Pub Date : 2024-06-28DOI: 10.1021/acsomega.4c00968
Zhuangyu Zhao, Nathan A. Rudman, Ivan J. Dmochowski
There is a need for photochemical tools that allow precise control of protein structure and function with visible light. We focus here on the s-tetrazine moiety, which can be installed at a specific protein site via the reaction between dichlorotetrazine and two adjacent sulfhydryl groups. Tetrazine’s compact size enables structural mimicry of native amino acid linkages, such as an intramolecular salt bridge or disulfide bond. In this study, we investigated tetrazine installation in three different proteins, where it was confirmed that the cross-linking reaction is highly efficient in aqueous conditions and site-specific when two cysteines are located proximally: the S–S distance was 4–10 Å. As shown in maltose binding protein, the tetrazine cross-linker can replace an interdomain salt bridge crucial for xenon binding and serve as a visible-light photoswitch to modulate 129Xe NMR contrast. This work highlights the ease of aqueous tetrazine bioconjugation and its applications for protein photoregulation.
{"title":"A Site-Specific Cross-Linker for Visible-Light Control of Proteins","authors":"Zhuangyu Zhao, Nathan A. Rudman, Ivan J. Dmochowski","doi":"10.1021/acsomega.4c00968","DOIUrl":"https://doi.org/10.1021/acsomega.4c00968","url":null,"abstract":"There is a need for photochemical tools that allow precise control of protein structure and function with visible light. We focus here on the <i>s</i>-tetrazine moiety, which can be installed at a specific protein site via the reaction between dichlorotetrazine and two adjacent sulfhydryl groups. Tetrazine’s compact size enables structural mimicry of native amino acid linkages, such as an intramolecular salt bridge or disulfide bond. In this study, we investigated tetrazine installation in three different proteins, where it was confirmed that the cross-linking reaction is highly efficient in aqueous conditions and site-specific when two cysteines are located proximally: the S–S distance was 4–10 Å. As shown in maltose binding protein, the tetrazine cross-linker can replace an interdomain salt bridge crucial for xenon binding and serve as a visible-light photoswitch to modulate <sup>129</sup>Xe NMR contrast. This work highlights the ease of aqueous tetrazine bioconjugation and its applications for protein photoregulation.","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":null,"pages":null},"PeriodicalIF":4.1,"publicationDate":"2024-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141524348","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}
Pub Date : 2024-06-28DOI: 10.1021/acsomega.4c03234
Dhruv Sharma, Dong Su Kim, Shin Young Oh, Kun Woong Lee, Won Seok Yang, Xuan Zhang, Sanjay Kumar Swami, Hyung Koun Cho, Sung Woon Cho
The implementation of photoelectrochemical water purification technology can address prevailing environmental challenges that impede the advancement and prosperity of human society. In this study, Cu, which is abundant on Earth, was fabricated using an electrochemical deposition process, in which the preferential orientation direction and carrier concentration of the Cu-based oxide semiconductor were artificially adjusted by carefully controlling the OH– and applied voltage. In particular, Cu2O grown with a sufficient supply of OH– ions exhibited the (111) preferred orientation, and the (200) surface facet was exposed, independently achieving 90% decomposition efficiency in a methyl orange (MO) solution for 100 min. This specialized method minimizes the recombination loss of electron–hole pairs by increasing the charge separation and transport efficiency of the bulk and surface of the Cu2O multifunctional absorption layer. These discoveries and comprehension not only offer valuable perspectives on mitigating self-photocorrosion in Cu2O absorbing layers but also provide a convenient and expeditious method for the mass production of water purification systems that harness unlimited solar energy. These properties enable significant energy saving and promote high-speed independent removal of organic pollutants (i.e., MO reduction) during the water purification process.
