Faraday Discussions最新文献

Investigating temperature influences on shell growth and microstructural variations in bay scallops: insights from multiscale microscopy. 研究温度对海湾扇贝壳生长和微观结构变化的影响：来自多尺度显微镜的见解。

IF 3.3 3区化学

Faraday Discussions Pub Date : 2025-05-27 DOI: 10.1039/d5fd00023h

Benazir Khurshid, Arnaud Benchetrite, Lise Guichaoua, Nicolas Brodusch, Bryce D Stewart, Roland Kröger, Raynald Gauvin, Martin Mallet, Réjean Tremblay, Natalie Reznikov

{"title":"Investigating temperature influences on shell growth and microstructural variations in bay scallops: insights from multiscale microscopy.","authors":"Benazir Khurshid, Arnaud Benchetrite, Lise Guichaoua, Nicolas Brodusch, Bryce D Stewart, Roland Kröger, Raynald Gauvin, Martin Mallet, Réjean Tremblay, Natalie Reznikov","doi":"10.1039/d5fd00023h","DOIUrl":"https://doi.org/10.1039/d5fd00023h","url":null,"abstract":"Scallops (order Pectinida) are well-known for their robust and beautiful calcitic shells that protect them from external impacts and predators. Scallops respond to environmental conditions, including water temperature, salinity, and food supply, which are reflected in the shell growth rates and patterning. The bay scallop (Argopecten irradians) is a species of high ecological and aquacultural value in North America, and its habitat may expand towards higher latitudes with inevitable global warming. To investigate the effect of water temperature on the accretion rate and the polycrystalline microstructure of the Bay scallop shell, we conducted a controlled growth experiment on juveniles, 4 weeks following their larval metamorphosis. Approximately 400 individuals, collected from a hatchery 4 weeks after metamorphosis, were then reared in reconstituted seawater for 9 weeks at 23 °C and 26 °C. At 7-, 9-, 11-, and 13-weeks post-metamorphosis, calcein was added to the water for 7 hours for fluorescent staining, and then equal batches of scallops were collected and fixed. Morphologic characterization of bay scallop shells included micro-computed X-ray tomography for 3D measurements to measure shell thickness, and fluorescence light microscopy for accretion rate assessment. We used mechanical testing of complete shells in compression to assess their stiffness, strength and toughness. Microstructural analysis of the shells included scanning electron microscopy and crystallographic analysis by electron backscattered diffraction. The scallops reared in warmer water exhibited a faster growth rate with shells showing higher calcite grain misorientation, no difference in relative shell thickness, and inconclusive difference in the shell mechanical properties. This study may help us to understand the multifarious implications of climate change.","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144148705","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

Three-dimensional imaging of vasculature and forming quail femur using cryo-correlative light and electron microscopy (cryo-CLEM). 用低温相关光电子显微镜（cryo-CLEM）观察鹌鹑股骨血管和成形的三维成像。

IF 3.3 3区化学

Faraday Discussions Pub Date : 2025-05-27 DOI: 10.1039/d5fd00022j

Anne Seewald, Jingxiao Zhong, Macarena Siri, Peter Fratzl, Emeline Raguin

{"title":"Three-dimensional imaging of vasculature and forming quail femur using cryo-correlative light and electron microscopy (cryo-CLEM).","authors":"Anne Seewald, Jingxiao Zhong, Macarena Siri, Peter Fratzl, Emeline Raguin","doi":"10.1039/d5fd00022j","DOIUrl":"https://doi.org/10.1039/d5fd00022j","url":null,"abstract":"Bone mineralization during embryonic development requires the transport and deposition of an enormous amount of mineral precursors. In avian embryos, blood vessels play a dual role in this context: facilitating the demineralization of the eggshell to supply calcium and other minerals on the one hand, and mediating their deposition into the developing skeleton on the other. Understanding the interface between blood vessels and the surrounding tissues is therefore crucial for unraveling the mechanisms underlying biomineralization. However, visualizing this interface poses significant challenges and requires imaging methods that preserve the ultrastructure in a close-to-native state. Here we present a detailed methodology for a cryogenic correlative light and electron microscopy (cryo-CLEM) workflow to investigate the transport of mineral precursors in blood vessels of the femur of quail embryos during bone development. To achieve this, we use a fluorophore-conjugated antibody to label endothelial cells, which form the inner lining of blood vessels and which mediate exchanges between the bloodstream and developing tissues. This approach enables precise localization of blood vessels through fluorescence microscopy, which is subsequently correlated with 3D high-resolution electron microscopy using Focused Ion Beam-Scanning Electron Microscopy (FIB-SEM). This methodology allows imaging of a sufficient volume to observe both the lumen of the blood vessels and the surrounding matrix, providing deeper insights into calcium transport and bone mineralization during quail embryogenesis.","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144148707","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

