Faraday Discussions最新文献_第10页

IF 3.4 3区化学

Faraday Discussions Pub Date : 2024-07-11 DOI: 10.1039/D4FD00102H

Daniel Speckhard, Tim Bechtel, Luca M. Ghiringhelli, Martin Kuban, Santiago Rigamonti and Claudia Draxl

引用次数: 0

Seeing nanoscale electrocatalytic reactions at individual MoS2 particles under an optical microscope: probing sub-mM oxygen reduction reaction† 在光学显微镜下观察单个 MoS2 颗粒的纳米级电催化反应：探测亚毫微米级的氧还原反应

IF 3.4 3区化学

Faraday Discussions Pub Date : 2024-07-10 DOI: 10.1039/D4FD00132J

Nikan Afsahi, Zhu Zhang, Sanli Faez, Jean-Marc Noël, Manas Ranjan Panda, Mainak Majumder, Naimeh Naseri, Jean-François Lemineur and Frédéric Kanoufi

{"title":"Seeing nanoscale electrocatalytic reactions at individual MoS2 particles under an optical microscope: probing sub-mM oxygen reduction reaction†","authors":"Nikan Afsahi, Zhu Zhang, Sanli Faez, Jean-Marc Noël, Manas Ranjan Panda, Mainak Majumder, Naimeh Naseri, Jean-François Lemineur and Frédéric Kanoufi","doi":"10.1039/D4FD00132J","DOIUrl":"10.1039/D4FD00132J","url":null,"abstract":"MoS2 is a promising electrocatalytic material for replacing noble metals. Nanoelectrochemistry studies, such as using nanoelectrochemical cell confinement, have particularly helped in demonstrating the preferential electrocatalytic activity of MoS2 edges. These findings have been accompanied by considerable research efforts to synthesize edge-abundant nanomaterials. However, to fully apprehend their electrocatalytic performance, at the single particle level, new instrumental developments are also needed. Here, we feature a highly sensitive refractive index based optical microscopy technique, namely interferometric scattering microscopy (iSCAT), for monitoring local electrochemistry at single MoS2 petal-like sub-microparticles. This work focuses on the oxygen reduction reaction (ORR), which operates at low current densities and thus requires high-sensitivity imaging techniques. By employing a precipitation reaction to reveal the ORR activity and utilizing the high spatial resolution and contrast of iSCAT, we achieve the sensitivity required to evaluate the ORR activity at single MoS2 particles.","PeriodicalId":49075,"journal":{"name":"Faraday Discussions","volume":"257 ","pages":" 107-125"},"PeriodicalIF":3.4,"publicationDate":"2024-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/fd/d4fd00132j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141578049","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Optical materials discovery and design with federated databases and machine learning† 通过联合数据库和机器学习发现和设计光学材料

IF 3.4 3区化学

Faraday Discussions Pub Date : 2024-07-10 DOI: 10.1039/D4FD00092G

Victor Trinquet, Matthew L. Evans, Cameron J. Hargreaves, Pierre-Paul De Breuck and Gian-Marco Rignanese

{"title":"Optical materials discovery and design with federated databases and machine learning†","authors":"Victor Trinquet, Matthew L. Evans, Cameron J. Hargreaves, Pierre-Paul De Breuck and Gian-Marco Rignanese","doi":"10.1039/D4FD00092G","DOIUrl":"10.1039/D4FD00092G","url":null,"abstract":"Combinatorial and guided screening of materials space with density-functional theory and related approaches has provided a wealth of hypothetical inorganic materials, which are increasingly tabulated in open databases. The OPTIMADE API is a standardised format for representing crystal structures, their measured and computed properties, and the methods for querying and filtering them from remote resources. Currently, the OPTIMADE federation spans over 20 data providers, rendering over 30 million structures accessible in this way, many of which are novel and have only recently been suggested by machine learning-based approaches. In this work, we outline our approach to non-exhaustively screen this dynamic trove of structures for the next-generation of optical materials. By applying MODNet, a neural network-based model for property prediction, within a combined active learning and high-throughput computation framework, we isolate particular structures and chemistries that should be most fruitful for further theoretical calculations and for experimental study as high-refractive-index materials. By making explicit use of automated calculations, federated dataset curation and machine learning, and by releasing these publicly, the workflows presented here can be periodically re-assessed as new databases implement OPTIMADE, and new hypothetical materials are suggested.","PeriodicalId":49075,"journal":{"name":"Faraday Discussions","volume":"256 ","pages":" 459-482"},"PeriodicalIF":3.4,"publicationDate":"2024-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141573174","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Single-molecule electrochemical imaging of ‘split waves’ in the electrocatalytic (EC′) mechanism† 对电催化（EC）机制中的 "分裂波 "进行单分子电化学成像

