{"title":"(Invited) Electrochemical Conversion of CO<sub>2</sub> Into Oxygen/ and C/CO in Molten Carbonate","authors":"Huayi Yin, Dihua Wang","doi":"10.1149/ma2023-01562737mtgabs","DOIUrl":"https://doi.org/10.1149/ma2023-01562737mtgabs","url":null,"abstract":"The molten salt CO 2 capture and electrochemical transformation (MSCC-ET) process has been demonstrated as an effective approach to capturing and converting CO 2 into oxygen and C/CO [1-2]. The effective CO 2 capture and electrochemical conversion rely on the high-temperature molten carbonate electrolytes and the cost-effective inert oxygen-evolution anode. In recent years, we have focused on the electrolyte engineering to modulate the reactions at both the cathode and anode as well as the CO 2 capture efficiency [3-4]. Besides, we insist on developing iron- and nickel-base oxygen-evolution inert anodes in terms of revealing the fundamental principles and basic guidelines for choosing proper materials and fabrication processes [5]. By doing so, we can prepare functional carbon materials or CO at the cathode with a high current efficiency of over 90%, and produce oxygen at the inert anode. In addition, the kilo-ampere scale electrolyzer was built to produce oxygen, carbon or CO with an energy efficiency of over 50%. Therefore, the molten carbonate CO 2 electrolyzer shows its potential to convert CO 2 on the Mars to produce oxygen and fuels to support the future exploration of outer space. References [1] H. Y. Yin, D. H. Wang*, et al., Capture and electrochemical conversion of CO 2 to value-added carbon and oxygen by molten salt electrolysis. Energy & Environmental Science, 2013, 6: 1538-1545. [2] R. Jiang, M. X. Gao, X. H. Mao, D. H. Wang*. Advancements and potentials of molten salt CO 2 capture and electrochemical transformation (MSCC-ET) process, Current Opinion in Electrochemistry, 2019, 17: 38-46. [3] B. W. Deng, J. J. Tang, X. H. Mao, Y. Q. Song, H. Zhu, W. Xiao, D. H. Wang*. Kinetic and Thermodynamic Characterization of Enhanced Carbon Dioxide Absorption Process with Lithium Oxide-Containing Ternary Molten Carbonate, Environmental Science & Technology, 2016, 50(19): 10588-10595. [4] Z. S Yang, B. W. Deng, K. F. Du, H. Y. Yin*, D. H. Wang*, A general descriptor for guiding the electrolysis of CO2 in molten carbonate, 2022, in press. [5] P. L. Wang, K. F. Du, Y. P. Dou, H. Zhu, D. H. Wang*, Corrosion behaviour and mechanism of nickel anode in SO42- containing molten Li2CO3-Na2CO3-K2CO3. Corrosion Science 2022, 166. Figure 1","PeriodicalId":11461,"journal":{"name":"ECS Meeting Abstracts","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135088640","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":"Progress of the Evaluation and Analysis Methods for Durability of SOFC Stacks","authors":"Teruhisa Horita","doi":"10.1149/ma2023-0154208mtgabs","DOIUrl":"https://doi.org/10.1149/ma2023-0154208mtgabs","url":null,"abstract":"Recent progress in the development of R&D for the evaluation and analytical methods of SOFC stack durability is reported under the NEDO Japanese national project. The goal of this project is the following two points: (1) to develop the advanced evaluation and analytical methods for the cell stacks which show a lifetime over 15 years (130 kh) with high efficiency of over 65% LHV, and (2) to develop the evaluation and analytical methods for dynamic operation mode such as rapid start-stop and load cycling. Three practical stacks were supplied by the stack developers and tested over 10,000 hours with high fuel utilization (Uf~85%). Relatively stable performances were reported for these stacks and degradation factors were considered taking into account the degradation mechanisms at cells and stacks. Under high Uf conditions, some specific degradation mechanisms are now analyzed in the cells. For rapid starts of stacks, evaluation protocols are considered taking into account the mechanical stress arising from the thermal distribution in the cells. Simulation methods are considered for the evaluation of performance after 15 years of operation in the stacks.","PeriodicalId":11461,"journal":{"name":"ECS