bluuebunny/crossref_metadata_2025 huggingface dataset:
Electrocatalytic Conversion of CH4 to High Value-Added Liquid Fuel over Binary Metal Oxide Tandem Catalysts
Authors: Xu Nengneng , Wang Yudong , He Zizhou , Zhou Xiao-Dong
Published: August 2024

As the main component (> 85%) of combustible ice and shale gas, methane (CH4), plays a significant role in the greenhouse effect.(1) Although CH4 was widely used to synthesize high value-added Cx oxygenates via indirect industrial reforming with high-energy consumption. The accurate control of oxidation degree in CH4 conversion remains a great challenge.(2) Therefore, it is difficult to achieve high conversion rate and high selectivity at the same time. The convenience and reliability of the control of reaction potential, as one of the advantages of electrocatalysis technology, can effectively address the above problems.(1, 3) Electrochemical technologies of CH4-to-Cx oxygenates are regarded as one of the most attractive pathways to produce bulk industrial liquid fuels.(4) Especially in the premise of clean energy as an energy source, the electrochemical conversion of methane demonstrates very advantageous market potential. In this work, we prepared a ZrO2 modified FeOx binary metal oxides tandem catalyst to accelerate partial oxidation of CH4 under ambient condition. With CO3
2- as an oxidant, ZrO2@FeOx tandem catalyst shows remarkable CH4 conversion performance with large current density gap (13.65 mA cm-2) and long-term electrochemical stability (negligible attenuation (8 %) after 48 hours) in three-electrodes cell. In addition, in a flow reactor, ZrO2@FeOx-based electrode also exhibits a highly stable operating lifespan over 72 hours at a large current density 50 mA cm-2 and achieve a feasible CH4-liqid fuel conversion with high total faradaic efficiency.

References

F. Liu, Y. Yan, G. Chen and D. Wang, Green Chemistry, 26, 655 (2024).

S. Yuan, Y. Li, J. Peng, Y. M. Questell-Santiago, K. Akkiraju, L. Giordano, D. J. Zheng, S. Bagi, Y. Román-Leshkov and Y. Shao-Horn, Advanced Energy Materials, 10, 2002154 (2020).

M. R. A. Kishore, S. Lee and J. S. Yoo, Adv Sci (Weinh), 10, e2301912 (2023).

L. Fu, R. Zhang, J. Yang, J. Shi, H. Y. Jiang and J. Tang, Advanced Energy Materials, 13 (2023).
Electrosynthesis for the Development of Selective Organic Reactions
Authors: Malapit Christian
Published: August 2024

The development of efficient and selective reactions play a vital role in chemical synthesis and drug discovery, serving as crucial drivers for advancements in these fields. Electrosynthesis has emerged as a versatile and powerful tool within organic chemistry, enabling the exploration and development of new organic reactions. This state-of-the-art technique harnesses the power of electricity to propel chemical transformations, paving the way for synthetic chemists to create intricate organic molecules. In this presentation, we will showcase notable discoveries from the Malapit Lab, highlighting the innovative application of electrochemistry in the exploration of novel and transformative reactions. Among these groundbreaking findings are a site-selective C–H functionalization reaction and the utilization of organoboron reagents to generate diverse carbon-heteroatom products through radical intermediates. These reactions hold promise for the late-stage functionalization of numerous biologically active compounds, presenting exciting opportunities for drug development and synthesis.
Intrinsically Disordered Proteins on Au Surfaces
Authors: Martic Sanela
Published: August 2024

Intrinsically disordered protein Tau, is a neuronal protein and one of the biomarkers of neurodegenerative diseases. Tau protein undergoes conformational changes, post-translational modifications, and aggregation, and is a viable drug target. We reported on using electrochemical impedance spectroscopy and cyclic voltammetry to study various aspects of tau protein biochemistry on Au surfaces (1-2). By immobilizing the tau protein onto the Au surface, the interactions with other proteins, ligands, and enzymes were investigated. Data show that the electrochemical methods are viable biophysical tools that provide new biochemical information which is not always possible with traditional biochemical methods.

References

A) Carlin, N., Martic-Milne, S. (2018). Anti-tau antibodies based electrochemical sensor for detection of tau protein. J. Electrochem. Soc.165: G3018-G3025. B) Jahshan, A., Esteves, J.O.V., Martic-Milne, S. (2016). Evaluation of ferritin and transferrin binding to tau protein. J. Inorg. Biochem. 162: 127-134.

Trzeciakiewicz, H., Esteves, J.O.V., Carlin, N., Martic, S. (2015). Electrochemistry of heparin binding to tau protein on Au surfaces. Electrochim. Acta. 162: 24-30.
Packaging and pH Effects on Meat Discoloration through Electrochemistry
Authors: Ayabadda Devage Sachinthani , Kasthuri Dias Sandun Bogahawaththa Bogahawaththa , Bhandari Silan , Avery Athena , Kumar Rishav , Ramanathan Ranjith , Krishnan Sadagopan
Published: August 2024

