Materials Chemistry Commons^™

Feasibility Studies For Use Of Copper Slag In Clinker Manufacture, Suresh Vanguri, Suresh Palla, Gonthi Prasad, Sanjeev Kumar Chaturvedi, Bibekananda Mohapatra

Makara Journal of Science

This study investigated the feasibility of using copper slag (CS-C) as a raw material in the production of Portland cement (PC). The effect of addition of 0%-3.5% CS-C on the clinkerization process, mineralogy, microstructure, and compressive strength development was studied. The Presence of CS-C in the raw mix resulted in the reduced temperature of clinkerization by about 50 °C. The quality of clinker prepared from the raw mix containing 3% CS-C and burned at 1400 °C was comparable to that of clinker prepared from the raw mix containing no CS-C and burned at 1450 °C. Gradual polymorphic modification of alite …

Carbon-Al Interface Effect On The Performance Of Ionic Liquid-Based Supercapacitor At 3 V And 65 OC, Zhen-Zhen Ye, Shu-Ting Zhang, Xin-Qi Chen, Jin Wang, Ying Jin, Chao-Jie Cui, Lei Zhang, Lu-Ming Qian, Gang Zhang, Wei-Zhong Qian

Journal of Electrochemistry

Ionic liquid (IL) electrolyte-based supercapacitors (SCs) have advantages of high operating voltage window, high energy density and nonflammability, as compared to conventional acetonitrile-based organic electrolyte SCs, and are typically suitable for the large-scale energy storage in the era of carbon neutrality full of renewable, but unstable electricity. However, current efforts were concentrated on the study with coin-cell type of IL-SCs, and less has been reported on the pouch type of IL-SCs for a long cycling time yet. To fabricate a reliable SC for the life time test or for the accelerated aging test under high temperature, one should concern the …

Application Of Artificial Intelligence To Lithium-Ion Battery Research And Development, Zhen-Wei Zhu, Jing-Yi Qiu, Li Wang, Gao-Ping Cao, Xiang-Ming He, Jing Wang, Hao Zhang

Journal of Electrochemistry

Lithium-ion batteries (LIBs) have become one of the best solutions to the energy storage issue in modern society. However, the battery materials and device development are both complex, and involve multivariable problems. Traditional trial-and-error approach, which relies on researchers to conduct experiments, has encountered bottlenecks in the improvement of the battery performance. Artificial intelligence (AI) is the most potential technology to deal with this issue due to its powerful high-speed and capabilities of processing massive data. In particular, the capability of machine learning (ML) algorithms in assessing multidimensional data variables and discovering patterns in the sets are expected to assist …

Advances On Composite Cathodes For Lithium-Sulfur Batteries, Xi-Yao Li, Chang-Xin Zhao, Bo-Quan Li, Jia-Qi Huang, Qiang Zhang

Journal of Electrochemistry

Lithium-sulfur (Li-S) batteries are deemed as high-promising next-generation energy storage technique due to their ultrahigh theoretical energy density, where the sulfur cathodes with high specific capacity guarantee the energy density advantage and directly determine the battery performances. After decades of exploration, the most promising sulfur cathodes are sulfur/carbon composite (S/C) cathodes and sulfurized polyacrylonitrile (SPAN) cathodes. In this manuscript, recent advances on S/C and SPAN cathodes in Li-S batteries are comprehensively reviewed. The electrochemical reaction circumstances on S/C and SPAN cathodes are firstly introduced and compared to reveal the working mechanisms of the two types of Li-S batteries. The S/C …

Multi-Electron Reaction-Boosted High Energy Density Batteries: Material And System Innovation, Rui-Qi Guo, Feng Wu, Xin-Ran Wang, Ying Bai, Chuan Wu

Journal of Electrochemistry

The continuous development of the global energy structure transformation has put forward higher demands upon the development of batteries. The improvements of the energy density have become one of the important indicators and hot topic for novel secondary batteries. The energy density of existing lithium-ion battery has encountered a bottleneck due to the limitations of material and systems. Herein, this paper introduces the concept and development of multi-electron reaction materials over the past twenty years. Guided by the multi-electron reaction, light weight electrode and multi-ion effect, current development strategies and future trends of high-energy-density batteries are highlighted from the perspective …