Meeting Abstracts","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135088644","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":"Unraveling Electrochemical Lignin Degradation in Organic Solvent for Production of Valuable Fuels and Chemicals","authors":"Mahmudul Hasan, Lauren F Greenlee","doi":"10.1149/ma2023-01422362mtgabs","DOIUrl":"https://doi.org/10.1149/ma2023-01422362mtgabs","url":null,"abstract":"Lignin is the second most abundant biopolymer in nature after cellulose. Due to its distinctive aromatic backbone, it is also one of the most unique biopolymers. The aromatic components in lignin provide structural support to plants and comprises about 30% of the plant material. These aromatic groups can be used to produce renewable aromatic compounds. Also, these aromatic compounds can be used to produce biofuels which can be promising alternative to fossil-based fuels and chemicals. Besides, from previous studies it is found that about 40 to 60 million tons of lignin are generated from pulp and paper industry, mostly as wastes. So, developing novel and attractive strategies for fragmentation of lignin is gaining increased interest among scientific community for valorizing this underexploited material. Also, by valorizing lignin the sustainability of biorefinery and paper industry can be enhanced. However, the present technologies used for degradation of lignin generally requires the use of metallic catalysts at high temperatures and harsh reaction conditions. As a result, catalyst recovery and decomposition often become difficult under such harsh conditions and the process becomes impractical. Also, these technologies suffer from poor selectivity and usually produce the desired fragmentation products in low yields. Compared to the thermocatalytic transformation of lignin, electrocatalytic approaches have several advantages like it is environmentally friendly, have mild reaction conditions and the cost is low. Besides, there is a lack of studies incorporating electrocatalytic oxidation and reduction of lignin in organic solvent. In this project, the main goal was to overcome the challenge of using isolated lignin from various industrial processes by electrochemical depolymerization of lignin in organic solvent like tetrahydrofuran. Tetrahydrofuran is mainly used in Co-solvent Enhanced Lignocellulosic Fractionation (CELF) process. So, electrocatalytic degradation of lignin in this solvent is beneficial because the product from CELF process can be directly used here and thus it can work as a secondary treatment process for CELF process. Cyclic voltammetry (CV) and Chronoamperometry (CA) which are important tools for identifying redox reactions happening in the system is used here. In this presentation, for varying concentrations of Lignin, Tetrahydrofuran and sulfuric acid the results found from CV and CA will be discussed with practical significance. Keywords: Recalcitrant biopolymer, Lignin in organic solvent, controlled electrocatalysis, secondary treatment for CELF process, Cyclic Voltammetry","PeriodicalId":11461,"journal":{"name":"ECS Meeting Abstracts","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135088673","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}
Ryan H. DeBlock, Hunter O. Ford, Christopher N. Chervin, Debra R. Rolison, Michelle D. Johannes, Jeffrey W. Long
{"title":"Uncovering Electrochemical Cation-Storage Mechanisms in Defective Vanadium Ferrites Using Synchrotron-Quality, in-Lab X-Ray Absorption Spectroscopy","authors":"Ryan H. DeBlock, Hunter O. Ford, Christopher N. Chervin, Debra R. Rolison, Michelle D. Johannes, Jeffrey W. Long","doi":"10.1149/ma2023-01472520mtgabs","DOIUrl":"https://doi.org/10.1149/ma2023-01472520mtgabs","url":null,"abstract":"X-ray absorption spectroscopy (XAS) is a critical tool for investigating new materials for electrochemical energy storage, providing important information on metal oxidation state and element-specific coordination. Historically, XAS measurements had required the energy specificity and brilliance of a synchrotron facility, but recent advances in detectors and optics are bringing XAS capabilities to the laboratory setting with multiple commercial instruments available. At the Naval Research Laboratory, we use laboratory-based XAS to study a class of disordered vanadium ferrite (VFe 2 O x ) aerogels that exhibit promising performance for electrochemical energy-storage applications such as rechargeable lithium-ion batteries. 