Physical Chemistry Commons^™

Quantum Transport Of The 2d Surface State In A Nonsymmorphic Semimetal, Xue Liu, Jin Hu, Jiang Wei, Chunlei Yue, Sergey V. Erohin, Yanglin Zhu, Abin Joshy, Jinyu Liu, Ana M. Sanchez, David Graf, Pavel B. Sorokin, Zinqiang Mao

Physics Faculty Publications and Presentations

In a topological semimetal with Dirac or Weyl points, the bulk-boundary correspondence principle predicts a gapless edge mode if the essential symmetry is still preserved at the surface. The detection of such topological surface state has been considered as the fingerprint prove for crystals with nontrivial topological bulk band. On the contrary, it has been proposed that even with symmetry broken at the surface, a new surface band can emerge in nonsymmorphic topological semimetals. The symmetry reduction at the surface lifts the bulk band degeneracies and produces an unusual “floating” surface band with trivial topology. Here, we first report quantum …

High Performance Mixed-Matrix Electrospun Membranes For Ammonium Removal From Wastewaters, Shu-Ting Chen, Sumith Ranil Wickramasinghe, Xianghong Qian

Chemical Engineering Faculty Publications and Presentations

Mixed-matrix electrospun membranes were developed to investigate ammonium removal from low ammonium concentration wastewaters for the first time. Particles derived from the inexpensive zeolite 13X were successfully incorporated into polyethersulfone (PES) matrices. The fabricated mixed-matrix electrospun membranes demonstrate high ammonium removal capacity reaching over 55 mg/g_zeolite, more than 2.5 times higher than the previously fabricated mixed-matrix membranes via non-solvent induced phase inversion. Moreover, the membranes fabricated exhibit high permeability and ease of regeneration. Over 90% of total ammonium nitrogen (TAN) can be removed from low TAN wastewaters such as aquaculture wastewaters. In addition to zeolite 13X, other zeolite …

Remote Performance Modulation Of Ultrafiltration Membranes By Magnetically And Thermally Responsive Polymer Chains, Arijit Sengupta, Anh Vu, Xianghong Qian, Sumith R. Wickramasinghe

Chemical Engineering Faculty Publications and Presentations

Ultrafiltration membranes, that respond to an external magnetic field and local temperature have been developed. Surface-initiated activator-generated electron transfer (AGET) atom transfer radical polymerization (ATRP) has been used to graft poly(N-isopropylacrylamide) (PNIPAm) from the surface of 300 kDa regenerated cellulose membranes. The polymerization initiator was selectively attached to the entire membrane surface, only the outer membrane surface or only the inner pore surface. A superparamagnetic nanoparticle was attached to the end of the polymer chain. The DI water flux as well as the flux and rejection of bovine serum albumin were investigated in the absence and presence of a 20 …

Preparation And Characterization Of "Water-In-Salt" Polymer Electrolyte For Lithium-Ion Batteries, Xu Hou, Xin He, Jie Li

Journal of Electrochemistry

Since the development of wearable and flexible electronic products, the demand of flexible energy storage devices such as batteries and super capacitors is in urgent. To enhance the safety and cycling stability for flexible lithium-ion batteries, “water-in-salt” polymer electrolyte was prepared by introducing 21 mol·kg^-1 LiTFSI electrolyte into cross-linked polyacrylamide (PAM) after freeze-drying. A great amount of holes with the size range of 10 ~ 20 μm can be found on the surface and in the bulk of polyacrylamide, which is benefited from the freeze-drying process and acts as a great support for the electrolyte uptake. The “water-in-salt” polymer …

Application Of Atomically Precise Metal Nanoclusters In Electrocatalysis, Zhi-Hua Zhuang, Wei Chen

Journal of Electrochemistry

Metal nanoclusters (M NCs) consist of only several to a few hundred of metal atoms and possess core sizes less than 2 nm. Owing to the quantum size effect, the electronic states of M NCs evolve to discrete levels similar to the molecule energy gaps, other than a continuous density of states to produce plasmon characteristic of bulk metal nanoparticles (M NPs). In comparison with the conventional M NPs, M NCs exhibit dramatically unique electronic and optical properties, such as molecule-like energy gaps, strong photoluminescence and high catalytic properties, which make them promising for potential application in numerous fields, such …

