Electrochemical science advances最新文献

{"title":"Fleet-Based Degradation State Quantification for Industrial Water Electrolyzers","authors":"Xuqian Yan,&nbsp;Lennard Helmers,&nbsp;Kunyuan Zhou,&nbsp;Astrid Nieße","doi":"10.1002/elsa.70002","DOIUrl":"https://doi.org/10.1002/elsa.70002","url":null,"abstract":"<p>A reliable and continuous assessment of the degradation state of industrial water electrolyzers is crucial for maintenance planning and dispatch optimization, thus facilitating risk management for both suppliers and operators. Although voltage is a widely used and easily measurable degradation indicator, its effectiveness is compromised in industrial settings due to the impact of arbitrary operating conditions. Existing methods to correct the impact of operating conditions often rely on measuring characteristic curves, which typically only provide a single-dimensional correction and do not allow varying corrections over time. We propose a data-driven method for degradation state quantification that adjusts the measured voltage under arbitrary operating conditions to a reference condition, using an empirical voltage model and degradation history from a fleet of electrolyzers. This method involves fitting the empirical voltage model for each time series segment and calculating the voltage under the reference condition. To assist model fitting under limited data coverage, the method utilizes a Bayesian approach to incorporate fleet knowledge–an aggregation of the degradation trajectories of the electrolyzer fleet. This method was validated using both synthetic data and operation data from 12 industrial electrolyzers with 1–3 years of operation history, including in-depth sensitivity analyses on the data coverage, fleet–target discrepancy, and fleet size. Results proved the superiority of the proposed fleet-based method over the benchmark method without using fleet knowledge.</p>","PeriodicalId":93746,"journal":{"name":"Electrochemical science advances","volume":"5 3","pages":""},"PeriodicalIF":2.9,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/elsa.70002","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144300434","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Electrodeposited p-Cu2O Films – Role of Redox-Active Compounds Under Photoelectrochemical Operation Revisited","authors":"Michael Neumann-Spallart,&nbsp;Dharini Bhagat,&nbsp;Šárka Paušová,&nbsp;Josef Krýsa,&nbsp;Indrajit Mukhopadhyay","doi":"10.1002/elsa.70003","DOIUrl":"https://doi.org/10.1002/elsa.70003","url":null,"abstract":"<p>The p-type semiconducting copper oxides CuO and Cu₂O are of interest for the conversion of solar energy due to their medium-wide bandgap and the position of their conduction band, allowing for reductive processes in junctions with electrolytes under irradiation. In this work, on Cu₂O, the efficiency of several such processes in competition with self-reduction is critically reviewed and experimentally studied. Up to 2000 nm thick films were obtained via potentiostatic electrodeposition on fluorine-doped tin oxide on glass from alkaline solutions of CuSO₄ using lactic acid as a complexant. The films consisted of a dense arrangement of crystallites as seen by scanning electron microscopy and were of phase pure Cu₂O as shown by X-ray diffraction (XRD). The films were specular, with an absorption coefficient of 50,000 cm⁻¹ at 480 nm and a direct bandgap of 2.5 eV. In junctions with aqueous electrolytes, the material was found to be p-type. Under electrical bias, cathodic and photocathodic currents passed and increased dramatically when reducible redox compounds were added. The influence of various redox couples (O₂, H₂O₂, and methylviologen [MV, 1,1'-dimethyl-4,4'-bipyridinium]) and their concentration in the electrolyte on the stability of the electrodes was studied. Long-time experiments showed that to avoid degradation of the electrodes, the use of oxygen-saturated solutions was mandatory when no other redox couple was added. H₂O₂-containing electrolytes gave rise to constant photocurrents and no alteration of the electrodes was found by XRD. MV yielded cathodic photocurrents. Reoxidation of its reduced form by dissolved oxygen was necessary in order to hinder dimerization or further reduction to MV⁰ and association of the latter to MV⁰_n, producing a whitish layer on top of the electrodes which led to their inactivation.</p>","PeriodicalId":93746,"journal":{"name":"Electrochemical science advances","volume":"5 2","pages":""},"PeriodicalIF":2.9,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/elsa.70003","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143835981","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Elucidating Parasitic Currents in Proton-Exchange-Membrane Electrolytic Cells via Physics-Based and Data-Driven Modeling","authors":"Violeta Karyofylli,&nbsp;K. Ashoke Raman,&nbsp;Linus Hammacher,&nbsp;Yannik Danner,&nbsp;Hans Kungl,&nbsp;André Karl,&nbsp;Eva Jodat,&nbsp;Rüdiger-A. Eichel","doi":"10.1002/elsa.70000","DOIUrl":"https://doi.org/10.1002/elsa.70000","url":null,"abstract":"<p>Proton-exchange membrane (PEM) water electrolysis is pivotal for green hydrogen production, necessitating accurate predictive models to manage their non-linearities and expedite commercial deployment. Understanding degradation mechanisms through macro-scale modeling and uncertainty quantification (UQ) is crucial for advancing this technology via efficiency enhancement and lifetime extension. This study primarily utilizes a one-dimensional physics-based model to elucidate the presence of electron transport within the PEM, another degradation phenomenon, besides gas crossover. This work also applies a machine learning (ML) algorithm, such as eXtreme Gradient Boosting (XGBoost), to model PEM electrolytic cell (PEMEC) operation based on a dataset generated from the previously mentioned physics-based model. The ML model excels in predicting the polarization behavior. Based on this surrogate model, UQ and sensitivity analysis are finally employed to enlighten the dependence of PEMECs performance and Faradaic efficiency on the effective electronic conductivity of PEM, especially when electronic pathways exist within the membrane and operating at low current densities.