bluuebunny/crossref_metadata_2025_split huggingface dataset:
Degradation Characteristics of Carbon-Supported Pt Via CO2 Detection during Startup/Shutdown of Polymer Electrolyte Membrane Fuel Cells
Authors: Ishikawa Seisho , Tanaka Akihisa , Oya Hirotaka , Koshiba Hideto , Yamashita Tsubasa , Hanaki Yasunari , Mizuno Yusuke , Nakao Masayuki , Nagato Keisuke 
Published: December 2024

One of the major factors that reduces the durability of polymer electrolyte membrane fuel cells (PEMFCs) is degradation of the carbon-supported Pt in the catalyst layer, which can be attributed to the aggregation of Pt and the corrosion of carbon [1]. In this study, the degradation characteristics of a PEMFC during startup/shutdown were evaluated through detection of the CO2 generated during power generation tests. Non dispersive infrared-type (NDIR) analyzers have been shown to provide immediate and accurate measurements of carbon dioxide concentrations [2], and a pathway for the immediate measurement of CO2 concentration was established by connecting an NDIR analyzer to a test bench for the power generation tests. The degradation test of the PEMFC was repeated 100 times, involving the voltage sweep to 1.5 and 1.0 V and a voltage hold at 0.6 V. The PEMFC performance was evaluated using linear sweep voltammetry before the start of the tests and after every 10 sets of degradation tests, and the CO2 concentration was measured in parallel with the tests. As a result, the generation of CO2 and degradation of the PEMFC performance were confirmed. Figure 1 shows measured CO2 concentration during the degradation test, and approximately 3 ppm of the initial value is an offset derived from the measurement system. More CO2 was generated when the voltage was raised from 0.3 to 1.5 V than when it was raised from 0.6 to 1.5 V. Furthermore, the amount of CO2 generation decreased as the degradation tests were repeated, which can be explained by the passivation of some carbon atoms on the surface above 0.6 V. The study will be extended to investigate the effects of the voltage profile and carbon support type on degradation characteristics, contributing to the improvement of the durability of PEMFCs.
References
[1] N. Macauley et al., Carbon Corrosion in PEM Fuel Cells and the Development of Accelerated Stress Tests, J Electrochem Soc, 16, F3148‒F3160 (2018).
[2] E. Niangar et al., Real-time CO2 Detection from Carbon Support Oxidation in PEM Fuel Cell Cathodes during Potential Cycling, ECS Trans, 50, 1599–1606 (2013).

Figure 1
Impedance Based Comparison of PEMFC Cathode Catalyst Layer Materials
Authors: Schwab Kersten , Weber Andre , Heider Emanuel Albert , Joos Markus 
Published: December 2024

The performance of Polymer Electrolyte Membrane Fuel Cells (PEMFC) is strongly dependent on the oxygen reduction reaction and therefore the cathode catalyst layer. Different catalyst layers with the same platinum loading can achieve vastly different performances. The exact composition of ionomer, carbon support and catalyst has a big impact on important electrode characteristic. These characteristics define the contributions of the loss processes that occur in the electrode. By improving one of the performance defining features of the catalyst layer, another one is oftentimes worsened. This creates a trade-off between the loss contributions and the catalyst design parameters.
Impedance spectroscopy (EIS) is a powerful tool to make these trade-offs visible. By calculating the distribution of relaxation times (DRT) the different loss processes can be deconvoluted and by fitting the impedance spectra to a physicochemical meaningful transmission line model, the loss processes can be quantified. In addition the electrochemical active surface area (ECSA) can be determined by cyclic voltammetry (CV) and correlated to the charge transfer losses.
In this contribution PEMFCs with different cathode catalyst layers and the same anodes are compared in a wide spectrum of operating conditions by means of EIS and DRT. On the basis of these measurements a transmission line model (TLM) is fitted to the impedance spectra and the loss contributions are quantified. The results enable a direct comparison of the cathode catalyst specific loss processes in different operating conditions. By means of CV and Hydrogen Underpotential Desorption, the ECSA is estimated and correlated with the loss contributions.
Cloud-Connected Labs of Future for Green Energy Materials
Authors: Malek Kourosh 
Published: December 2024