Electrochemiluminescence Imaging Hydrogen Evolution Reaction On Single Platinum Nanoparticles Using A Bipolar Nanoelectrode Array, Xiang Qin, Zhong-Qiu Li, Jian-Bin Pan, Jian Li, Kang Wang, Xing-Hua Xia

Journal of Electrochemistry

A high-density (5.7 × 10⁸ cm^-2) nanoelectrode array with the electrode diameter of 200 nm and the interelectrode distance of 450 nm were fabricated. The nanoelectrode array consisted of gold nanowires embedded in a porous anodic aluminum oxide (AAO) matrix, having regular nanoelectrode distribution and highly uniform nanoelectrode size. The gold nanoelectrode array was used as a closed bipolar nanoelectrode array combined with electrochemiluminescence (ECL) method to map the electrocatalytic activity of platinum nanoparticles toward hydrogen evolution reaction (HER) by modifying the catalysts on single nanoelectrodes. Results show that HER on single bipolar nanoelectrodes could be imaged …

Oxygen-Exposure Induced Rapid Oxidation Of Spiro-Ometad In Cspbibr2 Perovskite Solar Cells, Wei-Guo Wang, Tian Bai, Gao-Fei Xue, Mei-Dan Ye

Journal of Electrochemistry

2,2′,7,7′-tetrakis(N,N-di-p-methoxyphenyl-amine)-9,9′-spirobifluorene (Spiro-OMeTAD) is the most widely used hole transport material in perovskite solar cells (PSCs). However, its oxidation in the air takes a long time and results in the attack of perovskite by water. In this regard, we performed the oxidation process of Spiro-OMeTAD in oxygen, where perovskite can be protected from water, guaranteeing the integrity of perovskite. It was demonstrated that the champion Spiro-OMeTAD based CsPbIBr₂ PSCs after oxygen oxidation achieved a 7.19% power conversion efficiency (PCE), showing a higher PCE than 6.29% of the champion device oxidized in air. A series of electrochemical characterization methods were applied …

Theoretical Studies Of Metal-N-C For Oxygen Reduction And Hydrogen Evolution Reactions In Acid And Alkaline Solutions, Xue-Ping Qin, Shang-Qian Zhu, Lu-Lu Zhang, Shu-Hui Sun, Min-Hua Shao

Journal of Electrochemistry

Single atom catalysts (SAC) have been regarded as the promising alternatives to platinum group metals due to their low costs and potentially high catalytic activities in various electrocatalytic reactions. The atomic mechanism understanding of activity discrepancy among different metal and nitrogen co-doped carbon-based catalysts is still lacking. Here, non-precious metal and nitrogen co-doped carbons (Me-N-C, Me = Fe and Co) as the model catalysts are investigated by combining experimental and theoretical studies to explore the catalytic activities and corresponding reaction mechanisms toward oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER) at universal pHs. Atomic theoretical simulations suggest that Fe-N-C …

Electrochemical Surface-Enhanced Raman Spectroscopic Studies On Nickel Ultramicroelectrode, Li-Wen Wu, Wei Wang, Yi-Fan Huang

Journal of Electrochemistry

Nickel (Ni) electrodes are widely used in electrochemical researches. Understanding electrochemical processes on Ni electrodes through in-situ characterization of adsorbed species on their surfaces is helpful for rational optimization and application of Ni electrochemistry. Microelectrochemical surface-enhanced Raman spectroscopy (μEC-SERS) combines the mass transfer feature of ultramicroelectrode with high-sensitivity characterizations of molecular structures, which is a powerful method for studying Ni electrochemistry on polarization and non-equilibrium conditions. The key point of performing μEC-SERS is to make a SERS-active Ni ultramicroelectrode.
Here, we demonstrate a method of preparing a SERS-active Ni ultramicroelectrode through electrochemical deposition of several atomic layers of …

Electrochemical Gating Single-Molecule Circuits With Parallel Paths, Jun-Qing Su, Yi-Fan Zhou, Ling Tong, Ya-Hao Wang, Ju-Fang Zheng, Jing-Zhe Chen, Xiao-Shun Zhou

