Physical Chemistry Commons^™

Development Of An Electrochemical Immunosensor For Direct Detection Of Acrylamide In Food Samples, Pei Ying Lau

Student Works (2020-2029)

Acrylamide, a potential carcinogen which is mainly found in plant-based food such as potato chips, French fries, bread, biscuit, coffee and coco, after undergoing heating process at temperature above 120°C. The permissible maximum intake of acrylamide is 2.6 μg kg−1 of body weight per day to prevent cancer risk. Due to its neurotoxicity and carcinogenicity, a rapid detection method for acrylamide is strongly needed in food safety concern. Herein, a sample pre-treatment free electrochemical immunosensor was developed based on a displacement assay. In a displacement assay format, an antibody is initially bound to the surface immobilized hapten (analyte analogue) and …

In Situ Monitoring Of Catalytic Molecular Transformations On Noble Metal Nanocatalysts Using Surface-Enhanced Raman Spectroscopy, Hui Wang, Qingfeng Zhang, Esteban Villarreal, Hao Jing, Kexun Chen

Journal of the South Carolina Academy of Science

Noble metal nanoparticles have long been of tremendous interest in the nanophotonics and nanocatalysis communities owing to their intriguing size- and shape-dependent plasmonic and catalytic properties. The combination of tunable plasmon resonances with superior catalytic activities on the same noble metal nanoparticle, however, has long been challenging because the research on nanoplasmonics and nanocatalysis deals with nanoparticles in two drastically different size regimes. While tunable plasmon resonances are a unique feature of metallic nanoparticles in the sub-wavelength size regime, heterogeneous catalysis requires the use of substrate-supported sub-5 nm nanoparticulate catalysts. In this mini-review article, we share with the readers several …

A Possible Unaccounted Source Of Atmospheric Sulfate Formation: Amine-Promoted Hydrolysis And Non-Radical Oxidation Of Sulfur Dioxide, Shixian Wang, Xiao Cheng Zeng, Hui Li, Joseph S. Francisco

Xiao Cheng Zeng Publications

Numerous field and laboratory studies have shown that amines, especially dimethylamine (DMA), are crucial to atmospheric particulate nucleation. However, the molecular mechanism by which amines lead to atmospheric particulate formation is still not fully understood. Herein, we show that DMA molecules can also promote the conversion of atmospheric SO₂ to sulfate. Based on ab initio simulations, we find that in the presence of DMA, the originally endothermic and kinetically unfavourable hydrolysis reaction between gaseous SO₂ and water vapour can become both exothermic and kinetically favourable. The resulting product, bisulfite NH₂(CH₃)₂⁺ ∙ HSO …

Nanoscale Colocalization Of Fluorogenic Probes Reveals The Role Of Oxygen Vacancies In The Photocatalytic Activity Of Tungsten Oxide Nanowires, Meikun Shen, Tianben Ding, Steven T. Hartman, Fudong Wang, Christina Krucylak, Zheyu Wang, Che Tan, Bo Yin, Rohan Mishra, Matthew D. Lew, Bryce Sadtler

Electrical & Systems Engineering Publications and Presentations

Defect engineering is a strategy that has been widely used to design active semiconductor photocatalysts. However, understanding the role of defects, such as oxygen vacancies, in controlling photocatalytic activity remains a challenge. Here, we report the use of chemically triggered fluorogenic probes to study the spatial distribution of active regions in individual tungsten oxide nanowires using super-resolution fluorescence microscopy. The nanowires show significant heterogeneity along their lengths for the photocatalytic generation of hydroxyl radicals. Through quantitative, coordinate-based colocalization of multiple probe molecules activated by the same nanowires, we demonstrate that the nanoscale regions most active for the photocatalytic generation of …

Ni-Au Anodic Nano-Electrocatalyst For Direct Glucose Fuel Cells, Islam M. Al-Akraa, Aya S. Abdulhalim Eng, Yassr M. Asal Mr, Ahmad M. Mohammad Prof

