bluuebunny/crossref_metadata_2025_split huggingface dataset:
Engineering Lung-Inspired Flow Field Geometries for Redox Flow Batteries with Stereolithography 3D Printing
Authors: Muñoz Perales Vanesa , van der Heijden Maxime , Garcia-Salaberri Pablo A. , Vera Marcos , Forner-Cuenca Antoni 
Published: September 2023

Redox flow batteries are a promising electrochemical technology for low-cost, scalable and long-duration energy storage, but their energy market penetration is hampered by elevated costs1,2. One effective strategy is to increase the overall efficiency of the electrochemical stack. At the core of the electrochemical cells, the design of the flow fields—which distribute the electrolyte through the porous electrodes—determines, in combination with the electrode microstructure, the performance of the system3. To date, current designs are inspired on fuel cell technologies but have not been engineered for redox flow cells where single-phase reactive flows are sustained4.
In this work, we tailor lung-inspired flow field geometries for carbon paper electrodes using stereolithography 3D printing5,6. We propose two new lung-inspired geometries—with two and three channel levels—and compare them to a baseline interdigitated flow field. A two-step process based on stereolithography 3D printing followed by the application of a conductive coating is used to manufacture these complex flow field geometries. We employ a suite of electrochemical (i.e., polarization and electrochemical impedance spectroscopy) and fluid dynamic (pressure drop measurement) techniques together with numerical modelling to elucidate flow architecture-performance relationships. We find that lung-inspired structural patterns homogenize the electrolyte distribution into the electrode, accessing a larger electrode reaction area. These fractal geometries can outperform traditional interdigitated flow fields, providing a more favourable balance between low pressure drop and high electrochemical performance (Figure 1). In this talk, I aim to leverage lung-inspired flow field geometries as a promising prospect for engineering advanced flow cell architectures for emerging electrochemical devices.

References

1 E. Sánchez-Díez, J. Power Sources, 2021, 23.
2 L. F. Arenas, C. Ponce de León and F. C. Walsh, J. Energy Storage, 2017, 11, 119–153.
3 R. M. Darling and M. L. Perry, J. Electrochem. Soc., 2014, 161, A1381–A1387.
4 C. R. Dennison, E. Agar, B. Akuzum and E. C. Kumbur, J. Electrochem. Soc., 2016, 163, A5163–A5169.
5 J. Marschewski, L. Brenner, N. Ebejer, P. Ruch, B. Michel and D. Poulikakos, Energy Env. Sci, 2017, 10, 780–787.
6 M. P. Browne, E. Redondo and M. Pumera, Chem.
Rev., 2020, 120, 2783–2810.

Figure 1
Recycling of PFSA-Based Membranes and Their Re-Application in PEM Fuel Cells
Authors: Kutter Maximilian , Greve Christopher , Rosin Andreas , Herzig Eva M. , Gerdes Thorsten , Roth Christina 
Published: September 2023