Journal of Electrochemistry

Electrochemical gating has emerged as a feasible and powerful method to tune single-molecule conductance. Herein, we demonstrate that the electron transport through single-molecule circuits with two benzene rings in parallel could be efficiently gated by electrochemistry. The molecular junctions with two parallel paths are fabricated with Au electrodes by STM break junction (STM-BJ) technique. Their conductance value exhibits a 2.82-fold enhancement by the constructive quantum interference compared to single-molecule junctions with single path for electron tunneling. Furthermore, the conductance of para-benzene based molecule could be electrochemically tuned with a modulation ratio of about 333%·V^-1. With the help of …

Lithium Storage Performance Of Hard Carbons Anode Materials Prepared By Different Precursors, Zhen-Lang Liang, Yao Yang, Hao Li, Li-Ying Liu, Zhi-Cong Shi

Journal of Electrochemistry

Hard carbon is one of the most promising anode material for lithium ion batteries (LIBs) owing to its high stability, widespread availability, low-cost, and excellent performance. The electrochemical properties of hard carbon materials depend strongly on the type of precursors. It is, therefore, very important to choose an excellent hard carbon precursor. Polyacrylonitrile, petroleum pitch and peanut shells were used as raw materials to prepare different hard carbon anode materials for LIBs. These hard carbon anode materials were successfully synthesized in two steps. The selected precursor was firstly carbonized at 600℃ for 1 h in argon atmosphere using heating rate …

Pd-Based Electrocatalysts For Oxygen Reduction And Ethanol Oxidation Reactions: Some Recent Insights Into Structures And Mechanisms, Zhi-Peng Wu, Chuan-Jian Zhong

Journal of Electrochemistry

The development of efficient electrocatalysts for applications in fuel cells, including proton-exchange membrane fuel cell (PEMFC) and direct ethanol fuel cell (DEFC), has attracted extensive research attention in recent years. Oxygen reduction reaction and ethanol oxidation reaction are two of the key reactions where the design of active, stable and low-cost electrocatalysts is critical for the mass commercializations of PEMFCs and DEFCs. This challenge stems largely from the limited understanding of the catalyst structures and reaction mechanisms. Progress has been made in investigations of electrocatalysts derived from Pd-based alloy nanomaterials both experimentally and computationally. We highlight herein some of the …

Nitro Group Reduction For Use In Organic, Cathodic Materials, Brock G. Goeden

Honors Thesis

The industrial demand for higher capacity, light-weight battery materials has skyrocketed in recent years due to heavy investments in portable electronics, electronic vehicles, and renewable energy sources. However, rechargeable battery technology has seen little improvement since the invention of the Lithium-Ion battery in the 1980s. The low energy density of the traditionally utilized LiCoO2 cathodic material (specific capacity: 272 mAh g-1), has limited its potential to meet these increasing demands. To solve this problem, our research group is investigating new types of lightweight, organic, polymeric materials with conductive backbones as a possible replacement for the cathodic materials in Lithium-Ion batteries. …

Adsorption And Transport Of Colloids At Interface And In Bulk, Jingyun Lee

LSU Doctoral Dissertations

Colloids are suspensions of microscopic insoluble particles dispersed in a continuum phase such as liquid or gas. Colloids are found in our everyday life from food and cosmetic industries to pharmaceutical and biomedical applications. Depending on a global minimum of the free-energy landscape, colloidal suspensions can be classified as two major classes: equilibrium or active colloidal system. This Ph.D dissertation presents strategies to engineer equilibrium self-assembled structures and out-of-equilibrium active matter using various interparticle forces.

First, we introduce the means to promote the equilibrium self-assembled structures driven by adsorption of colloids at interface. Typically, adsorption of colloids at interface is …

Blood Driven Biopower Cells: Acquiring Energy From Reverse Electrodialysis Using Sodium Concentrations From The Flow Of Human Blood, Efecan Pakkaner, Chase Smith, Christina Trexler, Jamie Hestekin, Christa Hestekin

Chemical Engineering Faculty Publications and Presentations

With the growth of the healthcare industry, small scale power sources are needed to support advancements in medical implants, artificial organs, and sensors throughout the body. However, it remains a challenge to find safe, reliable, and stable power sources for these devices. In this study, a miniaturized reverse electrodialysis (RED) biopower cell design using physiological salinity concentration differences between renal bloodstreams is explored for its potential to be used as a power supply for implantable medical devices. Two small scale RED devices produced consistent power for up to three to ten days, depending on the device design. A two-fold decrease …

