ACS electrochemistry最新文献

英文中文

Optically Transparent Carbon Electrodes for Single Entity Electrochemistry.

ACS electrochemistry

Pub Date : 2024-10-08 eCollection Date: 2025-01-02 DOI: 10.1021/acselectrochem.4c00048

Kelly L Vernon, Tipsiri Pungsrisai, Oluwasegun J Wahab, Sasha E Alden, Yaxu Zhong, Myung-Hoon Choi, Ekta Verma, Anne K Bentley, Kathleen O Bailey, Sara E Skrabalak, Xingchen Ye, Katherine A Willets, Lane A Baker

We demonstrate the application and benefit of optically transparent carbon electrodes (OTCEs) for single entity nanoelectrochemistry. OTCEs are prepared by pyrolyzing thin photoresist films on fused quartz coverslips to create conductive, transparent, thin films. Optical, electrical, topographical, and electrochemical properties of OTCEs are characterized to evaluate their suitability for single entity electrochemistry. Nanoscale electrochemical imaging of the OTCEs using scanning electrochemical cell microscopy (SECCM) revealed uniform electrochemical activity for reduction of the hexaammineruthenium(III) redox complex, that was comparable to Au-coated glass, and in contrast to the heterogeneity observed with commonly used indium tin oxide (ITO) substrates. Additionally, we demonstrate the utility of the prepared OTCEs for correlative SECCM-scanning electron microscopy studies of the hydrogen evolution reaction at the surface of Au nanocubes. Lastly, we demonstrate the benefit of OTCEs for optoelectrochemical experiments by optically monitoring the electrodissolution of Au nanocrystals. These results establish OTCE as a viable transparent support electrode for multimode electrochemical and optical microscopy of nanocrystals and other entities.

{"title":"Optically Transparent Carbon Electrodes for Single Entity Electrochemistry.","authors":"Kelly L Vernon, Tipsiri Pungsrisai, Oluwasegun J Wahab, Sasha E Alden, Yaxu Zhong, Myung-Hoon Choi, Ekta Verma, Anne K Bentley, Kathleen O Bailey, Sara E Skrabalak, Xingchen Ye, Katherine A Willets, Lane A Baker","doi":"10.1021/acselectrochem.4c00048","DOIUrl":"10.1021/acselectrochem.4c00048","url":null,"abstract":"We demonstrate the application and benefit of optically transparent carbon electrodes (OTCEs) for single entity nanoelectrochemistry. OTCEs are prepared by pyrolyzing thin photoresist films on fused quartz coverslips to create conductive, transparent, thin films. Optical, electrical, topographical, and electrochemical properties of OTCEs are characterized to evaluate their suitability for single entity electrochemistry. Nanoscale electrochemical imaging of the OTCEs using scanning electrochemical cell microscopy (SECCM) revealed uniform electrochemical activity for reduction of the hexaammineruthenium(III) redox complex, that was comparable to Au-coated glass, and in contrast to the heterogeneity observed with commonly used indium tin oxide (ITO) substrates. Additionally, we demonstrate the utility of the prepared OTCEs for correlative SECCM-scanning electron microscopy studies of the hydrogen evolution reaction at the surface of Au nanocubes. Lastly, we demonstrate the benefit of OTCEs for optoelectrochemical experiments by optically monitoring the electrodissolution of Au nanocrystals. These results establish OTCE as a viable transparent support electrode for multimode electrochemical and optical microscopy of nanocrystals and other entities.","PeriodicalId":520400,"journal":{"name":"ACS electrochemistry","volume":"1 1","pages":"93-102"},"PeriodicalIF":0.0,"publicationDate":"2024-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11728714/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143061845","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

Redox-Detecting Deep Learning for Mechanism Discernment in Cyclic Voltammograms of Multiple Redox Events.

ACS electrochemistry

Pub Date : 2024-10-03 eCollection Date: 2025-01-02 DOI: 10.1021/acselectrochem.4c00014

Benjamin B Hoar, Weitong Zhang, Yuanzhou Chen, Jingwen Sun, Hongyuan Sheng, Yucheng Zhang, Yisi Chen, Jenny Y Yang, Cyrille Costentin, Quanquan Gu, Chong Liu

In electrochemical analysis, mechanism assignment is fundamental to understanding the chemistry of a system. The detection and classification of electrochemical mechanisms in cyclic voltammetry set the foundation for subsequent quantitative evaluation and practical application, but are often based on relatively subjective visual analyses. Deep-learning (DL) techniques provide an alternative, automated means that can support experimentalists in mechanism assignment. Herein, we present a custom DL architecture dubbed as EchemNet, capable of assigning both voltage windows and mechanism classes to electrochemical events within cyclic voltammograms of multiple redox events. The developed technique detects over 96% of all electrochemical events in simulated test data and shows a classification accuracy of up to 97.2% on redox events with 8 known mechanisms. This newly developed DL model, the first of its kind, proves the feasibility of redox-event detection and electrochemical mechanism classification with minimal a priori knowledge. The DL model will augment human researchers' productivity and constitute a critical component in a general-purpose autonomous electrochemistry laboratory.

