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5. A Novel Antimicrobial Electrochemical Glucose Biosensor Based on Silver-Prussian Blue Modified TiO$_2$ Nanotube Arrays

Author

Farajpour, Nasim, Deivanayagam, Ram, Phakatkar, Abhijit, Narayanan, Surya, Shahbazian-Yassar, Reza, and Shokuhfar, Tolou

Subjects
Quantitative Biology - Biomolecules, Physics - Applied Physics
Abstract

Glucose biosensors play an important role in the diagnosis and continued monitoring of the disease, diabetes mellitus. This report proposes the development of a novel enzymatic electrochemical glucose biosensor based on TiO$_2$ nanotubes modified by AgO and Prussian blue (PB) nanoparticles (NPs), which has an additional advantage of possessing antimicrobial properties for implantable biosensor applications. In this study, we developed two high performance glucose biosensors based on the immobilization of glucose oxidase (GOx) onto Prussian blue (PB) modified TiO$_2$ nanotube arrays functionalized by Au and AgO NPs. AgO-deposited TiO$_2$ nanotubes were synthesized through an electrochemical anodization process followed by Ag electroplating process in the same electrolyte. Deposition of PB particles was performed from an acidic ferricyanide solution. The surface morphology and elemental composition of the two fabricated biosensors were investigated by scanning electron microscopy (SEM) and energy-dispersive X-ray spectroscopy (EDS) which indicate the successful deposition of Au and AgO nanoparticles as well as PB nanocrystals. Cyclic voltammetry and chronoamperometry were used to investigate the performance of the modified electrochemical biosensors. The results show that the developed electrochemical biosensors display excellent properties in terms of electron transmission, low detection limit as well as high stability for the determination of glucose. Under the optimized conditions, the amperometric response shows a linear dependence on the glucose concentration to a detection limit down to 4.91 $\mu$M with sensitivity of 185.1 mA M$^{-1}$ cm$^{-2]$ in Au modified biosensor and detection limit of 58.7 $\mu$M with 29.1 mA M$^{-1}$ cm$^{-2]$ sensitivity in AgO modified biosensor.

Published
2021
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6. Gold-like activity copper-like selectivity of heteroatomic transition metal carbides for electrocatalytic carbon dioxide reduction reaction.

Author

Esmaeilirad, Mohammadreza, Baskin, Artem, Kondori, Alireza, Sanz-Matias, Ana, Qian, Jin, Song, Boao, Tamadoni Saray, Mahmoud, Kucuk, Kamil, Belmonte, Andres Ruiz, Delgado, Pablo Navarro Munoz, Park, Junwon, Azari, Rahman, Segre, Carlo U, Shahbazian-Yassar, Reza, Prendergast, David, and Asadi, Mohammad

Abstract

An overarching challenge of the electrochemical carbon dioxide reduction reaction (eCO2RR) is finding an earth-abundant, highly active catalyst that selectively produces hydrocarbons at relatively low overpotentials. Here, we report the eCO2RR performance of two-dimensional transition metal carbide class of materials. Our results indicate a maximum methane (CH4) current density of -421.63 mA/cm2 and a CH4 faradic efficiency of 82.7% ± 2% for di-tungsten carbide (W2C) nanoflakes in a hybrid electrolyte of 3 M potassium hydroxide and 2 M choline-chloride. Powered by a triple junction photovoltaic cell, we demonstrate a flow electrolyzer that uses humidified CO2 to produce CH4 in a 700-h process under one sun illumination with a CO2RR energy efficiency of about 62.3% and a solar-to-fuel efficiency of 20.7%. Density functional theory calculations reveal that dissociation of water, chemisorption of CO2 and cleavage of the C-O bond-the most energy consuming elementary steps in other catalysts such as copper-become nearly spontaneous at the W2C surface. This results in instantaneous formation of adsorbed CO-an important reaction intermediate-and an unlimited source of protons near the tungsten surface sites that are the main reasons for the observed superior activity, selectivity, and small potential.