</p>","PeriodicalId":93746,"journal":{"name":"Electrochemical science advances","volume":"5 3","pages":""},"PeriodicalIF":2.9,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/elsa.70000","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144299800","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Spearhead Metal Ultramicroelectrodes Based on Carbon Nanoelectrodes as Local Voltammetric pH Sensors","authors":"Thomas Quast,&nbsp;Stefan Dieckhöfer,&nbsp;Wolfgang Schuhmann","doi":"10.1002/elsa.70004","DOIUrl":"https://doi.org/10.1002/elsa.70004","url":null,"abstract":"<p>We suggest a new method for preparing metal electrodes based on carbon nanoelectrodes (CNEs), which are suitable for application in shearforce scanning electrochemical microscopy (SECM). The as-prepared CNEs were focused ion beam (FIB)-processed, subsequently thermally recessed, and finally, Pt or Au were electrodeposited into the cavity of the recessed CNEs leading to insulator-free metal electrodes with sizes of around 2 µm in diameter. For their application as local voltammetric pH sensors, the electrodes were calibrated in a concentration range of 11.6 M H⁺ to 9 M OH⁻. As a case study, we determined the local pH in situ using the developed Pt microelectrode positioned in close proximity to an Ag-based gas diffusion electrode (GDE) which was operated for the oxygen reduction reaction (ORR). We could observe a shift of the Pt_ox reduction peak of Δ<i>E</i> = −700 mV, which is exceeding previous observations at Ag-based GDEs by far. This novel type of electrode will pave the way to perform shearforce SECM with an even higher spatial resolution due to their spearhead shape.</p>","PeriodicalId":93746,"journal":{"name":"Electrochemical science advances","volume":"5 3","pages":""},"PeriodicalIF":2.9,"publicationDate":"2025-03-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/elsa.70004","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144299523","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Ramping-Up Electrolyser Manufacturing for the Green Hydrogen Transition: A Planning Approach for Scalable Factory Concepts","authors":"Michael Riesener,&nbsp;Esben Schukat,&nbsp;Niklas Schäfer,&nbsp;Nils Lehde genannt Kettler,&nbsp;Sebastian Junglas","doi":"10.1002/elsa.70005","DOIUrl":"https://doi.org/10.1002/elsa.70005","url":null,"abstract":"<p>In pursuit of more sustainable energy systems, green hydrogen supports renewable energy supply and enables flexible energy storage. To achieve both nationally and globally set goals of the green hydrogen transition, affordable hydrogen electrolysers need to be available. However, only small-scale production facilities have yet been established. Manufacturing companies are struggling to scale up production capacities to meet the rising yet fluctuating and uncertain market demands. However, existing factory planning methods do not satisfy the associated requirements. Therefore, we introduce a planning approach for developing scalable factory concepts that enable industrial high-scale production. The proposed planning approach is structured around a five-step procedure model that outlines the necessary planning tasks, both for the production system and IT system design. To automate the planning tasks, we describe a prototype implementation, which we apply to an electrolyser manufacturing company's use case in the series production of electrolysers in the gigawatt range (SEGIWA) research project on scalable electrolyser manufacturing. The project's technological focus is proton exchange membrane (PEM) electrolysis. Various planning scenarios are derived and validated by digital tools with 3D factory models. Finally, we discuss the advantages and shortcomings of the planning approach, which provides a framework for adapting production systems to the challenges posed by new technologies and dynamic market conditions. Thus, our contribution empowers manufacturers to design industrial production systems for scaling up electrolyser manufacturing, thereby contributing practically to the green hydrogen transition.