The commercialization of PEM fuel cells offers a promising opportunity to overcome our dependence on fossil fuels and provides an attractive alternative for automotive and stationary power applications.[1] However, PEMFCs are still costly in production, with the main cost factor due to the fabrication of the perfluorosulfonic acid (PFSA)-based proton exchange membrane and the noble metal catalysts.[2,3] Recycling of these components could increase the economic attractiveness of PEMFCs. However, while the high resistance of the ionomer membrane to thermal and chemical degradation is favorable for their use in fuel cells, it also makes membrane recycling a major challenge.
Here, we present a newly developed recycling strategy to recover PFSA-based membranes after operation by a hydrothermal treatment. Both short side chain (SSC) and long side chain (LSC) ionomers with EWs of 800 and 1000 were investigated. In contrast to previously published methods, we were able to recover the PFSA ionomer by using water instead of high-boiling organic solvents, such as DMF or DMSO.[4,5] The recycled membranes were obtained from the recycled PFSA ionomer solution by doctor-blading. They were investigated by in-situ Raman techniques for studying the water uptake and analyzed by IR and small-angle X-ray scattering (SAXS) techniques to get a more detailed insight into their morphology. In single cell tests at standard (80 °C) and enhanced (up to 130 °C) PEMFC operating temperatures, the recycled membranes showed an increased cell performance as compared to the pristine 3M-800EW membrane. Solid-state NMR measurements confirmed that no chemical changes in the membrane occurred due to the heat-treatment process.
We assume that the observed performance boost can be attributed to an increased water uptake and retention. Furthermore, a change in the polymer matrix formation may be responsible for the observed behavior, which led to an expanded water filled channel structure, where water can accumulate to facilitate proton diffusion as H3O+ through the channels. To confirm this assumption, the morphology of the recycled membranes will be investigated by in situ SAXS measurements at different temperatures and degrees of hydration.
[1] I. Staffell, D. Scamman, A. Velazquez Abad, P. Balcombe, P. E. Dodds, P. Ekins, N. Shah, K. R. Ward, Energy Environ. Sci.
2019, 12, 463–491.
[2] J. Fan, M. Chen, Z. Zhao, Z. Zhang, S. Ye, S. Xu, H. Wang, H. Li, Nat. Energy
2021, 6, 475–486.
[3] D. Papageorgopoulos, Fuel Cell R&D Overview. 2019 Annual Merit Review and Peer Evaluation Meeting, 2019.
[4] Q. Xu, X. Chen, S. Wang, C. Guo, Y. Niu, R. Zuo, Z. Yang, Y. Zhou, C. Xu, Energies
2022, 15, 8717.
[5] H. F. Xu, X. Wang, Z. G. Shao, I. M. Hsing, J. Appl. Electrochem.
2002, 32, 1337–1340.
Oxidative Desorption of Adsorbed Sulfur on Platinum Surfaces Modified with Cerium Species
Authors: Morooka Tetsuro , Nakanishi Takuya , Masuda Takuya 
Published: September 2023

In polymer electrolyte membrane fuel cells, hydrogen oxidation and oxygen reduction reaction occur at platinum (Pt) catalyst surface. Pollutants in air and hydrogen fuel, especially, sulfur (S) species, often strongly adsorb on the Pt surface, resulting in reduced electrochemically active surface area, namely poisoning effect. Because such poisoning causes the significant deterioration of cell performance and durability, understanding and control of adsorption behavior of S species are very important. Thus, it is necessary to develop a new method or material for recovery from S poisoning in anode.
In this study, a Pt(111) single crystal electrode was modified with a Ce species and its electrochemical property was compared with a bare Pt electrode. The modification with Ce species was accomplished by immersion in a Ce (NO3)3 + HClO4 aqueous solution with bubbling Ar + H2 gas through the solution for 1 h or applying the potential at -0.2 V in a Ce (NO3)3 + HClO4 aqueous solution. The modification of Pt(111) electrode with Ce species drastically changed the electrochemical responses; hydrogen adsorption/desorption waves become smaller and adsorption/desorption waves of hydroxy group disappeared because of the presence of adsorbed Ce species. Adsorbed species was identified as a Ce3+ ion by XANES spectrum.
After the bare Pt(111) electrode was immersed in an aqueous solution containing sodium sulfide, three types of adsorbed S species, HS and S/Sn were detected by XPS. HS was reductively desorbed from Pt electrode surface at potential cycling between 0.0 and 0.2 V vs. RHE (-0.2 and 0.0 V vs. Ag/AgCl). S/Sn species remained during this potential cycling but oxidatively desorbed when the positive limit of potential cycling was 0.6 V vs. RHE (0.8 V vs. Ag/AgCl). The hydrogen adsorption/desorption current gradually increased as repeating potential cycling between 0.0 and 1.0 V vs. RHE (-0.2 V and 0.8 V vs. Ag/AgCl).
After the Ce-modified Pt(111) electrode was immersed in an aqueous solution containing sodium sulfide, an anodic current assignable to the oxidative desorption of S species appeared at 0.3 V. The peak current decreased as repeating potential cycling between 0.0 and 0.7 V vs. RHE (-0.2 V and 0.5 V vs. Ag/AgCl). After this potential cycling, the peak area of S2p region of XPS spectra decreased as well as Ce 3d peak. The oxidative desorption of S and Sn on the Ce-modified Pt(111) electrode took place at 0.5 V vs RHE (0.3 V vs. Ag/AgCl) which is much more negative than that of bare Pt(111) electrode (1.0 V vs. RHE (0.8 V vs. Ag/AgCl)). Thus, modification of Pt(111) electrode with Ce species promoted the oxidative desorption of S species.
(Invited) Recent Development of Electrochemical Nitrate Reduction
Authors: Lim Jeonghoon , McCloskey Bryan D. , Lee Seung Woo , Hatzell Marta 
Published: September 2023