1,2 The structure and composition of these materials are readily varied via modifications to the epoxide-promoted sol–gel reaction of iron chloride and vanadium isopropoxide (e.g., substitution with other cations such as Al 3+ ), 2 as well as post-synthesis thermal treatments that render disordered, defective, or nanocrystalline forms of a given composition. The resulting series of VFe 2 O x materials are evaluated by XAS in both ex situ and in situ configurations, including as powder-composite cathodes versus lithium metal in pouch cells with conventional nonaqueous lithium-ion electrolyte. X-ray Absorption Near-edge Spectroscopy (XANES) at the V K-edge and Fe K-edge is used to track V and Fe oxidation state, respectively, permitting the assignment of metal-centered redox across the broad potential range over which these materials are electrochemically active (2–3.4 V vs Li/Li + ). Extended X-ray Absorption Fine Structure (EXAFS) analysis provides information on V- or Fe-specific coordination as a function of composition, structure, and state-of-charge. Parallel computation efforts using Density-Functional Theory offer a complementary feedback loop with experimental XANES and EXAFS to achieve a sophisticated description of these complex battery materials. 1. C. N. Chervin, J. S. Ko, B. W. Miller, L. Dudek, A. N. Mansour, M. D. Donakowski, T. Brintlinger, P. Gogotsi, S. Chattopadhyay, T. Shibata, J. F. Parker, B. P. Hahn, D. R. Rolison, and J. W. Long, J. Mater. Chem. A 3 , 12059 (2015). 2. C. N. Chervin, R. H. DeBlock, J. F. Parker, B. M. Hudak, N. L. Skeele, J. S. Ko, D. R. Rolison, and J. W. Long, RSC Adv. 11 , 14495 (2021).","PeriodicalId":11461,"journal":{"name":"ECS Meeting Abstracts","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135088684","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}
Alexander George Zestos, Michelle Hadad, Nadine Hadad
{"title":"Electroanalytical Measurement of Steroid Hormone with Carbon Electrode Sensor","authors":"Alexander George Zestos, Michelle Hadad, Nadine Hadad","doi":"10.1149/ma2023-01482526mtgabs","DOIUrl":"https://doi.org/10.1149/ma2023-01482526mtgabs","url":null,"abstract":"Cortisol is a vital steroid hormone that has been known as the “stress hormone,” which is elevated during times of high stress and anxiety. The improved detection of cortisol is critically important as it will help further our understanding of stress during several physiological states. Several methods exist to detect cortisol, however, they suffer from low biocompatibility, spatiotemporal resolution, and are relatively slow. In this study, we developed an assay to measure cortisol with carbon fiber microelectrodes (CFMEs) and fast-scan cyclic voltammetry (FSCV). FSCV is typically utilized to measure small molecule neurotransmitters by producing a readout CV for the specific detection of biomolecules on a fast, subsecond timescale with biocompatible CFMEs. It has seen enhanced utility in measuring peptides and other larger and more complex molecules. We developed a waveform to electro-reduce cortisol at the surface of CFMEs. The sensitivity of cortisol was found to be 5 nA/uM and was adsorption controlled on the surface of CFMEs and stable over several hours. Cortisol was co-detected with several other biomolecules such as dopamine and serotonin, and the waveform was fouling resistant to repeated injections of cortisol on the surface of the CFMEs. Furthermore, we also measured exogenously applied cortisol onto brain tissue and simulated urine to demonstrate biocompatibility and potential use in vivo . The specific biocompatible detection of cortisol with high spatiotemporal resolution will help further elucidate its biological significance and further understand its physiological importance in the brain.","PeriodicalId":11461,"journal":{"name":"ECS Meeting Abstracts","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135088689","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}
