Faraday Discussions最新文献

{"title":"Spectroelectrochemistry and light active process at nanointerface: general discussion","authors":"Zhifeng Ding, Andrew G. Ewing, Kaiyu X. Fu, Caleb M. Hill, Kaoru Hiramoto, Frédéric Kanoufi, John J. Kasianowicz, Christine Kranz, Christian Kuttner, Shuang-Yan Lang, Fei Li, Liang Liu, Jin Lu, Andrew R. Mount, Hang Ren, Yuanhua Shao, Mei Shen, Yasufumi Takahashi, Wei Wang, Fan Xia, Guohui Zhang, Ziwen Zhao and Yige Zhou","doi":"10.1039/D4FD90070G","DOIUrl":"10.1039/D4FD90070G","url":null,"abstract":"","PeriodicalId":49075,"journal":{"name":"Faraday Discussions","volume":"257 ","pages":" 151-164"},"PeriodicalIF":3.4,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143044979","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}

{"title":"Low-cost electrochemical gas sensing of vertical differences in wintertime air composition (CO, NO, NO2, O3) in Fairbanks, Alaska†","authors":"Tjarda J. Roberts, Meeta Cesler-Maloney and William R. Simpson","doi":"10.1039/D4FD00177J","DOIUrl":"10.1039/D4FD00177J","url":null,"abstract":"<p >Wintertime Fairbanks, Alaska, experiences episodes of severely poor air quality, when local emissions (<em>e.g.</em>, home-heating, vehicular) are enhanced by cold conditions and are trapped by temperature inversions. Monitoring of atmospheric composition, and in particular vertical gradients in composition, is challenging under cold Arctic conditions. This study demonstrates that multiple sets of low-cost electrochemical sensors can provide accurate measurement of CO, NO, NO<small>₂</small>, and O<small>₃</small> air composition across wide-ranging cold Arctic temperatures (0 °C to −30 °C). The sensors quantify vertical gradients in downtown Fairbanks’ atmospheric composition during winter 2021. Low-cost electrochemical sensors (with temperature co-measured) were characterised by cross-comparison to a regulatory air-quality monitoring site. We demonstrate excellent agreement of the electrochemical sensors with the reference monitors (<em>R</em><small>²</small> &gt; 0.86–0.98), with mean absolute errors &lt;5 ppbv (NO, NO<small>₂</small>, O<small>₃</small>) and &lt;50 ppbv (CO) over gas-ranges of 10–100’s, and 3000 ppbv, respectively, sufficient for using the low-cost electrochemical sensors to quantitatively investigate NO–NO<small>₂</small>–O<small>₃</small> atmospheric chemistry. During four weeks in February–March 2021, sensors placed on the rooftop (20 m) and base (3 m) of a building in downtown Fairbanks identified strong gradients in atmospheric composition over a very short &lt;20 m vertical scale at times when near-surface temperature inversions were present. At night, CO and NO<small>_<em>x</em></small> were more concentrated at the surface than aloft, and surface ozone was depleted whilst sometimes being present aloft. During the daytime, when solar radiation heated the surface, inversions were disrupted by efficient vertical mixing that mixed in ozone-rich air from above. The low-cost sensor observations demonstrate that near-surface pollutant trapping was correlated with thermal inversions and trace O<small>₃</small>–NO<small>_<em>x</em></small> atmospheric chemistry, and quantify a local O<small>_<em>x</em></small> source from direct “primary” NO<small>₂</small> emissions, with a directly emitted NO<small>₂</small> : NO<small>_<em>x</em></small> ratio of 0.13 mol mol<small>⁻¹</small>. The sensors also characterise NO<small>_<em>x</em></small> emissions, finding a NO<small>_<em>x</em></small> : CO of 0.15 mol mol<small>⁻¹</small>. When well-characterised, low-cost electrochemical sensors can provide valuable measurements of local emissions and vertically-resolved atmospheric composition, with sufficient accuracy to trace atmospheric chemistry in cold and stable wintertime urban environments.</p>","PeriodicalId":49075,"journal":{"name":"Faraday Discussions","volume":"258 ","pages":" 307-327"},"PeriodicalIF":3.4,"publicationDate":"2025-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/fd/d4fd00177j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143571694","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}