Myoglobin is the sarcoplasmic heme protein that determines the color of the meat. The oxidation state of myoglobin results in different forms of myoglobin, such as deoxy-, oxy-, and metmyoglobin. As the deviation from the bright red color of beef affects consumers' purchase decisions, meat packaging is done to retain the meat color and delay spoilage. In these studies, UV-spectrophotometric analysis is combined with the electrochemical method. Meat packaged under different conditions was considered. Two packaging conditions, vacuum and polyvinyl chloride, were compared with the normal unpackaged sarcoplasmic beef sample. Electrochemical regions of both positive and negative potential were diagnosed for sensory peaks where the data of vacuum packaging implied more color stability. To assess the effect of pH on meat discoloration, pH conditions of the physiological state (pH 7.4) and post-mortem meat (pH 5.6) were mainly considered. The rate of meat discoloration was higher at pH 5.6 than at pH 7.4. Electrochemical insights with regard to various packaging effects on meat discoloration will be discussed further.
Molecular Simulations Study of the Ionic Adsorption on Oscillating Carbon Electrodes
Authors: Gaudy Nicolas , Salanne Mathieu , Merlet Céline
Published: August 2024

Molecular dynamics simulations are a method of choice to study, at microscopic scales, the adsorption of electrolyte ions onto the electrodes of capacitive storage systems such as supercapacitors1.

Here, we use all-atom molecular dynamics simulations to model a pure ionic liquid electrolyte ([EMIM][TFSI], 1-ethyl-3-methylimidazolium trifluoromethanesulfonylimide) in contact with graphite electrodes (Figure:
Supercapacitor composed of graphite electrodes (in light blue) in contact with a pure ionic liquid electrolyte ([EMIM][TFSI], atoms colored according to the atom type. The arrows illustrate the oscillations of electrodes used to probe the influence of such a motion on the interfacial liquid.)

When applying a potential difference between the two carbon electrodes, a migration of counter ions is observed, ultimately leading to a compensation of the charges carried by the electrode atoms. The adsorption dynamics depend on several parameters (electrostatic interactions, coordination number, viscosity of the electrolyte, size of the ions etc.) and influence the power of these capacitive systems2. In order to improve the performance of supercapacitors, it is then important to describe and understand interfacial properties at a molecular scale.

Experimentally, an Electrochemical Quartz Crystal Microbalance (EQCM) can be used to study ion flow on top of the electrode. The frequency variations recorded by the EQCM are linked to variations in the mass adsorbed on the quartz surface, thus making it possible to study the dynamics of ion adsorption during the charge of a supercapacitor.3

However, variations in quartz frequency can influence the stability of the electrode-electrolyte interface, thus modifying ionic interactions and adsorption dynamics at the electrode surface4.

Here, thanks to molecular simulations, we have access to the adsorption rate of ions, to their re-orientation, to the variation of charge of the electrode atoms during adsorption etc. This allows us to study in detail the mechanisms governing the electrolyte-electrode interface during the charging of supercapacitors as part of EQCM. And study the extent to which perturbations caused by quartz oscillations in the ionic liquid affect electrode-electrolyte interfacial properties.

References

1 K. Xu, H. Shao, Z. Lin, C. Merlet, G. Feng, et al.. ENERGY & ENVIRONMENTAL MATERIALS, 3, 235-246 (2020)

2C. Péan, B. Rotenberg, P. Simon, M. Salanne, ELECTROCHIM. ACTA, 206, 504-512 (2016)

3Y-C. Wu, J. Ye, G. Jiang, K. Ni, N. Shu, P-L. Taberna, Y. Zhu, P. Simon, ANGEW. CHEM. INT. ED., 60, 13317-13322 (2021)

4Nikolai V. Priezjev, MICROFLUIDICS AND NANOFLUIDICS, 14, 225-233 (2013)

Figure 1
An Electrochemical Phase Field Model Applied to Molten Salt Dealloying Corrosion of Ni-Alloys
Authors: Bieberdorf Nathan , Bognarova Xueyang , Capolungo Laurent , Asta Mark
Published: August 2024

Metal alloys in contact with molten salts are known to corrode via a dealloying process, wherein the less-noble alloy elements (e.g. Cr) are selectively oxidized and dissolved, leaving behind a corroded structure that is enriched in the more-noble elements (e.g. Ni). In some cases, this can lead to molten salt infiltration into the alloy through discrete channels along specific microstructural features (e.g. grain boundaries). However, in other cases the dealloying process promotes a more full-scale attack of the alloy, generating a fine-scale ligament structure. This process can severely degrade the alloy’s structural integrity, which limits the practicality of these material systems in otherwise promising applications (e.g. molten salt-cooled power reactors).

The thermokinetic conditions for dealloying corrosion depend on the salt chemistry and the metal microstructure, which together inform the reaction process occurring at their interface. The salt chemistry and oxidant content set the electrochemical potential for selective oxidation of the less-noble elements. The associated oxidation rate is expected to depend on the presence of an interfacial structure (e.g. double layer) and also on the transport rates of reactants towards the interface (e.g. species diffusion in the metal and oxidizer transport in the salt) and reaction products away from the interface (cation transport in the salt). The corrosion rate and morphology will also depend strongly on the rate of transport laterally along the metal-salt interface, since the reorganization of the more-noble species (Ni) towards ligament formation facilitates the attack of the alloy by the corrosive agent. It has been hypothesized that molten salts enhance this rate of solute diffusion along the metal interface.

