the solvent of media. Each section has been subdivided respect to the temperature of the transformations. All categorizations has been accomplished to the green media. The authors has also calculated the atom economy of each reaction on behalf of green chemistry concept.     

交流阻抗法研究铝合金表面脉冲氧化膜

本 文采用宽 频阻抗 法首次测 得了 铝合 金表 面 脉冲 氧化 膜 的 Ｂｏｄｅ 图 ．实 验表 明： 脉冲氧化膜 与直流 氧化膜的 主要差别 在于多 孔层,脉 冲氧化膜 比较 均匀, 基本 无缺 陷．通 过显 微观 察及 Ｖ Ｉ 特性 曲线等测 定手段, 进一步佐 证了交 流阻抗测 试的部分 结果．     

电弧直读光谱仪的开发与应用

介绍一种国内首创的电弧直读光谱仪。该仪器由交/直流电弧激发光源、凹面光栅分光系统、光电倍增管接收器及智能测控系统所组成。研制成功地质样品专用的"交流电弧直读光谱仪"和高纯金属专用的"直流电弧直读光谱仪"可取代1m或2m光栅摄谱仪,省去了光谱相板、洗相及译谱等繁琐的操作程序。在优化的分析条件下,可直接对粉末状地球化学样品及高纯金属氧化物中的多种微量元素同时进行直读光谱测定,具有灵敏、准确、快速的特点,各项技术指标符合所属领域的"国家标准"及"行业规范"的要求。现已有多家使用单位采用"交流电弧直读光谱仪"分析了十几万件地球化学样品中的银、锡和硼等元素,取得了良好的应用效果。     

Dielectrophoretic focusing of particles in a microchannel constriction using DC‐biased AC flectric fields

This paper presents a fundamental study of particle electrokinetic focusing in a single microchannel constriction. Through both experiments and simulations, we demonstrate that such dielectrophoresis‐induced particle focusing can be implemented in a much smaller magnitude of DC‐biased AC electric fields (10 kV/m in total) as compared to pure DC electric fields (up to 100 kV/m). This is attributed to the increase in the ratio of cross‐stream particle dielectrophoretic velocity to streamwise electrokinetic velocity as only the DC field component contributes to the latter. The effects of the 1 kHz frequency AC to DC electric field ratio on particle trajectories and velocity variations through the microchannel constriction are also examined, which are found to agree with the simulation results.