{"title":"Systems nanoelectrochemistry from single entity to ensemble: general discussion","authors":"Paolo Actis, Koichi Aoki, Lane A. Baker, Giada Caniglia, Ning Dang, Zhifeng Ding, Andrew G. Ewing, Kaiyu X. Fu, J. Justin Gooding, Kaoru Hiramoto, Dechen Jiang, Frédéric Kanoufi, John J. Kasianowicz, Christine Kranz, Shuang-Yan Lang, Fei Li, Haoran Li, Liang Liu, Yi-Tao Long, Jin Lu, Si-Min Lu, Kim McKelvey, Andrew R. Mount, Hang Ren, Yuanhua Shao, Mei Shen, Zuzanna S. Siwy, Yasufumi Takahashi, Juan Tang, Haiyan Wang, Jun-Gang Wang, Kang Wang, Liang Wang, Yunong Wang, Fan Xia, Ruo-Chen Xie, Yi-Lun Ying, Guohui Zhang and Ziwen Zhao","doi":"10.1039/D4FD90068E","DOIUrl":"10.1039/D4FD90068E","url":null,"abstract":"","PeriodicalId":49075,"journal":{"name":"Faraday Discussions","volume":"257 ","pages":" 399-424"},"PeriodicalIF":3.4,"publicationDate":"2025-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143031682","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}

{"title":"Confined nanopore electrochemistry: general discussion","authors":"Paolo Actis, Koichi Aoki, Lane A. Baker, Zhifeng Ding, Andrew G. Ewing, Kaiyu X. Fu, J. Justin Gooding, Jun Huang, Frédéric Kanoufi, John J. Kasianowicz, Moonjoo Kim, Christine Kranz, Christian Kuttner, Fei Li, Liang Liu, Wei Liu, Jin Lu, Si-Min Lu, Kim McKelvey, Andrew R. Mount, Hang Ren, Yuanhua Shao, Yasufumi Takahashi, Shuo Tan, Juan Tang, Haiyan Wang, Kang Wang, Liang Wang, Weihua Wang, Fan Xia, Tianyi Xiong, Yi-Lun Ying, Yueming Zhai, Ziwen Zhao and Yige Zhou","doi":"10.1039/D4FD90067G","DOIUrl":"10.1039/D4FD90067G","url":null,"abstract":"","PeriodicalId":49075,"journal":{"name":"Faraday Discussions","volume":"257 ","pages":" 88-106"},"PeriodicalIF":3.4,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143021282","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}

{"title":"Programming two-component peptide self-assembly by tuning the hydrophobic linker†","authors":"Sangshuang Li, Huayang Liu, Yu Fang, Yaoting Li, Laicheng Zhou, Dinghao Chen, Juan Liang and Huaimin Wang","doi":"10.1039/D4FD00209A","DOIUrl":"10.1039/D4FD00209A","url":null,"abstract":"<p >Molecular self-assembly enables the formation of intricate networks through non-covalent interactions, serving as a key strategy for constructing structures ranging from molecules to macroscopic forms. While zero-dimensional and one-dimensional nanostructures have been widely achieved, two-dimensional nanostrip structures present unique advantages in biomedical and other applications due to their high surface area and potential for functionalization. However, their efficient design and precise regulation remain challenging. This study systematically explores how different hydrophobic amino acid linkers impact the microscopic morphology in two-component co-assembly systems with strong electrostatic interactions. The introduction of the AA linker resulted in distinctive 2D nanostrips, which stacked to form bilayer sheets, whereas VV, LL, and NleNle linkers formed one-dimensional fibers. In contrast, GG and PP linkers did not produce stable aggregates. Our findings highlight the role of intermolecular interactions in the development of 2D assemblies, providing new insights into the design and application of 2D materials.</p>","PeriodicalId":49075,"journal":{"name":"Faraday Discussions","volume":"260 ","pages":" 403-416"},"PeriodicalIF":3.1,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143955872","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}

