{"title":"(Keynote) Electrochemical Proton-Coupled Electron Transfer Theory","authors":"Sharon Hammes-Schiffer","doi":"10.1149/ma2023-01452453mtgabs","DOIUrl":"https://doi.org/10.1149/ma2023-01452453mtgabs","url":null,"abstract":"Proton-coupled electron transfer (PCET) plays a vital role in a wide range of electrochemical processes. This talk will describe theoretical and computational methods that have been developed to study electrochemical PCET and a variety of applications to molecular and heterogeneous electrocatalysis. My group has formulated a general PCET theory that includes the quantum mechanical effects of the electrons and transferring protons, as well as the motions of the donor-acceptor modes and solvent or protein environment. This PCET theory enables the calculation of rate constants and kinetic isotope effects for comparison to experiment. Our extension of this theory to electrochemical PCET incorporates the electronic structure of the electrode and the interfacial electric fields arising from the electrical double layer. Theoretical formulations for both homogeneous and heterogeneous electrochemical PCET provide analytical expressions for the rate constants and current densities as functions of applied potential. This theory has been applied to proton discharge on metal electrodes, as well as PCET at metal oxides and graphite-conjugated catalysts. These applications highlight the importance of using a theory that quantizes the transferring proton and includes the effects of hydrogen tunneling and excited electron-proton vibronic states. The insights from these theoretical studies are useful for the design of electrocatalytic systems to control the movement and coupling of electrons and protons for energy conversion processes. References Venkataraman, A. V. Soudackov, and S. Hammes-Schiffer, Theoretical formulation of nonadiabatic electrochemical proton-coupled electron transfer at metal-solution interfaces, J. Phys. Chem. C 112 , 12386-12397 (2008). K. Goldsmith, Y. C. Lam, A V. Soudackov, and S. Hammes-Schiffer, Proton discharge on a gold electrode from triethylammonium in acetonitrile: Theoretical modeling of potential-dependent kinetic isotope effects, J. Am. Chem. Soc. 141 , 1084-1090 (2019). C. Lam, A. V. Soudackov, and S. Hammes-Schiffer, Kinetics of proton discharge on metal electrodes: Effects of vibrational nonadiabaticity and solvent dynamics, J. Phys. Chem. Lett. 10 , 5312-5217 (2019). E. Warburton, P. Hutchison, M. N. Jackson, M. L. Pegis, Y. Surendranath, and S. Hammes-Schiffer, “Interfacial field-driven proton-coupled electron transfer at graphite-conjugated organic acids,” J. Am. Chem. Soc. 142 , 20855-20864 (2020). E. Warburton, A. V. Soudackov, and S. Hammes-Schiffer, Theoretical modeling of electrochemical proton-coupled electron transfer, Chem. Rev. 122 , 10599-10650 (2022).","PeriodicalId":11461,"journal":{"name":"ECS Meeting Abstracts","volume":"127 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135089382","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Mengxue Huang, Ruimin Ding, Lifang Chen, Jingchao Chen, Chaoqi Han, Wenwen Shi, Jie Yang, Shanshan Liu, Xi Yin
{"title":"(Digital Presentation) Structure-Activity Relationship of M-N-C Electrocatalysts Synthesized Using a General Solution-Phase Coordination Approach","authors":"Mengxue Huang, Ruimin Ding, Lifang Chen, Jingchao Chen, Chaoqi Han, Wenwen Shi, Jie Yang, Shanshan Liu, Xi Yin","doi":"10.1149/ma2023-01382294mtgabs","DOIUrl":"https://doi.org/10.1149/ma2023-01382294mtgabs","url":null,"abstract":"Metal- and nitrogen-doped carbon (M-N-C) catalysts have great potential in heterogeneous catalysis. They are used to catalyze various crucial electrochemical reactions, such as the oxygen reduction reaction (ORR), the hydrogen evolution reaction (HER), the oxygen evolution reaction (OER), and the CO 2 reduction reaction (CO 2 RR). 1-4 The nitrogen-coordinated metal sites (MN x ) have been considered the main active sites in these M-N-C catalysts. However, the synthesis of MN x moieties often undergoes a high-temperature heat-treatment step, resulting in low site density. On the other side, the coordination environment in the MN x sites is also affected by the metal species which induced the site formation. Therefore, it is challenging to single out the role of central metal in the structure-activity relationships for these MN x sites. In this presentation, we will discuss our recent progress in the development of a solution-phase coordination synthesis approach targeting M-N-C catalysts with high active-site density and well-defined coordination environments. 