IF 3.4 3区化学

Faraday Discussions Pub Date : 2024-07-06 DOI: 10.1039/D4FD00126E

Wandong Zhao and Jin Lu

引用次数: 0

Electrochemical nucleation and growth kinetics: insights from single particle scanning electrochemical cell microscopy studies† 电化学成核和生长动力学：单颗粒扫描电化学电池显微镜研究的启示

IF 3.4 3区化学

Faraday Discussions Pub Date : 2024-07-06 DOI: 10.1039/D4FD00131A

Kenneth Osoro, Sinthia Rahman and Caleb M. Hill

{"title":"Electrochemical nucleation and growth kinetics: insights from single particle scanning electrochemical cell microscopy studies†","authors":"Kenneth Osoro, Sinthia Rahman and Caleb M. Hill","doi":"10.1039/D4FD00131A","DOIUrl":"10.1039/D4FD00131A","url":null,"abstract":"The kinetics of particle nucleation and growth are critical to a wide variety of electrochemical systems. While studies carried out at the single particle level are promising for improving our understanding of nucleation and growth processes, conventional analytical frameworks commonly employed in bulk studies may not be appropriate for single particle experiments. Here, we present scanning electrochemical cell microscopy (SECCM) studies of Ag nucleation and growth on carbon and indium tin oxide (ITO) electrodes. Statistical analyses of the data from these experiments reveal significant discrepancies with traditional, quasi-equilibrium kinetic models commonly employed in the analysis of particle nucleation in electrochemical systems. Time-dependent kinetic models are presented capable of appropriately analysing the data generated via SECCM to extract meaningful chemical quantities such as surface energies and kinetic rate constants. These results demonstrate a powerful new approach to the analysis of single particle nucleation and growth data which could be leveraged in differentiating behavior within spatially heterogeneous systems.","PeriodicalId":49075,"journal":{"name":"Faraday Discussions","volume":"257 ","pages":" 126-136"},"PeriodicalIF":3.4,"publicationDate":"2024-07-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/fd/d4fd00131a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141573175","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Advanced algorithm for step detection in single-entity electrochemistry: a comparative study of wavelet transforms and convolutional neural networks† 单实体电化学中阶跃检测的先进算法：小波变换和卷积神经网络的比较研究

IF 3.4 3区化学

Faraday Discussions Pub Date : 2024-07-04 DOI: 10.1039/D4FD00130C

Ziwen Zhao, Arunava Naha, Nikolaos Kostopoulos and Alina Sekretareva

引用次数: 0

Integrated scanning electrochemical cell microscopy platform with local electrochemical impedance spectroscopy using a preamplifier† 利用前置放大器进行局部电化学阻抗光谱分析的集成扫描电化学细胞显微镜平台