Chemical Engineering

This study aims at the sequential assembling of a nickel oxide (NiOx: cauliflower-like nanostructure, 90 nm) and gold (Au; spherical, 95 nm in an average particle size) onto the GC surface nanocatalyst on a glassy carbon (GC) electrode (will be abbreviated as Ni-Au/GC) for the glucose electro−oxidation (GO); the principal anodic reaction in the direct glucose fuel cells (DGFCs). The charge of the Ni deposition on the GC surface (will be abbreviated as Ni/GC electrode) was initially optimized to obtain the highest catalytic activity toward GO which attained at (339.8 Ag−1) by applying 15 mC in the Ni deposition. Yet, …

Tuning The Activity And Stability Of Platinum Nanoparticles Toward The Catalysis Of The Formic Acid Electrooxidation, Islam M. Al-Akraa, Bilquis A. Al-Qodami, Santosh Sridhar Mysore Dr, R. Viswanatha Dr, Abdul Kareem Thottoli, Ahmad M. Mohammad

Chemical Engineering

No abstract provided.

Development Of Supported Pd-Based Catalysts For Carbon-Carbon Cross-Coupling And Oxidation Reactions, Mrinmoy Das

Theses and Dissertations

Heterogeneous catalysts are a crucial part of chemistry used for various chemical synthesis stages, pharmaceutical, and environmental applications. The use of nanoparticles or rather nanocatalysts enhances the heterogeneous catalytic applications. Both chemical and physical methods can be used to synthesize nanocatalysts. Chemical synthesis methods require comparatively fewer instruments and can easily synthesize a large amount of nanocatalysts. Nevertheless, chemical synthesis methods require reducing agents and solvents that can be toxic or harmful materials. They often need harsh reaction conditions as well, like high temperature and pressure. On the other hand, physical synthesis methods often require complex instrument setup, but their …

Enhanced Glucose Electrooxidation At Ni-Cu Binary Oxide Nanocatalyst, Islam M. Al-Akraa, Mahmoud M. Abouzaid Eng, Yaser M. Asal Mr, Ahmad M. Mohammad Prof

Chemical Engineering

The aim of this study is to fabricate a nickel (NiOx) and copper (CuOx) oxide nanocatalyst on a glassy carbon (GC) electrode (will be abbreviated as Ni-Cu/GC) for glucose oxidation (GO). A sequential electrodepositon mode was applied to assemble NiOx and CuOx in the fabrication scheme. The optimization of Ni loading on the GC surface (will be abbreviated as Ni/GC electrode) was achieved first to attain the maximum catalytic efficiency in terms of the specific current toward GO. This (409 Ag1)was obtained by applying 15 mC/cm2 in the deposition of Ni. However, unfortunately the NiOx/GC could not support a long-term …

Correlating The Physicochemical Properties Of Magnesium Stearate With Tablet Dissolution And Lubrication, Julie L. Calahan

Theses and Dissertations--Pharmacy

Magnesium stearate (MgSt) is the most commonly used pharmaceutical excipient and is present in over half the tablet formulations on the market. In spite of its popularity as an effective lubricant, it has been repeatedly recognized that there is significant variability between MgSt samples, which can cause inconsistent lubrication between batches of MgSt. The hypothesis of this research is that the batch-to-batch variability in tablet lubrication and dissolution observed in tablet formulations containing different MgSt samples can be correlated with differences in MgSt physicochemical properties (fatty acid salt composition, crystal hydrate form, particle size and surface area). Developing correlations between …

Carbon Oxidation At The Atomic Level: A Computational Study On Oxidative Graphene Etching And Pitting Of Graphitic Carbon Surfaces, Simon Schmitt

Theses and Dissertations--Mechanical and Aerospace Engineering

In order to understand the oxidation of solid carbon materials by oxygen-containing gases, carbon oxidation has to be studied on the atomic level where the surface reactions occur. Graphene and graphite are etched by oxygen to form characteristic pits that are scattered across the material surface, and pitting in turn leads to microstructural changes that determine the macroscopic oxidation behavior. While this is a well-documented phenomenon, it is heretofore poorly understood due to the notorious difficulty of experiments and a lack of comprehensive computational studies. The main objective of the present work is the development of a computational framework from …

Effect Of The Electrodeposition Potential Of Platinum On The Catalytic Activity Of A Pt/Gc Catalyst Toward Formic Acid Electro−Oxidation, Islam M. Al-Akraa, Bilquis A. Al-Qodami Ms., Ahmad M. Mohammad Prof