5, 6 A series of M-N-C catalysts are synthesized via this approach by coordinating electroactive target metal ions with the nitrogen-coordinated metal-vacancy (MVN x ) sites in N-C templated by sacrificial metals. With a combined experimental and computational approach, we explore the role of sacrificial metals, including s -, p -, 3 d -, 4 d -, and f -block metals, in forming various MVN x sites with unique coordination configurations. The structure-activity relationship between the coordination environment and the catalytic activity for ORR, HER, OER, and CO 2 RR is established by comparing the MN x site structures induced by various sacrificial metals. Furthermore, we will present the activity series of metal centers in M-N-C catalysts with the same and well-defined coordination environment for ORR, HER, OER, and CO 2 RR. These results will guide the future development of M-N-C catalysts. Acknowledgments Financial support from the State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences is greatly appreciated. This study is financially supported by the Shanxi Province grant (Grant No. 20210302123011, 202203021212007, and 202103021224442), and Key Research and Development (R&D) Projects of Shanxi Province (202102070301018). References J. Cui, Q. Chen, X. Li and S. Zhang. Recent advances in non-precious metal electrocatalysts for oxygen reduction in acidic media and PEMFCs: an activity, stability and mechanism study. Green Chemistry , 23 , 6898 (2021). H. He, H. H. Wang, J. Liu, X. Liu, W. Li and Y. Wang. Research Progress and Application of Single-Atom Catalysts: A Review. Molecules , 26 , 6501 (2021). U. Martinez, S. Komini Babu, E. F. Holby, H. T. Chung, X. Yin and P. Zelenay. Progress in the Development of Fe-Based PGM-Free Electrocatalysts for the Oxygen Reduction Reaction. Advanced Materials , 31 , 1806545 (2019). Y. Wang, X. Cui, L. Peng, ","PeriodicalId":11461,"journal":{"name":"ECS Meeting Abstracts","volume":"12 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135089398","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Patrick Teppor, Rutha Jäger, Jaak Nerut, Miriam Koppel, Jaan Aruväli, Olga Volobujeva, Enn Lust
{"title":"Valorization of Naturally Abundant Low-Value Peat into Highly Active Non-Platinum Group Metal Oxygen Reduction Catalysts","authors":"Patrick Teppor, Rutha Jäger, Jaak Nerut, Miriam Koppel, Jaan Aruväli, Olga Volobujeva, Enn Lust","doi":"10.1149/ma2023-01382287mtgabs","DOIUrl":"https://doi.org/10.1149/ma2023-01382287mtgabs","url":null,"abstract":"As society continues to adopt an increasingly eco-friendly stance, the efficient usage of natural resources needs to be maximised. For instance, energy obtained from biomass covers roughly a tenth of the global demand. This biomass can instead be used as a carbon source to produce value-added materials such as tnon-platinum group metal (NPGM) oxygen reduction catalysts, which are desperately sought after as global demand for fuel cells continues to rise [1,2]. For example, peat is an extremely abundant biomass material in Estonia covering roughly 20% of the country [3]. Herein, the viability of using peat-based catalysts as oxygen reduction catalysts in alkaline media was investigated. The peat sourced from a local peatland was processed and modified with inexpensive iron and nitrogen precursors through the common double-pyrolysis and acid washing synthesis procedure into peat-based NPGM catalysts. Additionally, zinc chloride was used as a pore forming agent. The influence of several principal synthesis parameters, e.g. precursor compound type and amount, on the physical and electrochemical properties of these materials was investigated using various characterization methods. The NPGM catalysts obtained from naturally abundant peat were highly microporous systems due to the inclusion of zinc chloride in the synthesis mixture. High onset (~0.93 V vs RHE) and half-wave potential (~0.83 V vs RHE) values were obtained for most of the materials in activity screening experiments conducted with a rotating disc electrode setup using 0.1 M KOH. However, using an excessive amount of the nitrogen precursor in the synthesis proved to be detrimental to the obtained activity. The high activity of the obtained peat-derived catalysts was further investigated in a rotating ring disc electrode setup where the influence of the studied synthesis parameters on the oxygen reduction reaction selectivity was more evident. Acknowledgments This work was supported by the EU through the European Regional Development Fund under projects TK141 “Advanced materials and high-technology devices for energy recuperation systems” (2014-2020.4.01.15-0011), NAMUR “Nanomaterials - research and applications” (3.2.0304.12-0397), NAMUR+ core facility funded by the Estonian Research Council (TT 13), PRG676 “Development of express analysis methods for micro-mesoporous materials for Estonian peat derived carbon supercapacitors” (01.01.2020–31.12.2024) and PUT1581 (1.01.2017–31.12.2020). References F. Jaouen, D. Jones, N. Coutard, V. Artero, P. Strasser, A. Kucernak, Johns. Matthey Technol Rev. 2018, 62, 231. E4tech, 2022, The Fuel Cell Industry Review 2021 . M. Orru, H. Orru, Est. J. Earth Sci. 2008, 57, 87.","PeriodicalId":11461,"journal":{"name":"ECS Meeting Abstracts","volume":"43 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135089406","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Keisuke Obata, Xinyi Zhang, Tabea Thiel, Michael Schwarze, Reinhard Schomäcker, Roel van de Krol, Fatwa Firdaus Abdi
{"title":"Solar-Driven Upgrading of Biomass by Coupled Hydrogenation Using in Situ Photoelectrochemically Generated H<sub>2</sub>","authors":"Keisuke Obata, Xinyi Zhang, Tabea Thiel, Michael Schwarze, Reinhard Schomäcker, Roel van de Krol, Fatwa Firdaus Abdi","doi":"10.1149/ma2023-01372128mtgabs","DOIUrl":"https://doi.org/10.1149/ma2023-01372128mtgabs","url":null,"abstract":"Green H 2 has been recognized as an important element in efforts to decarbonize our fossil fuel-dependent society. One approach to produce green H 2 is solar water splitting in a photoelectrochemical (PEC) device. Solar-to-hydrogen (STH) efficiencies of up to 30% have been demonstrated 1 but studies have shown that this approach still results in a relatively high levelized cost of hydrogen (LCOH) of ~10 US$ per kg of H 2 . 2-3 This is ca. one order of magnitude higher than that of hydrogen produced via steam methane reforming (SMR), which forms the bulk of the currently produced H 2 . A possible solution is to incorporate an upgrading process of biomass feedstock that generates valuable chemicals into the solar water splitting device. This is expected to not only decrease the overall LCOH but also introduce an alternative renewable pathway in chemical manufacturing. In this study, we propose the concept of solar-driven hydrogenation of biomass-derived feedstock. Photoelectrochemically generated H 2 in our solar water splitting device is coupled in situ with the homogenously catalyzed hydrogenation of itaconic acid (IA) to methyl succinic acid (MSA). IA has been identified by the US Department of Energy as one of the twelve building blocks that possess the potential to be transformed subsequently into several high-value bio-based chemicals or materials. 4 MSA is a valuable chemical compound with an estimated global market size of up to ~15,000 tonnes, whose derivatives are ubiquitously used as solvents in cosmetics, 5 polymer synthesis, 6 binders in powder coatings, 7 and organic synthesis, especially for pharmaceutical synthesis. 8-9 Our coupled hydrogenation approach—performed in the PV-electrolyzer and PEC configurations using III-V PV cells and BiVO 4 -based photoelectrode, respectively—successfully demonstrate solar-driven H 2 -to-MSA conversion efficiencies as high as 60%. In comparison to the non-coupled approach (i.e., direct hydrogenation), our coupled system offers synergistic benefits in terms of prolonged durability and a higher degree of flexibility toward other important chemical transformation reactions. In addition, life-cycle net energy assessment and technoeconomic analysis results show that adding the coupled hydrogenation process significantly lowers the energy payback time and the LCOH, respectively, to a point that is competitive even with SMR-produced H 2 . Further implications and optimization potentials of the coupled PEC hydrogenation approach will be discussed. References Kim, J. H.; Hansora, D.; Sharma, P.; Jang, J.-W.; Lee, J. S., Toward practical solar hydrogen production – an artificial photosynthetic leaf-to-farm challenge. Chem. Soc. Rev. 2019, 48 (7), 1908-1971. Shaner, M. R.; Atwater, H. A.; Lewis, N. S.; McFarland, E. W., A comparative technoeconomic analysis of renewable hydrogen production using solar energy. Energy Environ. Sci. 2016, 9 (7), 2354-2371. Pinaud, B. A.; Benck, J. D.; Seitz, L. C.; Forman, A. J.;","PeriodicalId":11461,"journal":{"name":"ECS Meeting Abstracts","volume":"50 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135089415","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Mateusz Cieślik, Krzysztof Formela, Mariusz Banasiak, Pawel Niedzialkowski, Robert Bogdanowicz, Jacek Ryl