{"title":"Phytantriol and monoolein in aqueous deep eutectic solvent and protic ionic liquid solutions†","authors":"Karen J. Edler, Gregory G. Warr, Alexander M. Djerdjev, Minh Thu Lam, Adrian M. Hawley and Stephen Mudie","doi":"10.1039/D5FD00004A","DOIUrl":"10.1039/D5FD00004A","url":null,"abstract":"<p >Lyotropic liquid crystal gels of phytantriol and monoolein are well known examples of self-assembled systems in water, which have multiple applications across biomedical and materials science. However aqueous systems can be restricted by rapid solvent evaporation, and the limited solubility of some species in water. Here we explore the formation of liquid crystalline phases of phytantriol and monoolein in mixtures of water with two protic ionic liquids, ethylammonium nitrate (EAN) and ethanolammonium nitrate (EtAN), and three deep eutectic solvents (DES) formed from mixtures of choline chloride with urea, fructose or citric acid. The structures of the gel phase in excess solvent were measured using small angle X-ray scattering for a fixed lipid concentration (5% w/w) as a function of temperature. The phase diagrams of both lipids in DES–water mixtures and the non-amphiphilic ionic liquid, EtAN, indicate that higher negative curvature inverse hexagonal structures are favoured by addition of water. However, the amphiphilic ionic liquid EAN swells and stabilises the cubic <em>Pn</em>3<em>m</em> structure. The interplay of solvent structure, polarity and molecular size are key to understanding the formation and stability of lyotropic liquid crystalline gels in these systems.</p>","PeriodicalId":49075,"journal":{"name":"Faraday Discussions","volume":"260 ","pages":" 94-112"},"PeriodicalIF":3.1,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/fd/d5fd00004a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144075071","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}

{"title":"Fiber formation seen through the high-resolution computational microscope†","authors":"Tomasz K. Piskorz, Vasudevan Lakshminarayanan, Alex H. de Vries and Jan H. van Esch","doi":"10.1039/D4FD00188E","DOIUrl":"10.1039/D4FD00188E","url":null,"abstract":"<p >Supramolecular fibers draw widespread attention due to their role in biological systems and ability to form complex materials exhibiting rich and dynamic behavior. Although the information about the supramolecular structure is encoded in their molecular blocks, a complete understanding of how this information translates into the final structure requires detailed insights into the energy landscape of the process and the possible routes across this landscape. Here, we study the formation of 1,3,5-cyclohexanetricarboxamide fibers by a Markov state model of molecular dynamics simulations with the polarizable CHARMM Drude force-field. We provide insights into all stages of supramolecular fiber formation up to microsecond timescales, starting from primary nucleation, through fiber elongation and secondary nucleation, and finally, the assembly of single fibers into bundles. Our results show that nucleation involves a rapid collapse of dissolved monomers into disordered assemblies, which gradually transform into nuclei and then grow into elongated fibers. Moreover, elongation and secondary nucleation appeared to be competing processes, depending on the density of the monomers adsorbed at the fiber–liquid interface. Finally, bundling involves the initial association of fibers by interactions between surface-exposed groups, followed by stabilization of the bundle by surface reorganization, which allows for favorable interactions between aromatic groups.</p>","PeriodicalId":49075,"journal":{"name":"Faraday Discussions","volume":"260 ","pages":" 269-282"},"PeriodicalIF":3.1,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/fd/d4fd00188e?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144126252","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}