In this work, we propose an electrochemical phase field model to predict the microstructural evolution of model Ni-alloys undergoing dealloying corrosion in molten fluoride salts. The model incorporates metal oxidation and dissolution via experimentally determined redox potentials and activity coefficients for metal species in the molten salt. We show that the corrosion rate and development of pores is strongly dependent on solute transport rates within the metal and also along their solid-liquid interface. In particular, we reveal a mechanism in which grain boundaries couple with the solid-liquid corrosion front to promote rapid dealloying and molten salt attack. Oxidant content in the salt and double-layer formation at the interface are discussed for their roles in setting the electrochemical potential and reaction rate at the metal-salt interface. Finally, we discuss how the model leverages insights from atomistic modeling and highlight key knowledge gaps in the mesoscale modeling of electrochemical molten salt corrosion.
Pouch Cell Case Laminate with Integrated Thermal Management Topologies
Authors: Robert Brian Joseph , Lee Andre , Johnson Tyler Nathaniel
Published: August 2024

With increased adoption of pouch-type battery cells in electrified vehicles there are evolving challenges for cell-to-array battery design. Trends of higher capacity and energy density as well as demands for reduced cost inspire integration opportunities of traditionally discrete functional components. Focusing on how battery cell active materials are packaged, specifically the polymer/aluminum laminate case, the formation of thermal transfer features at the pouch case surface would increase heat transfer efficiency and simplify the battery system by reducing components, weight, and volume. Designed topologies, from localized pin fins and straight channels to complex flow fields (Table 1), have been demonstrated at the pouch case laminate enabling a new design space at the cell level. This presentation will explore prototype designs, fabrication methods, and improvement areas for this technology.

Table 1 - Extrusion roller press designs and demonstrated prototypes for variable spaced channel arrays, pin fin topologies, and flow field patterns

Figure 1
(Invited) LIOVIX® Technology: Lithium Metal Anode Manufacturing at Scale
Authors: Yakovleva Marina , Fitch Brian , Xia Jian
Published: August 2024

Next generation battery technologies critically depend on giga factory scale for production of the battery components, such as thin lithium anodes. The core of Livent innovative and sustainable solution is LIOVIX®, proprietary Printable Lithium Formulation. The ability to print lithium metal anodes opens the pathway for the various ranges of anode’s width and thickness and allows cell manufacturer to easier change cell design and format to meet application requirements.
Integrating Polymer Electrolytes-Based Thick Composite Cathodes in All-Polymer Solid-State Lithium Metal Batteries
Authors: Ock Jiyoung , Owensby Kyra D'Yana , Chen Xi Chelsea , Sahore Ritu
Published: August 2024

High energy density solid-state batteries require high areal loading composite cathodes (>4 mAh/cm2). However, increasing the cathode loading or thickness can introduce additional challenges apart from the expected rate capability limitations, which are much less pronounced in low loading or thin composite cathodes. These include greater volume changes during cycling at the cell level, which can introduce stresses at the various interfaces. While there are many successful reports showing long-term stable cycling of high loading composite cathode in all-inorganic solid-state cells, these cells are typically cycled under high pressures (>10 MPa), which may be impractical to commercialize. Such high pressures can alleviate the interfacial contact loss issues generated due to volume changes during cycling. Polymer electrolytes are non-rigid and can potentially accommodate strains to maintain contact at the interfaces during cycling, given sufficient adhesion. In this work, we will show some of the design strategies that were implemented to alleviate the contact loss issue at the polymer electrolyte separator/composite cathode interface in order to achieve stable cycling with thick polymer electrolyte-based composite cathodes in coil-cell configuration. Nickel-rich NMC (LiNixMnyCozO2) cathodes (NMC811 or 622) were used as the active materials. Since polymer electrolytes are known to be unstable with high voltage cathodes such as NMCs, the contribution of oxidative instability to the overall capacity decay will also be discussed by comparing two polymer electrolytes with different oxidative stability (a PEO-based dual-ion polymer electrolyte, and a single-ion polymer electrolyte).

This research was sponsored by the U.S. Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy for the Vehicle Technologies Office’s Advanced Battery Materials Research Program (Simon Thompson, Program Manager). A part of this research was sponsored by the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory (ORNL), managed by UT-Battelle, LLC for the U.S. Department of Energy under Contract No. DE-AC05-00OR22725. The SEM in this work was performed and supported at the Center for Nanophase Materials Sciences in Oak Ridge National Lab, a DOE Office of Science user facility.
Hydrogen Evolution Atomic Cluster Catalysts-Decorated Hierarchical Nanoporous Zinc for on-Demand Hydrogen Generation By Metal Hydrolysis
Authors: Kubota Jo , Liu Jiaxin , Detsi Eric
Published: August 2024