{"title":"(Invited) Poly(lactic acid)-Nanodiamond Composites for Electroanalytical Applications","authors":"Mateusz Cieślik, Krzysztof Formela, Mariusz Banasiak, Pawel Niedzialkowski, Robert Bogdanowicz, Jacek Ryl","doi":"10.1149/ma2023-01221586mtgabs","DOIUrl":"https://doi.org/10.1149/ma2023-01221586mtgabs","url":null,"abstract":"There has been an exponential increase in the popularity of 3D printing technology in the last few years, also in everyday life. Numerous applications are reported for poly(lactic acid) (PLA) based polymer composites with various conductive carbon fillers for electrochemical needs, such as sensors, batteries, water remediation, etc. The bulk of these reports is based on commercially available 3D printing filaments, with carbon black, graphene or carbon nanotubes as fillers. Regardless of good conductivity, these materials possess characteristics that are suboptimal for electrochemical applications, including charge transfer kinetics, stability to oxidation, electrolytic window, etc. 3D printouts offer versatility in terms of ease of cheap and on-demand fabrication of free-standing multielectrode setups e.g. by dual-extruder printing. However, to fully embrace their advantages enhancement of charge transfer kinetics by removing an excess of PLA and uncovering the nanofillers, is needed. Recently we have demonstrated laser ablation for locally sculptured effective modification of the electrochemical response of these materials. There is a great focus on the development of new conductive filaments that exhibit better mechanical, electric, thermal, and electrochemical properties. We have evaluated for the first time various forms of conductive nanodiamonds (ND), i.e. detonation nanodiamonds and diamond-phase rich boron-doped carbon nanowalls, as fillers for PLA-based composites for 3D printing. The goal of the research was to investigate and thoroughly understand the interactions between composite components and those that affect the mechanical parameters and electrochemical characteristics of printed elements, studying how ND addition to PLA matrix affects material strength, rheology, and melting temperature. In particular, the enhancement of electrode kinetics and electrochemically available surface area by ND was revealed and discussed. The authors acknowledge the financial support by The National Science Centre (Republic of Poland) SONATA BIS 2020/38/E/ST8/00409.","PeriodicalId":11461,"journal":{"name":"ECS Meeting Abstracts","volume":"15 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135089427","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Julia Elizabeth Huddy, Anand P Tiwari, William Joseph Scheideler
{"title":"Modeling Mesoporous 3D-Printed Lattice Electrodes for Energy Storage","authors":"Julia Elizabeth Huddy, Anand P Tiwari, William Joseph Scheideler","doi":"10.1149/ma2023-01241597mtgabs","DOIUrl":"https://doi.org/10.1149/ma2023-01241597mtgabs","url":null,"abstract":"3D printing could offer the versatility to design and manufacture energy storage devices on demand. The precision and material flexibility of 3D printing is ideal for integrating porous electrodes that can enhance electrochemical performance [1] . This work analyzes the electrical conductivity of 3D-printed mesoscale strut lattices at the 100 μm – 1 mm scale with 40 – 90 % volumetric porosity to develop optimal electrodes for energy storage devices. We use a graph-theory-based model [2] to compute the conductivity of multiple 3D lattice types with either solid conducting struts or struts coated with conductive material. These structures show 3 – 5X higher conductivity than random conductive foams that lack an internal periodic mesostructure [3] . Using microstereolithography, we 3D print samples with high-resolution struts (< 70 µm) that maintain their shape and achieve high conductivity after carbonization at 700 ˚C. By tuning the lattice architecture, we manipulate the tradeoff between conductivity, weight, and porosity, validating our simulations with experimental measurements. These results demonstrate that that body-centered cubic (BCC) strut lattices have optimal conductivity per weight compared with other lattice types. Implementing these 3D-printed conductive lattices as supercapacitor electrodes, we see that the lattice architecture impacts the gravimetric capacitance of the devices as well as the mechanical strength, with octet structures outperforming both cubic and BCC lattices. Electrochemical impedance spectroscopy (EIS) shows that 3D-printed electrodes with higher porosity exhibit higher gravimetric double layer capacitance and lower charge transfer resistance, making them ideal candidates for use in supercapacitor electrodes as free-standing 3D hosts for active materials. CV characterization of the electrodes also illustrates how our graph theory-based model for 3D lattices can predict