Preparation Of Highly-Cyclized Sulfurized Polyacrylonitrile For Lithium-Sulfur Batteries, Xuan Ji, Jia-Yu Wang, An-Bang Wang, Wei-Kun Wang, Ming Yao, Ya-Qin Huang

Journal of Electrochemistry

Sulfurized polyacrylonitrile (SPAN) is regarded as an attractive cathode candidate of lithium-sulfur (Li-S) batteries for its non-dissolution mechanism and effective alleviation of polysulfides shuttling issue in Li-S batteries, displaying high utilization of cathode active material, outstanding cycle stability and structural stability. However, the relation between cyclization degree and cycle stability of SPAN is still unveiled. In this work, SPAN-C-V composites were synthesized by co-introduction of CuSO₄ and zinc n-ethyl-n-phenyldithiocarbamate (ZDB) in the co-heating of sulfur and polyacrylonitrile. The co-introduction of CuSO₄ and ZDB reduced the cyclization reaction onset temperature of PAN while increased the C—C/C=C within SPAN-C-V, thus …

Investigating The Electrochemical Behavior Of Dihydropyrrolopyroles For Use As Anodically Coloring Electrochromes, Perry Skiouris, Ally Kisiel, Valentino Sorto, Julia Mauro, Graham Collier

Symposium of Student Scholars

Electrochromic materials have found widespread use in consumer electronics, energy saving windows, and military applications. They contain unique electronic properties allowing them to undergo a color change in a redox reaction. One classification of these molecules is known as anodically coloring electrochromes (ACEs). When in solution, these compounds are transmissive in the neutral (ground) state and absorb visible light upon oxidation, by the formation of a radical cation, thus making them colored. The focus of this study is the electronic transitions of this radical cation and how chemical modifications to the structures produce a variable color profile. To design prospective …

Perfect Polar Alignment Of Parallel Beloamphiphile Monolayers: Synthesis, Characterization, And Crystal Architectures Of Unsymmetrical Phenoxy-Substituted Acetophenone Azines, Harmeet Bhoday, Michael Lewis, Steven P. Kelley, Rainer Glaser

Chemistry Faculty Research & Creative Works

It remains a great challenge to achieve polar order in organic molecular crystals because anti-parallel alignment of side-by-side molecules is intrinsically preferred. We have addressed this problem with a rational design that focuses on the polar stacking of parallel beloamphiphile monolayers (PBAMs) with strong lateral quadrupole-quadrupole attractions. We employ arene-arene interactions as lateral synthons. The first successes were achieved with unsymmetrical donor (X), acceptor (Y) substituted acetophenone azines which form polar PBAMs with double T-contacts between the azines. Near-perfect alignment was achieved with the methoxy series of (MeO, Y)-azines with Y=Cl, Br, I. Here, we report on the synthesis, the …

Elucidation Of Active Site And Mechanism Of Metal Catalysts Supported In Nu-1000, Hafeera Shabbir

All Dissertations

Advances in extraction of shale oil and gas has increased the production of geographically stranded natural gas (primarily consisting of methane (C1) and ethane (C2)) that is burned on site. A potential utilization strategy for shale gas is to convert it into fuel range hydrocarbons by catalytic dehydrogenation followed by oligomerization by direct efficient catalysts. This work focuses on understanding metal cation catalysts supported on metal-organic framework (MOF) NU-1000 that will actively and selectively do this transformation under mild reaction conditions, while remaining stable to deactivation (via metal agglomeration or sintering). I built computational models validated by experimental methods to …

Synthesis And Electrochemical Characterization Of Alkali Metal Borides As Redox Active Anion Frameworks, Michael R. Shabetai

LSU New Orleans Theses and Dissertations

Redox activity in intercalation cathodes is commonly attributed to changes in oxidation states of transition metal ions. Recently, a growing body of evidence revealed that the redox activity of oxygen contributes to the capacity of some known cathodes. We focused on designing an oxygen free intercalation cathode with redox-active anions. In order to overcome the entropic driving force for the decomposition of a charged redox active anion cathode, we looked for chemistries with solid (no gases) possible decomposition products. Additionally, the involvement of anions in a network of covalent bonds with shared electrons was considered as a possible way for …