Understanding the complexities of nitrogen cycle is critical because when the cycle is not in balance, excess reduced and oxidized nitrogen compounds could result in harmful impacts to life. Electrocatalytic conversion of waste nitrate (NO3
-) to benign dinitrogen (N2) and ammonia (NH3) fuel is an appealing strategy that may easily integrate with renewable energy. The process does not require chemical addition and thus requires operating costs lower than thermal routes. Nearly all nitrogen-based fertilizers rely on ammonia as a feedstock, and thus the demand for this chemical is heavily dependent on the global population and food demand. Over the next three decades, the global population will continue to dictate the market size and value for ammonia, which consequently will have a significant impact on our energy infrastructure. While electrochemical nitrogen reduction reaction (NRR) requires multiple proton and electron transfer process, ammonia production from nitrate reduction (NO3RR) is catalytic easier than NRR because the adsorbed/activated ion reactants (nitrate and nitrite) have an advantage of a lower dissociation energy for the N−O and N=O bonds (204 and 607 kJ mol-1) than that of N≡N bond (941 kJ mol-1). The synergistic effect between Cu and Pd has shown a high nitrate conversion yield and nitrogen selectivity. Engineering the Pd and Cu sites is critical but examination of the use of secondary metals in shape-controlled nanoparticle and atomic reconstruction are rare.
Here, we controlled Cu surface coverage on Pd nanocube nanoparticle to steer the selectivity between nitrogen and ammonia. In addition, the engineered the atomic structure of Pd and Cu nanoparticles showed high nitrate conversion yield, excellent dinitrogen selectivity, and outstanding cyclic stability. This study provides insights into the rational design of NO3RR electrocatalyst for efficiently transforming nitrate into nitrogen and ammonia.
(Digital Presentation) SOFC - Enabler for Highly Efficient Power Generation
Authors: Reiter Bernd 
Published: September 2023

SOFC technology offers power generation with very high efficiencies > 60 %. This leads to a high future demand for decentralized power generation for a secure energy supply.
Based on the current extreme load shedding in South Africa, the SOFC System industrialization between AVL and Mitochondria will be presented.
In addition, SOFC in marine applications will be discussed:
In April 2018, the IMO Marine Environment Protection Committee (MEPC) adopted a first strategy to reduce greenhouse gas emissions from international shipping. The first strategy defined the following targets: Reduce CO2 emissions by 40% by 2030 and by 70% by 2050 compared to 2008 levels, and reduce total greenhouse gas emissions from shipping by at least 50% by 2050.
For some applications, fuel cell technologies for propulsion and auxiliary power are seen as one of the most promising solutions to achieve not only decarbonization but also other emission reduction targets in maritime transport. Fuel cell systems are considered serious competitors to internal combustion engines for several reasons: high electrical efficiency of 60% at about 25% load, low emissions, and nearly silent operation
An Atomic Scale Simulation Framework to Decipher the Complex, High-Temperature Solid Oxide Electrolysis Cell Electro-Chemistries
Authors: Hossain Md Jamil , Pawar Gorakh Machindranath , Gaikwad Prashik , Shin Yun Kyung , Schulze Jessica , Penrod Kate , van Duin Adri 
Published: September 2023