Published
2021

7. Extreme mixing in nanoscale transition metal alloys

Author

Yao, Yonggang, Huang, Zhennan, Hughes, Lauren A, Gao, Jinlong, Li, Tangyuan, Morris, David, Zeltmann, Steven Eric, Savitzky, Benjamin H, Ophus, Colin, Finfrock, Y Zou, Dong, Qi, Jiao, Miaolun, Mao, Yimin, Chi, Miaofang, Zhang, Peng, Li, Ju, Minor, Andrew M, Shahbazian-Yassar, Reza, and Hu, Liangbing

Abstract

The ability to alloy different elements is critical for property tuning and materials discovery. However, general alloying at the nanoscale remains extremely challenging due to strong immiscibility and easy oxidation, particularly for early transition metals that are highly reactive. Here, we report nanoscale alloying using a high-temperature- and high-entropy-based strategy (T∗ΔSmix) to significantly expand the possible alloys and include early transition metals. While high-temperature synthesis favors alloy formation and metal reduction, the high-entropy compositional design is critical to further extending the alloying to strongly repelling combinations (e.g., Au-W) and easily oxidized elements (e.g., Zr). In particular, we explicitly characterized a record 15-element nanoalloy, which showed a solid-solution structure featuring localized strain and lattice distortions as a result of extreme mixing. Our study significantly broadens available compositions of nanoalloys and provides clear guidelines by utilizing the less-explored entropic chemistry.

Published
2021

20. High-throughput, combinatorial synthesis of multimetallic nanoclusters

Author

Yao, Yonggang, Huang, Zhennan, Li, Tangyuan, Wang, Hang, Liu, Yifan, Stein, Helge S., Mao, Yimin, Gao, Jinlong, Jiao, Miaolun, Dong, Qi, Dai, Jiaqi, Xie, Pengfei, Xie, Hua, Lacey, Steven D., Takeuchi, Ichiro, Gregoire, John M., Jiang, Rongzhong, Wang, Chao, Taylor, Andre D., Shahbazian-Yassar, Reza, and Hu, Liangbing

Published
2020

22. Multi‐Step Crystallization of Barium Carbonate: Rapid Interconversion of Amorphous and Crystalline Precursors

Author

Whittaker, Michael L, Smeets, Paul JM, Asayesh‐Ardakani, Hasti, Shahbazian‐Yassar, Reza, and Joester, Derk

Subjects
amorphous materials, barium carbonate, crystal growth, metastable compounds, multi-step crystallization, Chemical Sciences, Organic Chemistry
Abstract

The direct observation of amorphous barium carbonate (ABC), which transforms into a previously unknown barium carbonate hydrate (herewith named gortatowskite) within a few hundred milliseconds of formation, is described. In situ X-ray scattering, cryo-, and low-dose electron microscopy were used to capture the transformation of nanoparticulate ABC into gortatowskite crystals, highly anisotropic sheets that are up to 1 μm in width, yet only about 10 nm in thickness. Recrystallization of gortatowskite to witherite starts within 30 seconds. We describe a bulk synthesis and report a first assessment of the composition, vibrational spectra, and structure of gortatowskite. Our findings indicate that transient amorphous and crystalline precursors can play a role in aqueous precipitation pathways that may often be overlooked owing to their extremely short lifetimes and small dimensions. However, such transient precursors may be integral to the formation of more stable phases.

Published
2017

23. In Situ High Temperature Synthesis of Single-Component Metallic Nanoparticles

Author

Yao, Yonggang, Chen, Fengjuan, Nie, Anmin, Lacey, Steven D, Jacob, Rohit Jiji, Xu, Shaomao, Huang, Zhennan, Fu, Kun, Dai, Jiaqi, Salamanca-Riba, Lourdes, Zachariah, Michael R, Shahbazian-Yassar, Reza, and Hu, Liangbing

Subjects
Bioengineering, Nanotechnology, Affordable and Clean Energy, Chemical Sciences
Abstract

Nanoparticles (NPs) dispersed within a conductive host are essential for a range of applications including electrochemical energy storage, catalysis, and energetic devices. However, manufacturing high quality NPs in an efficient manner remains a challenge, especially due to agglomeration during assembly processes. Here we report a rapid thermal shock method to in situ synthesize well-dispersed NPs on a conductive fiber matrix using metal precursor salts. The temperature of the carbon nanofibers (CNFs) coated with metal salts was ramped from room temperature to ∼2000 K in 5 ms, which corresponds to a rate of 400,000 K/s. Metal salts decompose rapidly at such high temperatures and nucleate into metallic nanoparticles during the rapid cooling step (cooling rate of ∼100,000 K/s). The high temperature duration plays a critical role in the size and distribution of the nanoparticles: the faster the process is, the smaller the nanoparticles are, and the narrower the size distribution is. We also demonstrated that the peak temperature of thermal shock can reach ∼3000 K, much higher than the decomposition temperature of many salts, which ensures the possibility of synthesizing various types of nanoparticles. This universal, in situ, high temperature thermal shock method offers considerable potential for the bulk synthesis of unagglomerated nanoparticles stabilized within a matrix.

