Catalysis and Reaction Engineering Commons^™

Analyzing The Surface Chemistry Of Ni-Fe Hydroxide Alloy Nanoparticles As Catalysts For The Oxygen Evolution Reaction By X-Ray Photoelectron Spectroscopy Analysis, Lauren B. Shepard

Chemical Engineering Undergraduate Honors Theses

Water electrolysis has been proposed as a renewable source of hydrogen, a possible replacement to harmful fossil fuels. This process can be broken down into two half reactions, the hydrogen evolution reaction and the oxygen evolution reaction. Because the oxygen evolution reaction has slow kinetics and a high overpotential to overcome, a catalyst is needed to speed up the kinetics and ensure faster and more efficient production of molecular hydrogen. The use of Ni-Fe hydroxide alloy nanoparticles as a catalyst has been shown to significantly improve the efficiency of the reaction by decreasing the overpotential, making the process more energy …

Structural, Charge Transport, Gas Sensing, Magnetic, Pseudocapacitive, And Electrocatalytic Properties Of Perovskite Oxides., Surendra Bahadur Karki

Electronic Theses and Dissertations

Perovskites are functional materials with the general formula ABO₃ (A = alkali, alkaline earth or lanthanoid cations and B = transition metal or main group cations). These materials are marked by a variety of crystal structures and interesting properties such as colossal magnetoresistance, ferroelectricity, multiferroicity, superconductivity, pseudocapacitance, gas sensing, charge transport, and electrocatalytic properties. The formula of perovskite can be written as AA’BB’O₆, when there is ordering between two cations over A and B-sites. Such compounds are called double perovskite oxides. Some amount of oxygen could be lost from crystal structure without decomposition of the phase. Such …

Engineering Lewis Acidic Materials For Biomass Conversion And Battery Applications., Md Anwar Hossain

Electronic Theses and Dissertations

My long-term goal is to develop catalytic systems to produce renewable energy for a sustainable society. The overall research objective of my dissertation is to advance understanding of Lewis acidic materials for (1) conversion of renewable lignin into phenolics and (2) enhanced cycling stability of lithium metal batteries to safely store renewable electricity from wind and solar, thereby laying the groundwork for our transition to a sustainable society. Petroleum is a conventional feedstock for current transportation fuels (gasoline, diesel, and jet fuels). However, petroleum is a finite resource and produces greenhouse gases (CO₂ and CH₄) upon processing, …

Development Of Porous Solid Acid Catalysts For Lignocellulose And Plastic Upcycling., Mohammad Shahinur Rahaman

Electronic Theses and Dissertations

My goal is to develop chemical processes for transforming waste to solve environmental problems and enhance sustainability. Environmental problems such as pollution and massive amounts of waste are the main drivers that stimulate my research ideas. I focused on creating novel, efficient catalytic processes for converting polymeric waste "feedstocks" into high-value chemicals by integrating my expertise in catalysis, materials science, and synthetic chemistry to develop porous solid catalytic materials. During my Ph.D., I focused on two polymeric feedstocks, lignocellulose, and discarded plastic.

Early in my Ph.D. journey, I focused on catalytic upcycling of lignocellulose. Lignocellulosic biomass is cost-effective, abundant, and …

Optimizing Virus Prefiltration For Biopharmaceutical Manufacturing, Solomon Isu

Graduate Theses and Dissertations

Virus filters are single-use devices that use a size-based separation process. In virus filters, contaminating virus particles are retained while the therapeutic molecules pass through the membrane pores. Virus filters are an essential component of the overall virus clearance strategy. Sections 1 and 2 of this dissertation provide an introduction and extensive review of monoclonal antibody (mAb) process development, where virus filtration is pivotal. In section 3, prefiltration studies were performed with an industrially relevant IgG1 type mAb using adsorptive and size-exclusion-based prefilters with different mechanisms of action. This mAb has an isoelectric point range of 7.1 to 8.0 and …

Adjusting The Alloying Degree Of Pt3Zn To Improve Acid Oxygen Reduction Activity And Stability, Tian-En Zhang, Ya-Ni Yan, Jun-Ming Zhang, Xi-Ming Qu, Yan-Rong Li, Yan-Xia Jiang