Bonho Koo, Jinkyu Chung, Juwon Kim, Hyejeong Hyun, Dimitrios Fraggedakis, Jian Wang, Namdong Kim, Markus Weigand, Tae Joo Shin, Daan Hein Alsem, Norman Salmon, Martin Z. Bazant, Jongwoo Lim
{"title":"High C-Rate Dynamic Lithium (de)Insertion Pathway Investigated via Synchrotron-Based Operando XRD and Operando Scanning x-Ray Microscopy","authors":"Bonho Koo, Jinkyu Chung, Juwon Kim, Hyejeong Hyun, Dimitrios Fraggedakis, Jian Wang, Namdong Kim, Markus Weigand, Tae Joo Shin, Daan Hein Alsem, Norman Salmon, Martin Z. Bazant, Jongwoo Lim","doi":"10.1149/ma2023-01472522mtgabs","DOIUrl":"https://doi.org/10.1149/ma2023-01472522mtgabs","url":null,"abstract":"Lithium-ion insertion kinetics fundamentally hinges upon phase transformation behavior during (dis)charging and understanding the rate-dependent kinetics is crucial for the development of high-power batteries. At high c-rates, kinetic hysteresis is amplified and phase evolution becomes heterogeneous and unpredictable. Specifically, discharge becomes more sluggish than charging of most battery electrodes including LiNi x Mn y Co z O 2 (NMC) and LiFePO 4 (LFP). Here, we developed an operando soft x-ray microscopy to simultaneously observe surface charge transfer and bulk lithium diffusion in facet-controlled individual battery particles over a wide range of cycling rates (0.01 – 10C). Our result unambiguously reveals that dynamic asymmetry between fast charging and discharging originates from auto-inhibitory Li-rich and autocatalytic Li-poor surface domains, respectively. In addition, we developed synchrotron-based operando fast XRD to track phase evolution during fast cycling. We directly observed that sluggish Li diffusion at high Li content induces different phase transformations during charging and discharging, with strong phase separation and homogeneous phase transformation during charging and discharging, respectively. Moreover, by electrochemically manipulating the lithium-ion concentration distribution within NCM particles, phase separation pathway could be redirected to solid-solution kinetics even at 7 C-rate. Our work lays the groundwork for developing high-power applications and ultrafast charging protocols Figure 1","PeriodicalId":11461,"journal":{"name":"ECS Meeting Abstracts","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135088707","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}
Dohyoung Kim, Sang Hun Kim, Jiwon Oh, Yoonmi Nam, Heesu Hwang, Jin-Ha Hwang
{"title":"Application of Machine Learning to In<sub>2</sub>O<sub>3</sub>-Based Semiconducting Oxide Gas Sensors for High-Performance Gas Discrimination Against Ambient Humidity and Temperature Variations","authors":"Dohyoung Kim, Sang Hun Kim, Jiwon Oh, Yoonmi Nam, Heesu Hwang, Jin-Ha Hwang","doi":"10.1149/ma2023-01522614mtgabs","DOIUrl":"https://doi.org/10.1149/ma2023-01522614mtgabs","url":null,"abstract":"Since the advent of the 4 th industrial revolution characteristic of smart living standards, physical and/or chemical sensors have been gaining their academic/industrial interests in association with cloud-based data management, artificial intelligence and big data thanks to ever-increasing computing power and communication technology. In particular, machine learning-operated sensor networks are advancing to offer predictive, prescriptive, and even deductive analytics, overcoming basic descriptive functions. Regardless of the type of sensor, i.e., physical or chemical, homogeneously and/or heterogeneously configured sensor arrays can provide physical status and chemical information that have been impossible to achieve using single-mode sensors alone. This teaming of technology has opened up unprecedented applications that may be possible through sensor network implementation. Electronic nose with semiconducting gas sensors array can be regarded as a promising platform to find new functionality in the recognition of smells and odors through machine learning. Oxide semiconductor gas