</p>","PeriodicalId":93746,"journal":{"name":"Electrochemical science advances","volume":"5 3","pages":""},"PeriodicalIF":2.9,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/elsa.70005","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144300496","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Design and Analysis of Carbon-Supported NiMo HER Catalysts and Electrodes for High Performance All PGM-Free AEM Electrolysers","authors":"Lukas Heinius,&nbsp;Malte Klingenhof,&nbsp;Gregor Weiser,&nbsp;Pierre Schröer,&nbsp;Lukas Metzler,&nbsp;Susanne Koch,&nbsp;Sören Selve,&nbsp;Severin Vierrath,&nbsp;Peter Strasser","doi":"10.1002/elsa.202400027","DOIUrl":"https://doi.org/10.1002/elsa.202400027","url":null,"abstract":"<p>The influence of the nature of carbon-support materials on the structure and the electrochemical performance of NiMo cathode catalysts is investigated. Carbon materials addressed in this study include Ketjen Black, Vulcan and MWCNT-COOH. A one pot, easily scalable, hydrothermal microwave synthesis with a subsequent hydrogen reduction step was applied for the preparation of the catalyst materials. The structures and compositions of the catalysts were characterized by TEM/SEM, XRD, ICP-OES, BET and STEM-EDX. The performance of the catalysts was tested using rotating disc electrode (RDE) and anion exchange membrane (AEM) single-cell electrolyser to downselect the most active material. The influence of pH, catalyst loading and type of carbon support was investigated to optimize the operating conditions. By increasing the KOH concentration from 0.1 to 1 M in an AEM electrolysis cell, the current density could be more than doubled, whereas the introduction of a carbon support raised the current density by a factor of seven. Finally, it is demonstrated how applying a novel bar-coating preparation of the electrodes in a PGM-free AEM electrolyser enabled a favourable current density of 1 A cm⁻² at 2.04 V. This performance is comparable to earlier systems but requires only a fraction of the catalyst loading.</p>","PeriodicalId":93746,"journal":{"name":"Electrochemical science advances","volume":"5 3","pages":""},"PeriodicalIF":2.9,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/elsa.202400027","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144300122","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Extending Equivalent Circuit Models for State of Charge and Lifetime Estimation","authors":"Limei Jin,&nbsp;Franz Philipp Bereck,&nbsp;Josef Granwehr,&nbsp;Christoph Scheurer","doi":"10.1002/elsa.202400024","DOIUrl":"https://doi.org/10.1002/elsa.202400024","url":null,"abstract":"<p>Equivalent circuit modelling (ECM) of electrochemical impedance spectroscopy (EIS) data is a common technique to describe the state-dependent response of electrochemical systems such as batteries or fuel cells. To use EIS for predictive assessments of the future behaviour of such a system or its state of health (SOH), a more elaborate digital twin model is needed. Developing a robust and continuous SOH estimation poses a formidable challenge. In this study, a framework is presented where ECM parameters are expanded in a high-dimensional Chebyshev space. It facilitates not only a mapping of the state of charge dependence with robust boundary conditions but also an extension towards a more abstract SOH description is possible. Such methods can bridge the gap between the experiment and purely data-driven techniques that do not rely on fitting of experimental data using a priori defined models. In the absence of long-time impedance measurements of a battery, quasi-Monte Carlo sampling can be employed to generate differently aged synthetic battery models with limited experimental impedance data. As additional data becomes available, the space spanning the possible states of a battery can be gradually refined. The developed framework, therefore, allows for the training of big data models starting with very little experimental information and assuming random fluctuations of the model parameters consistent with available data.</p>","PeriodicalId":93746,"journal":{"name":"Electrochemical science advances","volume":"5 2","pages":""},"PeriodicalIF":2.9,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/elsa.202400024","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143836164","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Water Electrolysis Facing the Gigawatt Challenge—Comprehensive De-Risking of Proton Exchange Membrane and Anion Exchange Membrane Electrolyser Technology","authors":"André Karl,&nbsp;Eva Jodat,&nbsp;Hans Kungl,&nbsp;Ladislaus Dobrenizki,&nbsp;Günter Schmid,&nbsp;Peter Geskes,&nbsp;Rüdiger-A. Eichel","doi":"10.1002/elsa.202400041","DOIUrl":"https://doi.org/10.1002/elsa.202400041","url":null,"abstract":"<p>Green Hydrogen (H₂) is generally considered to play a key role in enabling sustainable energy storage, as well as a renewable feedstock to various industrial sectors. Accordingly, the production of H₂ by water electrolysis at an industrial scale is a key prerequisite for a transformation of our energy system. With respect to water electrolysis, proton exchange membrane (PEM) electrolysers are generally considered a technology option for the production of green H₂ on a large scale. Prior to market ramp-up PEM electrolysers have to undergo substantial de-risking for a technology ramp-up. For a comprehensive de-risking, a fundamental and holistic understanding of the degradation phenomena of electrolysers on an industrially relevant scale is a prerequisite. Field data with different application-specific load profiles needs to be acquired in order to develop countermeasures against possible degradation patterns induced by the operational mode. This is not only crucial for the more mature PEM technology but also in the future relevant for other more novel membrane electrolysis technologies such as anion exchange membrane (AEM) looking to make the step from laboratory operation to large-scale production and deployment. This editorial aims to outline the current status and general workflow of the de-risking process and serve as an introduction to the topics of this special issue ranging from fundamental studies on degradation processes on the catalyst level up to novel factory concepts for ramping up of electrolyser production.