{"title":"Characterization of lipid chain order and dynamics in asymmetric membranes by solid-state NMR spectroscopy†","authors":"Oskar Engberg, Viola Döbel, Kathrin M. Engel and Daniel Huster","doi":"10.1039/D4FD00192C","DOIUrl":"10.1039/D4FD00192C","url":null,"abstract":"<p >We studied the structure and dynamics of asymmetric POPC<small>^out</small>/(POPE/POPG)<small>ⁱⁿ</small> and POPS<small>^out</small>/(POPE/POPG)<small>ⁱⁿ</small> lipid membranes. To this end, the outer layer of multilamellar POPE/POPG (molar ratio 9 : 1) vesicles was exchanged (using methyl-β-cyclodextrin) by either chain deuterated POPC-<em>d</em><small>₃₁</small> or POPS-<em>d</em><small>₃₁</small>, for which <small>²</small>H NMR order parameters were measured. As controls, we prepared symmetric POPC-<em>d</em><small>₃₁</small>/POPE/POPG and POPS-<em>d</em><small>₃₁</small>/POPE/POPG membranes of the composition of just the outer membrane of the asymmetric multilamellar vesicles and pure POPC-<em>d</em><small>₃₁</small> or POPS-<em>d</em><small>₃₁</small> multilamellar vesicles. Compared to symmetric membranes of the same lipid composition, chain order parameters (<em>S</em>) of the asymmetric preparations were higher in the upper half of the chain and lower in the lower half. This reshuffling of acyl chain order is also expressed in higher <small>²</small>H NMR Zeeman order relaxation rates (<em>R</em><small>_1Z</small>) of the chain segments in asymmetric membranes indicating alterations in the elastic properties of asymmetric bilayers as inferred from plots of <em>R</em><small>_1Z</small><em>vs. S</em><small>²</small>. Asymmetric membranes showed increased stiffness and rigidity although the lipid acyl chain composition between the inner and outer leaflets were identical. There were no indications for chain interdigitation between the two leaflets in the NMR spectra, which led us to speculate that the interleaflet coupling could be accomplished by sensing the differences in lipid packing densities between the two leaflets. These alterations in leaflet properties should have consequences for lipid protein interaction and ultimately protein function.</p>","PeriodicalId":49075,"journal":{"name":"Faraday Discussions","volume":"259 ","pages":" 282-299"},"PeriodicalIF":3.1,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/fd/d4fd00192c?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143953415","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}

{"title":"Transport of continental particulate over the Labrador Sea and entrainment are important pathways for glaciation of remote marine clouds†","authors":"Hugh Coe, Huihui Wu, Nicholas Marsden, Michael Biggart, Keith N. Bower, Tom Choularton, Michael Flynn, Martin W. Gallagher, Kezhen Hu, Gary Lloyd, Graeme J. Nott, Paul F. Field and Benjamin J. Murray","doi":"10.1039/D5FD00005J","DOIUrl":"10.1039/D5FD00005J","url":null,"abstract":"<p >Marine Arctic clouds greatly influence the radiative balance across the Arctic region and their effectiveness at scattering radiation changes considerably depending on cloud phase. Glaciation of these clouds relies on the presence of ice nucleating particles, which are often limited in number, so often clouds may be liquid even at temperatures well below 0 °C. As the Arctic region warms, cloud feedbacks may accelerate change or lessen absorbed solar radiation. Understanding aerosol–cloud interactions and the sources and pathways of aerosol particles across the Arctic region is central to improving our knowledge of these poorly understood processes. In this paper, aircraft observations of single particle chemical and physical properties are presented and the composition of cloud residuals in both warm and glaciated clouds are examined using a single-particle laser ablation aerosol particle mass spectrometer (LAAPToF). In cloud, the LAAPToF sampled behind a Counterflow Virtual Impactor (CVI) to detect cloud particle residuals, separated into liquid, mixed phase and ice clouds using <em>in situ</em> observations of the fractional ice water content. Three different air mass regimes were sampled: northerly winds in both the marine boundary layer and the lower free troposphere; westerly winds from Canada in both the marine boundary layer and the free troposphere; and periods when the boundary layer winds were northerly but the air immediately above the boundary layer was from continental Canada. When the air in the boundary layer and free troposphere was from the north, most clouds were in the liquid phase, however, considerably more glaciation was observed when the air immediately above the boundary layer clouds was from Canada regardless of the flow direction in the boundary layer. Sea salt particles dominate the observed out of cloud aerosol particle population and liquid cloud particle residuals. However, in the detected mixed phase and ice cloud particle residuals dust and bioaerosol particles were substantial in number. Since these are known to be effective ice-nucleating particles, the observations suggest that long range transport of continental air and entrainment is an important pathway for the supply of aerosol to the remote Arctic boundary layer.</p>","PeriodicalId":49075,"journal":{"name":"Faraday Discussions","volume":"258 ","pages":" 147-170"},"PeriodicalIF":3.4,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/fd/d5fd00005j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143539676","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}

{"title":"Poster list","authors":"","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":49075,"journal":{"name":"Faraday Discussions","volume":"256 ","pages":""},"PeriodicalIF":3.4,"publicationDate":"2025-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142976251","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}