Physical Chemistry Commons^™

Electrochemical And In Situ X-Ray Absorption Fine Structure Study Of Li-Rich Cathode Materials, Meng-Yan Hou, Hong-Liang Bao, Ke Wang, Jian-Qiang Wang, Yong-Yao Xia

Journal of Electrochemistry

A series of the lithium-rich and manganese-based layered structure xLi₂MnO₃•(1-x)LiMn_1/3Ni_1/3Co_1/3O₂ (x = 0.3,0.5,0.7) materials were synthesized by a co-precipitation method, and followed by a solid-state reaction process. By comparing the first cycle efficiency, the reversible discharge capacity, the cycling stability and the voltage decay during the charge/discharge cycling process, the material with the composition of 0.5Li₂MnO₃•0.5LiMn_1/3Ni_1/3Co_1/3O₂was found to show the best electrochemical performance. The lithium storage mechanism and thermal stability of the de-lithiated compound were also investigated …

The Progress Of Order-Structured Membrane Electrode Assembly, Shang-Feng Jiang, Bao-Lian Yi

Journal of Electrochemistry

Performances of proton exchange membrane fuel cells (PEMFCs) have been recently improved. However, the cost and Pt loading must be further reduced for the commercialization of PEMFCs. Previous researches have proved that the order-structured electrode is beneficial to the effective utilization of Pt-based catalysts, decreasing the Pt loading and increasing the three-phase boundary for reaction. Especially, the nanostructure thin films (NSTFs) electrode, an ultra-thin catalytic layer developed by 3M Company, demonstrates high performance and durability. Besides, some other researchers have employed the high conductive carbon nanotube arrays or high stable metal oxide arrays as the order-structured catalyst supports for fundamental …

Uniform Nanoshells For Functional Materials: Constructions And Applications, Shu-Yi Duan, Wei Zhang, Jun-Yu Piao, An-Min Cao, Li-Jun Wan

Journal of Electrochemistry

As a significant protocol for materials treatment, surface modification has found broad applications in different fields including catalyst, photochemistry, and electrochemistry. Herein, we introduced the representative synthetic methodologies for the constructions of different functional materials with a focus on their core-shell structures. By taking the electrode materials in lithium ion batteries as an example, we demonstrated the importance of surface modification on the electrode materials. Different coating materials ranging from metal oxides, metal phosphates to carbon have been discussed. We also showed that an accurate control on the surface layer can be crucial for optimizing the electrochemical performances of the …

Recent Progress In Solid-State Nmr Study Of Electrode/Electrolyte Materials For Lithium/Sodium Ion Batteries, Gui-Ming Zhong, Zi-Geng Liu, Da-Wei Wang, Qi Li, Ri-Qiang Fu, Yong Yang

Journal of Electrochemistry

Solid state NMR technique is a powerful tool for characterizing the local structure and compositions of solid materials quantitatively. A comprehensive understanding of the structure evolution during the electrochemical reactions of the materials for lithium/sodium ion batteries will be obtained with the combination of solid state NMR, XRD, and XAS methods. Through analyzing solid state NMR spectra, we can obtain the compositions, local structures and ion diffusion dynamics of electrodes, electrolytes and surface layers for lithium/sodium ion batteries, providing an important theoretical support for the design and development of high-performance materials for batteries. In this paper, we review the recent …

3, 4-Ethylenedioxythiophene Monomer As Safety-Enhancing Additive For Lithium Ion Batteries, Wei-Xiao Ji, Feng Wang, Jiang-Feng Qian, Yu-Liang Cao, Xin-Ping Ai, Han-Xi Yang

Journal of Electrochemistry

Safety concern is a major obstacle hindering the wide applications of large-capacity lithium ion batteries (LIBs) in electric vehicles. In this paper, a polymerizable monomer of 3, 4-ethylenedioxythiophene (EDOT) was proposed and tested as an electrolyte additive for enhancing the safety of LIBs. The electro-oxidative polymerization behaviors and influence of PEDOT additive on the thermal behavior of LiCoO₂ cathode, as well as the safety performance and electrochemical properties of LiCoO₂-based LIBs were investigated. The results from cyclic voltammetry (CV) and transmission electron microscope (TEM) characterizations indicated that the monomer additive can be electro-oxidatively polymerized to form a …

