ACS electrochemistry最新文献_第2页

Effect of Trace Amounts of Chloride on Roughening of Au(111) Single-Crystal Electrode Surface in Sulfuric Acid Solution during Oxidation-Reduction Cycles. 微量氯化物对Au（111）单晶电极表面氧化还原过程中粗化的影响

ACS electrochemistry Pub Date : 2025-03-03 eCollection Date: 2025-07-03 DOI: 10.1021/acselectrochem.4c00226

Saeid Behjati, Marc T M Koper

{"title":"Effect of Trace Amounts of Chloride on Roughening of Au(111) Single-Crystal Electrode Surface in Sulfuric Acid Solution during Oxidation-Reduction Cycles.","authors":"Saeid Behjati, Marc T M Koper","doi":"10.1021/acselectrochem.4c00226","DOIUrl":"10.1021/acselectrochem.4c00226","url":null,"abstract":"This study investigates the impact of varying trace-level chloride ion concentrations on the roughening of a Au(111) electrode during oxidation-reduction cycles (ORCs) in 0.1 M sulfuric acid by in situ scanning tunneling microscopy (STM). At the higher chloride concentration (50 μM), rapid dissolution of Au atoms and step line recession are observed in the recorded in situ STM images. The high surface mobility of Au atoms resulted in a lack of detectable vacancy islands in the images with minimal changes in cyclic voltammograms (CVs) and the complete absence of nano-island formation, which is observed in pure sulfuric acid. At moderate concentration (10 μM), the dissolution rate decreased substantially, so the initial step lines are still distinguishable after the 200 ORCs. The lower surface mobility leads to the formation of vacancy islands in the terraces, and these newly formed step sites give rise to additional peaks in the CVs. At the lowest concentration (1 μM), nano-island formation is observed. However, inhomogeneous chloride adsorption (showing as darker areas in the EC-STM images) on the sample at high enough anodic potential (0.9 V) led to previously unreported behavior, showing very inhomogeneous roughening, with parts on the surface showing reduced Au atom mobility and minimal changes even after 200 ORCs.","PeriodicalId":520400,"journal":{"name":"ACS electrochemistry","volume":"1 7","pages":"1082-1092"},"PeriodicalIF":0.0,"publicationDate":"2025-03-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12235628/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144602698","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}

引用次数: 0

Structural Evolution of Silicon Nitride Anodes during Electrochemical Lithiation. 电化学锂化过程中氮化硅阳极的结构演变。

ACS electrochemistry Pub Date : 2025-02-28 eCollection Date: 2025-06-05 DOI: 10.1021/acselectrochem.4c00230

Adam J Lovett, Máté Füredi, Liam Bird, Samia Said, Brandon Frost, Paul R Shearing, Stefan Guldin, Thomas S Miller

{"title":"Structural Evolution of Silicon Nitride Anodes during Electrochemical Lithiation.","authors":"Adam J Lovett, Máté Füredi, Liam Bird, Samia Said, Brandon Frost, Paul R Shearing, Stefan Guldin, Thomas S Miller","doi":"10.1021/acselectrochem.4c00230","DOIUrl":"10.1021/acselectrochem.4c00230","url":null,"abstract":"Silicon nitride (SiN x ), a conversion-alloying lithium-ion battery electrode with excellent potential to replace silicon and graphite anodes, offers improved cycle stability and fast-charging capabilities. During the formation cycle(s), SiN x irreversibly converts into a mixture of lithiated silicon and nitridosilicate matrix. However, beyond this basic understanding, there is limited fundamental insight into how the post-conversion structure results in improved electrochemical performance. This significantly hinders the optimization and commercialization prospects of SiN x anodes. Herein, operando electrochemical atomic force microscopy is used to uncover the morphological and chemo-mechanical changes of SiN x thin films during the conversion reaction. We elucidate that the post-conversion SiN x forms silicon domains embedded within a matrix with a core-shell-like structure comprised of a stiff outer nitridosilicate surface and softer inner Si-rich core. The silicon domains that form have very stable dimensions (∼100 nm in diameter) that, crucially, remain smaller than the critical cracking threshold of silicon. This results in a more mechanically robust anode, anticipated to be free from the adverse effects of cracking, pulverization, and subsequent capacity fade. Our work marks an important advance in the fundamental understanding of silicon nitride anodes and offers a pathway to their incorporation into next-generation batteries.","PeriodicalId":520400,"journal":{"name":"ACS electrochemistry","volume":"1 6","pages":"962-973"},"PeriodicalIF":0.0,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12147161/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144268353","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}