Fiber formation seen through the high-resolution computational microscope. 通过高分辨率计算机显微镜观察到的纤维形成。

IF 3.3 3区化学

Faraday Discussions Pub Date : 2025-05-23 DOI: 10.1039/d4fd00188e

Tomasz K Piskorz, Vasudevan Lakshminarayanan, Alex H de Vries, Jan H van Esch

{"title":"Fiber formation seen through the high-resolution computational microscope.","authors":"Tomasz K Piskorz, Vasudevan Lakshminarayanan, Alex H de Vries, Jan H van Esch","doi":"10.1039/d4fd00188e","DOIUrl":"https://doi.org/10.1039/d4fd00188e","url":null,"abstract":"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.","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-05-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","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":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Revealing enameloid shark chemistry at the nanoscale. 在纳米尺度上揭示类搪瓷鲨鱼的化学性质。

IF 3.3 3区化学

Faraday Discussions Pub Date : 2025-05-23 DOI: 10.1039/d5fd00019j

Alberto Perez-Huerta, Eshita Samajpati, Gabriela A Farfan

{"title":"Revealing enameloid shark chemistry at the nanoscale.","authors":"Alberto Perez-Huerta, Eshita Samajpati, Gabriela A Farfan","doi":"10.1039/d5fd00019j","DOIUrl":"https://doi.org/10.1039/d5fd00019j","url":null,"abstract":"Shark teeth are considered excellent bio-archives because of their high abundance and preservation potential. Chemical proxies recorded by the teeth enameloid layers are used to interpret ecological and environmental parameters throughout the geological record. The use of these proxies relies on the assumption that biomineralization processes for enameloid formation have remained constant during shark evolution. Here, we test such an assumption by comparing the chemical composition at the nanoscale, using the technique of atom probe tomography (APT), of enameloid in modern and fossil shark teeth. Results indicate that there are clear differences in the chemistry at the core and inter-crystalline grain boundaries of fluorapatite crystals. These boundaries are enriched in strontium in all shark teeth, whereas there are differences in the distribution of magnesium, sodium, and iron. Teeth of the modern shark Isurus oxyrinchus have magnesium and sodium distributed at the inter-crystalline grain boundaries. Teeth of Eocene fossil sharks, Striatolamia macrota and Macrorhizodus praecursor, have a unique distribution of iron, at the inter-crystalline boundaries, and sodium, at the core of the crystals. This observation may indicate that biomineralization processes resulting in enameloid formation are not constant across the phylogeny of sharks. Overall, our findings strongly suggest that the enameloid content and distribution of magnesium, iron, strontium, and sodium are highly controlled by biomineralization processes. The role of magnesium and sodium seems to be similar in mammalian enamel and shark enameloid formation. Yet, nanoscale chemical differences, such as the presence of strontium in tooth enameloid, are likely associated to functional morphology.","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-05-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144126253","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

Multiphase chemistry: general discussion. 多相化学：一般讨论。

IF 3.3 3区化学

Faraday Discussions Pub Date : 2025-05-22 DOI: 10.1039/d5fd90014j

Sarah Albertin, Markus Ammann, Patrick Ayotte, Thorsten Bartels-Rausch, Hendrik Bluhm, James Brean, Natalie Brett, Lucy V Brown, Tillmann Buttersack, Lucy J Carpenter, Rohit Chikkaraddy, Hugh Coe, Jenée D Cyran, Natasha Garner, Dwayne Heard, Deanna Huff, Saewung Kim, Jingqiu Mao, Jennifer G Murphy, Christian Pfrang, Kerri A Pratt, Matti Rissanen, Joel Savarino, Céline Toubin, Thomas Whale, Megan Willis