Reduced Graphene Oxide (Rgo) Hollow Network Cages For High-Performance Electrochemical Energy Storage, Chi Zhang, Xu-Jun He, Gao-Ren Li

Journal of Electrochemistry

The reduced graphese oxide (RGO) hollow network cages were synthesized via zinc oxide (ZnO) template-assisted electrodeposition. The as-prepared RGO hollow network cages exhibited the multi-level architectures, from nano sheets, porous structures, networks, to 3D microscaled hollow cages, which can simultaneously optimize transport of electroactive species, utilization rate of electrode material, and super capacitive performance. Electrochemical measurements confirmed the superior performance of RGO hollow network cages for supercapacitors (SCs), such as high Csp (393 F⋅g^-1 at 1.0 A⋅g^-1), excellent rate capability (21.2% Csp loss from 1.0 to 20 A⋅g^-1), and superior cycling stability (< 1% Csp loss after 10000 cycles).

Electrochemiluminescence Immunosensor Based On Platinum Nanoparticles For The Determination Of Apolipoprotein A1, Ni Liao, Ying Zhuo, Ruo Yuan

Journal of Electrochemistry

In this paper, a novel electrochemiluminescence (ECL) immunosensor for the detection of apolipoprotein A1 was constructed based on flower-like platinum nanoparticles (PtNFs) via a one-pot chemical synthesis method. The PtNFs was used to immobilize the secondary antibody and enzyme (GOD). Then the prepared bioconjugates were introduced onto the electrode via sandwich immunoreactions. Accordingly, the ECL luminophore peroxydisulfate (S₂O₈^2-) was presented in the working buffer solution containing an appropriate amount of glucose. Through the ECL responses of S₂O₈^2- and O₂, a dramatically amplified ECL signal was obtained for the reason …

Developments Of Photo-Assisted Fuel Cells, Ling-Ling Zhang, Shao-Jun Dong

Journal of Electrochemistry

The exploitation and utilization of fossil fuels have led to serious energy crisis and environmental pollution. In this case, the development of renewable energy is an alternative to traditional energy consumption. Fuel cells (FCs) can convert chemical energy into electricity via the electrochemical reaction, which is green and environment-friendly. Photo-assisted FCs integrate photo-responsive components into FCs, leading to the dual routes of energy conversion including light energy to electricity and chemical energy to electricity, and thus, improving the energy utilization efficiency. The development of photo-assisted FCs is significant for practical application and promising to solve the coming energy crisis. In …

Aqueous Photochemistry Of Glyoxylic Acid, Alexis J. Eugene, Sha-Sha Xia, Marcelo I. Guzman

Chemistry Faculty Publications

Aerosols affect climate change, the energy balance of the atmosphere, and public health due to their variable chemical composition, size, and shape. While the formation of secondary organic aerosols (SOA) from gas phase precursors is relatively well understood, studying aqueous chemical reactions contributing to the total SOA budget is the current focus of major attention. Field measurements have revealed that mono-, di-, and oxo-carboxylic acids are abundant species present in SOA and atmospheric waters. This work explores the fate of one of these 2-oxocarboxylic acids, glyoxylic acid, which can photogenerate reactive species under solar irradiation. Additionally, the dark thermal aging …

Energy Transfer And Localization In Molecular Crystals, Mitchell A. Wood

Open Access Dissertations

With the aim of developing new technologies for the detection and defeat of energetic materials, this collection of work was focused on using simulations to characterize materials at extremes of temperature, pressure and radiation. Each branch of the work here is collected by which material response is potentially used as the detectable signal.