In recent years, there has been an increasing interest in nanoporous metals due to their wide range of applications, including catalysis, electrocatalysis, energy storage, actuation, and plasmonics. However, considerable attention has been given to precious nanoporous metals such as nanoporous Au, Pd, Pt, Ag, and Cu due to their low chemical reactivity, which makes them relatively easy to synthesize and characterize. Less precious nanoporous metals such as nanoporous Zn, Al, and Mg have been rarely fabricated and characterized because of their relatively high chemical reactivity 1. In this talk, I will present a novel, highly scalable approach to making hierarchical nanoporous zinc (NP-Zn) decorated with atomic clusters of hydrogen evolution catalysts for on-demand hydrogen generation by metal hydrolysis. Our approach involves selective etching in combination with galvanic replacement reactions. The conventional selective etching method requires several days to create a monolithic piece of NP-Zn 2. Our approach creates the same amount of hierarchical NP-Zn in less than 5 minutes, instead of several days. In our work, we used focused ion beam/scanning electron microscopy techniques to reveal the internal nanoscale morphology of the hierarchical NP-Zn, and small-angle X-ray scattering to analyze the pore size distribution. In general, when NP-Zn is used for hydrogen generation by metal hydrolysis, the hydrogen generation yield is low, typically around 20%. This is because zinc is naturally a poor hydrogen evolution material. Our process overcomes this issue by creating NP-Zn with its interface decorated with clusters of hydrogen evolution catalysts, which enables hydrogen generation yield exceeding 90% depending on the catalyst loading.

References

(1) Fu, J.; Welborn, S. S.; Detsi, E. Dealloyed Air- and Water-Sensitive Nanoporous Metals and Metalloids for Emerging Energy Applications. ACS Appl. Energy Mater.
2022, 5 (6), 6516–6544. https://doi.org/10.1021/acsaem.2c00405.

(2) Fu, J.; Deng, Z.; Lee, T.; Corsi, J. S.; Wang, Z.; Zhang, D.; Detsi, E. pH-Controlled Dealloying Route to Hierarchical Bulk Nanoporous Zn Derived from Metastable Alloy for Hydrogen Generation by Hydrolysis of Zn in Neutral Water. ACS Appl. Energy Mater.
2018, 1 (7), 3198–3205. https://doi.org/10.1021/acsaem.8b00419.
(Sensor Division Early Career Award) Portable Diagnostics for Cancer Management at Printed Strips
Authors: Cinti Stefano
Published: August 2024

Point-of-care testing (PoC) is revolutionizing the healthcare sector improving patient care in daily hospital practice and allowing reaching even remote areas. In the frame of cancer management, the design and validation of PoC enabling the non-invasive, rapid detection of cancer markers is urgently required to implement liquid biopsy. However, despite substantial advances in sensing technologies, the development, preparation, and use of self-testing devices is still confined to specialist laboratories and users. Decentralized analytical devices will enormously impact daily lives, enabling people to analyze diverse clinical, environmental, and food samples, evaluate them and make predictions to improve quality of life, particularly in remote, resource-scarce areas. In recent years, paper-based analytical tools have attracted a great deal of attention; the well-known properties of paper, such as abundance, affordability, lightness, and biodegradability, combined with features of printed electrochemical sensors, have enabled the development of sustainable devices that drive (bio)sensors beyond the state of the art. Their blindness toward colored/turbid matrices (i.e., blood, soil), their portability, and the capacity of paper to autonomously filter/purge/react with target species make such devices powerful in establishing point-of-need tools for use by non-specialists. Depending on analytical requisites, different types of paper (filter, office) and configurations (1D, 2D, 3D) can be adopted. Focusing on stable blood-based markers with high-specificity, such as miRNAs, is of crucial importance. A wide overview regarding application ranging from DNA to miRNA detection will be provided, with the aim in showing the potentialities of portable electrochemical biosensors for improving society involvement in monitoring circulating nucleic acids associated to diverse conditions, i.e. cancer, Alzheimer’s disease, HIV.
(Invited) Recent Progress in Functional Nanomaterials for Biosensing and Theranostics
Authors: Lin Yuehe
Published: August 2024

In this talk, I will present an overview of our pioneering research in functional nanomaterials for biosensing and theranostics. Our work primarily focuses on novel materials such as protein cages, peptoids, single-atom nanozymes, and nanoflowers, and their applications in the field of biosensing and theranostics.

Building on my extensive background in developing materials and systems for biosensors, including immunosensors and microfluidic devices, we have explored the development of various smartphone-based biosensors. These biosensors are primarily based on DNA assays and immunoassays for point-of-care diagnostics, significantly enhancing the detection of disease biomarkers. Our research utilizes nanomaterials loaded with optical or electroactive signal molecules as amplification tags, dramatically improving the sensitivity in detecting disease biomarkers and food pathogens.

An exciting frontier in our research is the application of nano-peptoids in cell imaging, single-particle tracking, and cancer theranostics. The unique properties of nano-peptoids, including their biocompatibility and the ability for precise control over interactions, have opened new avenues in biomedicine and healthcare. These advancements hold promise for groundbreaking applications, particularly in enhancing the efficacy and precision of cancer diagnostics and treatment.

Moreover, the integration of 3D printing technology has enabled us to fabricate compact and efficient devices, a testament to our commitment to innovation in biosensor technology.