Preparations And Electrocatalytic Ethanol Properties Of Palladium Intercalated Hydrotalcite, Shou-Xun Hu, Liang Li, Jun-Hao Yang, Liu-Qiang Li, Zhi-Hao Jin

Journal of Electrochemistry

High-performance electrocatalysts play a vital role in the commercial application of direct fuel cells. Current anode materials still have such problems as low activity, easy poisoning and high cost. In this study, a new type of nano- palladium (Pd) catalyst was prepared by dipping method using layered double hydroxides (LDHs) as the carrier. X-ray diffractometer, scanning electron microscope (SEM), inductively coupled plasma mass spectrometer (ICP-MS), energy spectrometer, transmission electron microscope (TEM), cyclic voltammetry, chronoamperometry and electrochemical impedance spectroscope were used to analyze the structure and electrocatalytic performance of the catalyst. The results showed that the newly prepared Pd/Mg-Al-LDHs still maintained …

Theoretical Study On Electrical Properties Of Molecular Junctions Of Viologen Derivatives, Zhuan-Yun Cai, Jia Liu, Si-Yuan Guan, De-Yin Wu, Zhong-Qun Tian

Journal of Electrochemistry

In this paper, the electrical properties of molecular junctions formed N,N′-bis(4-thioalkyl)-4,4′-bipyridinium (viologen) moiety between two gold (Au) electrodes have been investigated by combining density functional theory and non-equilibrium Green’s functional approach. To modulate the viologen molecule to be a cation with one and two positive charges (V⁺ and V²⁺), we introduce one and two trifluoroacetic acid ions (TFA^-) around the molecule, respectively. The valence states of V⁺ and V²⁺ are confirmed by checking Mulliken and NBO charges. Then the relationship between molecular conductance and electronic structures of the neutral state …

Study On Li3Bo3 Interface Modification Of Garnet Solid Electrolyte, Gui-Wei Chen, Zheng-Liang Gong

Journal of Electrochemistry

Garnet solid-state electrolytes have become the research hotspot due to their high ionic conductivity, wide electrochemical stability window and good air stability. However, there are still a series of problems to be solved. The poor contact between the lithium (Li) metal and garnet pellet make it difficult to build stable ion diffusion channels, resulting in large interfacial resistance. The continuous growth of lithium dendrites can penetrate the electrolyte pellet and cause a short circuit in the solid-state battery. Herein, a novel strategy is proposed to improve the wettability of LLZTO electrolyte with Li metal, via interfacial modification of LLZTO electrolyte …

Preparation Of Pdcoir Tetrahedron Nanocatalysts And Its Performance Toward Ethanol Oxidation Reaction, Zhi-Yuan Yu, Rui Huang, Jie Liu, Guang Li, Qian-Tong Song, Shi-Gang Sun

Journal of Electrochemistry

As a new energy conversion device, direct ethanol fuel cells (DEFCs) are widely concerned because of their remarkable advantages such as high theoretical energy density and wide fuel sources. However, the rapid development of DEFCs has been severely impeded due to the sluggish kinetic process and toxic intermediates especially in their anodic reactions. Palladium (Pd)-based materials are considered to be excellent anode catalysts for DEFCs, especially under alkaline conditions. And further improving their performance is an important direction to promote the development of DEFCs. Surface structure and composition are the key factors affecting the performance of catalysts which can be …

Research Progress On Transition State Of Organic Electrode Materials, Xue-Qian Zhang, Zhou-Guang Lu, Wei-Wei Huang

Journal of Electrochemistry

With the increasing requirements for high energy density, long lifetime, high safety, environmentally friendly fabrication, and sustainable development of large energy storage devices, the society calls for new electrode materials in rechargeable batteries beyond traditional inorganic materials which are limited by specific capacity. Organic electrode materials have been widely used in rechargeable batteries due to their advantages of large theoretical capacity, designable structures and environmentally friendly fabrications. In this review, the radical intermediates of organic electrode materials produced in the charging-discharging process (redox reaction) and their types are systematically reviewed. The stability of radical intermediates controlled by changing the structure …