引用次数: 0

Unveiling the structure of protein-based hydrogels by overcoming cryo-SEM sample preparation challenges. 通过克服低温扫描电镜样品制备挑战揭示蛋白质基水凝胶的结构。

IF 3.3 3区化学

Faraday Discussions Pub Date : 2025-05-22 DOI: 10.1039/d4fd00204k

Dimitra Katrantzi, Stuart Micklethwaite, Nicole Hondow, Andy Brown, Lorna Dougan

{"title":"Unveiling the structure of protein-based hydrogels by overcoming cryo-SEM sample preparation challenges.","authors":"Dimitra Katrantzi, Stuart Micklethwaite, Nicole Hondow, Andy Brown, Lorna Dougan","doi":"10.1039/d4fd00204k","DOIUrl":"https://doi.org/10.1039/d4fd00204k","url":null,"abstract":"Protein-based hydrogels have gained significant attention for their potential use in applications such as drug delivery and tissue engineering. Their internal structure is complex, spans across multiple length scales and affects their functionality, yet is not well understood because of folded proteins' sensitivity to physical and chemical perturbations and the high water content of hydrogels. Cryo-scanning electron microscopy (cryo-SEM) has the potential to reveal such hierarchical structure when hydrated hydrogels are prepared with appropriate cryofixation. We show for photochemically cross-linked, folded globular bovine serum albumin (BSA) protein hydrogels that preparation artefacts are reduced by in situ gelation, high pressure freezing (HPF), plasma focused ion beam (pFIB) milling, sublimation, and low dose secondary electron imaging. Cryo-SEM of folded BSA protein hydrogels prepared in this way reveals a heterogeneous network with nanoscale porosity (∼60 nm pores) surrounded by high secondary electron emission regions (∼30 nm diameter) interconnected by narrower, lower emission regions (∼20 nm length). This heterogeneous network structure is consistent with small angle scattering studies of folded protein hydrogels, with fractal-like clusters connected by intercluster regions. We further test the potential of cryo-SEM to detect the impact of protein unfolding on hydrogel network formation and reveal nanoscale differences in cluster sizes consistent with those derived from scattering data. Importantly, cryo-SEM directly images pores for sizing in both systems, with initial results on BSA suggesting protein unfolding induces an increase of ∼10 nm in pore sizes. Our findings on cryo-SEM sample preparation challenges and solutions provide new opportunities to link hydrogel structure to function.","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144118371","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

Co-assembled supramolecular hydrogels: nano-IR sheds light on tripeptide assemblies. 共组装的超分子水凝胶：纳米红外揭示了三肽组装。

IF 3.3 3区化学

Faraday Discussions Pub Date : 2025-05-21 DOI: 10.1039/d4fd00193a

Paola Alletto, Ana M Garcia, Federica Piccirilli, Silvia Marchesan

引用次数: 0

Transport and chemistry: general discussion. 运输和化学：一般性讨论。

IF 3.3 3区化学

Faraday Discussions Pub Date : 2025-05-21 DOI: 10.1039/d5fd90013a

Markus Ammann, James Brean, Lucy J Carpenter, Rohit Chikkaraddy, Martyn P Chipperfield, Barbara D'Anna, Valerio Ferracci, Markus M Frey, Dwayne E Heard, Saffron G Heddell, Alicia Hoffman, Deanna Huff, Bianca Lauster, Kathy S Law, Jingqiu Mao, Claudia Mohr, Jennifer G Murphy, Peter K Peterson, Kerri A Pratt, Tjarda J Roberts, Joel Savarino, Freya Squires, Jochen Stutz, Megan Willis, Xin Yang

引用次数: 0

Multicomponent supramolecular hydrogels composed of cationic phenylalanine derivatives and anionic amino acids. 由阳离子苯丙氨酸衍生物和阴离子氨基酸组成的多组分超分子水凝胶。