引用次数: 0

Determination of Enantiomeric Excess in Confined Aprotic Solvent. 非质子溶剂中过量对映体的测定。

ACS electrochemistry Pub Date : 2025-02-26 eCollection Date: 2025-06-05 DOI: 10.1021/acselectrochem.4c00219

Emer B Farrell, Fionn McNeill, Dominik Duleba, Adria Martínez-Aviño, Patrick J Guiry, Robert P Johnson

{"title":"Determination of Enantiomeric Excess in Confined Aprotic Solvent.","authors":"Emer B Farrell, Fionn McNeill, Dominik Duleba, Adria Martínez-Aviño, Patrick J Guiry, Robert P Johnson","doi":"10.1021/acselectrochem.4c00219","DOIUrl":"10.1021/acselectrochem.4c00219","url":null,"abstract":"The validation of the stereochemical purity of synthesized compounds is a requisite for the fine-chemical industry, particularly in the production of enantiopure drug compounds. However, most methodologies employed in the determination of enantiopurity require carefully chosen chiral GC or HPLC columns, increasing associated cost, analysis time, and complexity. Herein, we present a nanopore-based technology for the determination of enantiopurity, exploiting changes in ion-current rectification of quartz nanopipettes containing an aprotic organic electrolyte. Changes in solvent ordering at the quartz surface upon enantiomerically preferential adsorption give rise to distinguishable current-voltage responses. The applicability of our simple and cost-effective platform is demonstrated through the determination of the enantiomeric excess of commercially available (R)- and (S)-enantiomers of 4-methoxy-α-methylbenzylamine and duloxetine hydrochloride, as well as the product of a decarboxylative asymmetric allylic alkylation. Ion-current rectification (ICR)-based enantiomeric excess determination is completed within minutes, using negligible sample volumes and with simple low-cost electrical instrumentation.","PeriodicalId":520400,"journal":{"name":"ACS electrochemistry","volume":"1 6","pages":"928-939"},"PeriodicalIF":0.0,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12147146/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144268348","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}

引用次数: 0

Effect of Coordination Environment and Electronic Coupling on Redox Entropy in a Family of Dinuclear Complexes. 配位环境和电子耦合对一类双核配合物氧化还原熵的影响

ACS electrochemistry Pub Date : 2025-02-18 eCollection Date: 2025-05-01 DOI: 10.1021/acselectrochem.4c00186

Daniela Carmona-Pérez, Meiqin Gao, Samantha Andes, William W Brennessel, Agnes E Thorarinsdottir