Visible Light-Assisted Deconstruction/Refunctionalization Of Strained And Unstrained N-Cycloalkylanilines, Elvis Duah Boateng

Graduate Theses and Dissertations

The exploitation of ring strain as a driving force to facilitate chemical reactions is a well-appreciated principle in organic chemistry. Of the strained carbocycles frequently explored in this respect, cyclopropane ring systems have drawn considerably more interest among synthetic chemists than their homolog, the cyclobutane ring systems, even though the strain energy of cyclobutane (26.7 kcal/mol) is similar to that of cyclopropane (27.5 kcal/mol). We have previously developed a [4+2] annulation reaction for the synthesis of aniline-substituted six-membered carbocycles under photoredox catalysis via the oxidative cleavage of N-cyclobutylanilines. The key reaction involved in this method is a ring-opening process of …

A Study On Interactions Between Metal-Organic Frameworks And Biological Materials, Josh Phipps

Graduate Theses and Dissertations

Metal-organic frameworks or MOFs are an extremely useful tool in many areas of applications. Their popularity in recent years has arisen from their high efficiency in catalytic chemical reactions. This is made possible due to their porous interior and the ability of the MOFs components to be functionalized. These same traits make MOFs excellent for use in protein encapsulation or immobilization and have the potential to become excellent drug carriers. Their development in this utilization has been limited dramatically compared to MOFs chemical applications. This is due in part to the nature of biological processes taking longer to study, but …

Efficient Interface Enabled By Nano-Hydroxyapatite@Porous Carbon For Lithium-Sulfur Batteries, Jia-Yu Wang, Xue-Feng Tong, Qi-Fan Peng, Yue-Peng Guan, Wei-Kun Wang, An-Bang Wang, Nai-Qiang Liu, Ya-Qin Huang

Journal of Electrochemistry

The dissolution and “shuttle effect” of lithium polysulfides (LiPSs) hinder the application of lithium-sulfur (Li-S) batteries. To solve those problems, inspired by natural materials, a nano-hydroxyapatite@porous carbon derived from chicken cartilage (nano-HA@CCPC) was fabricated by employing a simple pre-carbonization and carbonization method, and applied in Li-S batteries. The nano-HA@CCPC would provide a reactive interface that allows efficient LiPSs reduction. With a strong affinity for LiPSs and an excellent electronic conductive path for converting LiPSs, the shuttle effect of LiPSs was confined and the redox kinetics of LiPSs was substantially enhanced. Li-S batteries employing nano-HA@CCPC-modified separators exhibited long cycle life and …

Which Factor Dominates Battery Performance: Metal Ion Solvation Structure-Derived Interfacial Behavior Or Solid Electrolyte Interphase Layer?, Hao-Ran Cheng, Zheng Ma, Ying-Jun Guo, Chun-Sheng Sun, Qian Li, Jun Ming

Journal of Electrochemistry

Solid-electrolyte interphase (SEI) layer formed on the electrode by electrolyte decomposition has been considered to be one of the most important factors affecting the battery performance. We discover that the metal ion solvation structure can also influence the performance, particularly, it can elucidate many phenomena that the SEI cannot. In this review, we summarize the importance of the metal ion solvation structure and the derived metal ion de-solvation behaviors, by which we can build an interfacial model to show the relationship between the interfacial behavior and electrode performance, and then apply to different electrode and battery systems. We emphasize the …

Advances And Atomistic Insights Of Electrolytes For Lithium-Ion Batteries And Beyond, Tingzheng Hou, Xiang Chen, Lu Jiang, Cheng Tang

Journal of Electrochemistry

Electrolytes and the associated electrode-electrolyte interfaces are crucial for the development and application of high-capacity energy storage systems. Specifically, a variety of electrolyte properties, ranging from mechanical (compressibility, viscosity), thermal (heat conductivity and capacity), to chemical (solubility, activity, reactivity), transport, and electrochemical (interfacial and interphasial), are correlated to the performance of the resultant full energy storage device. In order to facilitate the operation of novel electrode materials, extensive experimental efforts have been devoted to improving these electrolyte properties by tuning the physical design and/or chemical composition. Meanwhile, the recent development of theoretical modeling methods is providing atomistic understandings of the …