the optimal structure for energy storage. This model can also serve to predict electrode performance and tailor design for integration of higher surface area nanoporous materials on these conductive 3D printed scaffolds. This allows us to guide the design of 3D printed electrodes to minimize charge transfer resistance and achieve an optimal balance between gravimetric and volumetric energy density for device applications. [1] J. Zhao, Y. Zhang, X. Zhao, R. Wang, J. Xie, C. Yang, J. Wang, Q. Zhang, L. Li, C. Lu, Y. Yao, Advanced Functional Materials 2019 , 29 , 1900809. [2] J. E. Huddy, M. S. Rahman, A. B. Hamlin, Y. Ye, W. J. Scheideler, Cell Reports Physical Science 2022 , 3 , 100786. [3] F. G. Cuevas, J. M. Montes, J. Cintas, P. Urban, J Porous Mater 2008 , 16 , 675. Figure showing (a) designed octet (blue), cubic (orange), and BCC (red) lattice types as well as (b) SEM images of their experimental 3D-printed counterparts and (c) measured electrical resistance. Figure 1","PeriodicalId":11461,"journal":{"name":"ECS Meeting Abstracts","volume":"127 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135089429","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"(Invited) A Closer Look at Impact Ionization Coefficients in Wide Band Gap Semiconductors: Theoretical Models and Measured Data","authors":"Enrico Bellotti, Masahiko Matsubara","doi":"10.1149/ma2023-01321819mtgabs","DOIUrl":"https://doi.org/10.1149/ma2023-01321819mtgabs","url":null,"abstract":"The direct measurement of ionization coefficients in wide band gap semiconductor materials is challenging due to the need to operate at high field strengths and the requirement of specific test structures that enable single carrier injection. More often than not, ionization coefficients are inferred from current multiplication data measured in p-n junctions or transistors structures. Unfortunately, sub-par material quality, processing issues and inappropriate measuring techniques have led to ionization coefficients values that are contradictory and with large variation among different datasets. As a result, theoretical models that attempt to predict the values of the carriers’ ionization coefficients are important since they provide an estimate of the expected values and a first order evaluation of the material performance. Developing theoretical models presents its own set of challenges. The established approach is based on a full electronics structure description of the semiconductor material and a suitable model to quantify the interaction of carriers with phonons, impurities and material imperfections. While this methodology has been successful with conventional elemental and compound semiconductors, and it has been applied to some wide band gap materials such as GaN, 4H-SiC [1,2] and diamond, a number of open issues still exists. The main difficulty is the determination of the carrier-phonon scattering strength at high electric field strengths that cannot be inferred from low-field mobility measurements. Among all wide band gap semiconductors, 4H-SiC [3] and GaN [4] are the material for which ionization coefficients have been measured by several groups. In the case of GaN, different measured ionization coefficients datasets are available and seems to provide a consistent indication of the expected values. Corresponding theoretical models based on full-band Monte Carlo simulations have been able to predict the correct trends, namely the fact that holes dominate the ionization process, but a quantitative agreement between predicted and measured values has only been achieved recently [5]. This talk will provide an overview of the currently available experimentally measured ionization coefficients for wide band gap semiconductors and compare them to the ones obtained with theoretical models of different complexity. Specifically the development of the theoretical models for high-field transport for 4H-SiC, GaN will be discussed. Three different approaches, one based on empirical carrier-phonon scattering rates, one using the rigid pseudo ion model, and the direct evaluation of the interaction parameters based on a ab-initio DFT approach will be compared, and the outcome for each one of them benchmarked against the measured values. Additionally, the models will be applied to determine the ionization coefficients in AlGaN alloys, cubic BN and diamond. [1] E. Bellotti et al., J. Appl. Phys., 87, (8), p.3864, 15 April 2000. [2] F. Bertazzi et al., J.","PeriodicalId":11461,"journal":{"name":"ECS Meeting Abstracts","volume":"75 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135089434","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Kai Fan, Kuei-Lin Liu, Jun-Hsuan Chung, Zong-Hong Lin