IF 3.4 3区化学

Faraday Discussions Pub Date : 2024-07-02 DOI: 10.1039/D4FD00122B

Ancheng Wang, Rong Jin and Dechen Jiang

引用次数: 0

The electrochemical modulation of single molecule fluorescence† 单分子荧光的电化学调制

IF 3.4 3区化学

Faraday Discussions Pub Date : 2024-07-02 DOI: 10.1039/D4FD00111G

Ying Yang, Yuanqing Ma and J. Justin Gooding

{"title":"The electrochemical modulation of single molecule fluorescence†","authors":"Ying Yang, Yuanqing Ma and J. Justin Gooding","doi":"10.1039/D4FD00111G","DOIUrl":"10.1039/D4FD00111G","url":null,"abstract":"Recently it has been shown that electrochemistry, instead of using high intensity lasers, can be used to modulate the intensity of emission of fluorophores and even switch fluorophores between their ON and OFF states as required for single molecule localisation microscopy. This modulation of fluorescence does not necessarily correlate with direct oxidation and reduction of the dyes. Questions arise from this unexpected observation related to what is the electrochemistry that occurs, what are the important variables in switching fluorophores electrochemically and what range of dyes can be modulated with electrochemistry. Herein we seek to answer some of these questions. We demonstrate how to effectively modulate the fluorescence intensity of organic dye-labelled cell samples on an indium tin oxide surface using electrochemistry with redox-active mediators present in an oxygen scavenger buffer. We showed the electrochemical fluorescence modulation is sensitive to the applied potential and the excitation laser intensity, indicating the possibility of coupled photochemical and electrochemical reactions occurring. We also compared the electrochemical fluorescence modulation of representative oxazine, rhodamine, and cyanine dyes using ATTO 655, Alexa Fluor 488, and Alexa Fluor 647. Different dyes with distinctly different structural cores show fluorescence modulation to different extents. The electrochemical fluorescence modulation will be applicable in fluorescence imaging techniques as well as biosensing.","PeriodicalId":49075,"journal":{"name":"Faraday Discussions","volume":"257 ","pages":" 333-343"},"PeriodicalIF":3.4,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141527889","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

High-throughput calculations and machine learning modeling of 17O NMR in non-magnetic oxides 非磁性氧化物中 $^{17}text{O}$ NMR 的高通量计算和机器学习建模

IF 3.4 3区化学

Faraday Discussions Pub Date : 2024-07-01 DOI: 10.1039/D4FD00128A

Zhiyuan Li, Bo Zhao, Hongbin Zhang and Yixuan Zhang

{"title":"High-throughput calculations and machine learning modeling of 17O NMR in non-magnetic oxides","authors":"Zhiyuan Li, Bo Zhao, Hongbin Zhang and Yixuan Zhang","doi":"10.1039/D4FD00128A","DOIUrl":"10.1039/D4FD00128A","url":null,"abstract":"The only NMR-active oxygen isotope, oxygen-17 (17O), serves as a sensitive probe due to its large chemical shift range, the electric field gradient at the oxygen site, and the quadrupolar interaction. Consequently, 17O solid-state NMR offers unique insights into local structures and finds significant applications in the studies of disorder, reactivity, and host–guest chemistry. Despite recent advances in sensitivity enhancement, isotopic labeling, and NMR crystallography, the application of 17O solid-state NMR is still hindered by low natural abundance, costly enrichment, and challenges in handling spectrum signals. Density functional theory calculations and machine learning techniques offer an alternative approach to mapping the local crystal structures to NMR parameters. However, the lack of high-quality data remains a challenge, despite the establishment of some datasets. In this study, we implement and execute a high-throughput workflow combining AiiDA and CASTEP to evaluate the NMR parameters. Focusing on non-magnetic oxides, we have chosen over 7100 binary, ternary, and quaternary compounds from the Materials Project database and performed calculations. Furthermore, using various descriptors for the local crystalline environments, we model the 17O NMR parameters using machine learning techniques, further enhancing our ability to predict and understand 17O NMR parameters in oxide crystals.","PeriodicalId":49075,"journal":{"name":"Faraday Discussions","volume":" 0","pages":" 72-87"},"PeriodicalIF":3.4,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141527890","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Delivery of carbon dioxide to an electrode surface using a nanopipette 使用纳米管将二氧化碳输送到电极表面

IF 3.4 3区化学

Faraday Discussions Pub Date : 2024-07-01 DOI: 10.1039/D4FD00124A

Jaimy Monteiro, Harry Dunne and Kim McKelvey

引用次数: 0