Review On Oxygen-Free Vanadium-Based Cathodes For Aqueous Zinc-Ion Batteries, Xiao-Ru Yun, Yu-Fang Chen, Pei-Tao Xiao, Chun-Man Zheng

Journal of Electrochemistry

Aqueous zinc-ion batteries (AZIBs) are considered as one of the most promising next-generation electrochemical energy storage systems owing to their high-power density, environmental benign, intrinsic safety, and the low cost of the abundant zinc resources. However, their further development is still plagued by the inferior electrochemical performance of cathode materials. Though extensive research has been conducted to investigate various cathode materials (including manganese oxides, vanadium oxides, Prussian blues analogy, and organic materials), design of high-performance cathodes with satisfying capacity and long-term cycling stability still faces great challenges. Oxygen-free vanadium-based compounds, owing to their better conductivity, larger interlayer spacing, lower ion …

Oligomeric Ionic Liquids: Bulk, Interface And Electrochemical Application In Energy Storage, Dan-Dan Li, Xiang-Yu Ji, Ming Chen, Yan-Ru Yang, Xiao-Dong Wang, Guang Feng

Journal of Electrochemistry

Over recent years, oligomer ionic liquids (OILs), a novel class of ionic liquids, are becoming preferential electrolytes for high-performance energy-storage devices, such as supercapacitors with enhanced energy density and non-flammable lithium-ion batteries (LIBs). Herein, structures, properties, and their associations of the up-to-the-minute formulated OILs are systematically summarized and elaborately interpreted, especially for dicationic ionic liquids and tricationic ionic liquids. The physicochemical and electrochemical properties of OIL-based electrolytes are presented and analyzed, which are vitally important for supercapacitors and LIBs. Subsequently, the applications of OILs as electrolytes for supercapacitors and LIBs are summarized, with the comparisons of the energy-storage mechanisms and …

Insight Into The Effects Of Cation Disorder And Surface Chemical Residues On The Initial Coulombic Efficiency Of Layered Oxide Cathode, Jin-Li Liu, Han-Feng Wu, Zhi-Bei Liu, Ying-Qiang Wu, Li Wang, Feng-Li Bei, Xiang-Ming He

Journal of Electrochemistry

Lithium layered oxide LiNi_0.6Co_0.2Mn_0.2O₂ (NCM622) is one of the most promising cathode materials in high-energy lithium-ion batteries for electric vehicles. However, one drawback for NCM622 is that its initial coulombic efficiency (ICE) is only about 87%, which is at least 6% lower than that of LiCoO₂ or LiFePO₄. In this work, we investigated the effects of surface chemical residues (e.g., LiOH and Li₂CO₃) and Li/Ni cation disorder resulted during the sintering on the ICE. We found that the ICE of the as-prepared samples could be boosted …

Ferrocenium Salt Aided Substitution Reactions And Synthesis Of Glycosylated Curcumin Derivatives, Deva Saroja Talasila

Dissertations

Organic synthesis has been significantly advanced with the employment of transition metal complexes. The discovery of transition metal catalysts provided the synthetic community with powerful tools for accelerating reactions and making them more selective and efficient. Many chemical reactions do not happen without a catalyst.

Iron-based catalysts have several advantages for the chemical industry because it is a non-toxic and ecologically friendly metal. Our group previously found that ferrocenium cations with a 3+ oxidation state of iron-catalyzed propargylic substitution reactions at low temperatures. The sandwich structure of ferrocenes allows substituents to be introduced on the cyclopentadienyl rings, which allows for …

Electrochemical Syntheses Of Nanomaterials And Small Molecules For Electrolytic Hydrogen Production, Jia-Qi Wei, Xiao-Dong Chen, Shu-Zhou Li