Journal of Electrochemistry

Proton exchange membrane fuel cell (PEMFC) is a new type of energy device, a relatively excellent way to achieve carbon neutrality. However, due to the relatively slow reaction rate of oxygen reduction reaction (ORR) at the cathode, platinum (Pt) is the key material of the cathode catalyst. However, Pt is a kind of noble metal, and its high cost restricts the PEMFC commercialization process. At present, the main approach is to combine transition metals with Pt to prepare Pt-based alloys and to reduce the use of Pt. Pt-based alloys are excellent catalysts for ORR, improving both the activity and stability, …

Preparation Of Pt@Basrtio3 Nanostructure And Its Properties Towards Photoelectrochemical Ammonia Synthesis, Jing Zhang, Rui-Xia Guo, Jian-Jun Fu, Shi-Bin Yin, Pei-Kang Shen, Xin-Yi Zhang

Journal of Electrochemistry

Ammonia is an important industrial raw material and a potential green energy. Using renewable energy to convert nitrogen into ammonia under ambient condition is an attractive method. However, the development of efficient photoelectrochemical ammonia synthesis catalysts remains a challenge. Perovskite such as BaSrTiO₃ (BST) is a good photocatalytic material. However, BST is active under ultraviolet light and has a high recombination rate of photogenerated electron-hole pairs. By dispersing precious metals, it can effectively regulate the absorption of sunlight by BST. In this work, we used a two-step method to prepare BST. The H₂PtCl₆·6H₂O …

In-Situ/Operando57Fe Mössbauer Spectroscopic Technique And Its Applications In Nife-Based Electrocatalysts For Oxygen Evolution Reaction, Jafar Hussain Shah, Qi-Xian Xie, Zhi-Chong Kuang, Ri-Le Ge, Wen-Hui Zhou, Duo-Rong Liu, Alexandre I. Rykov, Xu-Ning Li, Jing-Shan Luo, Jun-Hu Wang

Journal of Electrochemistry

The development of highly efficient and cost-effective electrocatalysts for the sluggish oxygen evolution reaction (OER) remains a significant barrier to establish effective utilization of renewable energy storage systems and water splitting to produce clean fuel. The current status of the research in developing OER catalysts shows that NiFe-based oxygen evolution catalysts (OECs) have been proven as excellent and remarkable candidates for this purpose. But it is critically important to understand the factors that influence their activity and underlying mechanism for the development of state-of-the-art OER catalysts. Therefore, the development of in-situ/operando characterizations is urgently required to detect key intermediates along …

In Situ Characterization Of Electrode Structure And Catalytic Processes In The Electrocatalytic Oxygen Reduction Reaction, Ya-Chen Feng, Xiang Wang, Yu-Qi Wang, Hui-Juan Yan, Dong Wang

Journal of Electrochemistry

As an electrochemical energy conversion system, fuel cell has the advantages of high energy conversion efficiency and high cleanliness. Oxygen reduction reaction (ORR), as an important cathode reaction in fuel cells, has received extensive attention. At present, the electrocatalysts are still one of the key materials restricting the further commercialization of fuel cells. The fundamental understanding on the catalytic mechanism of ORR is conducive to the development of electrocatalysts with the enhanced activity and high selectivity. This review aims to summarize the in situ characterization techniques used to study ORR. From this perspective, we first briefly introduce the advantages of …

Microcystin-Lr Removal From Water Via Enzymatic Linearization And Ultrafiltration, Abelline Fionah, Cannon Hackett, Hazim Aljewari, Laura Brady, Faisal Alqhtani, Isabel C. Escobar, Audie K. Thompson

Chemical Engineering Faculty Publications and Presentations

Microcystin-LR (MC-LR) is a toxin produced by cyanobacteria that can bloom in freshwater supplies. This study describes a new strategy for remediation of MC-LR that combines linearization of the toxin using microcystinase A, MlrA, enzyme with rejection of linearized byproducts using membrane filtration. The MlrA enzyme was expressed in Escherichia coli (E. coli) and purified via a His-tag with 95% purity. Additionally, composite membranes made of 95% polysulfone and 5% sulfonated polyether ether ketone (SPEEK) were fabricated and used to filter a solution containing cyclic and linearized MC-LR. Tests were also performed to measure the adsorption and desorption of MC-LR …

Computational Study Of The Reactions Of Heteroatomic Compounds On Ceo2, Suman Bhasker Ranganath