{"title":"Photoassisted Water Purification through an Electrochemically Artificially Adjusted p-Cu2O Light Absorption Layer","authors":"Dhruv Sharma, Dong Su Kim, Shin Young Oh, Kun Woong Lee, Won Seok Yang, Xuan Zhang, Sanjay Kumar Swami, Hyung Koun Cho, Sung Woon Cho","doi":"10.1021/acsomega.4c03234","DOIUrl":"https://doi.org/10.1021/acsomega.4c03234","url":null,"abstract":"The implementation of photoelectrochemical water purification technology can address prevailing environmental challenges that impede the advancement and prosperity of human society. In this study, Cu, which is abundant on Earth, was fabricated using an electrochemical deposition process, in which the preferential orientation direction and carrier concentration of the Cu-based oxide semiconductor were artificially adjusted by carefully controlling the OH<sup>–</sup> and applied voltage. In particular, Cu<sub>2</sub>O grown with a sufficient supply of OH<sup>–</sup> ions exhibited the (111) preferred orientation, and the (200) surface facet was exposed, independently achieving 90% decomposition efficiency in a methyl orange (MO) solution for 100 min. This specialized method minimizes the recombination loss of electron–hole pairs by increasing the charge separation and transport efficiency of the bulk and surface of the Cu<sub>2</sub>O multifunctional absorption layer. These discoveries and comprehension not only offer valuable perspectives on mitigating self-photocorrosion in Cu<sub>2</sub>O absorbing layers but also provide a convenient and expeditious method for the mass production of water purification systems that harness unlimited solar energy. These properties enable significant energy saving and promote high-speed independent removal of organic pollutants (i.e., MO reduction) during the water purification process.","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":null,"pages":null},"PeriodicalIF":4.1,"publicationDate":"2024-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141524354","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}
Pub Date : 2024-06-28DOI: 10.1021/acsomega.3c09035
Rafał Podgórski, Michał Wojasiński, Artur Małolepszy, Jakub Jaroszewicz, Tomasz Ciach
3D printing is a promising technique for producing bone implants, but there is still a need to adjust efficiency, facilitate production, and improve biocompatibility. Porous materials have a proven positive effect on the regeneration of bone tissue, but their production is associated with numerous limitations. In this work, we described a simple method of producing polymer or polymer-ceramic filaments for 3D-printing scaffolds by adding micrometer-scale porous structures on scaffold surfaces. Scaffolds included polycaprolactone (PCL) as the primary polymer, β-tricalcium phosphate (β-TCP) as the ceramic filler, and poly(ethylene glycol) (PEG) as a porogen. The pressurized filament extrusion gave flexible filaments composed of PCL, β-TCP, and PEG, which are ready to use in fused filament fabrication (FFF) 3D printers. Washing of 3D-printed scaffolds in ethanol solution removed PEG and revealed a microporous structure and ceramic particles on the scaffold’s surfaces. Furthermore, 3D-printed materials exhibit good printing precision, no cytotoxic properties, and highly impact MG63 cell alignment. Although combining PCL, PEG, and β-TCP is quite popular, the presented method allows the production of porous scaffolds with a well-organized structure without advanced equipment, and the produced filaments can be used to 3D print scaffolds on a simple commercially available 3D printer.
{"title":"Fabrication of 3D-Printed Scaffolds with Multiscale Porosity","authors":"Rafał Podgórski, Michał Wojasiński, Artur Małolepszy, Jakub Jaroszewicz, Tomasz Ciach","doi":"10.1021/acsomega.3c09035","DOIUrl":"https://doi.org/10.1021/acsomega.3c09035","url":null,"abstract":"3D printing is a promising technique for producing bone implants, but there is still a need to adjust efficiency, facilitate production, and improve biocompatibility. Porous materials have a proven positive effect on the regeneration of bone tissue, but their production is associated with numerous limitations. In this work, we described a simple method of producing polymer or polymer-ceramic filaments for 3D-printing scaffolds by adding micrometer-scale porous structures on scaffold surfaces. Scaffolds included polycaprolactone (PCL) as the primary polymer, β-tricalcium phosphate (β-TCP) as the ceramic filler, and poly(ethylene glycol) (PEG) as a porogen. The pressurized filament extrusion gave flexible filaments composed of PCL, β-TCP, and PEG, which are ready to use in fused filament fabrication (FFF) 3D printers. Washing of 3D-printed scaffolds in ethanol solution removed PEG and revealed a microporous structure and ceramic particles on the scaffold’s surfaces. Furthermore, 3D-printed materials exhibit good printing precision, no cytotoxic properties, and highly impact MG63 cell alignment. Although combining PCL, PEG, and β-TCP is quite popular, the presented method allows the production of porous scaffolds with a well-organized structure without advanced equipment, and the produced filaments can be used to 3D print scaffolds on a simple commercially available 3D printer.","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":null,"pages":null},"PeriodicalIF":4.1,"publicationDate":"2024-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141524350","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}
Pub Date : 2024-06-28DOI: 10.1021/acsomega.4c04218
Mutlu Karasoglu, Mustafa Özgür Öteyaka, Evren Yasa, Evren Tan, Melih Cemal Kuşhan