Chemical Engineering

The electrocatalytic activity of platinum (Pt)–modified glassy carbon (GC) (referred as Pt/GC) electrodes toward the formic acid electro−oxidation (FAO) was investigated. The Pt deposition on the GC substrate was carried out by a potentiostatic technique at different potentials (from 0.2 V to −0.2 V vs. Hg/Hg2Cl2/KCl (sat.) reference electrode) and the corresponding influence on the catalytic activity toward FAO was monitored. The electrocatalytic inspection revealed a potential role for the Pt deposition potential in boosting the catalytic efficiency of the catalyst toward FAO and further in mitigating the CO poisoning that eventually deactivate the catalyst. Interestingly, the highest activity toward …

A Spin-Coated Tiox/Pt Nanolayered Anodic Catalyst For The Direct Formic Acid Fuel Cells, Islam M. Al-Akraa, Ahmad M. Mohammad Prof

Chemical Engineering

The CO poisoning of the platinum anodic catalyst which typically functions the catalytic deterioration of the direct formic acid fuel cells could be minimized with a simple modification for Pt with titanium oxide. The fabrication scheme involved the spin-coating of a Ti precursor onto a Pt thin layer that was physically sputtered onto a Si substrate. The whole assembly was subjected to a post-annealing processing to produce the TiOx layer (60 nm) in a porous structure (mostly Anatase) atop of the Pt surface. The porous nature of the TiOx layer permitted the participation of Pt in the electrocatalysis of the …

Resolving The Puzzle Of Single-Atom Silver Dispersion On Nanosized Γ-Al2O3 Surface For High Catalytic Performance, Fei Wang, Jinzhu Ma, Shaohui Xin, Qiang Wang, Jun Xu, Changbin Zhang, Hong He, Xiao Cheng Zeng

Xiao Cheng Zeng Publications

Ag/γ-Al₂O₃ is widely used for catalyzing various reactions, and its performance depends on the valence state, morphology and dispersion of Ag species. However, detailed anchoring mechanism of Ag species on γ-Al₂O₃ remains largely unknown. Herein, we reveal that the terminal hydroxyls on γ-Al₂O₃ are responsible for anchoring Ag species. The abundant terminal hydroxyls existed on nanosized γ-Al₂O₃ can lead to single-atom silver dispersion, thereby resulting in markedly enhanced performance than the Ag cluster on microsized γ-Al₂O₃. Density-functional-theory calculations confirm that Ag atom is mainly …

Laser Ablation In Liquid For The Controlled Production Of Photoluminescent Graphene Quantum Dots And Upconverting Nanoparticles, Rosemary Lynn Calabro

Theses and Dissertations--Chemistry

Photoluminescent­ (PL) nanomaterials play an important role in areas including displays, sensing, solar, photocatalysis, and bio applications. Traditional methods to prepare PL materials suffer many drawbacks such as harsh chemical precursors, complicated synthetic steps, and production of many byproducts. Laser ablation in liquid (LAL) has emerged as a promising alternative to prepare materials that is single-step, fast, uses fewer precursors, produces fewer side products, and has simple purification steps. During LAL, a solid target is irradiated with a pulsed laser source. The laser pulses cause plasma plumes of the target material to form which are cooled, condensed, and can react …

Effects Of Hole Transporting Layers And Surface Ligands On Interface Energetics And Photovoltaic Performance Of Methylammonium Lead Iodide Perovskites, So Min Park

Theses and Dissertations--Chemical and Materials Engineering

Organic metal halide perovskites are promising materials for various optoelectronic device applications such as light emitting diodes (LED) and photovoltaic (PV) cells. Perovskite solar cells (PSCs) have shown dramatic increases in power conversion efficiency over the previous ten years, far exceeding the rate of improvement of all other PV technologies. PSCs have attracted significant attention due to their strong absorbance throughout the visible region, high charge carrier mobilities, color tunability, and ability to make ultralight weight devices. However, organic metal halide perovskites still face several challenges. For example, their environmental stability issue must be overcome to enable widespread commercialization. Meeting …

Towards The Rational Design Of Organic Semiconductors Through Computational Approaches, Qianxiang Ai