{"title":"Effect of Coordination Environment and Electronic Coupling on Redox Entropy in a Family of Dinuclear Complexes.","authors":"Daniela Carmona-Pérez, Meiqin Gao, Samantha Andes, William W Brennessel, Agnes E Thorarinsdottir","doi":"10.1021/acselectrochem.4c00186","DOIUrl":"https://doi.org/10.1021/acselectrochem.4c00186","url":null,"abstract":"The elucidation of factors that govern the temperature sensitivity of the electrochemical potential is essential to the development of electrochemical systems with target properties. Toward this end, we report a series of isostructural homo- and heterometallic M2 (M = FeII, FeIII, ZnII) complexes supported by a phenoxo-centered tetrapyridyl ligand and ancillary carboxylate ligands that enables independent change in (i) charge, (ii) coordination environment of the redox-active center(s), and (iii) electronic coupling strength between redox centers. Variable-temperature electrochemical analysis of the series reveals the temperature coefficient for Fe-based redox couples to be highly dependent on the coordination environment of the redox-active center(s), with Fe centers in a pseudo-octahedral [FeN3O3] coordination environment affording a 2-fold greater temperature coefficient for the FeIII/FeII redox couple than those in ancillary ferrocenyl groups. In contrast, identical temperature coefficients for the FeIII/FeII redox event in Fe2 and FeZn complexes establish electronic coupling strength to have a minimal impact on the temperature dependence of the Fe-based redox couple. Taken together, these results provide important insights for the design of molecular compounds with target redox properties, and they provide the first examination of how electronic coupling influences the temperature dependence of the redox potential and the associated redox entropy in molecular compounds.","PeriodicalId":520400,"journal":{"name":"ACS electrochemistry","volume":"1 5","pages":"741-753"},"PeriodicalIF":0.0,"publicationDate":"2025-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12051193/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144057622","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}

引用次数: 0

Sensitive Imaging of Electroactive Species in Plasmonic Electrochemical Microscopy Enabled by Nanoconfinement. 利用纳米约束实现电活性物质在等离子体电化学显微镜中的灵敏成像。

ACS electrochemistry Pub Date : 2025-02-17 eCollection Date: 2025-06-05 DOI: 10.1021/acselectrochem.4c00227

Samuel Groysman, Yisi Chen, Adaly Garcia, Christian Martinez, Kevin Diego-Perez, Miriam Benavides, Yi Chen, Zijian Wan, Shaopeng Wang, Rujia Liu, Dengchao Wang, Chong Liu, Yixian Wang

{"title":"Sensitive Imaging of Electroactive Species in Plasmonic Electrochemical Microscopy Enabled by Nanoconfinement.","authors":"Samuel Groysman, Yisi Chen, Adaly Garcia, Christian Martinez, Kevin Diego-Perez, Miriam Benavides, Yi Chen, Zijian Wan, Shaopeng Wang, Rujia Liu, Dengchao Wang, Chong Liu, Yixian Wang","doi":"10.1021/acselectrochem.4c00227","DOIUrl":"10.1021/acselectrochem.4c00227","url":null,"abstract":"Spatially resolved sensing is a burgeoning area of electrochemistry that, in contrast to traditional electrochemical techniques, allows for the analysis of heterogeneous systems such as neurotransmitter release from cells. Of these techniques, optical microscopy methods are valued for real-time high throughput sensing. However, improving the sensitivity of many optical techniques remains a challenge. Here, we modify the gold (Au) electrode of the standard plasmonic electrochemical microscopy (PEM) setup with a mesoporous silica film (MSF) to achieve sensitive imaging of the electroactive species. Sensitivity enhancement occurs via species nanoconfinement from the attraction of ions to the negatively charged silica films, thereby increasing the local concentration change and magnifying the PEM signal. The performance of Au-MSF electrodes in the PEM setup was investigated using 1,1'-ferrocenedimethanol, whose oxidized form carries a positive charge. Results revealed enhancement of the sensing signal, with up to 37-fold improvement in the detection limit and up to 23 times improvement in the sensitivity. Importantly, Au-MSF electrodes allowed for the quantification of detected concentrations, in contrast to Au electrodes, for which R2 values were unacceptably low. Furthermore, Au-MSF electrodes also showed increased sensitivity for dopamine detection compared to Au electrodes and were able to visualize localized dopamine release, showing this setup's great promise for biological applications, such as real-time imaging of the neurotransmitter release.","PeriodicalId":520400,"journal":{"name":"ACS electrochemistry","volume":"1 6","pages":"974-986"},"PeriodicalIF":0.0,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12147111/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144268351","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}