sensors with high sensitivity, simple structure, rapid response speed, excellent reversibility and facile integration have been widely employed to detect harmful, explosive, and toxic gases but the simple gas sensing mechanism involving charge transfer between the gas and oxide surfaces often leads to a lack of gas selectivity, hampering gas recognition. The machine learning ecosystem is capable of solving the pre-existing drawbacks encountered in chemical sensor domains. However, the recognition of gases under variations in ambient humidity and temperature has barely been investigated, and most studies have focused on the compensation of sensor signals using humidity and temperature sensor. Gas recognition under various humidity conditions by machine learning without the assistance of humidity sensors has never been achieved. Five In 2 O 3 -based semiconducting metal oxide (SMO) gas sensors were combined in the form of sensor arrays with machine learning methodologies with the aim to detecting and discriminating indoor volatile organic compounds (VOCs) such as benzene, xylene, toluene, formaldehyde, and ethanol against humidity and/or temperature variations. The SMO gas sensor performance was evaluated using principal component analysis (PCA) and neural network-based classification in terms of the gas sensor data type/amount, neural network algorithms, sensor combinations, and environmental factors. The PCA analyses revealed the limitations on the discrimination of VOCs under temperature- and/or humidity-interfered gas sensing environments. Gas detection/discrimination could be improved significantly by using neural network-based algorithms, i.e., artificial neural networks (ANNs), deep neural networks (DNNs), and 1-dimensional convolutional neural networks (1D CNNs). The neural network algorithm prediction based on the entire gas sensing/purge transient data outperfor","PeriodicalId":11461,"journal":{"name":"ECS Meeting Abstracts","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135088710","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}
Yifu Chen, Hengzhou Liu, Jungkuk Lee, Shuang Gu, Wenzhen Li
{"title":"(Invited) Green Ammonia-Mediated CO<sub>2</sub> Capture and Direct Electrochemical Reduction to Formate","authors":"Yifu Chen, Hengzhou Liu, Jungkuk Lee, Shuang Gu, Wenzhen Li","doi":"10.1149/ma2023-01392307mtgabs","DOIUrl":"https://doi.org/10.1149/ma2023-01392307mtgabs","url":null,"abstract":"Direct electrochemical conversion of CO 2 capture solutions (instead of gaseous CO 2 ) into valuable chemicals can circumvent the energy-intensive CO 2 regeneration and pressurization steps. While commonly used CO 2 capture agents include alkali and amine solutions, ammonia has been rarely investigated. In another aspect, mismanagement of reactive nitrogen (Nr) in waste has emerged as a major problem in water pollution to our ecosystems, causing severe eutrophication and health concerns. Sustainably recovering Nr [such as nitrate (NO 3 − )-N] and converting it into green ammonia (NH 3 ) could mitigate the environmental impacts of Nr and reduce the NH 3 demand from the carbon-intensive Haber-Bosch process, as well as a possible CO 2 capture agent due to its alkaline nature. In this talk, we will present our rencet research on integration of electrodialysis and electrocatalysis for ammonia synthesis from dilute waste Nr sources, and green ammonia-mediated CO 2 capture (to ammonium bicarbonate, NH 4 HCO 3 ) and subsequent reduction to ammonium formate (NH 4 HCO 2 ) as a new approach to CO 2 capture and utilization (CCU). We have demonstrated a record-high NO 3 − -to-NH 3 performance in a scalable, versatile, and cost-effective membrane-free alkaline electrolyzer (MFAEL): an unprecedented NH 3 partial current density of 4.22 ± 0.25 A cm −2 with a faradaic efficiency of 84.5 ± 4.9%. We also discovered that an ammonium bicarbonate (NH 4 HCO 3 )-fed electrolyzer with an anion exchange membrane (AEM) outperforms the state-of-the-art KHCO 3 electrolyzer with a bipolar membrane (BPM) owing to its favorable thermal decomposition property, which allows for a 3-fold increase in the in