Theses and Dissertations--Chemistry

Though organic semiconductors have illustrated potential as industry-relevant materials for electronics applications, there are few guidelines that can take one from molecular design to functional materials. This limitation is, in part, due to incomplete understanding as to how the atomic-scale construction of the π-conjugated molecules that comprise the organic semiconductors determines the nature and strength of both the noncovalent intramolecular interactions that govern molecular conformation and noncovalent intermolecular interactions that regulate the energetic preference for solid-state packing. Hence, there remain several fundamental questions that need to be resolved in order to design organic semiconductors from a priori knowledge, including: What …

Designing Metal-Halide Perovskites With Enhanced Optical Properties And Stability Using Surface Ligands, Md Aslam Uddin

Theses and Dissertations--Chemistry

Metal-halide perovskites (MHPs), with formula ABX₃ (A = methylammonium, formamidinium, or Cs⁺; B = Sn²⁺ or Pb²⁺; and X = Cl^-, Br^-, or I^-) are versatile and attractive materials because of their tunable optical and electronic properties. These optical and electronic properties include tunable direct band gaps, high absorption coefficients, low exciton binding energies, relatively high electron and hole mobilities, narrow emission line-widths, and high photoluminescence (PL) quantum yields (Φ_PL). Much of the initial excitement around organic metal-halide perovskites focused on their application in photovoltaics (PVs) …

Structure, Morphology And Composition-Property Elucidation Of Ni–Mo And Ni−Mo−P Nanocrystals For Water Splitting Reactions And Group Iv Alloy And Silicate Nanocrystals For Visible To Near Ir Optoelectronics, Ebtesam Hassan Abuelenein Eladgham

Theses and Dissertations

Abstract

Structure, Morphology and Composition-Property Elucidation of Ni–Mo and Ni−Mo−P Nanocrystals for Water Splitting Reactions and Group IV Alloy and Silicate Nanocrystals for Visible to Near IR Optoelectronics

by

Ebtesam Hassan Abuelenein Eladgham

A dissertation submitted in partial fulfillment of the requirements for the degree of Doctor of Philosophy at Virginia Commonwealth University.

Advisor: Indika U Arachchige

Associate Professor, Department of Chemistry

Nanomaterials have gained a great attention because of their unique physical properties with size intermediate between molecular materials and extended solids. They have a large surface to volume ratio and display size tunable physical properties that was not …

Metal-Oxide Nanostructures Fabricated From Reactive Laser Ablation In Liquid, Mallory G. John

Theses and Dissertations

The development of metal-oxide nanostructures is a growing area due to their applications in diverse fields spanning energy conversion and storage, chemical manufacturing, and en- vironmental technology. This interest in catalytically active nanomaterials has prompted the synthesis and investigation of highly functionalized nanoparticles (NPs), including core- shell, silicate-stabilized, and bi- and multi-metallic nanocomposites. While wet-chemical synthesis methods of metal-oxide nanostructures have led to several morphologies, compositions, and shapes, these syntheses often require high temperatures, toxic solvents or reducing agents, and long reaction times.

Laser synthesis and processing of colloids (LSPC) encompasses both ‘top down’ and ‘bottom up’ approaches to synthesize …

Morphology Controlled Preparations And Electrochemical Properties Of Znco2O4 Electrode Materials For Supercapacitors, Yue-Shen Zhou, Meng Li, Shuang Wu, Zhao-Lei Li, Yan-Min Gao

Journal of Electrochemistry

In this work, hydrothermal reaction and high temperature were used to grow ZnCo₂O₄ active materials on Ni foam. The crystal stuctures and surface morphlogies of four samples were investigated by X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM) and transmission electron microscopy (TEM). The electrochemical performances were characterized by cyclic voltammetry (CV), galvanostatic charge/discharge (GCD) testing and electrochemical impedance spectroscopy (EIS) on an electrochemical station. It can be seen that active materials tended to form denser stuctures with an increasing amount of NH₄F in the solution system and four different morphologies of ZnCo_{2 …}

Electrochemical Determination Of Trace Copper Ions In Drinking Water Source, Jing-Ji Peng, Hong Zheng, Yi-Song Zou, Guo-Kun Liu, Dong-Xing Yuan