Throughout this talk, we will delve into the intricate details of these innovations, discussing their implications for the future of biosensing and theranostics.
A Novel Cerium Oxide/Gold/Carbon Nanocomposite-Based Electrochemical Sensor for Detecting Hydroxyl Radicals
Authors: Ghaedamini Hamidreza , Alba-Rubio Ana , Kim Dong-Shik
Published: August 2024

Hydroxyl radicals (•OH), a type of reactive oxygen species (ROS), play a crucial role in maintaining the normal physiological processes of human cells. Nevertheless, an excessive accumulation of these radicals may perturb cellular mechanisms, so triggering the onset of severe diseases, including cancer, neurological disorders, and heart disease. The detection of •OH is thus of utmost importance in the early diagnosis of these disorders. The combination of an electrochemical methodology with a recognition system is considered as a promising approach for the detection of •OH. This is primarily due to its capacity to provide fast and direct readings without the need for any preliminary sample preparation. This study presents the development of a new electrochemical sensor for the detection of •OH. The sensor was developed by modifying a screen-printed carbon electrode (SPCE) with a nanocomposite consisting of cerium oxide nanoclusters (CeOx), gold nanoparticles (AuNPs), and a highly conductive carbon. The synthesis of AuNPs supported by carbon was carried out using a deposition-precipitation process. Subsequently, the meticulous deposition of CeOx nanoclusters onto the AuNPs was achieved by the use of surface organometallic chemistry (SOMC). Energy dispersive X-ray spectroscopy (EDS) and transmission electron microscopy (TEM) were applied to assess the distribution of AuNPs on the carbon substrate and their subsequent embellishment with CeOx nanoclusters. The actual loadings of Ce and Au present in the nanocomposite were measured using inductively coupled plasma optical emission spectroscopy (ICP-OES). Cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) were employed to analyze the electrochemical responses resulting from the interaction of the CeOx-Au/Carbon nanocomposite with •OH. The CV results demonstrated that the proposed sensor exhibited the capability to effectively identify the presence of •OH in the Fenton reaction, with a notably low limit of detection of 58 µM. The sensor demonstrated a linear correlation between the current response and the concentration of •OH, within the range of 0.05 to 5 mM. Compared to a sensor modified with CeOx/Carbon, the CeOx-Au/Carbon-modified sensor exhibited enhanced electrochemical performance, as demonstrated by an increased current response and a reduced peak potential difference when detecting •OH radicals. Furthermore, the EIS studies showed that the sensor could distinguish •OH from other comparable ROS, such as hydrogen peroxide (H2O2).
Disposable Carbon Electrochemical Sensor Modified with Gold Nanoparticles for Creatinine Detection
Authors: Azzi Deborah , Silva Luiz , Neumann Amanda , Gatti Alexandre , Janegitz Bruno
Published: August 2024

The social and economic impact of Chronic Kidney Disease on global health systems is devastating. It is estimated that annual spending on the treatment of Chronic Kidney Patients is in the order of 2 to 3% of annual health budgets. (1) In 2015, considering the United States, medical expenses for individuals with chronic kidney diseases were more than 64 billion dollars (1). Indeed, the early diagnosis of chronic kidney diseases is very important for the implementation of preventive measures that delay or even interrupt the progression to more advanced stages of the disease. In this context, this work aims to develop a disposable electrochemical sensor aimed at detecting creatinine for diagnosing kidney diseases. The flexible disposable lab made carbon sensor has been modified with gold nanoparticles. Morphological and electrochemical characterizations were carried out to better understand the proposed device. From cyclic voltammetry measurements, the proposed sensor showed reduction and oxidation peaks related to gold oxides formed on its surface. When adding creatinine there is a decrease in the electrochemical signal due to the adsorption of the target analyte. Therefore, it was inferred that it was possible to detect creatinine present in the solution from the reduction in the analytical response of the gold-modified electrode. Using the square wave voltammetry technique, in accordance with what was previously presented, when CNN was added to the solution, the Au-CNN interaction caused a reduction in the analytical response, therefore, with the increase in CNN concentration, this reduction increased linearly in the range of 0.5 to 10 µmol L-1 with a limit of detection and quantification, 0.15 and 0.45 µmol L-1, respectively, were calculated. Furthermore, it presented a sensitivity of 0.97 µA mol-1 L with a linear equation of Ipeak (µA) = 0.97 x C(CNN) + 0.23. Furthermore, the proposed sensor was successfully applied to determine creatinine in human serum samples and the recovery results were close to 100%. Therefore, the device modified with gold nanoparticles is an interesting alternative for creatinine detection.

References

(1) Luyckx V. A. et al. The global burden of kidney disease and the sustainable development goals, Bulletin of the World Health Organization Published online: 20 April 2018.
Bipolar Electrochemistry Enabled Synthesis and Application of 2D Materials
Authors: Pan Xian , Miao Kepei , Chowdhury Azmal Huda , Jafarizadeh Borzooye , Allagui Anis , Wang Chunlei
Published: August 2024

Graphene is a promising 2D material for biosensing and energy storage applications due to its unique properties such as high surface area and high charge mobility. However, there is a significant variation in the high quality graphene contents in commercial products. The conventional wet chemical and electrochemical exfoliation approaches rely on harsh chemicals and can introduce relatively high level of defects in the 2D materials. In our recent research, we have demonstrated a simple and cost-effective bipolar electrochemical (BPE) approach which has the advantages of producing high quality 2D materials such as graphene and phosphorene. Moreover the BPE can simultaneously achieve exfoliation, reduction and deposition which enables the production of high quality microelectrodes based on 2D materials. In one exemplary application, the BPE based graphene electrodes show enhanced areal capacitance and outstanding frequency behavior as supercapacitor electrodes. In another exemplary application, the BPE enabled reduced graphene oxide microelectrodes demonstrated high sensitivity and low detection limit as aptasensors. Furthermore, the mechanistic studies including the temperature effect were conducted in order to further tune the functionality and enhance the exfoliation rate of the 2D materials.
Empowering Navajo Nation's Water Quality Monitoring through State-of-the-Art Paper-Electrochemical Sensors
Authors: Billey Wayant , Platero Justin , Platero Joshua , Begay Makeiyla , Wilson Katelyn , Plummer Dallen , Spencer Davina , Nelwood Michael , Abdelazim Khaled , Soundappan Thiagarajan
Published: August 2024

