bluuebunny/crossref_metadata_2025_split huggingface dataset:
Electrochemical Oxidation of Biomass-Derived Wastewaters for Simultaneous H2 Production
Authors: Boruah Bhanupriya , Bhatwadekar Swanand Sadashiv , Riedel Nickolas W , Strange Lyndi E. , Lopez-Ruiz Juan A. 
Published: December 2024

As the world continues to search for new ways to support the growth of a sustainable energy future, biomass conversion emerges as a potential method to produce carbon-neutral biofuels and biochemicals. For example, hydrothermal liquefaction (HTL) can be used to convert biomass- and waste-derived feedstocks into bio-crudes, which then undergo catalytic upgrading with exogenous molecular hydrogen (H2) for biofuel production (gasoline, diesel, jet oil.). HTL also generates an aqueous phase (HTL-AP) that contains up to 5 wt.% of organic compounds that cannot be treated with traditional wastewater treatment technologies (e.g., anaerobic digestion). Instead, we propose to use the HTL-AP to in situ generate the H2 needed for biofuel production via the electrochemical oxidation (ECO) of HTL-AP.1
2

In this work, we evaluate how the HTL-AP composition of both organic and inorganic compounds as well as the applied potential affect the ECO activity, energy consumption, and electrode stability. Initially, our electrochemical experiments were performed in batch cells to understand the performance of anode and cathode for ECO and H2 generation in terms of onset potential, exchange current densities, and Tafel slopes. This was followed by a demonstration of ECO long-term stability in a continuous-flow electrolyzer. Our studies show that the presence of organic compounds decreases the current density at high potential region but increases at low potential region for some HTL-AP. The anode stability increased from 24 h to >3,000 h by optimizing the applied potential and the source of HTL-AP. However, the cathode performance and stability remained unaffected by the HTL-AP and potential. The resulting energy requirement for COD removal (kWh/kgCOD) of the optimized system is lower than that of the traditional wastewater treatment process. Furthermore, the energy requirement for H2 production (kWh/kgH2) is found to be almost half compared to the commercial electrolyzer.

References

(1) Andrews, E.; Lopez-Ruiz, J. A.; Egbert, J. D.; Koh, K.; Sanyal, U.; Song, M.; Li, D.; Karkamkar, A. J.; Derewinski, M. A.; Holladay, J. Performance of base and noble metals for electrocatalytic hydrogenation of bio-oil-derived oxygenated compounds. ACS sustainable chemistry & engineering
2020, 8 (11), 4407-4418.
(2) Qiu, Y.; Lopez-Ruiz, J. A.; Zhu, G.; Engelhard, M. H.; Gutiérrez, O. Y.; Holladay, J. D. Electrocatalytic decarboxylation of carboxylic acids over RuO2 and Pt nanoparticles. Applied Catalysis B: Environmental
2022, 305, 121060.

Figure 1
Quantifying Aging-Induced Irreversible Volume Change of Porous Electrodes
Authors: Garrick Taylor R. , Miao Yong , Macciomei Eric , Fernandez Miguel , Weidner John W. 
Published: December 2024

Automotive manufacturers are working to improve cell and pack design by increasing their performance, durability, and range. One of the critical factors to consider as the industry moves towards materials with higher energy density is the ability to consider the irreversible volume change characteristic of the accelerated SEI layer growth tied to the large volume change and particle cracking typically associated with active material strain. Here, we add to a previously developed mechano-electrochemical model[1-8] to more practically understand the impact of irreversible volume change, primarily assigned to SEI layer growth. As the time from initial design to manufacture of electric vehicle is decreased in order to rapidly respond to consumer demands and widespread adoption of electric vehicles, the ability to link aging and volume change to end of life vehicle requirements using virtual tools is critical.[9] In this study[10], we apply a model to determine the irreversible volume change at the electrode and cell level, allowing for virtual design iterations to predict the volume change at battery cell aged states, and probe possible changes in the SEI layer over life.
References:

T. R. Garrick, K. Kanneganti, X. Huang and J. W. Weidner, J Electrochem Soc, 161, E3297 (2014).

T. R. Garrick, Y. Dai, K. Higa, V. Srinivasan and J. W. Weidner, ECS Transactions, 72, 11 (2016).

T. R. Garrick, X. Huang, V. Srinivasan and J. W. Weidner, J Electrochem Soc, 164, E3552 (2017).

T. R. Garrick, K. Higa, S.-L. Wu, Y. Dai, X. Huang, V. Srinivasan and J. W. Weidner, J Electrochem Soc, 164, E3592 (2017).