Research Progress Of Sio2 Regrowth During Selective Etching Process In 3d Nand Manufacture Procedure, Zi-Han Zhou, Yun-Wen Wu, Ming Li, Su Wang

Journal of Electrochemistry

As one of the most significant memory chips in semiconductor market, NAND has been developed from two-dimension (2D) to three-dimension (3D). Due to the three-dimensional memory structure of 3D NAND, the capacity density, read-write speed and reliability of memory chips have been greatly improved, as well as the reduction of power dissipation. It is by nitride-oxide selective etching process in the alternate stacked structure of 3D NAND that the inter-dielectric layers can be obtained. The more stack layers, the better performance of chips will be. Meanwhile, however, silicon dioxide (SiO₂) would regrow on the corner of oxide layers, …

Preparation And Performance Investigation Of Li-Sgo Doped Semi-Ipns Porous Single Ion Conducting Polymer Electrolyte, Yun-Feng Zhang, Jia-Ming Dong, Chang Tan, Shi-Kang Huo, Jia-Ying Wang, Yang He, Ya-Ying Wang

Journal of Electrochemistry

Herein, the lithiated sulfonated graphene oxide (Li-SGO) was successfully prepared via three steps by sulfonation of graphene oxide with 3-merraptnpropylt rimethnxysilane, oxidation of thiol into sulfonate with hydrogen peroxide and lithiation of sulfonate with aqueous lithium hydroxide. The as-prepared Li-SGO was then introduced into the semi-interpenetrating networks of single ion conducting polymer electrolyte (Li-SGO-FPAS) and poly vinylidenefluoride-hexafluoro propylene (PVDF-HFP) binder by in-situ polymerization to fabricate the porous single ion conducting polymer electrolyte membrane (Li-SGO-po-FPAS) generated from the poor compatibility between aromatic Li-SGO-FPAS and aliphatic PVDF-HFP binder. The key properties such as morphology, porosity, solvent uptake, mechanical …

Combined Applications Of Photocurrent Spectroscopy, Photoluminescence Spectroscopy And Uv-Vis Spectroscopy For Nano-Semiconductor Based Photoelectric Devices, Si-Da Bian, Jian-Zhang Zhou, Zhong-Hua Lin

Journal of Electrochemistry

The electronic structures and properties of nano-semiconductors are quite different from those of bulk semiconductors due to the nano-size effect (such as quantum size effect). Moreover, when the nano-semiconductor materials are deposited onto the substrate to construct a device, their electronic properties are also affected by the substrate or other components, which may lead to different performances of nano-semiconductors based photoelectric devices, and consequently, different corresponding characterization methods are needed. The combination of photocurrent spectroscopy, photoluminescence spectroscopy with UV-Vis absorption spectroscopy can provide a more comprehensive characterization for the electronic properties and photoelectrochemical performances of nano-semiconductors in photoelectric devices. Our …

Influence Of Resveratrol On Performance Of Long-Term Storage’S Lithium-Ion Battery Electrolyte, Lei Zhang, Xu-Ping Zhang, Si-Wei Zhang, Quan-Chao Zhuang

Journal of Electrochemistry

Electrolyte of lithium-ion battery usually goes through processes of filling, transportation and storage from the completion of manufacture to the use. Understanding the influence of long-term storage process on performance of lithium-ion battery electrolyte is of theoretical significance for production of lithium-ion battery. Scanning electron microscope (SEM) images showed that the solid electrolyte interface (SEI) film formed on the surface of the graphite electrode was thicker in the base electrolyte after 6 months of storage. The charge/discharge test results showed that the reversible cycle capacity and cycle stability (capacity retention rate) of graphite electrode decreased significantly after 6 months of …

Research Progress In Electrodeposition Technology Of Titanium-Based Iridium Oxide Electrode, Dan-Dan Wu, Xu Wu