Where the chemical response is of interest, this work will explore the possibility of non-statistical chemical reactions in condensed-phase energetic materials via reactive molecular dynamics (MD) simulations. We characterize the response of three unique high energy density molecular crystals to different means of energy input: electric fields …

Preparation Parameters Optimization And Electrocatalytic Properties Of Supported Au Nanoparticles, Rui Yao, Yu-Jiang Song, Huan-Qiao Li, Jia Li, Jian-Guo Liu

Journal of Electrochemistry

Due to interesting size effect, physical and chemical properties, nano-scale gold materials have been commonly used to catalytic reactions. However, the application of gold nanomaterials in the field of electrocatalysis is limited. Herein, we report the synthesis of gold nanparticles supported on carbon through chemical reduction of HAuCl₄ by NaBH₄ under mild conditions in the presence of surfactants as soft templates, carbon black or graphene as a support. We investigated a series of key reaction parameters, including reagent concentration, temperature, the types of carbon supports and surfactants. With the optimum synthetic parameters, we successfully obtained supported 1 ~ …

Preparation And Performance Of 3d Graphene Type Porous Carbon Employing Nano Fe(Oh)3 As Template For Oxygen Reduction Catalyst, Chong-Yun Sun, Zhong-Fang Li, Xue-Wei Lu, Xi-Zhan Zhong, Yu-Rong Liu

Journal of Electrochemistry

The 3D graphene type porous carbon was prepared using coal tar pitch as carbon source and nano Fe(OH)₃ as template. Optimal conditions for the catalytic oxygen reduction performance were determined as: the mass ratio of coal tar, nano Fe(OH)₃ and KOH is 6:8:4; the pyrolysis temperature is 800 ^oC. SEM images show that the products have uniformly porous structure. TEM images demonstrate that the products are porous with foam shapes. HRTEM images further indicate that the products have formed several-layers 3D graphene structure, which are also supported by XRD and Raman data, and the pore size mainly …

Special Issue: Electrocatalyst And Electrocatalysis In Fuel Cells Preface, Zi-Dong Wei

Journal of Electrochemistry

/

Recent Progress In Non-Precious Metal Oxygen Reduction Reaction Catalysts With An Encapsulation Structure, Mei-Ling Xiao, Jian-Bing Zhu, Chang-Peng Liu, Jun-Jie Ge, Wei Xing

Journal of Electrochemistry

Platinum-based materials, the state-of-the-art catalysts for fuel cells, suffer from prohibitive costs, limited resources and insufficient durability. Accordingly, tremendous efforts were made in searching for efficient, durable and inexpensive alternatives to precious-metal electrocatalysts for the oxygen reduction reaction (ORR). Transition-metals (Fe, Co)/nitrogen co-doped hybrids, heteroatom (N, P, S, F, et al) doped carbons and composites with transition-metals encapsulated in graphitic layers are reported as the most efficient non-precious metal ORR catalysts. Among the various non-precious metal ORR catalysts, transition-metals encased in graphitic layer catalysts are a novel type of catalysts for ORR with high activity and durability, and thus, the …

Mini-Review: Possible Applications Of Scanning Electrochemical Microscopy (Secm) In Characterizations Of Oxygen Reduction Reaction And Oxygen Evolution Reaction, Xing-Xing Chen

Journal of Electrochemistry

Scanning electrochemical microscopy (SECM) has been proved to be a unique technique for combinatorial screening of localized phenomena for different electrocatalysts potentially used in new energy conversion and storage systems. This mini-review provides a brief summary of different SECM working modes, such as direct mode, feedback mode, generation-collection mode, redox competition mode and noise mode, which are especially applied for characterizing the oxygen reactions. Particularly, a series of important development in SECM screening of electrocatalysts for oxygen reduction reaction and oxygen evolution reaction from the author and W. Schuhmann’s group in Germany has been highlighted and overviewed. Finally, some prospects …

Multi-Scaled Carbon Supported Platinum As A Stable Electrocatalyst For Oxygen Reduction Reaction, Yu-Ping Li, Lu-Hua Jiang, Su-Li Wang, Gong-Quan Sun

Journal of Electrochemistry

The stability of carbon supports is essential for electrocatalysts of fuel cells. Herein, the mesoporous carbon with the high graphitic degree (highly graphitic mesoporous carbon, HGMC) was synthesized by using resorcinol as the carbon precursor, SiO₂ as the templates and urea as the reducing agent. The as-prepared HGMC was characterized by XRD, Raman spectroscopy, TEM, N2 adsorption. The stability of HGMC was evaluated by mimicking the start-up/shut-down conditions of fuel cells in a three-electrode system referring to the NREL standard. The obtained HGMC is of moderate surface area (187.4 m²•g^-1) and is chemically stable under …