The clean energy technology sector faces a major challenge with the pace of development trailing behind commercialization targets. The root cause hampering progress towards cleaner materials and technologies is that laboratories with complementary capabilities still largely operate in separation, with a lack of coordination among their efforts. The EU-funded DECODE project (DE-centralised ClOud Labs for inDustrialisation of Energy Materials) aims to break down these barriers by creating a decentralised and adaptive cloud-connect labs concept. DECODE aims at transforming the development and innovation process for clean energy materials and technologies. The project envisions the creation of a decentralized platform that connects multiple labs to enhance the effectiveness and accelerate the progress of research and development in the field of clean energy technology. The core elements of the platform consist of the DECODE FABRIC, a matrix-like structure that facilitates collaboration, and a scoring system to assess integration readiness of methods and tools. An AI-enabled CPU orchestrates contributions from partner labs.
The objective of DECODE is to digitally connect multiple labs, boost the effectiveness, and accelerate the development and integration of materials for sustainable hydrogen technologies. At its core, DECODE strives to develop and deploy three innovative modules: 1) the DECODE Foundry, a semantic search engine for assembling methods and tools into practical workflows, 2) the DECODE FABRIC, a matrix structure that connects modelling and characterisation suites, and 3) the DECODE CPU for end-to-end orchestration of a given materials development to integration pipeline. The platform, designed for unprecedented flexibility and interoperability, harnesses AI-driven data management and ontological mapping to enable the seamless collaboration among partner labs.
Initially focusing on hydrogen technologies, DECODE's vision may be expanded to other technologies including energy harvesting, storage, clean water and more. The platform strives for an unprecedented level of flexibility and adaptability, accommodating diverse strategies and technologies. In summary, DECODE accelerates clean energy innovation through interconnected labs, fostering a sustainable and cleaner future.
Prospects in the Design of Porous Vs. Rib/Channel Flow Fields for Polymer Electrolyte Membrane Fuel Cells
Authors: Garcia-Salaberri Pablo A. , Perego Andrea , Zenyuk Iryna V. 
Published: December 2024

Porous flow fields show promising characteristics to promote oxygen transport and improve performance of next-generation polymer electrolyte membrane fuel cells (PEMFCs) [1]. In this work, combined experimental and numerical work is conducted to examine the pros and cons of porous flow fields compared to conventional rib/channel flow fields (see Figure 1). The experimental performance data of a cathode porous flow field integrated into PEMFC is used to validate the numerical model, which is then used to perform a comprehensive parametric study involving both operational and constructive parameters [2]. The results show that the main advantages of the porous flow fields are: (i) the improvement of oxygen transport, (ii) the decrease of water saturation in the cathode MEA, reducing water flooding, and (iii) the increase of the distribution homogeneity (e.g., current density and temperature) in the in-plane direction [3,4]. In contrast, the main disadvantages are: (iv) the potential effect of electrical contact resistances between porous surfaces, and (v) the decrease of the water removal drag force in the cathode channel [5]. These issues can be mitigated with thinly manufactured foams and/or increasing the assembly compression ratio. In addition, hybrid porous flow fields incorporating a rib/channel pattern with fine pore-size porous ribs can be used to improve the contact between surfaces and increase the cathode gas flow velocity.
[1] G. Zhang et al., Porous Flow Field for Next-Generation Proton Exchange Membrane Fuel Cells: Materials, Characterization, Design, and Challenges, Chem. Rev. 123 (2023) 989-1039.
[2] P.A. García-Salaberri, I.V. Zenyuk, Boosting the Performance of Polymer Electrolyte Membrane Fuel Cells with Porous Flow Fields: Pros and Cons, Energy, In preparation.
[3] J.E. Park, Achieving breakthrough performance caused by optimized metal foam flow field in fuel cells, International Journal of Hydrogen Energy 44 (2019) 22074-22084.
[4] Y. Wu et al., Multi-length scale characterization of compression on metal foam flow-field based fuel cells using X-ray computed tomography and neutron radiography, Energy Conversion and Management 230 (2021) 113785.
[5] Y. Wu et al., Characterization of water management in metal foam flow-field based polymer electrolyte fuel cells using in-operando neutron radiography, International Journal of Hydrogen Energy 45 (2020) 2195-2205.
This work was supported by project PORHYDRO1 TED2021-131620B-C21/AEI European Union NextGenerationEU/PRTR, of the Ministry of Science and Innovation of Spain, Spanish Research Council.

Figure 1. Schematic of the combined experimental and numerical methodology used to examine the pros and cons of porous vs. rib/channel flow fields.