D. J. Pereira, J. W. Weidner and T. R. Garrick, J Electrochem Soc, 166, A1251 (2019).

D. J. Pereira, M. A. Fernandez, K. C. Streng, X. X. Hou, X. Gao, J. W. Weidner and T. R. Garrick, J Electrochem Soc, 167, 080515 (2020).

D. J. Pereira, A. M. Aleman, J. W. Weidner and T. R. Garrick, J Electrochem Soc, 169, 020577 (2022).

T. R. Garrick, M. A. Fernandez, M. Verbrugge, C. Labaza, R. Mollah, B. J. Koch, M. Jones, J. Gao, X. Gao and N. Irish, J. Electrochem. Soc., 170060548 (2023)

T. R. Garrick, Y. Zeng, J. B. Siegel, and V. R. Subramanian, J. Electrochem. Soc., 170113502 (2023)

T. R. Garrick, Y. Miao, E. Macciomei, M. Fernandez and J. W. Weidner, J Electrochem Soc, 170, 100513 (2023).
(Invited) Elucidating Redox Mechanisms in Battery Materials through Resonant Inelastic X-Ray Spectroscopy (RIXS)
Authors: Radin Max , Kunitsa Alexander 
Published: December 2024

Novel battery materials offer the promise of greatly increased energy densities for automative and other applications. However, their practical adoption is often limited by problems in electrochemical performance, such as poor rate capability, voltaic efficiency, and cyclability. Resonant Inelastic X-ray Spectroscopy (RIXS) has become a valuable tool for understanding the redox mechanisms in such materials, representing a first step towards solving problems in electrochemical performance. In many cases, however, the underlying origins of RIXS features are unclear. For example, redox mechanisms in Li-rich cathodes are associated with several absorption and emission features in oxygen RIXS measurements, but a clear picture of what redox mechanisms create these features remains elusive.
As a step towards identifying redox mechanisms in Li-rich and related cathode materials, this presentation reviews existing theories of reaction mechanisms in these compounds, revisits experimental RIXS data on these materials and related oxides, and presents ab initio calculations evaluating possible origins of commonly observed features. Results suggest that some features could arise from molecular oxygen residing in low-symmetry environments. Additionally, prospects for using error-corrected quantum computation to more accurately model such electronic structure problems will be discussed.
Leveraging Molecular Dynamics to Improve Porous Electrode Theory Modeling Predictions of Lithium-Ion Battery Cells
Authors: Dix Sean T. , Lowe Jeffrey , Rashvand Avei Mehdi , Garrick Taylor R. 
Published: December 2024

Lithium-ion battery cell modeling using physics-based approaches such as porous electrode theory is a powerful tool for battery design and performance analysis, both at the battery cell and system level1. Cell metrics such as resistance and thermal performance can be quickly calculated in a pseudo-two-dimensional (P2D) framework. For engineering of electric vehicle batteries, speed and fidelity of electrochemical models is paramount in a competitive landscape. Physics-based models allow for high fidelity but require detailed knowledge of the cell component material properties. Acquiring these material characteristics typically requires time-consuming and expensive experiments limiting the ability to quickly screen through cell designs. One approach to circumvent costly experiments is to use molecular dynamics to calculate electrolyte transport properties. We demonstrate how cell modeling using simulated transport properties enables predictions of cell level metrics, allowing for experiment-free component screening. We also show how the variation in transport property predictions from molecular dynamics affects the final cell level performance predictions2.
References

T. R. Garrick, Y. Zeng, J. B. Siegel, and V. R. Subramanian, J. Electrochem. Soc., 170, 113502 (2023).

S. T. Dix, J. S. Lowe, M. R. Avei, and T. R. Garrick, J. Electrochem. Soc., 170, 083503 (2023).
(Invited) Nonlinear Frequency Response Analysis – Basics and Application for Battery Analysis
Authors: Krewer Ulrike , Weber Andre , Ulrich Julian , Chan Hoon Seng 
Published: December 2024