Journal of Electrochemistry

Titanium-based iridium oxide electrode has been widely used in various fields, such as electrocatalytic oxidation, biomedical applications, hydrometallurgical metal recovery, electro-osmotic dewatering, etc. At present, it is mainly prepared by traditional thermal decomposition method, however, which has high cost, cumbersome process, mainly relying on manual labor and cannot be mass-produced yet. It is, therefore, urgently necessary to explore new preparation technologies by focusing on electrodeposition technology, with technological characteristics such as eco-friendly and sustainable development. This article systematically discusses the research progress in iridium oxide electrodeposition preparation technology from the aspects of deposition solution formulation, base material selection and treatment, …

Preparations And Electrochemical Properties Of Bc/Coni2S4@Ppy Flexible Composites For Supercapacitors, Si-Yuan Peng, Shi-Run Yang, Jing-Hong Zhou, Zhi-Jun Sui, Tao Zhang, Yi Shi, Xing-Gui Zhou

Journal of Electrochemistry

Flexible supercapacitor is one of the most promising energy storage devices for portable and wearable electronic products due to its advantages of high power density, fast charging and long cycle life. Therefore, self-supporting flexible electrode materials with high performance have attained more and more attention both in academia and in industry recently. In this work, using bacterial cellulose (BC) as a flexible substrate, the bacterial cellulose/nickel-cobalt sulfide@polypyrrole (BC/CoNi₂S₄@PPy) flexible composites with three-dimensional porous network and good conductivity were prepared by a combined solvothermal-in-situ polymerization-vacuum filtration method. The samples were characterized by X-ray diffraction, …

Syntheses Of Na3V2(Po4)2O2F As A Cathode For Sodium Ion Battery Application, Kai Wu

Journal of Electrochemistry

High-temperature solid-state method, hydro-thermal method and solvo-thermal method have been mainly employed to synthesize Na₃V₂(PO₄)₂O₂F (NVPF) cathode materials. However, these methods are energy consuming and complicated, which is not applicable for a large scale industrial production. In this study, a rather low-temperature (70℃) co-precipitation strategy was proposed to synthesize NVPF cathode materials. The as-prepared NVPF cathode materials showed a spherical shape with a diameter of 400 ~ 500 nm, and exhibited a sodium storage of 105.6 mAh·g^-1 and an efficiency of 90.06%. After a simple thermal process, the specific …

Computational Modelling Enables Robust Multidimensional Nanoscopy, Matthew D. Lew

Electrical & Systems Engineering Publications and Presentations

The following sections are included:

• Present State of Computational Modelling in Fluorescence Nanoscopy

• Recent Contributions to Computational Modelling in Fluorescence Nanoscopy

• Outlook on Computational Modelling in Fluorescence Nanoscopy

• Acknowledgments

• References

Effects Of Resin Chemistries On The Selective Removal Of Industrially Relevant Metal Ions Using Wafer-Enhanced Electrodeionization, Humeyra B. Ulusoy Erol, Christa N. Hestekin, Jamie A. Hestekin

Chemical Engineering Faculty Publications and Presentations

Wafer-enhanced electrodeionization (WE-EDI) is an electrically driven separations technology that occurs under the influence of an applied electric field and heavily depends on ion exchange resin chemistry. Unlike filtration processes, WE-EDI can be used to selectively remove ions even from high concentration systems. Because every excess ion transported increases the operating costs, the selective separation offered by WE-EDI can provide a more energy-efficient and cost-effective process, especially for highly concentrated salt solutions. This work reports the performance comparison of four commonly used cation exchange resins (Amberlite IR120 Na⁺, Amberlite IRP 69, Dowex MAC 3 H⁺, and …

Fluid Model Of Plasma-Liquid Interaction: The Effect Of Interfacial Boundary Conditions And Henry's Law Constants, Yifan Liu, Dingxin Liu, Jishen Zhang, Bowen Sun, Santu Luo, Hao Zhang, Li Guo, Mingzhe Rong, Michael G. Kong

Bioelectrics Publications

Plasma–liquid interaction is a critical area of plasma science, mainly because much remains unknown about the physicochemical processes occurring at the plasma–liquid interface. Besides a lot of experimental studies toward the interaction, a few fluid models have also been reported in recent years. However, the interfacial boundary conditions in the models are different and the Henry's law constants therein are uncertain; hence, the accuracy and robustness of the simulation results are doubtable. In view of this, three 1D fluid models are developed for the interaction between a plasma jet and deionized water, each of which has a unique interfacial boundary …