In this study, we investigated the effect of heat treatment (HT) and hot isostatic press (HIP) on the corrosion behavior of Ti6Al4 V, manufactured by electron beam melting (EBM) additive manufacturing. The preliminary results showed that the thermal process makes the columnar structure more pronounced and the α-lathe coarser compared to EBM. The β phase disappeared with the aging treatment and when increasing the HIP temperature treatment. According the open circuit potential (Eocp) behavior of samples, the HIP3 sample had performed more positive corrosion potential than rivals after 2 h of immersion probably due to equiaxed grain with coarser α-late and the absence of the β phase. In adverse, inferior corrosion behavior was observed for HIP1 because of a higher quantity of the β phase causing probably galvanic corrosion. The HIP process leads to a lower corrosion potential than EBM. At least one protective oxide layer formation was observed for all samples at the anodic branch, and the current density was lower for the HT3 sample. The microstructure analysis revealed the presence of the β-phase in the form of needle-like for the HT1 sample and HIP1 in the corroded area. Furthermore, the EDS line analysis showed the presence of aluminum with oxygen at the edge of the corrosion area for HIP1 suggesting aluminum plays a barrier against degradation. On the other hand, the HT1 showed higher impedance resistance due to the coarser α-lathe microstructure and well-defined β phase.
{"title":"Effect of Heat Treatment and Hot Isostatic Pressing on the Corrosion Behavior of Ti6Al4 V Parts Produced by Electron Beam Melting Additive Manufacturing Technology","authors":"Mutlu Karasoglu, Mustafa Özgür Öteyaka, Evren Yasa, Evren Tan, Melih Cemal Kuşhan","doi":"10.1021/acsomega.4c04218","DOIUrl":"https://doi.org/10.1021/acsomega.4c04218","url":null,"abstract":"In this study, we investigated the effect of heat treatment (HT) and hot isostatic press (HIP) on the corrosion behavior of Ti<sub>6</sub>Al<sub>4</sub> V, manufactured by electron beam melting (EBM) additive manufacturing. The preliminary results showed that the thermal process makes the columnar structure more pronounced and the α-lathe coarser compared to EBM. The β phase disappeared with the aging treatment and when increasing the HIP temperature treatment. According the open circuit potential (<i>E</i><sub>ocp</sub>) behavior of samples, the HIP3 sample had performed more positive corrosion potential than rivals after 2 h of immersion probably due to equiaxed grain with coarser α-late and the absence of the β phase. In adverse, inferior corrosion behavior was observed for HIP1 because of a higher quantity of the β phase causing probably galvanic corrosion. The HIP process leads to a lower corrosion potential than EBM. At least one protective oxide layer formation was observed for all samples at the anodic branch, and the current density was lower for the HT3 sample. The microstructure analysis revealed the presence of the β-phase in the form of needle-like for the HT1 sample and HIP1 in the corroded area. Furthermore, the EDS line analysis showed the presence of aluminum with oxygen at the edge of the corrosion area for HIP1 suggesting aluminum plays a barrier against degradation. On the other hand, the HT1 showed higher impedance resistance due to the coarser α-lathe microstructure and well-defined β phase.","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":null,"pages":null},"PeriodicalIF":4.1,"publicationDate":"2024-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141524138","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}
Pub Date : 2024-06-28DOI: 10.1021/acsomega.3c09738
Lan Wang, Ting Lu, Zhiping Li, Xiao Guo
The dissolution of elemental sulfur in acidic gas leads to its precipitation as gas pressure decreases, thereby causing potential damage to the formation due to the deposition of sulfur particles. Previous sulfur deposition prediction models often relied on the solubility of sulfur in acidic gas and the stress state of sulfur particles to determine the occurrence of deposition, thus establishing predictive models. However, in the presence of complex geological conditions, the multiphase flow through porous media and the adsorption of particles on pore throat walls can also influence sulfur particle deposition to some degree. It is well known that sulfur particle deposition during gas reservoir development exhibits instability, with multiple factors influencing the deposited sulfur particles. Particularly noteworthy is the influence of airflow velocity, which can resuspend sulfur particles that are physically adsorbed on pore throat surfaces, thereby reintegrating them into the gas phase. Additionally, the dynamic deposition of larger sulfur particles involves a dynamic process. This study elucidates the dynamic process of sulfur deposition by considering the diverse transport dynamics of sulfur particles. Physical adsorption and desorption behaviors of sulfur particles are determined based on variations in reservoir conditions. The desorption status of sulfur particles with different particle sizes within the formation is established by evaluating the equilibrium between the force exerted on the pore throat wall and the suspension force generated by gas flow. The critical conditions for sulfur deposition in Yuanba gas reservoir were obtained by substituting on-site parameters into calculations. Moreover, a mathematical model is proposed to describe the dynamic deposition and migration of sulfur particles, adopting principles from continuous porous media porous flow theory, fluid flow mass conservation, as well as sulfur particle desorption and migration. The formulated model is solved, and its resulting solution process and outcomes hold significant implications for numerical simulation and predictive assessment of the development impact on gas reservoirs, particularly in later stages.