The NSF-PREM research collaborative effort between Navajo Technical University (NTU) and Harvard University aims to address the critical issue of water contamination within the Navajo Nation. Decades of uranium mining and mineral extraction have left a lasting mark on the Navajo land and groundwater resources, necessitating effective solutions. The Nano-electrochemical Analysis and Energy Storage Laboratory (NEST LAB) at NTU has developed flexible paper-based sensors integrated with advanced electrochemical techniques to detect heavy metal concentrations in water samples. These sensors are cost-effective, easy to fabricate, and highly reliable, offering real-time monitoring capabilities. The projects core goal is to expedite water quality analysis and empower the Navajo community to detect potential contamination promptly. By distributing these sensors to local chapter houses, residents can independently assess groundwater quality, fostering a sense of ownership and proactive environmental stewardship. This partnership exemplifies the power of community-driven solutions and trains Navajo students to get involved in scientific innovation to safeguard the environment for future generations in the Navajo Nation.
Paper-Based Electrochemical Sensors for Cancer Biomarkers Detection
Authors: Begay Makeiyla , Wilson Katelyn , Platero Justin , Platero Joshua , Plummer Dallen , Billey Wayant , Spencer Davina , Soundappan Thiagarajan
Published: August 2024

Cancer is currently the third leading cause of death among the people of the Navajo Nation and is the most common cause of death worldwide. American Indians are often diagnosed when cancer has reached the advanced stages compared to other communities. Major contributors for the cancer inside the Navajo Nation is the exposure to uranium, other heavy metals, and radon gas. In the Navajo Nation, uranium mining boomed from 1944 to 1986; decades later, uranium tailings and toxic waste from the milling process have caused an increased rate of cancer in the Navajo Nation.

Further cancer detection and monitoring remain critical challenges in healthcare. This research explores the fabrication of paper-based electrochemical sensors modified with nanoparticles and antigens at the Nanoelectrochemical Analysis and Energy Storage Laboratory (NEST LAB) at Navajo Technical University (NTU) for the sensitive and selective detection of cancer biomarkers.

These electrochemical sensors harness the unique qualities of paper, such as low cost and ease of fabrication, combined with the specific binding capabilities of nanoparticles and antigens. Modifying paper electrode surfaces enhances sensitivity and selectivity, making these sensors a cost-effective and portable option for early cancer detection. In contrast to traditional methods like imaging and biopsies, electrochemical sensors are low-cost, offer minimally invasive screening, high sensitivity, and affordability, making them valuable tools in the early diagnosis and management of cancer. These sensors'accessibility and potential to detect cancer at its earliest stages can significantly improve patient outcomes, particularly in resource-limited areas such as Native American reservations.

Keywords: Cancer biomarkers, paper-based electrochemical sensors, nanoparticle modification, antigen modification, early detection, point-of-care diagnostics, cost-effective healthcare.
A Search for Suitable Water-Splitting Electrodes Using SEAL and Harpoon
Authors: Brodie Dustin K , Menningen Kenneth L , Riha Shannon C
Published: August 2024

The search for suitable electrodes for photoelectrochemical water splitting extends across the periodic table. While III-V semiconductors exhibit superior light gathering properties, metal oxide semiconductors generally cost less and are more robust.

The Solar Energy Activity Laboratory (SEAL) 1 and the Heterogeneous Anodes Rapidly Perused for Oxygen Overpotential Neutralization (HARPOON)2 are simple experiments that can quickly scan for suitable oxide semiconductors. The SEAL experiment measures photocurrent and the HARPOON experiment measures oxygen production efficiency.

Electrodes made of oxides of Fe, Pd, In, Ni, Zn, Cd, Ga, and W were produced in our laboratory and evaluated using the SEAL and HARPOON experiments. The relative performance of these oxides and their mixtures were evaluated.

REFERENCES

J. R. McKone et al., “The Solar Army: A Case Study in Outreach Based on Solar Photoelectrochemistry, “ Rev. Adv. Sci. Eng.
3, 288 (2014).