Recycling Mf Solid Waste Into Mesoporous Nitrogen-Doped Carbon With Iron Carbide Complex In Graphitic Layers As An Efficient Catalyst For Oxygen Reduction Reaction, Can-Yun Zhao, Lin Huang, Yong You, Ying-Fang Yao, Xiao-Gang Su, Hong Wan, Jian-Guo Liu, Cong-Ping Wu

Journal of Electrochemistry

Nitrogen-doped carbon materials with iron ions are known as catalytic growth agents for the oxygen reduction reaction (ORR) in fuel cells, but the design and synthesis of high-performance and low-cost catalysts still remain a significant challenge. Herein, we present a cost-effective approach to dispose of MF solid waste as the precursor for the synthesis of MCFes catalyst with the favorable structure features such as the high specific surface area, abundant active sites and suitable pore structure. The results showed that the MCFe-10/10/2 had specific surface area as high as 780.7 m²•g^-1 and high efficient catalytic activity comparable …

Recent Progresses In Molybdenum-Based Electrocatalysts For The Hydrogen Evolution Reaction, Ze-Xing Wu, Jie Wang, Jun-Po Guo, Jing Zhu, De-Li Wang

Journal of Electrochemistry

Electrochemical catalytic production of hydrogen has been considered as a promising and sustainable strategy for clean and renewable energy technologies. Molybdenum-based non noble metal catalysts for the hydrogen evolution reaction have attracted extensive attention due to its effective catalytic performance. In this review, the recent progresses in molybdenum-carbide, phosphide, nitride and sulfide electrocatalysts are presented. In addition, the strategies to improve the catalytic performance are analyzed and the prospects for the future development trends are expected.

Syntheses Of Carbon Paper Supported High-Index Faceted Pt Nanoparticles And Their Performance In Direct Formic Acid Fuel Cells, Long Huang, Mei Zhan, Yu-Cheng Wang, Yan-Fen Lin, Shuo Liu, Ting Yuan, Hui Yang, Shi-Gang Sun

Journal of Electrochemistry

Direct formic acid fuel fuels (DFAFCs) are promising energy source for portable electronic devices. Palladium (Pd) is more active than platinum (Pt) for the formic acid electrooxidation. However, the stability of Pd is much poorer than that of Pt. Unfortunately, the ultra-low natural abundance of the Pt makes it extremely expensive and limits its application as a fuel cell catalyst. Boosting both the activity and stability of Pt nanoparticles to enhance their efficiency is urgent. As previous works illustrated, nanoparticles enclosed with high-index facets usually bare a higher activity toward fuel cell related reactions than those nanoparticles with low-index facet. …

Dynamic Simulation Of Oxygen Reduction Reaction In Pt/C Electrode For Proton Exchange Membrane Fuel Cells, Shang Li, Fen Zhou, Lei Chen, Mu Pan

Journal of Electrochemistry

It is an urgent need to reduce the Pt loading in electrode for practical fuel cell applications worldwide. Herein, we theoretically investigate the oxygen distribution, generated current, and minimum Pt loading of Pt/C electrode for practical applications based on kinetic model of oxygen reduction reaction. The results indicate that with increasing electrode effective thickness to 40 mm, serious concentration polarization is expected for Pt/C electrode. To generate a power density of 1.4 W⋅cm^-2 (2.1A⋅cm^-2@0.67 V) for fuel cell, the cathode catalyst layer thickness in PEMFC should be as thin as 3 mm. The minimum Pt loading will …

Synthesis Of Structurally Ordered Platinum-Iron Catalysts With Enhanced Oxygen Reduction Reaction Activity, Ye-Zheng Cai, Ming-Chuan Luo, Fang-Hui Wang, Zhao-Nan Sun, Hong Zhu