Figure 1
Influence of the Clamping Force and the Formation of Liquid Water Along the Channel on the Local Diffusion Processes in PEMFCs
Authors: Fischer Yannick , Oppek Philipp , Chuang Po-Ya Abel , Weber Andre 
Published: December 2024

The success of PEMFCs in heavy duty applications depends on achieving high power densities while maintaining exceptional durability. Under high current density operating conditions, the transport of oxygen from the gas channel via the GDL and MPL to the active Pt-particles in the catalyst layer becomes performance limiting. In the different layers, oxygen transport takes place via various transport processes, such as Knudsen, molecular and ionomer diffusion. Gas transport in a fuel cell is influenced to varying degrees by the operating conditions, geometry of the flow channel, and the properties of the porous media. Porosity and tortuosity of the diffusion media depend on the local clamping force and the amount of liquid water present. In a large-active-area cell, the clamping force and liquid water as well as oxygen concentration, pressure and temperature can vary significantly between the inlets and the exits, which results in a spatially varying oxygen transport resistance and local performance along the channel. To enable targeted optimization of the operating strategy and component design for high current density operation, a comprehensive understand of the local diffusion processes and their dependencies is essential.
In our study, limiting current measurement is used as a diagnostic tool in combination with a segmented cell to determine the local oxygen transport resistance [1, 2]. In the measurement setup, the clamping force is manually set for each segment and recorded continuously throughout the experiment. By systematically varying the operating conditions (p, RH, T), clamping force and cathode gas composition (N2/He), we aim to deconvolute each transport mechanism and the allocation of the transport resistance to each individual layer. The local operating conditions, such as pressure and temperature, are simulated using empirical models based on local measurement data. The combined results allow us to obtain the local oxygen transport resistance as a function of local operating conditions and the clamping force along the flow channel.
In this study, the distribution of different gas diffusion processes and their impact on fuel cell performance along the channel are presented. In particular, the effect of the clamping force and the formation of liquid water along the channel on local porosity and tortuosity in the GDL are discussed. Furthermore, our results demonstrate how the overall performance of the cell can be optimized by adjusting the clamping force distribution along the flow channel.
References:

M. A. Rahman, M. Sarker, F. Mojica, P.-Y.A. Chuang, Electrochimica Acta 320 (2019), 134601

T. V. Reshetenko, J. St-Pierre, J. Electrochem. Soc. 161 (2014), 10, F1089-F1089
Nondestructive Nano-Imaging and Nano-Spectroscopy of Buried Battery Interfaces: Advancing in Situ and Operando Infrared Characterization Schemes for Basic Energy Storage Science
Authors: Larson Jonathan M. , He Xin , Bechtel Hans A. , Kostecki Robert 
Published: December 2024

A critical component to the advancement and realization of beyond Li-ion electrical energy storage technologies is the careful study and characterization of the electrochemically active interfaces that govern the function and performance of such devices. Ideally, characterization of interfaces, and the interphases that grow therein, would be done in an inherently non-destructive way, while within its undisturbed native environment, and with nanoscale resolution over microscale areas (to resolve the kinds, and distribution, of the interphase building blocks). The practical realization of this, though, is extremely challenging because these interfaces and interphases are buried, highly reactive, nano-thin, and structurally and chemically heterogenous.
In this talk, we’ll discuss a brief history of an emerging and evolving infrared near-field methodology aimed at overcoming as many of these challenges as possible, to study electrochemical energy storage materials and interfaces in their native environment, non-destructively, and with nanoscale resolution. This is accomplished by employing a combination of precisely engineered and electrochemically controlled graphene/electrolyte interfaces, and diffraction-limit-breaking near-field optical probes capable of chemical imaging and vibrational spectroscopy at the nanoscale. We will present works published on graphene/liquid-electrolyte interfaces,1 and anode-free-based Li/polymer-electrolyte interfaces.2 We will show that in the former case, operando potential step voltammetry + nano-FTIR is capable of sensing concentration changes in the electric double layer.1 Furthermore, in the latter case, where we will spend most our time, in situ multimodal nano-FTIR, ATR-FTIR, infrared nano-imaging, and atomic force microscopy reveal nanoscale structural and chemical heterogeneities intrinsic to the solid polymer electrolyte initiate a cascade of additional interfacial nanoscale heterogeneities during Li plating and stripping, including Li-ion conductivity, electrolyte decomposition, and interphase formation.2

1.) Y.-H. Lu,* J.M. Larson,* A. Baskin, X. Zhao, P. Ashby, D. Prendergast, H. Bechtel, R. Kostecki, and M. Salmeron, Nano Lett
19, 5388-5393 (2019).