Solid oxide electrolysis cells (SOECs) have received a significant attention due to their high
hydrogen (H2) generation efficiency. However, the major scientific challenges such as low
faradaic efficiency of SOECs affects the costs per kilogram of H2 and the large-scale adoption of
H2 as a fuel. Therefore, it is imperative to address the fundamental issues surrounding the low
faradaic efficiency bottleneck and pave the way for a better SOEC design with a relatively higher
faradaic efficiency. In the present research, we present eReaxFF atomic scale simulations
workflow that can reproduce quantum mechanical (QM) calculations on relevant condensed
phase and cluster systems of solid oxide materials describing oxygen vacancies, vacancy
migrations, water adsorption, water splitting and hydrogen generation on the solid oxide material
surfaces in a typical electrocatalysis process. We used barium zirconate doped with 20 mol% of
yttrium (BZY20) solid oxide as model system. Using the developed eReaxFF force field, we
performed zero-voltage molecular dynamics simulations to observe water adsorption and the
steps leading to the eventual hydrogen production. In addition, the introduction of explicit
electron concept to the force field led to the understanding of the non-zero-voltage effects on
hydrogen generation. Based on our simulation results, we conclude that this force field opens an
avenue to simulate electron conductivity, electron leakage and provide us a far-reaching
molecular understanding of improving the faradaic efficiency of SOECs.
Technology Development for Hydrogen Production Using Nuclear Energy
Authors: Li Hongqiang , Stolberg Lorne , Patel Jayesh , Ibeh Blessing , Vega Adrian , Suppiah Sam 
Published: September 2023

Nuclear energy is a low-carbon energy source which can provide both electricity and high-temperature heat. Nuclear-based hydrogen production offers a unique opportunity to mitigate carbon emissions. Canadian Nuclear Laboratories (CNL) has been actively developing technologies for nuclear hydrogen production. This poster will highlight CNL’s capability and achievements on the Cu-Cl thermochemical process (CNL trademarked as HCuTECTM) and Solid oxide electrolysis (SOE).
HCuTECTM has four main steps in the process: Electrolysis, Separation, Hydrolysis and Thermolysis. The maximum temperature of the HCuTECTM process is 530 oC, which is lower than other thermochemical processes and makes its coupling with some small modular reactors and the supercritical water nuclear reactor ideal since these reactors can supply heat above 600 oC. CNL has extensively studied these individual steps and demonstrated an integrated laboratory system (shown in Figure 1) with a hydrogen production capacity of 100 g/d. CNL is interested in scaling up the process with industrial partners.
SOE is also being researched and advanced for hydrogen and clean fuel production at CNL. Current effort is focused on the materials development for oxygen conducting cells. Several CNL cells were made with in-house materials and tested on single cell stations. Preliminary results of CNL cells showed very promising performance for hydrogen production. In the meantime, CNL is assessing the economic benefit of different options to integrate SOE with high-temperature nuclear reactors for both hydrogen and clean fuel production.

Figure 1
Electro-Oxidative Polymerization of Aromatic Monomers without an Electric Power Supply
Authors: Inagi Shinsuke , Iwai Suguru 
Published: September 2023