Journal of Electrochemistry

Hydrogen is a clean, efficient, renewable energy resource and the most promising alternative to fossil fuels for future carbon-neutral energy supply. Therefore, sustainable hydrogen production is highly attractive and urgently demanded, especially via water electrolysis that has clean, abundant precursors and zero emission. However, current water electrolysis is hindered by the sluggish kinetics and low cost/energy efficiency of both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). In this regard, electrochemical synthesis offers prospects to raise the efficiency and benefit of water electrolysis by fabricating advanced electrocatalysts and providing more efficient/value-adding co-electrolysis alternatives. It is an eco-friendly and facile …

Catalytic Effect Of Disordered Ru-O Configurations For Electrochemical Hydrogen Evolution, Xue Sun, Ya-Jie Song, Ren-Long Li, Jia-Jun Wang

Journal of Electrochemistry

Phase engineering is considered as an effective method for modulating the electronic structure and catalytic activity of catalysts. The disordered conformation of amorphous materials allows flexible reforming of the surface electronic structure, showing their attractiveness as catalysts for hydrogen evolution reaction (HER). Herein, we designed and developed an amorphous ruthenium dioxide (a-RuO₂) catalyst with a disordered Ru-O configuration. The conformational relationship between Ru-O ordering and HER performance is established by combining advanced electron microscopic techniques with detailed electrochemical tests. Specifically, the disordered Ru-O coordination significantly enhanced the HER catalytic activity in both acidic and alkaline media, ultimately leading …

Alkaline Water Electrolysis For Efficient Hydrogen Production, Wen-Fu Xie, Ming-Fei Shao

Journal of Electrochemistry

Hydrogen production from water electrolysis is a sustainable and environmentally benign strategy in comparison with fossil fuel-based hydrogen. However, this promising technique suffers from the high energy consumption and unsatisfactory cost due to the sluggish kinetics of both half reaction and inferior stability of electrocatalysts. To address this challenge, herein, we present a timely and comprehensive review on advances in alkaline water electrolysis that is already commercialized for large scale hydrogen production. The design principles and strategies with aiming to promote the performance of hydrogen generation are discussed from the view of electrocatalyst, electrode, reaction and system. The challenges and …

Alkaline Seawater Electrolysis At Industrial Level:Recent Progress And Perspective, Tao Zhang, Yi-Pu Liu, Qi-Tong Ye, Hong-Jin Fan

Journal of Electrochemistry

Industrial hydrogen generation through water splitting, powered by renewable energy such as solar, wind and marine, paves a potential way for energy and environment sustainability. However, state-of-the-art electrolysis using high purity water as hydrogen source at an industrial level would bring about crisis of freshwater resource. Seawater splitting provides a practical path to solve potable water shortage, but still faces great challenges for large-scale industrial operation. Here we summarize recent developments in seawater splitting, covering general mechanisms, design criteria for electrodes, and industrial electrolyzer for direct seawater splitting. Multi-objective optimization methods to address the key challenges of active sites, reaction …

A Self-Supported Ru-Cu3P Catalyst Toward Alkaline Hydrogen Evolution, Zi-Xuan Wan, Chao-Hui Wang, Xiong-Wu Kang

Journal of Electrochemistry

Transition metal phosphide (TMP) is a kind of effective catalysts toward hydrogen evolution reaction (HER) in alkaline electrolytes. However, the performance of TMP catalysts is strongly limited by water splitting. In this work, we developed a method to prepare a copper foam (CF) supported Ru-doped Cu₃P catalyst (Ru-Cu₃P/CF) by a consecutive growth of Cu(OH)₂ nanoarrays, soaking in RuCl₃ solution and phosphorization. A large surface area was obtained by the self-supported catalysts with the appropriative Ru doping. As an excellent HER catalyst, it exhibited a low overpotential of 95.6 mV at a current density of …

Synthesis Of Carbon Nanohoops And Macrocycles Via Alkyne Metathesis, Xin Zhou

LSU Doctoral Dissertations

Cycloparaphenyleneacetylene (CPPA) and cycloparaphenylene (CPP) are called carbon nanohoops; they are fully conjugated macrocycles with radially oriented aromatic groups. Though many syntheses of CPPA and CPP were reported, in the macrocyclization step, the yields were usually not satisfying, as the reactions were irreversible. Our group utilizes alkyne metathesis to address this problem. Chapter 1 provides backgrounds and an introduction to the carbon nanohoops and alkyne metathesis.