Nonlinear frequency response analysis (NFRA), also known as nonlinear impedance spectroscopy is the younger, less well-known sibling of impedance spectroscopy (EIS). In contrast to EIS, a large sinusoidal current or potential input is used; the output signal then contains higher harmonics, which are a nonlinear fingerprint of the electrochemical system under investigation. Why is this nonlinear response of practical relevance? Because electrochemical reactions have typically a nonlinear relation of current and potential. NFRA thus allows to discriminate between different reactions that give a similar linear response (i.e. EIS), to identify and parameterise reaction kinetics or surface/degradation changes, or to simply check if a process in EIS is nonlinear. Recent applications comprise batteries, electrosyntheses, and fuel cells. [1]
This talk thrives to make NFRA more accessible to the electrochemistry and battery community. It introduces the NFRA technique (left Fig.) and its application to Li-ion batteries [3-6]. It gives an insight how to conduct reliable measurements, and which nonlinearities can be expected from reaction and transport processes [2]. Applied to Li-ion batteries, i.a. the potential for state-of-health estimation [3], for uniquely detecting Li-Plating (right Fig) or in-depth analysis on the impact of particle size on aging [5] is demonstrated. Models are shown to aid interpreting the NFR spectra. [6]

Figure. Illustration of nonlinear frequency response analysis [2] (left) and spectra showing clear changes between plating (-10°C) vs. classical aging (25°C) [4](right).

References:

[1] Vidakovic-Koch et al., Curr. Opin. Electrochem. 30, 100851, 2021
[2] Wolff et al., Europ. Phys. J. - ST 227 (18), 2617-2640, 2019.
[3] Chan et al., J. Power Sources 542, 231814, 2022
[4] Harting, Wolff, Krewer, Electrochim. Acta 281, 378-385, 2018
[5] Chan et al., Batteries Supercap. 6(10), e202300203, 2023
[6] Wolff et al., Electrochim. Acta 260, 614-622, 2018

Figure 1
Impedance Analysis of Ultramicroelectrodes for Neural Stimulation
Authors: Biney Bernard W. , Carvalho Sophia , Eluagu Cynthia C. , Olivo Elizabeth , Dong QiWei , Wu Yupeng , Cogan Stuart , Otto Kevin John , Orazem Mark E. 
Published: December 2024

Most neural stimulation techniques rely on macroelectrodes, which generate electric fields that impact neuronal groups rather than specific neurons, often resulting in unintended side effects.1,2 Ultramicroelectrodes (UMEs) offer enhanced spatial resolution, holding promise for precise targeting of specific neurons to optimize therapeutic outcomes while mitigating adverse effects. However, ultramicroelectrodes present challenges. For example, delivery of required charge may require current densities that can damage the electrode or adjacent tissue.
Impedance measurements of UMEs were conducted and analyzed to understand stimulation currents and potential damage to the electrodes and tissue. The measurement-model technique was used to identify the optimal frequency range for regression analysis, to quantify the stochastic error structure, and to identify inconsistencies with the Kramers-Kronig relations. Understanding of the error structure is vital for interpretation.3 The regressions were weighted using the inverse of the variance for the stochastic error structures, and quality of fits were determined by the weighted chi-square statistic.
Process modeling was used to understand and characterize the underlying physical and chemical processes that occur at the electrode-electrolyte interface and electrode-tissue interface during neural stimulation. Constant-phase element (CPE) parameters, Q and alpha, corresponding to the behavior of the electrode-tissue interface, were obtained from this model. In addition, parameters associated with a capacitive loop were identified. Work is in progress to identify the origin of this loop.
References
(1) Otto, K. J.; Schmidt, C. E. Neuron-Targeted Electrical Modulation. Science. March 20, 2020, pp 1303–1304. https://doi.org/10.1126/science.abb0216.
(2) Orazem, M. E.; Otto, K. J., Alexander, C. L., Electrochemistry in Action-Engineering the Neuronal Response to Electrical Microstimulation. Electrochemical Society Interface
2023, 32 (1), 40–42. https://doi.org/10.1149/2.F06231IF.
(3) Orazem, M. E.; Agarwal, P.; Jansen, A. N.; Wojcik, P. T.; Garcia-Rubio, L. H. Development of Physico-Chemical Models for Electrochemical Impedance Spectroscopy. Electrochim Acta
1993, 38 (14), 1903–1911.
Phase-Selective Synthesis of Cobalt Oxide Materials Via Electrochemical Chloride-Mediated Oxidation
Authors: Kim MinJeong , Nam Ki Min , Park Gisang , Park Joon Yong 
Published: December 2024