{"title":"Redox-Detecting Deep Learning for Mechanism Discernment in Cyclic Voltammograms of Multiple Redox Events.","authors":"Benjamin B Hoar, Weitong Zhang, Yuanzhou Chen, Jingwen Sun, Hongyuan Sheng, Yucheng Zhang, Yisi Chen, Jenny Y Yang, Cyrille Costentin, Quanquan Gu, Chong Liu","doi":"10.1021/acselectrochem.4c00014","DOIUrl":"10.1021/acselectrochem.4c00014","url":null,"abstract":"In electrochemical analysis, mechanism assignment is fundamental to understanding the chemistry of a system. The detection and classification of electrochemical mechanisms in cyclic voltammetry set the foundation for subsequent quantitative evaluation and practical application, but are often based on relatively subjective visual analyses. Deep-learning (DL) techniques provide an alternative, automated means that can support experimentalists in mechanism assignment. Herein, we present a custom DL architecture dubbed as EchemNet, capable of assigning both voltage windows and mechanism classes to electrochemical events within cyclic voltammograms of multiple redox events. The developed technique detects over 96% of all electrochemical events in simulated test data and shows a classification accuracy of up to 97.2% on redox events with 8 known mechanisms. This newly developed DL model, the first of its kind, proves the feasibility of redox-event detection and electrochemical mechanism classification with minimal a priori knowledge. The DL model will augment human researchers' productivity and constitute a critical component in a general-purpose autonomous electrochemistry laboratory.","PeriodicalId":520400,"journal":{"name":"ACS electrochemistry","volume":"1 1","pages":"52-62"},"PeriodicalIF":0.0,"publicationDate":"2024-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11728721/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143061804","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

The Role of Surfactant in Electrocatalytic Carbon Dioxide Reduction in the Absence of Metal Cations.

ACS electrochemistry

Pub Date : 2024-10-03 eCollection Date: 2025-01-02 DOI: 10.1021/acselectrochem.4c00040

Hansaem Jang, Adrian M Gardner, Lucy J Walters, Alex R Neale, Laurence J Hardwick, Alexander J Cowan

Carbon dioxide electroreduction does not occur on Au when metal cations are absent from the electrode surfaces. Here we show that the electroreduction can be enabled without metal cations, albeit with low efficiency, by the presence of cationic surfactants on Au. The findings demonstrate that in addition to possibly stabilizing CO₂ reduction intermediates the presence of surfactants plays a role in suppressing the competing reactions. At potentials negative of a critical potential, a cationic surfactant adsorbs onto the electrode surface, displacing interfacial water molecules, hampering the access of proton donors to the electrode surface and inhibiting hydrogen evolution during electrolysis.

引用次数: 0

类型

全部化学•材料生命科学医学物理工程技术环境•农林材料科学地球科学法学管理学化学环境科学与生态学计算机科学教育学经济学农林科学人文科学生物学数学物理与天体物理心理学综合性期刊其他工业工程理学历史学农学文学信息工程

数据库

全部 ACS Publications Elsevier ieeexplore Springer The Royal Society of Chemistry Wiley

期刊

ACS electrochemistry

全部 Acc. Chem. Res. ACS Applied Bio Materials ACS Appl. Electron. Mater. ACS Appl. Energy Mater. ACS Appl. Mater. Interfaces ACS Appl. Nano Mater. ACS Appl. Polym. Mater. ACS BIOMATER-SCI ENG ACS Catal. ACS Cent. Sci. ACS Chem. Biol. ACS Chemical Health & Safety ACS Chem. Neurosci. ACS Comb. Sci. ACS Earth Space Chem. ACS Energy Lett. ACS Infect. Dis. ACS Macro Lett. ACS Mater. Lett. ACS Med. Chem. Lett. ACS Nano ACS Omega ACS Photonics ACS Sens. ACS Sustainable Chem. Eng. ACS Synth. Biol. Anal. Chem. BIOCHEMISTRY-US Bioconjugate Chem. BIOMACROMOLECULES Chem. Res. Toxicol. Chem. Rev. Chem. Mater. CRYST GROWTH DES ENERG FUEL Environ. Sci. Technol. Environ. Sci. Technol. Lett. Eur. J. Inorg. Chem. IND ENG CHEM RES Inorg. Chem. J. Agric. Food. Chem. J. Chem. Eng. Data J. Chem. Educ. J. Chem. Inf. Model. J. Chem. Theory Comput. J. Med. Chem. J. Nat. Prod. J PROTEOME RES J. Am. Chem. Soc. LANGMUIR MACROMOLECULES Mol. Pharmaceutics Nano Lett. Org. Lett. ORG PROCESS RES DEV ORGANOMETALLICS J. Org. Chem. J. Phys. Chem. J. Phys. Chem. A J. Phys. Chem. B J. Phys. Chem. C J. Phys. Chem. Lett. Analyst Anal. Methods Biomater. Sci. Catal. Sci. Technol. Chem. Commun. Chem. Soc. Rev. CHEM EDUC RES PRACT CRYSTENGCOMM Dalton Trans. Energy Environ. Sci. ENVIRON SCI-NANO ENVIRON SCI-PROC IMP ENVIRON SCI-WAT RES Faraday Discuss. Food Funct. Green Chem. Inorg. Chem. Front. Integr. Biol. J. Anal. At. Spectrom. J. Mater. Chem. A J. Mater. Chem. B J. Mater. Chem. C Lab Chip Mater. Chem. Front. Mater. Horiz. MEDCHEMCOMM Metallomics Mol. Biosyst. Mol. Syst. Des. Eng. Nanoscale Nanoscale Horiz. Nat. Prod. Rep. New J. Chem. Org. Biomol. Chem. Org. Chem. Front. PHOTOCH PHOTOBIO SCI PCCP Polym. Chem.

﹀