{"title":"Development of Wearable Microneedle-Based Platform for Real-Time Biomarkers Sensing","authors":"Kai Fan, Kuei-Lin Liu, Jun-Hsuan Chung, Zong-Hong Lin","doi":"10.1149/ma2023-01341936mtgabs","DOIUrl":"https://doi.org/10.1149/ma2023-01341936mtgabs","url":null,"abstract":"The wearable device technology plays a huge role in the healthcare sector owing to the aging global population and increased acquisition of the internet of things (IoT). Further, the Coronavirus Disease-2019 (COVID-19) pandemic has accelerated the emergence of wearable medical devices in the market. The patients with chronic diseases are more focused on tracking single or multiple nutrients and biomarkers in the body. Diabetes is a classic example of chronic disease where the patients need to monitor their blood glucose level for a long time. In addition, diabetic patients also face electrolyte imbalance which gives rise to several other diseases. There is an immense urgency to develop a sensing platform that can detect the essential ions as well as biomarkers from the interstitial fluid (ISF) as it contains valuable information about the physiological status of a person. According to Centers for Disease Control and Prevention (CDC), imbalance of sodium concentration in the body may lead to stroke, hypertension, and epilepsy; for potassium: arrhythmia, chronic kidney disease (CKD), and dizziness; for calcium: depression, osteoporosis, and other bone-related disease; for pH of body fluid: urinary tract infection, respiratory acidosis, and sleep apnea. Within this advent of wearables, microneedle (MN)-based transdermal sensors are well positioned to play a key role in combining the significant benefits of dermal interstitial fluid (ISF) as a source of clinical indicators and minimally invasive skin puncturing to allow the collection of real-time diagnostic data. In this context, we have developed a MNs based versatile platform for the transdermal amperometric detection of glucose and different clinically relevant biomarkers such as K + , Na + , Ca 2+ in the body fluid in a robust, reliable, and cost-effective way. Here, stainless steel microneedle (SS-MN) is used as an ideal candidate for multiplex sensing due to its great chemical stability as well as the rigidity for accurate and painless puncture. The device is fabricated with ion selective electrode (ISM) coating on each needle for their corresponding electrolyte and enzyme for glucose detection. In vitro experiments performed in artificial ISF samples yielded excellent sensitivity and a good linear response. The sensor is successfully applied for in vivo detection of glucose and these ions in SD rats for validating their feasibility as a real-time sensing device. Overall, this developed concept comprises of significant progress in the sensing of glucose and other ions in relation to an electrolyte imbalance in the humans that holds relevance in controlling several diseases.","PeriodicalId":11461,"journal":{"name":"ECS Meeting Abstracts","volume":"75 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135089436","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"A Flexible and Stretchable Temperature Sensor Based on Contact Electrification for Robotic Sensing","authors":"Kee Chin Lim, Shuo-Wen Chen, Yung-Hsin Chen, Yan-Tsz Huang, Arnab Pal, Zong-Hong Lin","doi":"10.1149/ma2023-01341877mtgabs","DOIUrl":"https://doi.org/10.1149/ma2023-01341877mtgabs","url":null,"abstract":"With the rapid development of robotic systems, an increasing number of various sensitive sensors are needed to meet the requirement of data collection for unmanned detection and monitoring technology. Among various external stimuli information, temperature sensing is an essential important function that can avoid high-temperature scalding injuries, achieve robot detection of environmental, and human-machine interfaces applications. However, most of the existing temperature sensors for robotic sensing are realized by rigid materials, which have the disadvantage of not being able to adapt to an arbitrarily curved surface. Also, most of the sensors are thermistor-based approaches, which faces challenges in developing a low-cost robotic system since external power is required to obtain the sensing signal. In this work, a self-powered and stretchable temperature sensor based on Triboelectric Nanogenerator (TENG) technology was developed. The principle of TENG is the coupling effect of triboelectric charge transfer and electrostatic induction effects, which can generate different magnitudes of electrical signals when subjected to external stimuli, including temperature. To this end, this