{"title":"Microscopic Mechanism and Percolation Model of Dynamic Deposition of Elemental Sulfur Particles in Acidic Gas Reservoirs","authors":"Lan Wang, Ting Lu, Zhiping Li, Xiao Guo","doi":"10.1021/acsomega.3c09738","DOIUrl":"https://doi.org/10.1021/acsomega.3c09738","url":null,"abstract":"The dissolution of elemental sulfur in acidic gas leads to its precipitation as gas pressure decreases, thereby causing potential damage to the formation due to the deposition of sulfur particles. Previous sulfur deposition prediction models often relied on the solubility of sulfur in acidic gas and the stress state of sulfur particles to determine the occurrence of deposition, thus establishing predictive models. However, in the presence of complex geological conditions, the multiphase flow through porous media and the adsorption of particles on pore throat walls can also influence sulfur particle deposition to some degree. It is well known that sulfur particle deposition during gas reservoir development exhibits instability, with multiple factors influencing the deposited sulfur particles. Particularly noteworthy is the influence of airflow velocity, which can resuspend sulfur particles that are physically adsorbed on pore throat surfaces, thereby reintegrating them into the gas phase. Additionally, the dynamic deposition of larger sulfur particles involves a dynamic process. This study elucidates the dynamic process of sulfur deposition by considering the diverse transport dynamics of sulfur particles. Physical adsorption and desorption behaviors of sulfur particles are determined based on variations in reservoir conditions. The desorption status of sulfur particles with different particle sizes within the formation is established by evaluating the equilibrium between the force exerted on the pore throat wall and the suspension force generated by gas flow. The critical conditions for sulfur deposition in Yuanba gas reservoir were obtained by substituting on-site parameters into calculations. Moreover, a mathematical model is proposed to describe the dynamic deposition and migration of sulfur particles, adopting principles from continuous porous media porous flow theory, fluid flow mass conservation, as well as sulfur particle desorption and migration. The formulated model is solved, and its resulting solution process and outcomes hold significant implications for numerical simulation and predictive assessment of the development impact on gas reservoirs, particularly in later stages.","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":null,"pages":null},"PeriodicalIF":4.1,"publicationDate":"2024-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141524351","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}
This study examined the surface modification of titanium (Ti) implants to enhance early-stage osseointegration, which reduced the failure rate of internal fixation in osteoporotic fractures that inherently decrease in bone mass and strength. We employed a layer-by-layer electroassembly technique to deposit catalpol-containing hyaluronic acid/chitosan multilayers onto the surface of Ti implants. To evaluate the in vitro osteoinductive effects of catalpol-coated Ti implants, the robust osteoblast differentiation capacity of the murine preosteoblast cell line, MC3T3-E1, was employed. Furthermore, the performance of these implants was evaluated in vivo through femoral intramedullary implantation in Sprague–Dawley rats. The engineered implant effectively regulated catalpol release, promoting increased bone formation during the initial stages of implantation. The in vitro findings demonstrated that catalpol-coated Ti surfaces boosted ALP activity, cell proliferation as measured by CCK-8, and osteogenic protein expression via WB analysis, surpassing the uncoated Ti group (P < 0.05). In vivo micro-computed tomography (CT) and histological analyses revealed that catalpol-coated Ti significantly facilitated the formation and remodeling of new bone in osteoporotic rats at 14 days post-implantation. This study outlines a comprehensive and straightforward methodology for the fabrication of biofunctional Ti implants to address osteoporosis.