The rapid growth of the global economy has led to an elevating human demand for energy and chemicals, which is heavily reliant on the utilization and conversion of fossil fuels. Electrochemical conversion is arising as a viable strategy for synthesizing a various high-value chemicals thanks to the mild operation conditions, adjustable selectivity, and potential for scalability in industrial settings. Chlor-alkali process can be utilized for removing microorganisms, disinfecting water, and so on. Furthermore, in an electrochemical system, the oxidation half reaction of the chloride oxidation can be coupled with a value-added reduction in half reaction, such as H2 evolution, N2 reduction, CO2 reduction, and organic reduction.
In this study, β-CoOOH and γ-CoOOH, distinct cobalt oxyhydroxides, were synthesized via a chloride-mediated electrochemical oxidation process. This method employed heterogeneous reactions, where the oxidation of metal hydroxides was facilitated by electrochemically generated oxidants—active chlorine species—directly formed on the electrode surface through the oxidation of chloride ions. Characterization through X-ray diffraction (XRD) confirmed the synthesis of these two distinct metal oxide phases, elucidating their phase purity and crystal structures. Furthermore, the adjustable surface morphology and composition of intercalated ions were observed under varying electrosynthetic conditions. This synthetic strategy can be extended to the fabrication of other metal oxides, including manganese oxides. The resulting cobalt oxyhydroxide and manganese dioxide materials display versatile properties suitable for a wide range of applications in energy, environmental, and biotechnological fields.
Structural Regulation and Advanced Transmission Electron Microscopy Characterization of the Oxygen Reduction Reaction Electrocatalysts
Authors: Gong Mingxing 
Published: December 2024

Fuel cells (FCs) are regarded as the most promising green energy conversion technology in the 21st century because of their advantages. However, the industrialization process of FCs is restricted by several key problems, one of which is the cathode catalyst. The Oxygen Reduction Reaction (ORR) of FCs is a complex process involving 4 electrons, which has sluggish kinetics and high over-potential. Therefore, it is usually necessary to use a large number of precious metal platinum (Pt) catalysts to improve the reaction efficiency, but the characteristics of small reserves of Pt, high price, and easy to be poisoned and deactivated increase the operating cost of the whole system. It is imperative to develop substitutes for non-Pt-based ORR catalysts and reveal their structure-activity relationship with advanced characterization techniques.
There are two ways to solve this problem: one is to improve the utilization rate of platinum-based catalyst, the other is to develop non-platinum-based catalysts. In terms of improving the utilization rate of Pt, our research group mainly constructed new Pt-based ordered intermetallic compound catalytic materials, and improved the surface structure, alloying degree and electronic structure of Pt-based catalysts by changing the atomic types, proportions and post-treatment temperatures of Pt and transition metals, so as to regulate their electrocatalytic properties. On the other hand, the morphology control of ordered intermetallic compounds has always been a major challenge in this field, and we have made a preliminary attempt in the morphology control. At the same time, with the help of modern characterization techniques, it is of great significance to study the changes of structure and components during the service of Pd-based catalysts, and to understand their failure behavior and performance attenuation mechanism for the subsequent optimization and commercialization of Pd-based catalysts. Among them, visualization technology based on transmission electron microscopy (TEM) has become a research hotspot because it can directly observe the failure process of catalysts in service.
Influence of Process Parameters on Electrochemical CO2 Reduction to C2+ Products
Authors: Pradellok Florian , Hüwels Jan , Wessling Matthias , Keller Robert 
Published: December 2024