Journal of Electrochemistry

To improve oxygen reduction reaction catalytic activity of the precious metals platinum for fuel cell, the precursors of carbon-supported structurally disordered platinum-iron alloy (D-Pt₃Fe/C and D-PtFe/C) catalysts with different compositions were synthesized via a modified polyol reduction method. Then, by optimizing the annealing conditions in the inert gas, we turned the structurally disordered platinum-iron alloy to the structurally ordered platinum-iron alloy (O-Pt₃Fe/C and O-PtFe/C) catalysts. The structural characterizations of the as-prepared catalysts were performed by X-ray powder diffraction (XRD), transmission electron microscopy (TEM), inductively coupled plasma-atomic emission spectroscopy (ICP-AES), and X-ray photoelectron spectroscopy (XPS). The results …

Rambling Between "Zhong Yong" And "Catalysis", Zi-Dong Wei

Journal of Electrochemistry

“Zhong Yong” represents a traditional Chinese wisdom, which was first proposed by Confucius and continuously richened by his followers. “Zhong Yong” pursues the balances among all kinds of contradictions, and insists that neither “too much” nor “not enough” is good. For a successful catalyst, on which the adsorption of reactants must be not so strong and not so weak either. On this point of view, there are the same pursuits for “Zhong Yong” and catalysis. In this paper, the author starts his story with a conversation between Confucius and his student, followed by 3 interesting stories happening in the ancient …

Nitrogen, Fluorine Co-Doped Silk-Derived Carbon For Electrochemical Oxygen Reduction With High Performance In Alkaline Solution, Fang-Fang Liu, Hong-Liang Peng, Shi-Jun Liao

Journal of Electrochemistry

A high-performance, doped carbon-based catalyst was synthesized by pyrolyzing hydrothermally treated silkworm cocoon. The effects of preparation conditions and fluorine promotion on various catalysts’ performance were investigated. The catalyst prepared under optimal conditions and doped with nitrogen and fluorine possessed the high specific surface area of more than 1000 m^2⋅g^-1 and contained 3.5 and 7.3% (by mass, the same below) N and F, respectively. The activity of the catalyst toward oxygen reduction reaction in an alkaline medium was comparable to that of commercial Pt/C, showing both superior tolerance to methanol poisoning and better durability. Doping with fluorine …

Mutlifunctional Platforms For Gene And Drug Delivery For Cancer Therapy, Jeffery J. Ambrose Jr.

Doctoral Dissertations

The National Cancer Institute and the American Cancer Society estimate that 1.6 million new cancer incidences and over half a million cancer related deaths occur annually [1][2]. Cancer the second most common cause of death in the United States [1], [2]. Although the causes of cancer can vary depending on cell type, all or almost all instances of cancer arise from a mutation or from an abnormal activation of the cellular genes that control cell growth and mitosis [3].

Treatment of a given cancer type depends on the subtype, stage and progression of the cancer. Varieties of cancer therapy include …

Electrochemical H2O2 Sensor Based On The Co-Immobilization Of Phosphmolybdic Acid And Graphene On Pedot Film Electrode With Nafion, Hao-Xian Zhou, Jun-Ming Zhang, Zhi-Yu Qu, Pan-Yu Zhang, You-Jun Fan

Journal of Electrochemistry

With a glassy carbon electrode (GCE) as the substrate, the poly(3,4-ethylenedioxythiophene) (PEDOT) film electrode was prepared through the electrochemical polymerization method, then a novel non-enzymatic electrochemical H₂O₂ sensor was fabricated by co-immobilizing phosphomolybdic acid and graphene with Nafion on the PEDOT/GCE electrode. The modified electrodes were characterized by scanning electron microscopy (SEM), while the responsive properties of the sensor to H₂O₂ were investigated by cyclic voltammetry and chronoamperometry. The results demonstrated that, under the optimized conditions, the sensor exhibited good electrocatalytic performance for H₂O₂ reduction. The current response of the sensor …

Improving The Electrochemical Properties Of Polyaniline By Doping With Silver Ions, Hui Xu, Jin-Juan Pu, Yong Chen, Jian Liu

Journal of Electrochemistry

Polyaniline (PANI) is an attractive candidate among the various conductive polymers based on its unique doping/de-doping behavior, intrinsic electrical conductivity, facile synthesis, and environmental stability. However, the poor conductivity and cycle stability in an acid medium have restricted its applications. Our work aims at solving the above problems effectively by doping silver ions into PANI. The PANI and PANI doped with silver ions (PANI/Ag⁺) were synthesized by a facile interfacial polymerization process, which used aniline as a starting material in toluene in contact with an aqueous solution of silver nitrate varied from 0.04 mol•L^-1 to 0.20 mol⋅L …