LSU Doctoral Dissertations

The mechanisms of ambient-temperature reactions of heteroatomic compounds catalyzed by ceria (CeO₂), an archetypical reducible oxide, for enzyme mimetics, environmental protection, and chemical synthesis are investigated in this dissertation using theoretical methods. CeO₂ is modeled with thermodynamically stable low-index surfaces exposed by commonly studied ceria thin films and nano particles. To understand phosphatase-like dephosphorylation activity, stable adsorption states and surface reactions of model phosphates are examined. Binding of the central P-atom to surface lattice oxygen (O_latt) supplemented by phosphoryl O-Ce interaction is the only stable adsorption state for the un-dissociated molecule. Deprotonation of phosphate monoesters, …

Facet Dependent Oxygen Evolution Activity Of Spinel Cobalt Oxides, Li-Hua Zhang, Hong-Yuan Chuai, Hai Liu, Qun Fan, Si-Yu Kuang, Sheng Zhang, Xin-Bin Ma

Journal of Electrochemistry

Water splitting is a promising technology to produce clean hydrogen if powered by renewable energies, where oxygen evolution is the rate determining step at an anode. Here we adjust the different crystal planes of the cobalt oxides catalyst to expose more effective active sites through a hydrothermal process, so as to improve the reaction activity for oxygen evolution. The samples were well characterized by TEM, SEM and XRD. Among the three synthetic crystal planes (100), (111) and (110) of spinel cobalt oxides, the (100) crystal plane has the highest intrinsic activity. Combining in-situ infrared and DFT calculations, we …

Selective Co2 Reduction To Formate On Heterostructured Sn/Sno2 Nanoparticles Promoted By Carbon Layer Networks, Xue Teng, Yanli Niu, Shuaiqi Gong, Xuan Liu, Zuofeng Chen

Journal of Electrochemistry

Tin (Sn)-based materials have emerged as promising electrocatalysts for selective reduction of CO₂ to formate, but their overall performances are still limited by electrode structures which govern the accessibility to active sites, the electron transfer kinetics, and the catalytic stability. In this study, the heterostructured Sn/SnO₂ nanoparticles dispersed by N-doped carbon layer networks (Sn/SnO₂@NC) were synthesized by a melt-recrystallization method taking the low melting point of Sn (m.p. 232^oC). The N-doped carbon layer networks derived from polydopamine could attract more electrons on the electrocatalyst, serve as conductive agents and protect the ultrafine nanoparticles from …

Structural Degradation Of Ni-Rich Layered Oxide Cathode For Li-Ion Batteries, Jia-Yi Wang, Sheng-Nan Guo, Xin Wang, Lin Gu, Dong Su

Journal of Electrochemistry

Nickel(Ni)-rich layered oxide has been regarded as one of the most important cathode materials for the lithium-ion batteries because of its low cost and high energy density. However, the concerns in safety and durability of this compound are still challenging for its further development. On this account, the in-depth understanding in the structural factors determining its capacity attenuation is essential. In this review, we summarize the recent advances on the degradation mechanisms of Ni-rich layered oxide cathode. Progresses in the structure evolution of Ni-rich oxide are carefully combed in terms of inner evolution, surface evolution, and the property under thermal …

Recent Advances In Electrochemical Kinetics Simulations And Their Applications In Pt-Based Fuel Cells, Ji-Li Li, Ye-Fei Li, Zhi-Pan Liu

Journal of Electrochemistry

Theoretical simulations of electrocatalysis are vital for understanding the mechanism of the electrochemical process at the atomic level. It can help to reveal the in-situ structures of electrode surfaces and establish the microscopic mechanism of electrocatalysis, thereby solving the problems such as electrode oxidation and corrosion. However, there are still many problems in the theoretical electrochemical simulations, including the solvation effects, the electric double layer, and the structural transformation of electrodes. Here we review recent advances of theoretical methods in electrochemical modeling, in particular, the double reference approach, the periodic continuum solvation model based on the modified Poisson-Boltzmann …

Recent Advances In Structural Regulation On Non-Precious Metal Catalysts For Oxygen Reduction Reaction In Alkaline Electrolytes, Xue Wang, Li Zhang, Chang-Peng Liu, Jun-Jie Ge, Jian-Bing Zhu, Wei Xing