本研究探讨了如何对钛（Ti）植入物进行表面改性，以增强早期阶段的骨结合，从而降低骨质疏松性骨折内固定的失败率，因为骨质疏松性骨折本身就会降低骨量和骨强度。我们采用了逐层电装配技术，将含透明质酸/壳聚糖的梓醇多层膜沉积到钛植入物表面。为了评估梓醇涂层 Ti 植入体的体外骨诱导效应，我们采用了具有强大成骨细胞分化能力的小鼠前成骨细胞系 MC3T3-E1。此外，还通过在 Sprague-Dawley 大鼠的股骨髓内植入对这些植入物的性能进行了体内评估。工程植入物能有效调节梓醇的释放，在植入初期促进骨形成。体外研究结果表明，涂有 catalpol 的钛表面提高了 ALP 活性、CCK-8 测定的细胞增殖和 WB 分析的成骨蛋白表达，超过了未涂覆的钛组（P < 0.05）。体内显微计算机断层扫描（CT）和组织学分析表明，在植入后 14 天，梓醇涂层 Ti 显著促进了骨质疏松大鼠新骨的形成和重塑。这项研究为制造生物功能钛植入体解决骨质疏松症问题提供了一种全面而简单的方法。
{"title":"Enhancement of Local Osseointegration and Implant Stability of Titanium Implant in Osteoporotic Rats by Biomimetic Multilayered Structures Containing Catalpol","authors":"Jiayi Yang, Wei Zhang, Binghao Lin, Shuming Mao, Guangyao Liu, Kai Tan, Jiahao Tang","doi":"10.1021/acsomega.4c02322","DOIUrl":"https://doi.org/10.1021/acsomega.4c02322","url":null,"abstract":"This study examined the surface modification of titanium (Ti) implants to enhance early-stage osseointegration, which reduced the failure rate of internal fixation in osteoporotic fractures that inherently decrease in bone mass and strength. We employed a layer-by-layer electroassembly technique to deposit catalpol-containing hyaluronic acid/chitosan multilayers onto the surface of Ti implants. To evaluate the in vitro osteoinductive effects of catalpol-coated Ti implants, the robust osteoblast differentiation capacity of the murine preosteoblast cell line, MC3T3-E1, was employed. Furthermore, the performance of these implants was evaluated in vivo through femoral intramedullary implantation in Sprague–Dawley rats. The engineered implant effectively regulated catalpol release, promoting increased bone formation during the initial stages of implantation. The in vitro findings demonstrated that catalpol-coated Ti surfaces boosted ALP activity, cell proliferation as measured by CCK-8, and osteogenic protein expression via WB analysis, surpassing the uncoated Ti group (<i>P</i> < 0.05). In vivo micro-computed tomography (CT) and histological analyses revealed that catalpol-coated Ti significantly facilitated the formation and remodeling of new bone in osteoporotic rats at 14 days post-implantation. This study outlines a comprehensive and straightforward methodology for the fabrication of biofunctional Ti implants to address osteoporosis.","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":null,"pages":null},"PeriodicalIF":4.1,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141524211","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}
Pub Date : 2024-06-27DOI: 10.1021/acsomega.3c10033
Sascha Chur, Lennart Kulik, Volker Schulz-von der Gathen, Marc Böke, Judith Golda
Catalysts are critical components for chemical reactions in industrial applications. They are able to optimize selectivity, efficiency, and reaction rates, thus enabling more environmentally friendly processes. This work presents a novel approach to catalyst functionalization for the CO2 reduction reaction by combining the reactive species of an atmospheric pressure plasma jet with the electric fields and energy input of a laser. This leads to both a nanoscale structuring as well as a controllable chemical composition of the surface, which are important parameters for optimizing catalyst performance. The treatment is conducted on thin copper layers deposited by high power pulsed magnetron sputtering on silicon wafers. Because atomic oxygen plays a key role in oxidizing copper, two photon absorption fluorescence is used to investigate the atomic oxygen density in the interaction zone of the COST plasma jet and a copper surface. The used atmospheric pressure plasma jet provides an atomic oxygen density at the surface in a distance of 8 mm to the jet nozzle of approximately 2×1021