Journal of Electrochemistry

Aiming at the on-site and quick safety evaluation of the dissolved trace copper ions (Cu²⁺) in drinking water source, an electrochemical detection platform was developed on the basis of the square wave anodic stripping voltammetry using the gold nanoparticles (Au NPs) modified glassy carbon electrode, where Au NPs were deposited via electrochemical cyclic voltammetry. The proposed method displayed the limit of detection as low as 1.3 μg·L^-1 in the linear range of 2 ~ 50 μg·L^-1. The proposed method was applied to the determination of Cu²⁺ in the midstream of Minjiang River, one of …

Electrochemical Behaviors Of Azopurine On Gold Electrodes, Ming-Xue Li, Hang Shi, Jia Liu, Meng Zhang, Jian-Zhang Zhou, De-Yin Wu, Zhong-Qun Tian

Journal of Electrochemistry

In this paper, we studied the electrochemical behaviors of azopurine on polished gold electrodes with cyclic voltammetry (CV). On the basis of analyzing scan rate and peak current, it was supposed that the redox process belonged to a reversible process controlled by adsorption in 0.2 mol·L^-1 PBS (pH = 4.0 ~ 10.0) solutions. The potentials of redox peaks moved more negatively with increasing pH value. This proved that the H⁺ proton has participcted in the electrochemical reaction. The further data analysis and the calculation of surface adsorption excess demonstrated that the reaction was a two-proton and two-electron process. …

Electrochemical Cycling Stability Of Polyaniline Films In Different Color Ranges, Kun Xu, Kai-Ling Zhou, Hao Wang, Jing-Bing Liu, Hui Yan

Journal of Electrochemistry

The electrochromic behaviors of polyaniline films were investigated by potential step and cyclic voltammetry coupled with UV viscosity photometer. The polyaniline films show colorful changes from pale yellow to green and then to blue. Electrochromic stability, electrochemical behavior, coloring performance, optical properties and surface formations of the produced films were studied in detail. The working electrode was the flexible PANI electrode, and the counter electrode and the reference electrode were a platinum sheet and Ag/AgCl, respectively. The in situ optical transmittance of the PANI film at 650 nm was measured using an ultraviolet-visible-near-infrared spectrophotometer (Shimadzu UV-3101PC) combining with a square …

Polyaniline Coated Hollow Sulfur Prepared Using Sublimate 2,4,6-Tri(Propan-2-Yl)-1,3,5-Trioxane As Template For Sulfur Electrode, Zhang-Feng Li, Xiao-Rui Wang, Wen-Sheng Tian, Jin-Ze Yang, Ping Zhang, Li-Ping Ma, Yang Chen, Xiao-Li Cui, Zhi-Yu Jiang

Journal of Electrochemistry

An advance method for preparing polyaniline-coated hollow sulfur material using sublimate material ADD(2,4,6-tri(propan-2-yl)-1,3,5-trioxane) as a template was developed for lithium-sulfur battery. At first, the smashed ADD particles were coated by a sulfur layer through the reaction of Na₂S₂O₃ with diluted HCl. Then polyaniline layer was coated again on the surface of sulfur layer through the reaction of aniline with (NH₄)₂S₂O₈. After being dried at 60 ^oC for 12 h, the ADD in such a composite evaporated totally, and resulted in the formation of polyaniline-coated hollow sulfur …

Study On Electro-Sorption Of Heavy Metals And Sulfamethoxazole On Activated Carbon Fibers, Wen-Jun Zhao, Bing-Xin Jia, Ya-Nan Zhang, Jiu-Nian Guan, Jiao Qu, Ying Lu

Journal of Electrochemistry

To study the optimal removal condition, adsorption mechanism and comparative analysis of the three typical cationic pollutants, i.e., Zn(II), anionic pollutant Cr(VI) and molecular pollutant sulfamethoxazole (SMX), using self-made upflowed electro-sorption device for adsorptions of above three pollutants by modified activated carbon fiber were researched. The activated carbon fiber (ACF) was modified by hydrochloric acid. The ACF morphology and structure before and after modification were characterized by SEM, BET and FTIR. The characterization results show that the modified ACF had fewer surface impurities than the modified surface and the gully is more obvious, the specific surface area was increased by …

Bipolar-Membrane Electrodialysis Method To Treat Industrial High Saline Perfume Wastewater, Jian Zhang, Dong-Fang Niu, Shuo-Zhen Hu, Xin-Sheng Zhang