With an increasing concentration of carbon dioxide (CO2) in the atmosphere, greenhouse gas emissions must be mitigated to prevent further global warming. A promising technology to achieve this goal is the electrochemical reduction of CO2. Thereby, CO2 is converted to value-added chemicals using renewable electrical energy. Ethylene or ethanol are valuable C2+ products, which may be synthesized with copper based catalysts. However, many studies lack control of temperature and CO2 excess factors as well as the application of industrially relevant current densities above 200 mA cm-2. Additionally, recent literature proposes benefits of pulsed operation as opposed to static operation. Pulsed operation employing gas diffusion electrodes at elevated current densities must be studied in more detail to assess the full potential of dynamic operation.
This work demonstrates the continuous electrochemical reduction of CO2 to C2+ products at industrially relevant conditions. Current densities from 100 mA cm-2 to 400 mA cm-2 are applied to an electrochemical flow cell with a geometrical electrode area of 25 cm2. CuO nanoparticles were deposited on gas diffusion layers as catalyst via automated ultrasonic spray-coating. Throughout electrolysis experiments, constant electrolyte temperatures of 20 °C or 40 °C and constant CO2 excess factors of 2 or 5 are maintained. In contrast to statically applied current, pulsed current experiments focus on enhanced CO2 mass transfer to the catalyst layer.
Throughout static electrolysis, an increase in Faradaic efficiency from 30 % to 60 % for C2+ products is observed when the current density is increased from 100 mA cm-2 to 400 mA cm-2. This is attributed to a more alkaline pH in the catalyst layer caused by high current densities which is favorable to produce C2+ products. Furthermore, it was found that an electrolyte bulk temperature of 20 °C increases the Faradaic efficiency for C2+ products compared to experiments conducted at 40 °C. We hypothesize that this is due to less intermediate desorption from the catalyst. Furthermore, the reduction of CO2 excess leads to an increase in Faradaic efficiency for C2+ products. The highest Faradaic efficiency to C2+ products was found at 400 mA cm-2 with an electrolyte bulk temperature of 20 °C at a CO2 excess factor of 2. Additionally, the influence of pulsed current on the yield of C2+ products was investigated and different pulsing procedures were tested. The results show that pulsed current operation reduces the parasitic hydrogen evolution. However, the C2+ formation was not increased compared to static operation in an electrochemical flow cell at high current densities. In summary, this work shows how different process parameters influence the product distribution in electrochemical CO2 reduction on a CuO catalyst to improve the selectivity towards C2+ products. This is a further step towards a sustainable process to produce platform chemicals.
Zero-Emission Hydrogen Production at on-Site Hydrogen Refueling Station Using Excess Electricity in Kyushu
Authors: Tachikawa Yuya , Kobayashi Tomotake , Kawakami Keiji , Matsuo Yudai , Kumamoto Yoshiyasu , Morishima Ryoko , Yasutake Masahiro , Sasaki Kazunari 
Published: December 2024

Introduction

In Japan, the shift from CO2-emitting energy sources toward carbon neutrality is proceeding rapidly. Approximately 27% of the electricity generated in Japan is generated using zero CO2 emission energy sources including renewable energy. Especially in Kyushu island, located in the western region of Japan, approximately 58% of electric energy is provided by zero-emission power generation, and energy conversion is steadily progressing toward achieving carbon neutrality by 2050. The introduction of offshore wind power and other renewable energy facilities is planned for the Kyushu region in the future, which is expected to further reduce CO2 emissions in the power generation sector. Meanwhile, energy management issues have become apparent, such as the fact that some electricity generated cannot be used due to reasons such as the imbalance between supply and demand of electricity.
In this study, to investigate methods to store and use excess electricity and resolve the imbalance, we aims to clarify the effect of hydrogen production system on imbalance resolution. To evaluate its effect, demonstration studies are currently underway at an on-site hydrogen production type hydrogen station.

Research Issues

In this demonstration study, an on-site hydrogen station has been installed and demonstrated that can produce hydrogen using a water electrolyzer(Hitachi Zosen Corp.), compress hydrogen using a hydrogen compressor(Hydro-Pac. Inc.), and fill hydrogen using a hydrogen supply unit (TATSUNO Corp.) with a pre-cooling heat exchanger (ORION Machinery Co., Ltd.). Energy management equipment that makes effective use of electric power that cannot be used even if generated and equipment that associates the power required when operating facilities with zero-emission power sources have also been installed. And the realization of carbon neutrality for the entire hydrogen station's power consumption, its component power sources, and excess power usage status are being analyzed and examined in this study.
This presentation will report the results and its analysis of the demonstration of hydrogen production by zero-emission power source using the above facilities.

Acknowledgement

This research was supported by New Energy and Industrial Technology Development Organization (NEDO), project No. JPNP14026.