2.) X. He*, J. M. Larson*, H. A. Bechtel, and R. Kostecki, Nat Commun, 13, 1398 (2022).
(*: Denotes Equal Contribution)

Figure 1
Automating Energy Storage System Studies at the Advanced Photon Source: A Case Study of 11-BM
Authors: Wang Yang , Lapidus Saul 
Published: December 2024

Traditionally, energy storage system characterization involves labor-intensive processes, from sample preparation to data acquisition and analysis. However, the integration of automation technologies streamlines this workflow, enhancing efficiency and throughput while minimizing human intervention. The 11-BM beamline, equipped with high-resolution X-ray diffraction capabilities, serves as a versatile platform for investigating the structural and chemical properties of materials crucial for energy storage applications.
The key components of the automated workflow deployed at 11-BM, including robotic sample handling systems, real-time data acquisition algorithms, and advanced machine learning techniques for rapid data analysis. By interfacing with sophisticated automation system involving robotics like UR5e and KX2, researchers can remotely design experiments, execute protocols, and retrieve results with minimal manual intervention, thereby accelerating the pace of research and innovation in energy storage technology.
Optical and X-Ray Absorption Interrogation of Selenium-Based Redox in Carbon Nanofoam Supported SxSey Cathodes
Authors: Carter Rachel Elizabeth , DeBlock Ryan H. , Lefler Matthew , Neale Zachary Garbe , Love Corey T. , Sassin Megan B. , Rolison Debra R. , Long Jeffrey W. 
Published: December 2024

Sulfur-based batteries have emerged as a leading contender for next-generation energy storage owing to their high redox capacity and the global availability of elemental sulfur. Yet the electronically insulating nature of sulfur limits the applicability of this battery chemistry. Redox kinetics are enhanced by coating sulfur onto a conductive, porous carbon scaffold1 and atomically mixing with selenium.2 Electrochemical discharge of S/Se blends exhibit additional voltage plateaus compared to a pure S cathode and in-situ optical microscopy identifies a more direct reaction pathway with less active material dissolution.3 Lab scale in-operando X-ray absorption spectroscopy reveals shifts in the Se K-edge correlated with features in electrochemical charge-discharge profiles, providing critical insights on the redox mechanism in nanocomposites of sulfur and selenium.
1. Neale, Z.G.; Lefler, M.J.; Long, J.W.; Rolison, D.R.; Sassin, M.B.; Carter, R.; Freestanding Carbon Nanofoam Papers with Tunable Porosity as Lithium-Sulfur Battery Cathodes. Nanoscale,
2023, 15, 16924-16932.
2. Deblock, R.H.; Lefler, M..J.; Neale, Z.G.; Love, C.T.; Long, J.W.; Carter, R.; Optical and X-ray Absorption Interrogation of Selenium-based Re-dox in Li-SxSey batteries, Energy Advances, 2024, 2024, 3, 424-429.
3. Carter, R.; NewRingeisen, A.; Reed, D.; Atkinson, R.W.; Mukherjee, P.P.; Love, C.T.; Optical Microscopy Reveals the Ambient Sodium Sulfur Discharge Mechanism, ACS Sustainable Chem. Eng.
2021, 9, 1, 92–100.
Correlating the Battery Performance and the Texture of Electrodeposited Lithium Metal in Zero-Excess Solid-State Lithium Metal Batteries
Authors: Li Zhuo , Fan Austin , Hatzell Kelsey 
Published: December 2024

Zero-excess solid state lithium metal batteries are considered the next-generation battery system recognized for their high volumetric energy density and improved safety. However, the non-uniform plating behavior of lithium metal against the current collector leads to poor coulombic efficiency and lithium dendrite formation [1]. Thus, it is essential to understand and quantify the plating behaviors to optimize the system. The texture, or crystallographic orientation, of lithium metal can be used to evaluate the morphology of lithium metal within batteries [2]. In liquid batteries, a strong {110} texture has been correlated with a denser and dendrite-free morphology [2], which can lead to a better coulombic efficiency [3]. However, it is currently not understood how the crystallographic orientation is affected by the presence of hydrostatic stress which is common in zero-excess solid-state batteries. The lack of knowledge is in part because accessing buried solid-solid interfaces is challenging and even more challenging when considering the volatile nature of lithium metal. In this study, we addressed the challenge by adopting synchrotron-based X-ray pole figure measurements [4]. Both synchrotron-based and lab-based X-ray pole figure measurements were utilized to reveal the texture evolution of lithium metal understand various conditions such as hydrostatic stress and temperature. By combining texture measurement with electrochemistry, we deconvoluted the impact of accumulated capacity, temperature, and current density on the quality of plated lithium metal. Understanding the impact of these factors will enable better control of operating conditions to achieve a more uniform and dendrite free lithium deposition, thereby ensuring longer-lasting and more stable zero-excess solid-state lithium metal batteries.