Chapter 2 details the synthesis of the [3]CPP⁴A and [3]CPP⁵A, with good macrocyclization yields via alkyne metathesis. This study showed the error-correction ability of alkyne metathesis, especially with nonsymmetric substrates. …

Converting Hydrazone-Based Photoswitches Into Functional Materials, Sirun Yang

Dartmouth College Ph.D Dissertations

The development of new classes of molecular switches with enhanced performance and brand-new functionalities enables practitioners to push the frontiers of adaptive materials. In the realm of photoswitches, the bistability of hydrazones (i.e., molecules that incorporate the C=N-NH functional group) allows for the kinetic trapping of polymer and supramolecular assemblies resulting in multistate actuation and emergent phenomena that are not tractable with other photoswitches. This property has transformed hydrazone photoswitches into powerful tools that can be used in understanding fundamental molecular interactions and how to apply them in modulating the physicochemical properties of materials.

Progressing from disordered to …

Preface To Special Issue On Water Electrolysis For Hydrogen Production, Li Li, Jin-Song Hu, Zi-Dong Wei

Journal of Electrochemistry

No abstract provided.

Recent Development Of Low Iridium Electrocatalysts Toward Efficient Water Oxidation, Jing Ni, Zhao-Ping Shi, Xian Wang, Yi-Bo Wang, Hong-Xiang Wu, Chang-Peng Liu, Jun-Jie Ge, Wei Xing

Journal of Electrochemistry

Developing high-performance and low-cost electrocatalysts for oxygen evolution reaction (OER) is the key to implementing polymer electrolyte membrane water electrolyzer (PEMWE) for hydrogen production. To date, iridium (Ir) is the state-of-the-art OER catalyst, but still suffers from the insufficient activity and scarce earth abundance, which results in high cost both in stack and electricity. Design low-Ir catalysts with enhanced activity and stability that can match the requirements of high current and long-term operation in PEMWE is thus highly desired, which necessitate a deep understanding of acidic OER mechanisms, unique insights of material design strategies, and reliable performance evaluation norm, especially …

The Rapid Preparation Of Efficient Mofeco-Based Bifunctional Electrocatalysts Via Joule Heating For Overall Water Splitting, Ao Zhou, Wei-Jian Guo, Yue-Qing Wang, Jin-Tao Zhang

Journal of Electrochemistry

Water electrolysis is an available way to obtain green hydrogen. The development of highly efficient electrocatalysts is a current research hotspot for water splitting, but it remains challenging. Herein, we demonstrate the synthesis of a robust bifunctional multi-metal electrocatalysts toward water splitting via the rapid Joule-heating conversion of metal precursors. The composition and morphology were well regulated via altering the ratio of metal precursors. In particular, the trimetal MoC/FeO/CoO/carbon cloth (CC) electrode revealed the outstanding bifunctional electrocatalytic performance due to the unique composition and large electrochemical active surface area. Typically, the MoC/FeO/CoO/CC catalyst needed low overpotentials of 121 and 268 …

Perovskite-Type Water Oxidation Electrocatalysts, Xiao Liang, Ke-Xin Zhang, Yu-Cheng Shen, Ke Sun, Lei Shi, Hui Chen, Ke-Yan Zheng, Xiao-Xin Zou

Journal of Electrochemistry

The development of energy conversion/storage technologies can achieve the reliable and stable renewable energy supply, and bring us a sustainable future. As the core half-reaction of many energy-related systems, water oxidation is the bottleneck due to its sluggish kinetics of the four-concerted proton-electron transfer (CPET) process. This necessitates the exploitation of low cost, highly active and stable water oxidation electrocatalysts. Perovskite-type oxides possess diverse crystal structures, flexible compositions and unique electronic properties, enabling them ideal material platform for the optimization of catalytic performance. In this review, we provide a comprehensive summary for the crystal structures, electronic structures and synthetic methods …