situ CO 2 concentration, a maximum 23% increase in formate faradaic efficiency, and a 35% reduction in cell voltage by substituting BPM with the AEM. Our integrated process by combining NH 4 HCO 3 electrolysis with CO 2 capturing by on-site generated green ammonia from the electro-reduction of nitrate in MFAEL has shown a remarkable 99.8% utilization of CO 2 capturing agent. Such a multi-purpose process may offer a sustainable route for the simultaneous removal of N r wastes and streamlined CO 2 capturing and upgrading to valuable chemicals.","PeriodicalId":11461,"journal":{"name":"ECS Meeting Abstracts","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135088722","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 Structural Model for Transient Pt Oxidation during Fuel Cell Start-up Using Electrochemical X-Ray Photoelectron Spectroscopy","authors":"Hassan Nagra, Rik Mom, Axel Knop-Gericke","doi":"10.1149/ma2023-01382205mtgabs","DOIUrl":"https://doi.org/10.1149/ma2023-01382205mtgabs","url":null,"abstract":"Potential spikes during the start-up (SU) and shutdown (SD) of fuel cells are a major cause of platinum (Pt) electrocatalyst degradation, which limits the lifetime of the device. The electrochemical oxidation of Pt that occurs on the cathode during the potential spikes plays a key role in this degradation process. However, the composition of the oxide species formed, as well as their role in catalyst dissolution remains unclear. In this study, we employ a special arrangement of XPS (X-ray Photoelectron Spectroscopy), in which the Pt electrocatalyst is covered by graphene, making the in situ examination of the Pt oxidation/reduction under wet conditions possible. We use this assembly to investigate oxidation state changes of Pt within fuel cell relevant potential window. We show that above 1.1 V RHE , a mixed Pt δ+ /Pt 2+ /Pt 4+ surface oxide is formed, with an average oxidation state that gradually increases as the potential is increased. By comparing a model based on the XPS data to the oxidation charge measured during potential spikes, we show that our description of Pt oxidation is also valid during the transient conditions of fuel cell SU/SD. This is due to the rapid Pt oxidation kinetics during the pulses. As a result of the irreversibility of Pt oxidation, some remnants of oxidized Pt remain at typical fuel cell operating potentials after a pulse. Figure 1","PeriodicalId":11461,"journal":{"name":"ECS Meeting Abstracts","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135088766","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":"(Keynote) Electrochemical CO<sub>2</sub> Reduction on NiNC Single Metal Atom Catalysts Under Alkaline to Acidic pH Conditions","authors":"Peter Strasser","doi":"10.1149/ma2023-01492557mtgabs","DOIUrl":"https://doi.org/10.1149/ma2023-01492557mtgabs","url":null,"abstract":"The science and technology of the direct electrochemical CO 2 reduction reaction on both model electrodes in liquid-electrolyte H-cells and Gas Diffusion Electrodes (GDEs) in flow electrolyzers offer as many formidable challenges as intriguing opportunities. Controlling the selectivity (faradaic efficiency), while maximizing the energy efficiency by lowering the kinetic overpotentials remains key to turn this complex reaction into a practical process embedded in a process chain. In this talk, I will highlight some of our recent advances in the design and characterization of NiNC single site electrocatalysts for the electrochemical reduction of CO 2 to CO and CO 2 /CO mixed feeds into value-added fuels and chemicals in H-cell and Gas Diffusion Electrode (GDE) single cell electrolyzers. Further focus will be placed on the diagnosis of carbonate transport processes during electrolyzer cell operation using the experimentally accessible carbon crossover coefficient, CCC. Performance and its limitations of cell operation in alkaline and acid conditions will be contrasted and discussed.","PeriodicalId":11461,"journal":{"name":"ECS Meeting Abstracts","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135088771","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}