Electrochemistry is a powerful tool for organic synthesis based on electron transfer-driven reactions at the substrate/electrode interface. The use of electricity for synthetic reactions without the need for hazardous chemical oxidants and reductants is recognized as a green and sustainable approach. We have recently developed a split bipolar electrode (s-BPE) system [1], in which the redox reactions can be driven in a low electrolyte concentration, with batch [2,3] and flow [4] cells. Herein, we report a novel s-BPE system for organic electrosynthesis driven under a streaming potential condition with a pressure flow. As a proof-of-concept study on electrosynthesis without an electric power supply, electrochemical oxidative polymerization of aromatic monomers such as pyrrole successfully yielded the corresponding polymer films on an electrode surface at the upstream, which acted as an anode [5].
[1] Shida, N.; Zhou, Y.; Inagi, S. Chem. Res.
2019, 52, 2598-2608.
[2] Miyamoto, K.; Nishiyama, H.; Tomita, I.; Inagi, S. ChemElectroChem
2019, 6, 97-100.
[3] Shida, N.; Villani, E.; Sanuki, M.; Miyamoto, K.; Gotou, A.; Isogai, I.; Yamauchi, A.; Fuchigami, T.; Tomita, I.; Inagi, S. Electrochemistry, 2021, 89, 476-479.
[4] Sakagami, H.; Takenaka, H.; Iwai, S.; Shida, N.; Villani, E.; Gotou, A.; Isogai, T.; Yamauchi, A.; Kishikawa, Y.; Fuchigami, T.; Tomita, I.; Inagi, S. ChemElectroChem, 2022, 9, e202200084
[5] Iwai, S.; Suzuki, T.; Sakagami, H. Miyamoto, K.; Chen, Z.; Konishi, M.; Villani, E.; Shida, N.; Tomita, I.; Inagi, S. Commun. Chem., 2022, 5, 66.
Development of a Small Molecule Hydrogen Evolution Catalyst
Authors: Karr Dylan Thomas Mills , Pochkhua Luka , Staley Rachel , Smith Diane 
Published: September 2023

Based on prior work done by Diane K. Smith et al on redox responsive 3 hydrogen bond array dimers, a fundamental investigation on the nature of proton coupled electron transfer (PCET) was done by surveying a series of new electroactive “host” H-bond dimers. In these dimers, electron transfer should induce proton transfer across a H-bond, increasing the overall strength of hydrogen bond binding the “guest” and “host”. In particular, the goal was to investigate how electrochemical behavior and binding strength changes as the relative acidity of the electro-inactive “guest” changes in a 2-hydrogen bond array. For this task, amido pyridinium derivatives will be used as the redox active "hosts" and a series of different carboxylic acid, 2-hydroxypyridine, and amide derivatives as the electro-inactive "guests". Unexpectedly, in the presence of carboxylic acids, the amido pyridinium acts as a hydrogen evolution catalyst. During guest host cyclic voltammogram (CV) titrations, there was a large anodic shift of 500 mV and a catalytic increase in current, which is characteristic of an EC mechanism (figure 2). A series of investigations into this mechanism were done following the initial discovery, including scan rate and concentration dependence CV’s, spectro-electrochemical studies, bulk electrolysis, DEMS, and DFT calculations. These studies allowed us to propose the mechanism below (figure 1) for hydrogen evolution. This presentation will detail our efforts to characterize this hydrogen evolution catalyst, the relevance of small molecule hydrogen evolution catalyst, and how we intend to modify it for synthetic purposes.
Figure 1 (left image): Reduction of pyridinium amide with and without guests and proposed mechanism of hydrogen evolution
Figure 2 (right image): CV of pyridinium amide in the presence of dodecanoic acid

Figure 1
Anodic Oxidation of 9,9'-Spiro Bifluorenes
Authors: Becker James Y. , Golub Tatiana , Herath Ajith , West Robert 
Published: September 2023

Previously we investigated electrochemical properties [1] of various 2,3,4,5-tetraphenylsiloles (I) with different substituents attached to the Si atom. Major products include 1,2-dibenzoyl, 1,2-diphenylethene, tetraphenylfuran and tetraphenyldihydrofuran.
Later [2] we explored the redox properties of four silafluorenes of type (II). Major products after CPE involve both aromatic hydrocarbons and siloxane derivatives.
Recently [3] we studied the electrochemical redox properties of four spiro-derivatives (III) in which the central atom is C, Si, Ge or Sn, both by cyclic voltammetry and controlled potential electrolysis. The outcome from these measurements will be presented in this talk. It is noteworthy to indicate that each spiro derivative afford different products although their cyclic voltammograms are similar.
References
[1] A. Dhiman, Z.-R. Zhang, R. West, J. Y. Becker, J. Electroanal. Chem.,
2004, 569, 15-22; A. Dhiman, Z.-R. Zhang, R. West, J. Y. Becker, J. Electroanal. Chem.,
2004, 573, 139-146.
[2] A. C. Herath, R. West, J.Y. Becker, J. Electroanal. Chem., 2014, 728, 118-122.
[3] T. Golub-Sedinkin, A. C. Herath, R. West, and J. Y. Becker, ChemElectroChem
,
2019, 6, 1–6; J.Y. Becker, unpublished results (2021).