Adsorption Behavior Of Rhodamine 6g On Silver Surfaces Studied By Electrochemical Surface-Enhanced Raman Spectroscopy, Chan-Juan Chen, Cheng Zong, Guo-Kun Liu, Bin Ren

Journal of Electrochemistry

Rhodamine 6G (R6G) is one of the most common probe molecules employed in single molecule surface-enhanced Raman spectroscopy (SM-SERS). The study in adsorption behavior of R6G will help understand the interactions between R6G and surface. In this paper, we used electrochemical surface-enhanced Raman spectroscopy (SERS) to study the potential-dependent adsorption behavior of R6G on silver electrodes. Our results show that when the potential moved negatively, the orientation of R6G on silver surface changed from vertical to inclined adsorption. This result indicates that the abnormal SM-SERS spectra of R6G observed in the former SM-SERS studies from other research groups are due …

Electrochemical Detection Of Hydrogen Peroxide At Aunps Modified Electrode Using P-Hydroxyphenylboronic Acid As A Precursor, Chun-Yan Wang, Xiao-Qiu Liu, Ying-Xin Qi

Journal of Electrochemistry

We developed a new method for electrochemical detection of hydrogen peroxide (H₂O₂) based on boronate oxidation of p-hydroxyphenylboronic acid. This method using p-aminophenol which is produced from the reaction of H₂O₂ and p-aminophenylboronic acid as a well electrochemical probe, combined with a gold nanoparticles (AuNPs) modified electrode for an indirect detection of H₂O₂. Because of the large surface area and enhanced electrocatalytic behavior by the AuNPs modified electrode, the detection sensitivity was improved. The method could detect H₂O₂ in the concentration range of 1 ~ 100 …

Electrochemical Determination Of Hg(Ii) At Gold Nanoparticles@Carbonaceous Microspheres Modified Electrode, Tian-Yu Qiu, Ming-Chun Wang, Xian-Feng Du, Tian-Jia Jiang, Xing-Jiu Huang

Journal of Electrochemistry

The gold nanoparticles@carbonaceous microspheres (Au@CMSs) and  Au@CMSs modified glassy carbon electrode (GCE) were prepared. The Au@CMSs modified  GCE was further examined for possible sensitive detection of mercury ions (Hg(II)) in an aqueous solution by square wave anodic stripping voltammetry (SWASV). The excellent performance was found in the stripping analysis of Hg(II) in 0.1 mol•L^-1 NaAc-HAc(pH=5.0) with a sensitivity of 25.863 A•(mol•L^-1)^-1 and a detection limit of 3.69×10^-8 mol•L^-1 based on the 3σ method.

Fabrication Of Riboflavin Electrochemical Sensor Based On Au Nanoparticles/Polydopamine/Carbon Nanotubes Modified Glassy Carbon Electrode, Hua-Ping Peng, Mei-Ling Yu, Xin Liu, Pan Liu, Wei Chen, Ai-Lin Liu, Xin-Hua Lin

Journal of Electrochemistry

A novel electrochemical platform for the high sensitivity detection of riboflavin was constructed by Au nanoparticles/polydopamine/carbon nanotubes (Au-PDA-MWCNTs) nanocomposite modified glassy carbon electrode. The Au-PDA-MWCNTs nanocomposite was synthesized by in situ reduction method. The characteristics of the as-prepared Au-PDA-MWCNTs nanocomposite modified electrodes were investigated by using UV-Vis spectroscopy, scanning electron microscopy (SEM) and electrochemical methods. Cyclic voltammetry (CV) and differential pulse voltammetry (DPV) were used to study the electrochemical behavior of riboflavin (RF) at Au-PDA-MWCNTs nanocomposite modified electrodes. The results demonstrated that the present electrochemical sensor exhibited a wide linear range from 5×10^-9 mol•L^-1to 1×10^-5 mol•L …