引用次数: 0

Distinguishing between Photothermal and Photoelectric Effects in Li-Ion Batteries. 区分锂离子电池中的光热效应和光电效应。

ACS electrochemistry Pub Date : 2025-02-07 eCollection Date: 2025-06-05 DOI: 10.1021/acselectrochem.4c00212

Lifu Tan, Byung-Man Kim, Kohei Shimokawa, Su Jin Heo, Arvind Pujari, Michael De Volder

{"title":"Distinguishing between Photothermal and Photoelectric Effects in Li-Ion Batteries.","authors":"Lifu Tan, Byung-Man Kim, Kohei Shimokawa, Su Jin Heo, Arvind Pujari, Michael De Volder","doi":"10.1021/acselectrochem.4c00212","DOIUrl":"10.1021/acselectrochem.4c00212","url":null,"abstract":"Over the past decades, photo-enhanced batteries where light is used to improve the rate performance or recharge batteries have received increased attention in the academic community. However, the underlying mechanisms that contribute to performance enhancement in several photo-enhanced batteries are still under debate. For instance, photothermal effects, resulting from light absorption and subsequent conversion to heat through non-radiative relaxation, and photo-induced charge transfer, involving the generation and separation of electron-hole pairs under the illumination resulting in charge carrier transport, can be challenging to disentangle. This study aims to distinguish between the photothermal and photo-induced charge transfer in TiO2 and Fe2O3 as model systems because of their photoactivity and ability to store Li-ions. Using ultraviolet photoelectron spectroscopy (UPS) and UV-vis spectroscopy, we measure the band positions of these materials, and by a combination of different electrochemical processes, we demonstrate the transition from photothermal dominated to photoelectric effects in these materials. These results further illustrate the fact that different processes take place in photo-batteries, and this work provides a workflow to investigate these complex interactions.","PeriodicalId":520400,"journal":{"name":"ACS electrochemistry","volume":"1 6","pages":"921-927"},"PeriodicalIF":0.0,"publicationDate":"2025-02-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12147141/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144268349","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}

引用次数: 0

Porous Transport Layers for Anion Exchange Membrane Water Electrolysis: The Impact of Morphology and Composition. 阴离子交换膜电解水的多孔传输层：形态和组成的影响。

ACS electrochemistry Pub Date : 2025-02-07 eCollection Date: 2025-06-05 DOI: 10.1021/acselectrochem.4c00207

Melissa E Kreider, Ambar R Maldonado Santos, Arielle L Clauser, Matthew E Sweers, Leiming Hu, Emily K Volk, Ai-Lin Chan, Joshua D Sugar, Shaun M Alia

{"title":"Porous Transport Layers for Anion Exchange Membrane Water Electrolysis: The Impact of Morphology and Composition.","authors":"Melissa E Kreider, Ambar R Maldonado Santos, Arielle L Clauser, Matthew E Sweers, Leiming Hu, Emily K Volk, Ai-Lin Chan, Joshua D Sugar, Shaun M Alia","doi":"10.1021/acselectrochem.4c00207","DOIUrl":"10.1021/acselectrochem.4c00207","url":null,"abstract":"Anion exchange membrane water electrolysis (AEMWE) is an emerging technology for the low-cost production of hydrogen. However, the efficiency and durability of AEMWE devices is currently insufficient to compete with other low-temperature electrolysis technologies. The porous transport layer (PTL) is a critical cell component that remains relatively unoptimized for AEMWE. In this study, we demonstrate that device performance is significantly affected by the morphology and composition of the PTL. For Ni fiber-based PTLs with a ∼2 μm Co3O4 oxygen evolution reaction catalyst layer, decreasing the pore size and porosity resulted in a 20% increase in current density at 2 V in 1 M KOH supporting electrolyte. Alloy PTLs with even lower porosity had a higher performance; in particular, the stainless steel PTL gave an 80% increase in current density relative to Ni. Without Co3O4, the alloy PTLs still demonstrated high activity, indicating that the PTL material was catalytically active. However, characterization of the electrode and electrolyte after testing indicated that the alloy PTLs also underwent restructuring and corrosion processes that may limit long-term stability. This study demonstrates that the design of PTLs with improved morphology and composition is an important area of focus to achieve AEMWE performance targets.","PeriodicalId":520400,"journal":{"name":"ACS electrochemistry","volume":"1 6","pages":"897-909"},"PeriodicalIF":0.0,"publicationDate":"2025-02-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12147155/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144268350","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}