References:

[1] Christian Heubner, Sebastian Maletti, Henry Auer, Juliane Hüttl, Karsten Voigt, Oliver Lohrberg, Kristian Nikolowski, Mareike Partsch, and Alexander Michaelis. From Lithium-Metal toward Anode-Free Solid-State Batteries: Current Developments, Issues, and Challenges. Adv. Func. Mater. 2021, 31(51), 2106608.
[2] Shi, Feifei, Allen Pei, Arturas Vailionis, Jin Xie, Bofei Liu, Jie Zhao, Yongji Gong, and Yi Cui. "Strong texturing of lithium metal in batteries." Proceedings of the National Academy of Sciences 114, no. 46 (2017): 12138.
[3] Hu, Xitao, Yao Gao, Yongming Sun, Zhen Hou, Yufeng Luo, Danni Wang, Jiangpeng Wang, Biao Zhang, Zijian Zheng, and Quan Li. "Preserving the Li {110} Texture to Achieve Long Cycle Life in Li Metal Electrode at High Rates." Advanced Functional Materials 34, no. 11 (2024): 2307404.
[4] Wenk, H-R., and S. Grigull. "Synchrotron texture analysis with area detectors." Journal of applied crystallography 36, no. 4 (2003): 1040-1049.
Operando Bragg Coherent Diffraction Imaging of Commercial Polycrystalline and Single Crystal NMC811 Electrodes
Authors: Llewellyn Alice V. , Jervis Rhodri , Shearing Paul R 
Published: December 2024

Commercial candidates for electric vehicle batteries include Ni-rich Li(Ni0.8Mn0.1Co0.1)O2 (NMC811) cathodes due to their high specific capacity (200 mAh/g) and reduced cobalt content, which has positive socio-economic repercussions. Despite all of the advantages, these materials suffer from a range of degradation modes, many of which are associated with the redox and crystallographic behavior at high states of charge and are thought to be the cause of rapid capacity fade. NMC811 suffers from anisotropic changes in the crystal structure during cycling, which induce strain and can then lead to issues such as particle crack formation. Gathering data at multiple length scales is imperative for understanding the discrete mechanisms at play. Bragg Coherent Diffraction Imaging (BCDI) is a key tool for obtaining data at the nano-scale by providing high spatial resolution images of individual particles. BCDI also affords the unique opportunity to resolve the strain of individual crystals at the picometer scale, producing data with the highest quantifiable imaging resolution of battery electrodes and allowing for the detection of evolving defect modes such as shearing and stacking faults in the crystals during cycling.
NMC811 typically employs the archetypal cathode particle morphology, consisting of a secondary particle agglomerate (~ 10 μm) made up of nanometer-sized primary particles. It is widely accepted that crack formation occurs at grain boundaries between primary particles. One mitigation method is to switch to a single crystal morphology, reducing the number of grain boundaries within particles and therefore improving overall performance. However, there is still a limited understanding of the subtle mechanistic differences between the two morphologies during cycling.
In this work, Operando BCDI was employed to study both polycrystalline and single crystal NMC811 electrodes in both pristine and aged states. Non-uniform distributions of inter- and intracrystal strain were observed for both polycrystalline and single crystal morphologies, even in the pristine state. Strain values an order of magnitude higher were observed for polycrystalline NMC811 compared to single crystal NMC811, likely a cause for the single crystal morphology’s superior performance. The nucleation of crystal splitting was also observed for a pristine single crystal during cycling, which could subsequently result in intergranular cracking. This feature is only resolvable with extremely high-resolution techniques such as BCDI. This work ultimately adds to the understanding of the central role of crystal-scale dynamics during cycling and the potential ramifications for a cell's electrochemical performance, leading to informed material design.