Figure 1
Electrochemical Upcycling of Pollutants
Authors: Waldvogel Siegfried R 
Published: September 2023

The electrochemical conversion of pollutants provides a new and powerful way to upcycle these harmful substances into valuable intermediates. Electrosynthesis represents a future technology, which is characterized by its outstanding sustainability.[1] After carbon dioxide, sulfur dioxide is the most prominent pollutant in flue gas. The direct electrochemical incorporation into more elaborated molecules has started recently.[2] The anodic conversion of arenes and subsequent reaction with sulfur dioxide adducts yield sulfonamides,[3] sulfonates,[4] and sulfamides.[5]

Another pollutant from the era of highly chlorinated pesticides is hexachloro-cyclohexane. The non-suitable isomers of Lindane were piled-up in larges deposits ranging >7 Mio. t. By e-shuttle this can be converted to non-fossil benzene source.[6]

The talk will discuss in detail the mechanistic details which led to greener processes.

References:

[1] D. Pollok, S. R. Waldvogel, Chem. Sci.
2020, 11, 12375–12592.
[2] S. P. Blum, K. Hofman, G. Manolikakes, S. R. Waldvogel, Chem. Commun.
2021, 57, 8236–8249.
[3] S. P. Blum, T. Karakaya, D. Schollmeyer, A. Klapars, S. R. Waldvogel, Angew.
Chem. Int. Ed.
2021, 60, 5056–5062.
[4] S. P. Blum, D. Schollmeyer, M. Turks, S. R. Waldvogel, Chem. – Eur. J.
2020, 26, 8358–8362.
[5] S. P. Blum, L. Schäffer, D. Schollmeyer, S. R. Waldvogel, Chem.
Commun. 2021, 57, 4775–4778.
[6] X. Dong, J. L. Röckl, S. R. Waldvogel, B. Morandi, Science,
2021, 371, 507–514.

Figure 1
(Invited) Electroenzymatic Hydrogen Production: Mediated/Direct Electron Transfer Strategies and Continuous Product Analysis
Authors: Milton Ross 
Published: September 2023

Metalloenzymes such as hydrogenases and nitrogenases are of interest to electrochemists for mechanistic study as well as applied biotechnological hydrogen and ammonia production. In order to interface these enzymes with electrodes mediated and direct electron transfer methods have been reported, each having their strengths and weaknesses. In addition to establishing efficient electron transfer with enzymes, dynamic product analysis is also desirable since rates of product formation (and the distribution of products) can be determined during an experiment with varying electrode potential (and thermodynamic driving force for heterogeneous electron transfer).
Our recent efforts concerning the design of electrode:enzyme interfaces are presented here, including (i) mediated vs. direct electron transfer strategies, (ii) rotating ring disk electrochemistry, and (iii) continuous mass spectrometry and gas chromatography [1-2]. In this work, an [FeFe]-hydrogenase is employed as a model enzyme for molecular hydrogen formation, with a view to expand these approaches towards enzymatic electrocatalytic studies of nitrogenases. Limitations and difficulties of the presented approaches will be discussed.
References:
[1] Khushvakov, J., Nussbaum, R., Cadoux, C., Duan, J., Stripp, S.T. and Milton, R.D., Angewandte Chemie International Edition, 2021, 60 (18), 10001-10006.
[2] Liu, Y., Webb, S., Moreno Garcia, P., Kulkarni, A., Maroni, P., Broekmann, P. and Milton, R.D., Submitted.