引用次数: 0

Identifying and Quantifying Loss Sources in Anion-Exchange Membrane Water Electrolyzers. 阴离子交换膜水电解槽损耗源的识别与量化。

ACS electrochemistry Pub Date : 2025-01-17 eCollection Date: 2025-05-01 DOI: 10.1021/acselectrochem.4c00156

Karam Yassin, Rinat Attias, Yoed Tsur, Dario R Dekel

{"title":"Identifying and Quantifying Loss Sources in Anion-Exchange Membrane Water Electrolyzers.","authors":"Karam Yassin, Rinat Attias, Yoed Tsur, Dario R Dekel","doi":"10.1021/acselectrochem.4c00156","DOIUrl":"https://doi.org/10.1021/acselectrochem.4c00156","url":null,"abstract":"Anion-exchange membrane (AEM) water electrolyzers (AEMWEs) have gained significant attention for their ability to utilize precious-metal-free catalysts and environmentally friendly fluorine-free hydrocarbon polymeric membranes. In this study, we identify and quantify the sources of performance losses in operando AEMWEs using an innovative approach based on electrochemical impedance spectroscopy and MATLAB-based impedance spectroscopy genetic programming. Using this approach, we move beyond conventional equivalent circuit models to develop a proper and analytical model of the distribution function of relaxation times (DFRT), enabling a deeper analysis of Faradaic and non-Faradaic processes. We apply this framework to isolate the critical processes-ohmic, ionic transport, charge transfer, and mass transfer-across various conditions, including KOH concentration, dry cathode operation mode with different anode electrolytes (KOH, K2CO3, and pure water), cell temperature, and membrane type. Our results indicate a considerable performance reduction as the KOH concentration in the anode decreases, primarily due to the relatively high ionic transport resistance. Our observations show that the performance of dry cathode operation with KOH in the anode yields a comparable performance to dual-side electrolyte feeding due to sufficient water back-diffusion from the anode, which efficiently maintains cathode hydration. Conversely, using pure water as an electrolyte in the anode with a dry cathode significantly increases cell resistances and compromises ionic transport, underscoring the urgent need for highly conductive ionomeric materials and strategies. These insights indicate that using DFRT to evaluate the AEMWE operation by separating and associating the electrochemical phenomena could simplify system design while enabling more efficient generation of dry, pure hydrogen and advancing the technology toward commercial application.","PeriodicalId":520400,"journal":{"name":"ACS electrochemistry","volume":"1 5","pages":"655-666"},"PeriodicalIF":0.0,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12051194/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144002154","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}

引用次数: 0

Water-Assisted Electrosynthesis of a Lithium-Aluminum Intermetallic from a Lithium Chloride-Ionic Liquid Melt. 水辅助电合成氯化锂离子液体熔体中的锂-铝金属间化合物。

ACS electrochemistry Pub Date : 2025-01-17 eCollection Date: 2025-05-01 DOI: 10.1021/acselectrochem.4c00134

Fabrizio Bernini, Giovanni Bertoni, Adele Mucci, Andrea Marchetti, Daniele Malferrari, Gian Carlo Gazzadi, Marco Ricci, Sergio Marras, Remo Proietti Zaccaria, Enzo Rotunno, Alessio Nicolini, Nassima Yamini, Andrea Cornia, Marco Borsari, Andrea Paolella