S. E. Shaner et al., “Discovering Inexpensive, Effective Catalysts for Solar Energy Conversion: An Authentic Research Laboratory Experience,” J. Chem. Educ.
93, 650 (2016).
Two Dimensional Structured Electrode of Nickel Oxide for Enhanced Capacitive Behaviour
Authors: Phogat Peeyush , Shreya Shreya , Jha Ranjana , Singh Sukhvir
Published: August 2024

Two-dimensional (2D) nickel oxide (NiO) was synthesized using carbon as templates in a single step hydrothermal route. X-ray diffraction studies revealed the formation of a single phase NiO. Crystallite size and strain in the as synthesized material were calculated using the Williamson-Hall method and Size-Strain plot. UV-Vis spectroscopy investigations provided insight into the absorption region and optical band gap of NiO, including refractive index analysis. The optical absorption indicated that the material absorbs in both UV and part of visible region, with a reduced band gap of 1.9 eV. Microstructural analysis of NiO was carried out by using high resolution transmission electron microscope (HRTEM) which confirmed the presence of nanosheets. The selected area electron diffraction pattern (SAEDP) of the corresponding area revealed the polycrystalline nature of the as synthesized NiO, with fine crystallites oriented along (111) and (220) planes. Morphological analysis was performed using field emission scanning electron microscopy (FESEM), revealing the presence of 2D nano-sheets. Elemental compositional analysis was carried by using energy-dispersive X-ray spectroscopy (EDS) as an attachment of FESEM and TEM, which showed the presence of nickel and oxygen only. Nyquist plot and cyclic voltammetry depicts the capacitive behaviour, suggesting the material’s suitability for capacitor/supercapacitor applications.
The Flipped Classroom and Electrochemical Education
Authors: Suroviec Alice
Published: August 2024

The use of flipped classrooms in STEM education has been demonstrated to be a powerful learning technique for students. Faculty have been given freedom to experiment with different ways that that classroom content can be delivered to students. The ability to use pre-recorded videos that students engage with before lecture followed by time in class working on problems and answering questions allows students to deepen their understanding of the content. In this presentation examples of electrochemistry taught through flipped classroom will be presented as well as how cyclic voltammetry and other electrochemical techniques are taught in the lab.
Evaluation of Future Faculty Perspectives on Teaching and Learning of Electrochemistry & Thermochemistry: A Microstudy Approach
Authors: Azeez Ahmad Tijani , Mutambuki Jacinta
Published: August 2024

Education revolves around teaching and learning with instruction being at the center. This study seeks to investigate the whole trend of the perspectives of future faculty on the teaching and learning of critical chemical concepts “Electrochemistry” and “Thermochemistry”. The objectives are to study and extrapolate the trend and probe their applications to industry and other concepts in chemistry. Questionnaires were administered on graduate students including graduate assistants across universities in three continents: North America, Asia, and Africa. Result shows that the concepts require practical demonstration, interwoven and have applications to energy and power industries. It also reveals that learners’ motivation must be aroused prior to learning the concepts, including that learners’ attitudes is most vital in the classroom settings.
(Invited) Pilot Power Platform for Integrated Coupled Electrolysis of Furfural to Maleic Acid and Levulinic Acid to Valeric Acid
Authors: Zaffaroni Riccardo , Simões Catarina , Giling Erwin , Bubberman Saskia
Published: August 2024

In recent years it has become evident that electrification of the chemical industry is essential to shift from a fossil based society to a renewable and sustainable one. In this talk, we will address development of a pilot scale setup to upconvert bioderived feedstocks to relevant building blocks for the chemical industry. Specifically, we focused our attention to the concept of paired electrolysis: oxidation of furfural to maleic acid coupled with reduction of levulinic acid to valeric acid within the same electrochemical cell. Within the framework of this mentioned reaction, we will show different steps of the reactions optimization, scale up, process intensification that eventually led to the construction and testing of pilot power platform installation with electrochemical surface area of 1m2 (10 cell stack 1000cm2) and

productivities of about 6kg/day (Figure 1). We will also focus on downstream process needed to go from crude electrolyte to pure maleic acid and pure valeric acid. Finally, we will present insights from technoeconomic analysis.

Biography:

PERFORM: Highly selective electrochemical conversions (performproject.eu)

Figure 1. Developed infrastructure for electrochemical conversion of bioderived feedstocks to maleic acid and valeric acid. Left: upstream electrochemical Power Platform. Right: electrodialysis pilot, first downstream process of maleic acid purification

Figure 1
Controlled Assembly of Nanowires into Welded Nanowire Networks for Memristor Device Fabrication
Authors: Vaddiraju Sreeram , Choudhary Jitendra , Vidwans Niraj Ashutosh , Yanda Bhupesh Pydiraju
Published: August 2024

Next-generation electronic devices are essential for neuromorphic computing (or brain-inspired computing), which is essential for the high-speed processing of big data using artificial intelligence tools.(1) Memristors, an important constituent of these next-generation electronic devices, have been fabricated using many forms of metal oxides, including nanowires. Nanowires forms of oxides, although reduce the complexity of the memristive device fabrication process, need many technological advances for their widespread use in memristor fabrication.(1) For instance, the cyclability of devices needs to be improved. Furthermore, realizing the high density of nanowire-based memristor devices requires methods for addressing individual nanowires in large assemblies (i.e., arrays) of nanowires, strategies for which also need to be developed.(1) A possible avenue to address these problems is through the use of nanowire networks,(1) specifically those that have nanowires welded together via bridges that have the same chemical composition as those of the nanowires themselves.(2) In this configuration, the resistive switching of both the nanowires and the randomly-formed junctions between the nanowires can be employed to make mesoscale devices, circumventing the need to individually address each nanowire in the nanowire assemblies.(1) Realizing memristive devices based on welded nanowire networks, therefore, requires a strategy for assembly via welding of pre-synthesized nanowires into networks that offer the ability to control the chemical compositions of the interfaces between the nanowires and the densities of nanowires within the assemblies.(2, 3) In the presentation, strategies developed by our group for the assembly of semiconductor nanowires into welded nanowire networks of controlled densities will be discussed in detail. Specific devices that will be discussed include assembly via welding of Mg2Si, TiO2 and TiC nanowires.(2, 3) The assembly via welding of nanowires into networks is expected to accelerate the testing of mesoscale memristive devices, irrespective of the method employed for the synthesis of the nanowires used in the assemblies. This is expected to aid in accelerating both the science and technology needed for the deployment of memristive devices.