IF 3.3 3区化学

Faraday Discussions Pub Date : 2025-05-21 DOI: 10.1039/d4fd00198b

Shruti Ghosh, Hannah E Distaffen, Christopher W Jones, Bradley L Nilsson

{"title":"Multicomponent supramolecular hydrogels composed of cationic phenylalanine derivatives and anionic amino acids.","authors":"Shruti Ghosh, Hannah E Distaffen, Christopher W Jones, Bradley L Nilsson","doi":"10.1039/d4fd00198b","DOIUrl":"https://doi.org/10.1039/d4fd00198b","url":null,"abstract":"Supramolecular hydrogels composed of self-assembled fluorenylmethoxycarbonyl phenylalanine (Fmoc-Phe) derivatives have been the focus of intense study as novel materials for biological applications that include drug delivery, tissue engineering, and regenerative medicine. Cationic Fmoc-Phe derivatives functionalized with diaminopropane (Fmoc-Phe-DAP) have been shown to undergo self-assembly and hydrogelation upon an increase in solution ionic strength by the addition of inorganic salts that provide cation-shielding counterions. Further, the identity of the inorganic salts modifies the assembly morphology and emergent viscoelastic properties of the resulting materials. Herein, we report multicomponent hydrogels composed of Fmoc-Phe-DAP derivatives in which hydrogelation is promoted by the addition of anionic amino acids, monosodium aspartate or monosodium glutamate. Aspartate and glutamate salts both support supramolecular gelation of Fmoc-Phe-DAP derivatives, although only the glutamate gels remain stable over periods longer than one hour. The assemblies formed by Fmoc-Phe-DAP derivatives in the presence of aspartate and glutamate are morphologically distinct relative to those formed in the presence of sodium chloride. The viscoelastic properties of stable glutamate/Fmoc-Phe-DAP derivative hydrogels are sensitive to the ratios of glutamate to Fmoc-Phe-DAP derivative, with increased concentrations of glutamate corresponding to higher viscoelastic strength. These multicomponent systems demonstrate that comixing unfunctionalized amino acids with self-assembling Fmoc-Phe-DAP derivatives is yet another effective method to modify the emergent properties of the resulting materials.","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144109141","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

Silylated peptides as building blocks for material synthesis using sol-gel polymerization. 硅基化多肽作为溶胶-凝胶聚合材料合成的基石。

IF 3.3 3区化学

Faraday Discussions Pub Date : 2025-05-20 DOI: 10.1039/d5fd00014a

Mehmet B Karakaplan, Vinay S Tiwari, Omer Agazani, Cécile Echalier, Gilles Subra, Meital Reches

{"title":"Silylated peptides as building blocks for material synthesis using sol-gel polymerization.","authors":"Mehmet B Karakaplan, Vinay S Tiwari, Omer Agazani, Cécile Echalier, Gilles Subra, Meital Reches","doi":"10.1039/d5fd00014a","DOIUrl":"https://doi.org/10.1039/d5fd00014a","url":null,"abstract":"The bottom-up approach exploits simple building blocks to generate new materials with desired physical and chemical characteristics. Here, we combine two bottom-up routes that occur under mild conditions, self-assembly and sol-gel synthesis, to program the shape and structure of materials. While self-assembly occurs through non-covalent interactions, sol-gel synthesis involves forming covalent bonds. As a proof of concept, we chose the self-assembled peptide Phe-Phe and its fluorinated analogue Phe(4-F)-Phe(4-F) to template the sol-gel process. These peptides were silylated to allow their self-mineralization. Scanning electron microscopy and atomic force microscope analysis revealed the formation of rod-shaped structures for the silylated Phe-Phe while spherical particles were formed by its fluorinated analogue. The size of the particles ranges from nano to micron scale. Fourier transform infrared spectrometry suggested the presence of parallel β-sheet secondary structure and siloxane bond formation that can stabilize these structures. Overall this approach can be adopted for other self-assembled peptides for generating new materials using a bottom-up approach.","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144109143","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