{"title":"Water-Assisted Electrosynthesis of a Lithium-Aluminum Intermetallic from a Lithium Chloride-Ionic Liquid Melt.","authors":"Fabrizio Bernini, Giovanni Bertoni, Adele Mucci, Andrea Marchetti, Daniele Malferrari, Gian Carlo Gazzadi, Marco Ricci, Sergio Marras, Remo Proietti Zaccaria, Enzo Rotunno, Alessio Nicolini, Nassima Yamini, Andrea Cornia, Marco Borsari, Andrea Paolella","doi":"10.1021/acselectrochem.4c00134","DOIUrl":"https://doi.org/10.1021/acselectrochem.4c00134","url":null,"abstract":"Although water is considered detrimental for Li-ion battery technology, a 1% w/w amount of water in a melt of LiCl in ionic liquid 1-butyl-3-methylimidazolium chloride promotes the reduction of lithium into a LiAl intermetallic along with water oxidation to O2 gas. The electrodeposition of an intermetallic layer of several micrometers thickness is demonstrated by combining complementary techniques, such as galvanostatics, X-ray diffraction, electron energy-loss spectroscopy, mass spectrometry, and 1H nuclear magnetic resonance. The concentration of water in the ionic liquid is found to be a critical feature, as no Li is deposited when ionic liquid is dried. Our findings highlight an innovative and simple method to produce a LiAl intermetallic by using water and lithium chloride as chemical reagents.","PeriodicalId":520400,"journal":{"name":"ACS electrochemistry","volume":"1 5","pages":"599-606"},"PeriodicalIF":0.0,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12051454/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144061475","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}

引用次数: 0

Electrochemical Flow Reactors: Mass Transport, iR Drop, and Membrane-Free Performance with In-Line Analysis. 电化学流动反应器：质量传输，iR下降和无膜性能与在线分析。

ACS electrochemistry Pub Date : 2025-01-14 eCollection Date: 2025-04-03 DOI: 10.1021/acselectrochem.4c00167

W J Niels Klement, Elia Savino, Sarah Rooijmans, Patty P M F A Mulder, N Scott Lynn, Wesley R Browne, Elisabeth Verpoorte

{"title":"Electrochemical Flow Reactors: Mass Transport, iR Drop, and Membrane-Free Performance with In-Line Analysis.","authors":"W J Niels Klement, Elia Savino, Sarah Rooijmans, Patty P M F A Mulder, N Scott Lynn, Wesley R Browne, Elisabeth Verpoorte","doi":"10.1021/acselectrochem.4c00167","DOIUrl":"10.1021/acselectrochem.4c00167","url":null,"abstract":"Continuous flow reactors are promising for electrochemical conversions, in large part due to the potentially rapid refreshment of reagents over the electrode surface. Microfluidic reactors enable a high degree of control over the fluid flow. Diffusion to and from the electrode and electrode area determine the efficiency of electrochemical conversion. The effective electrode area is limited by the loss in electrode potential due to iR drop, and further electrode length (and hence area) is limited due to ineffective mass transport to and from the electrode. Here, we report on a microfluidic electrochemical device with large (long) area electrodes running in parallel, which both minimizes the iR drop and ensures a constant electrode potential along the whole length of the electrodes. The electrodes are separated by laminar flow in the channels, instead of by a membrane, thereby reducing cell resistance. Herringbone grooves are used to increase mass transport rates by inducing transverse flow. We confirm fluid flow behavior in the devices using computational fluid dynamics (CFD) and verify the results experimentally using in-line and off-line UV/vis absorption and resonance Raman spectroscopy. We anticipate that this approach will aid future development of electrochemical flow reactors, enabling larger area-electrodes and realizing greater efficiencies.","PeriodicalId":520400,"journal":{"name":"ACS electrochemistry","volume":"1 4","pages":"504-515"},"PeriodicalIF":0.0,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11973871/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143813314","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}

引用次数: 0