References:

Milano G, Porro S, Valov I, Ricciardi C. Recent developments and perspectives for memristive devices based on metal oxide nanowires. Advanced Electronic Materials. 2019;5(9):1800909.

Kang Y, Vaddiraju S. Solid-State Phase Transformation as a Route for the Simultaneous Synthesis and Welding of Single-Crystalline Mg2Si Nanowires. Chemistry of Materials. 2014;26(9):2814-9.

Chen Y, Kazerooni NA, Srinivasa A, Chapkin WA, Sihn S, Roy AK, et al. Shape memory polymer composites (SMPCs) using interconnected nanowire network foams as reinforcements. Nanotechnology. 2022;34(5):055601.
Molten Salt Preparation of Carbon Nanostructures for Metal-Ion Storage Applications
Authors: Kamali Ali Reza
Published: August 2024

Efficient electrical energy storage relies on the preparation of low-cost yet high-quality carbon nanostructures. This presentation introduces innovative molten salt approaches for generating such carbon materials, leveraging diverse carbon sources such as natural or synthetic graphite, biomass waste, and plastic materials. Electrochemical exfoliation of various graphite materials in molten salt is demonstrated to yield electrolytic carbon nanostructures, including graphene nanosheets, carbon nanotubes, and onion-like carbon nanoparticles. The distinctive morphology, structure, and electrical conductivity of these carbon materials are investigated, and their impact on Na-ion and Li-ion storage performances is thoroughly discussed. Furthermore, the presentation explores the molten salt-assisted carbonization of corn lignocellulosic waste, resulting in carbon materials with tailored morphological and compositional characteristics conducive to efficient Li-ion and Na-ion storage performance. Additionally, insights are provided into the transformation of waste plastic materials into graphene-based nanostructures through molten salt techniques, with a focus on their electrical and electrochemical performances. This comprehensive exploration not only underscores the versatility of molten salt methodologies in synthesizing diverse carbon nanostructures but also sheds light on their potential applications in advancing energy storage technologies.

References

A.R. Kamali*, H. Zhao, J. Alloy. Compd. 949 (2023) 169819

H. Zhao, A. Rezaei, A.R. Kamali*, J. Electrochem. Soc. 169 (2022) 054512

R. Li, A.R. Kamali*, Chem. Eng. Sci. 265 (2023) 118222

A.R. Kamali*, S. Li, Appl. Energy 334 (2023) 120692

A.R. Kamali*, J. Yang, Polym. Degrad. Stab. 177 (2020) 109184

A. Rezaei, B. Kamali, A.R. Kamali*, Measurement 150 (2020) 107087

A.R. Kamali* et al., J. Mater. Chem. A 5 (2017) 19126-19135

A.R. Kamali*, Carbon 123 (2017) 205-215
(Nanocarbons Division Richard E. Smalley Research Award) Fluorescence of Single-Walled Carbon Nanotubes: From Discovery to Real-World Applications
Authors: Weisman R. Bruce
Published: August 2024

The unique physical and chemical properties of single-walled carbon nanotubes (SWCNTs) continue to inspire extensive research by many basic and applied researchers. One of the most remarkable features of SWCNTs is their variety of pi-electronic structures associated with specific diameters and roll-up angles. Approximately two-thirds of these structural species are semiconducting and display near-infrared photoluminescence (fluorescence) through direct band gap transitions. I will describe the discovery of this SWCNT fluorescence and the assignment of specific spectral features to physical nanotube structures. Several illustrations of using SWCNT emission spectroscopy in research will then be described, including characterizing sample compositions, capturing images and spectra of single nanotubes in physical and biological environments, and guiding covalent tailoring of nanotube excitonic properties. Finally, I will present an update on an emerging technology for industrial strain measurement that uses SWCNTs as strain sensors that report through spectral shifts in their emission spectra.
(Invited) Semiconducting Single-Walled Carbon Nanotubes: Stimulated Emission, Electron Spin, and Beyond
Authors: Ma Xuedan
Published: August 2024

Great strides have been made in the understanding of electronic and optical properties of semiconducting single-walled carbon nanotubes (SWCNTs) in the past two decades. With optical transitions at near-infrared wavelengths, and diameter- and chirality-tunable electronic structures, SWCNTs are promising candidates for near-infrared nanolasers. In this talk, I will discuss our recent exploration of stimulated emission from SWCNTs by coupling them to whispering gallery modes supported by polymer microspheres through a self-assembly process.

In contrast to the many exciting developments in the excitonic frontier, electron spins, which are ubiquitous in solid state materials and highly relevant to spintronic and quantum information science, in SWCNTs are relatively less understood. In this talk, I will also discuss our recent study of electron spins in SWCNTs.