</p>","PeriodicalId":93746,"journal":{"name":"Electrochemical science advances","volume":"5 3","pages":""},"PeriodicalIF":2.9,"publicationDate":"2025-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/elsa.202400041","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144299602","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Tuning Proton Exchange Membrane Electrolytic Cell Performance by Conditioning Nafion N115-Based Membrane Electrode Assemblies","authors":"Niklas Wolf,&nbsp;Ali Javed,&nbsp;Leander Treutlein,&nbsp;Hans Kungl,&nbsp;André Karl,&nbsp;Eva Jodat,&nbsp;Rüdiger-A Eichel","doi":"10.1002/elsa.202400038","DOIUrl":"https://doi.org/10.1002/elsa.202400038","url":null,"abstract":"<p>Conditioning of the membrane electrode assembly (MEA) is an important step to establish functionality and obtain a consistent performance of the proton exchange membrane electrolytic cell (PEMEC) when setting it into operation. On a laboratory scale in an academic context, conditioning encompasses primary pre-treatment of the MEA by chemical or thermal procedures under defined mechanical conditions and, secondarily, the break-in procedure, during which the PEMEC is subjected to initial electrical loads before actual operation. This study demonstrates the effect of MEA conditioning on the short-term performance of PEMEC. The impact of mechanical, chemical and thermal conditions during pre-treatment was investigated for Nafion N115-based MEAs while keeping the break-in procedure invariant for all pre-treatment conditions. The electrochemical characterisation was performed using polarisation curves and electrochemical impedance spectroscopy. The impact of ex situ–before assembly of the cell–versus in situ–after assembly of the cell–conditioning resulted in markedly different mechanical conditions. The experimental results showed an improvement in PEMEC performance by pre-treating the MEA after cell assembly. Compared to pre-treatment with deionised water (DI water) at 60°C, treatment with acidic solution improved the performance, evidenced by a 21 mV reduction in cell voltage at 2 A·cm⁻². When compared with DI water at 60°C, a pre-treatment at 90°C with DI water reduced cell voltage by 23 mV.</p>","PeriodicalId":93746,"journal":{"name":"Electrochemical science advances","volume":"5 3","pages":""},"PeriodicalIF":2.9,"publicationDate":"2025-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/elsa.202400038","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144299974","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"A Finite Element Model of Transient Galvanic Corrosion Behaviour of Aluminium Alloy","authors":"Jieshun Tang,&nbsp;Mingyang Gao,&nbsp;Haitao Wang,&nbsp;Daokui Xu,&nbsp;Shu Guo,&nbsp;En-Hou Han","doi":"10.1002/elsa.202400031","DOIUrl":"https://doi.org/10.1002/elsa.202400031","url":null,"abstract":"<p>The environment in which aircraft are used is very complex, and factors such as high salinity, high humidity atmospheric conditions and mechanical loads applied to the aircraft during flight can lead to damage to the fuselage materials and compromise the safety of the aircraft. A large number of mechanical structural components in aircraft consist of aluminium alloys, which are susceptible to mechanical loads that erode mechanical properties and endanger the integrity of the aircraft. A time-dependent numerical model is developed in this study. The model provides insight into the complex effects of mechanical loading on the kinetics of galvanic coupling corrosion of AA7075 (aluminium alloy). Our results clearly show that mechanical loading accelerates galvanic corrosion, and the galvanic corrosion behaviour of aluminium alloys is significantly accelerated when loading induces plastic deformation; changes in the thickness of the thin liquid film affect the galvanic corrosion of the galvanic coupling model, which is suppressed when the film thickness is increased, and, in general, exhibits a stronger tendency to corrode homogeneously; the galvanic corrosion behaviour of aluminium alloys is significantly accelerated as the area of cathode increases; the simulation also reveals a higher localisation rate of the model when the boundary load is applied compared to the no-load case in the galvanic coupling corrosion behaviour. The numerical methodology illustrated in this study not only serves as a comprehensive tool for interpreting the intricate relationship between mechanical loading and corrosion behaviour, but also provides a framework for a deeper understanding of this multifaceted phenomenon. In practical applications, the model developed in this study can be used to check the safety of aluminium alloy structural components in service, which can be used as a reference for the design of aircraft wing skins.</p>","PeriodicalId":93746,"journal":{"name":"Electrochemical science advances","volume":"5 2","pages":""},"PeriodicalIF":2.9,"publicationDate":"2025-01-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/elsa.202400031","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143835961","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}