Published
2017

26. Composite PEDOT:PSS‐PEO Layers for Improving Lithium Batteries**.

Author

Ritter, Timothy G., Il Kim, Yong, Bezerra De Souza, Breno, Wang, Xinnian, Pan, Yayue, Yurkiv, Vitaliy, Yarin, Alexander L., and Shahbazian‐Yassar, Reza

Subjects
POLYETHYLENE oxide, YOUNG'S modulus, IONIC conductivity, THERMAL stability, THERMAL properties
Abstract

This work investigates the application of poly(3,4‐ethylenedioxythiophene) polystyrenesulfonate (PEDOT:PSS) with polyethylene oxide (PEO) in lithium batteries (LIBs). This composite film comprising PEDOT:PSS and PEO was 3D printed onto a carbon nanofiber (CNF) substrate to serve as a layer between the polypropylene (PP) separator and the lithium anode in LIBs. The resulting CNF‐PEDOT:PSS‐PEO film exhibited superior mechanical and thermal properties compared to conventional PP separators. Mechanical tests revealed a high Young's modulus and puncture strength for the composite film. Thermal stability tests indicated that the CNF‐PEDOT:PSS‐PEO film remained stable at higher temperatures compared to the commercial PP separator, and combustion tests confirmed its superior fire‐resistance properties. In terms of conductivity, the composite film maintained comparable ionic conductivity to the commercial PP separator. Electrochemical tests demonstrated that LIBs incorporating the CNF‐PEDOT:PSS‐PEO film exhibited slight improvement in cycling performance, with a 7.9 % increase in long‐term cycling capacity compared to LIBs using only the commercial PP separator. These findings indicate that the developed CNF‐PEDOT:PSS‐PEO composite film holds promise to improve safety, while maintaining the electrochemical performance of LIBs by reducing dendrite formation and enhancing thermal stability. [ABSTRACT FROM AUTHOR]

Published
2024
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27. Scalable Synthesis Methods for High‐Entropy Nanoparticles.

Author

Ritter, Timothy G., Pappu, Samhita, and Shahbazian‐Yassar, Reza

Subjects
MATERIALS science, HYDROGEN storage, FUEL cells, CRYSTAL structure, ELECTROCHEMISTRY
Abstract

High‐entropy materials (HEMs) represent a revolutionary class of materials that have garnered significant attention in the field of materials science due to their extraordinary properties in diverse fields of applications such as catalysis and electrochemistry. The past decade has witnessed a substantial increase in the study of these materials, exploring new synthesis routes and compositions. What began as the synthesis of high‐entropy alloys has expanded to encompass several classes of HEMs such as oxides, hydroxides, sulfides, nitrides, and carbides, among others. Several synthesis methods have been developed to produce these materials. This review therefore highlights the fundamental concepts of HEMs, including their core effects, with a major emphasis on their scalable synthesis routes. The advantages and drawbacks of these methods are also discussed. As HEMs transition from the lab to large‐scale production, there is a growing need for cost‐effective and scalable synthesis methods with high material yield suitable for a variety of applications like hydrogen storage, catalysis, batteries, supercapacitors, and fuel cells. Hence, this review serves as an introduction to scalable synthesis routes based on crystal structure, desired elements, synthesis times, and equipment costs. [ABSTRACT FROM AUTHOR]

Published
2024
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29. Continuous 2000 K droplet-to-particle synthesis

Author

Wang, Xizheng, Huang, Zhennan, Yao, Yonggang, Qiao, Haiyu, Zhong, Geng, Pei, Yong, Zheng, Chaolun, Kline, Dylan, Xia, Qinqin, Lin, Zhiwei, Dai, Jiaqi, Zachariah, Michael R., Yang, Bao, Shahbazian-Yassar, Reza, and Hu, Liangbing

Published
2020
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44. Carbothermal shock synthesis of high-entropy-alloy nanoparticles

Author

Yao, Yonggang, Huang, Zhennan, Xie, Pengfei, Lacey, Steven D., Jacob, Rohit Jiji, Xie, Hua, Chen, Fengjuan, Nie, Anmin, Pu, Tiancheng, Rehwoldt, Miles, Yu, Daiwei, Zachariah, Michael R., Wang, Chao, Shahbazian-Yassar, Reza, Li, Ju, and Hu, Liangbing

Published
2018

49. High temperature shockwave stabilized single atoms

Author

Yao, Yonggang, Huang, Zhennan, Xie, Pengfei, Wu, Lianping, Ma, Lu, Li, Tangyuan, Pang, Zhenqian, Jiao, Miaolun, Liang, Zhiqiang, Gao, Jinlong, He, Yang, Kline, Dylan Jacob, Zachariah, Michael R., Wang, Chongmin, Lu, Jun, Wu, Tianpin, Li, Teng, Wang, Chao, Shahbazian-Yassar, Reza, and Hu, Liangbing

Published
2019
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