Journal of Electrochemistry

Oxygen reduction reaction (ORR) in alkaline electrolytes is an important electrochemical process for metal-air batteries and anion exchange membrane fuel cells (AEMFCs). However, the sluggish kinetics spurs intensive research on searching robust electrocatalysts. Non-precious metal catalysts (NPMCs) that can circumvent the cost and scarcity issues associated with platinum (Pt)-based materials have been pursued and the challenges lie in the performance improvement to rival Pt-based benchmarks. As the composition and structure of the NPMCs have a significant impact on the catalytic performance, precise regulation on the catalyst structure holds great promise to bridge the activity gap between NPMCs and Pt-based benchmarks. …

Mass Loading Optimization For Ethylene Glycol Oxidation At Different Potential Regions, Sheng-Nan Sun, Zhi-Chuan Xu

Journal of Electrochemistry

Designing and fabricating the electrocatalysts is attracting more and more attention in recent years due to a global interest in developing techniques for electrochemical energy conversion and storage, as well as elelectro-synthesis of valuable chemicals. The activity is one of the key performance parameters for electrocatalysts, while the observed activity can be affected by mass loading of electrocatalysts. Here, we take cobalt oxide (Co₃O₄)/graphite paper electrode (Co₃O₄/GPE) as a model electrode to demon-strate how the mass loading of Co₃O₄ catalyst influences ethylene glycol (EG) oxidation in alkaline (KOH) by …

Understanding The Photodegradation Mechanism Of Gaseous Acetaldehyde Over Bi2wo6 – Modified Znwo4 Photocatalyst Under Uv Light Irradiation, Mirabbos Hojamberdiev, Ronald Vargas, Shahlo Daminova, Zuhra Kadirova

CHEMISTRY AND CHEMICAL ENGINEERING

Indoor air quality has a significant impact on human health as people spend more time indoors. As a common indoor air pollutant, acetaldehyde is considered toxic when exposed to it for a prolonged period. The aim of this study is the enhancement of the photocatalytic activity of ZnWO₄ with a monoclinic wolframite structure for degradation of gaseous acetaldehyde by modifying its surface with Bi₂WO₆ layered structure. The mechanisms behind the enhanced photocatalytic activity and the pathways for acetaldehyde photodegradation over the Bi₂WO₆-modified ZnWO₄ photocatalyst are discussed.

Modelling Of Reаctive Distillаtion Process For Etherificаtion Reаction, Adham Norkobilov, Olimjon Mаksudov, Abdulaziz Bаkhtiyorov, Orifjon Zаripov, Abbos Elmаnov

CHEMISTRY AND CHEMICAL ENGINEERING

А reаctive distillаtion system is exаmined to produce for the production of Ethyl tert butyl ether (ETBE) viа etherificаtion of isobutene with ethаnol. Optimizаtion methods using heаt integrаtion аre аlso conducted. The molаr reflux rаtio аnd reboiler duty аre cаlculаted using sensitivity аnаlysis. The bottom streаm with the sаtisfied purity of ETBE is integrаted for heаting the feed streаm to the column. Heаt integrаtion from reаctor heаt to the initiаl feed streаm аnd from bottom streаm of the column to the column inlet streаm with the purpose of аchieving tаrget feed temperаture leаds to high conversion in the reаctive distillаtion …

Synergistic Enhancement Of Formic Acid Electro-Oxidation On Ptxcuy Co-Electrodeposited Binary Catalysts, Yaser M. Asal, Ahmad M. Mohammad, Sayed S. Abd El Rehim, Islam M. Al-Akraa

Chemical Engineering

A propitious binary catalyst composed of Pt and Cu which were electrodeposited simultaneously onto a glassy carbon (GC) substrate was recommended for the formic acid (FA) electro-oxidation reaction (FAOR); the principal anodic reaction in the direct FA fuel cells (DFAFCs). The simultaneous co-electrodeposition of Pt and Cu in the catalyst provided an opportunity to tune the geometric functionality of the catalyst to resist the adsorption of poisoning CO at the Pt surface that represented the major impediment for DFAFCs marketing. The catalytic activity of the catalyst toward FAOR was significantly influenced by the (Pt4+/Cu2+) molar ratio of the electrolyte during …