study is a pilot effort toward validating the sensitivity of TENG electrical output on different temperature effects. The surface potential of materials is explored under different temperatures by Kelvin probe force microscopy (KPFM), which shows the feasibility of self-powered temperature sensor. The proposed temperature sensor is composed of highly resilient materials physiological saline as liquid electrode encapsulated with Ecoflex as triboelectric layer, which has the advantage of biocompatibility. The temperature sensing performance was successfully maintained at 200% stretch. Owing to its flexible, bendable and stretchable characteristics, the self-powered temperature-sensitive sensor has been successfully demonstrated on a robot hand, which can read the information and respond to different temperatures through the feedback system. Overall, this self-powered temperature-sensitive sensor has great potential to be an emerging tool for human-robot interaction and automatic detection.","PeriodicalId":11461,"journal":{"name":"ECS Meeting Abstracts","volume":"24 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135089446","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"(Invited) towards Continuous Health Monitoring Platforms By Enzyme-Free Electrochemical Sensors and Triboelectric Sensors for Noninvasive Lactate Detection","authors":"Min-Hsin Yeh","doi":"10.1149/ma2023-01341875mtgabs","DOIUrl":"https://doi.org/10.1149/ma2023-01341875mtgabs","url":null,"abstract":"Emerging wearable devices with non-invasively biosensing technics have drawn considerable attention to continuously monitor several metabolites in body fluids, such as a tear, saliva, and sweat, to diagnose human health conditions. Most importantly, wearable sensors could offer unique possibilities for online, real-time and non-invasive monitoring of health compared to traditional invasive biosensors. Among lots of analytes, lactic acid concentration in the human body exhibits a high relationship with several diseases such as acute heart diseases, hypoxia, muscle fatigue, meningitis, and cystic fibrosis, and it could also cause muscle pain in athletes. To further boost up the reproducibility and reliability of wearable biosensors to detect lactate concentration levels from human sweat, Ni-based layered double hydroxide (LDH) with various secondary transition metals (Fe and Co) was proposed as electrocatalysts in an enzyme-free electrochemical lactate sensor. According to the mechanism of lactate oxidation on the transition metal-based electrocatalyst, secondary transition metal of Co could serve as the active site for lactate oxidation and facilitate the adsorption of OH - in the alkaline electrolyte. To further increasing the active surface area for enhancing the sensitivity of Ni-based LDH, ZIF-67 derived NiCo LDH was synthesized as the electrocatalyst for non-enzymatic lactate detection. Co-based ZIF-67 served as self-sacrificial templates to fabricate hierarchically structural NiCo LDH with uniform porosity and high electrochemically active surface area to achieve outstanding electrocatalytic performance for lactate sensing. After optimizing the particle size of ZIF-67 and transformation times, ZIF-67 derived NiCo LDH reached the ultrahigh sensitivity of 83.98 μA mM - 1 cm - 2 at an applied potential of 0.55 V (vs. Ag/AgCl KCl sat’d) in the concentration range from 2 to 26 mM. On the other hand, pioneering works in biosensors for lactate detection in sweat has been encountered major challenges such as noble material usage, immobile power supply, and complicated circuit connection to realize the compact sustainable sensing systems. To solve these restrictions, herein, the self-powered molecular imprinted polymers based triboelectric sensor (MIP-TES) was designed to offer a multifunctional noninvasive approach for specific and simultaneous lactate detection. Free-standing PVDF/graphene flexible electrode modified poly(3-aminophenyl boronic acid) imprinted lactate molecule demonstrated the change of the surface properties afterlactate adsorption. MIP-modified electrode revealed the selective lactate sensing over non molecular imprinted polymers (NIP) electrode through the superior and stable signal change with variation of lactate concentration in human sweat. Moreover, MIP modified lactate sensor was further introduced in the triboelectric nanogenerator system to harvest mechanical energy from contact and separation into electrical output. The ","PeriodicalId":11461,"journal":{"name":"ECS Meeting Abstracts","volume":"71 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135089455","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}