Journal of Electrochemistry

Large amount of organic saline wastewater is generated from various chemical industries. The contents of organic saline wastewater are more and more complicated as they are created from different types of industries. Directly discharging the organic saline wastewater without pre-treatment can generate severe environmental problem and waste useful resources. It is necessary to use an economical method to treat the organic saline wastewater and recover the salt into useful materials to achieve resource reuse. Bipolar-membrane electrodialysis (BMED) is one of the methods that can remove salt from the wastewater and convert it into certain acid and base with higher value …

Transient Electrochemical Surface-Enhanced Raman Spectroscopic Study In Electrochemical Reduction Of P-Nitrothiophenol, Yun Ling, Jing Tang, Guo-Kun Liu, Cheng Zong

Journal of Electrochemistry

P-nitrothiophenol (PNTP) is one of the most common probe molecules studied by surface-enhanced Raman spectroscopy (SERS). The research in electrochemical reduction behavior of PNTP will help understanding the mechanism for the nitrobenzene reduction. In this paper, we used transient electrochemical surface-enhanced Raman spectroscopy (TEC-SERS) to study the SERS of PNTP with cyclic voltammetry and chronoamperometry on gold electrodes. The results show that the TEC-SERS provide a time resolution that equals the transient electrochemical methods, and we concluded that the reaction was so quick that we did not observe the spectral information of intermediate species described in the literatures with a …

Electrochemical Properties Of Sulfur In Different Carbon Support Materials, Bo Zhang, Jia Liu, Xiao-Chen Liu, De-Jun Li

Journal of Electrochemistry

In order to investigate the effect of carbon structure on electrochemical performance of sulfur/carbon composite in lithium-sulfur battery, in this paper, sublimation sulfur was incorporated into three types of carbon materials, namely, graphene, carbon black and porous carbon. The three sulfur/carbon composites were characterized by scanning electron microscopy (SEM), Brunauer-Emmett-Teller (BET), and X-ray diffraction (XRD) techniques, and their electrochemical performances were also studied. The results showed that the sulfur/porous carbon composite offered an initial discharge capacity of 1623.2 mA·h·g^-1 and remained 845 mA·h·g^-1 after 100 cycles. Compared with graphene and carbon black, the mesopores and micropores in porous …

Electrochemical Sensor Based On Magnetic Electrode Modified With Magnetic Molecularly Imprinted Nanoparticles Immobilized Hemoglobin For Determination Of Hydrogen Peroxide, Yang Yuan, Jia-Xin Wang, Yu-Hua Cao

Journal of Electrochemistry

In this work, the surface-imprinted technique was used to prepare magnetic hemoglobin (Hb) imprinted nanoparticles, using Fe₃O₄@SiO₂ NPs as the carrier, Hb as the template molecule, and tetraethyl orthosilicate (TEOS) as the imprinted polymer monomer. The nanoparticles had a core-shell structure, with magnetic Fe₃O₄ NPs as the core and Hb imprinted polymers as the shell. Therefore, Hb could be concentrated and fixed on the surface of the magnetic imprinted nanoparticles (MMIPs NPs). Furthermore, MMIPs NPs were immobilized with chitosan (CS) on the surface of a magnetic electrode to constitute Hb enzyme-like biosensor …

An Aptasensor Based On Aunps/Pani/Tnts Nanocomposite For Electrochemical Detection Of Tobramycin, Yong-Ling Nong, Ni-Na Qiao, Ying Liang

Journal of Electrochemistry

A novel well-constructed electrochemical aptamer-based sensor for the detection of tobramycin was presented, using differential pulse voltammetry (DPV) as a detection technique and methylene blue(MB) as an electrochemical indicator. A glassy carbon electrode modified with a nanocomposite of Au nanoparticles/polyaniline/titania nanotubes (AuNPs/PANI/TNTs) was constructed as the electrode scaffold. The nanocomposite was characterized by transmission electron microscopy and X-ray photoelectron spectroscopy in detail. The results of cyclic voltammetry and electrochemical impedance measurements demonstrated that the AuNPs/PANI/TNTs nanocomposites can improve greatly the electron transfer on the interface. For the detection of tobramycin, the DPV results showed a linear relationship between the current …