{"title":"Self-Organizing Sub-μm Surface Structures Stimulated by Microplasma Generated Reactive Species and Short-Pulsed Laser Irradiation","authors":"Sascha Chur, Lennart Kulik, Volker Schulz-von der Gathen, Marc Böke, Judith Golda","doi":"10.1021/acsomega.3c10033","DOIUrl":"https://doi.org/10.1021/acsomega.3c10033","url":null,"abstract":"Catalysts are critical components for chemical reactions in industrial applications. They are able to optimize selectivity, efficiency, and reaction rates, thus enabling more environmentally friendly processes. This work presents a novel approach to catalyst functionalization for the CO<sub>2</sub> reduction reaction by combining the reactive species of an atmospheric pressure plasma jet with the electric fields and energy input of a laser. This leads to both a nanoscale structuring as well as a controllable chemical composition of the surface, which are important parameters for optimizing catalyst performance. The treatment is conducted on thin copper layers deposited by high power pulsed magnetron sputtering on silicon wafers. Because atomic oxygen plays a key role in oxidizing copper, two photon absorption fluorescence is used to investigate the atomic oxygen density in the interaction zone of the COST plasma jet and a copper surface. The used atmospheric pressure plasma jet provides an atomic oxygen density at the surface in a distance of 8 mm to the jet nozzle of approximately <i></i><span style=\"color: inherit;\"></span><span data-mathml='<math xmlns=\"http://www.w3.org/1998/Math/MathML\" display=\"inline\"><mn>2</mn><mo>&#xD7;</mo><msup><mrow><mn>10</mn></mrow><mrow><mn>21</mn></mrow></msup><mfrac><mrow><mn>1</mn></mrow><mrow><msup><mrow><mi mathvariant=\"normal\">m</mi></mrow><mrow><mn>3</mn></mrow></msup></mrow></mfrac></math>' role=\"presentation\" style=\"position: relative;\" tabindex=\"0\"><nobr aria-hidden=\"true\"><span style=\"width: 4.461em; display: inline-block;\"><span style=\"display: inline-block; position: relative; width: 4.709em; height: 0px; font-size: 95%;\"><span style=\"position: absolute; clip: rect(1.427em, 1004.71em, 3.223em, -999.997em); top: -2.536em; left: 0em;\"><span><span style=\"font-family: STIXMathJax_Main;\">2</span><span style=\"font-family: STIXMathJax_Main; padding-left: 0.251em;\">×</span><span style=\"padding-left: 0.251em;\"><span style=\"display: inline-block; position: relative; width: 1.799em; height: 0px;\"><span style=\"position: absolute; clip: rect(3.161em, 1000.99em, 4.214em, -999.997em); top: -4.022em; left: 0em;\"><span><span style=\"font-family: STIXMathJax_Main;\">10</span></span><span style=\"display: inline-block; width: 0px; height: 4.028em;\"></span></span><span style=\"position: absolute; top: -4.455em; left: 0.994em;\"><span><span style=\"font-size: 70.7%; font-family: STIXMathJax_Main;\">21</span></span><span style=\"display: inline-block; width: 0px; height: 4.028em;\"></span></span></span></span><span><span style=\"display: inline-block; position: relative; width: 0.994em; height: 0px; margin-right: 0.127em; margin-left: 0.127em;\"><span style=\"position: absolute; clip: rect(3.347em, 1000.25em, 4.214em, -999.997em); ","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":null,"pages":null},"PeriodicalIF":4.1,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141524143","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}
As a photostabilizing agent for cyanine dye, methyl-β-cyclodextrin (MβCD) was investigated as a possible antifading agent for cyanine dye-labeled proteins. Cyanine-3 (Cy3)-labeled streptavidin (SA-Cy3) solutions containing MβCD exhibited improved resistance against photobleaching. Further research revealed that MβCD can be used as a coating material on the surface of gene chips. Chips loaded with cyanine dye (Cy3 and Cyanine-5 (Cy5))-conjugated model microbeads exhibited resistance against photobleaching with MβCD coatings. MβCD coatings improved the imaging quality of model chips and resulted in higher discrimination ratios (DR) of single base recognition by a set of control beads (NP68). In a whole genome genotyping assay for human samples, the MβCD-coated samples were found to have a better clustering performance than the noncoated ones for a group of randomly picked single nucleotide polymorphisms (SNPs).
{"title":"Screening of Methyl-β-cyclodextrins as an Antifading Agent for Cyanine Dye-Labeled Streptavidin to Improve the Performance of Genotyping Chips","authors":"Yuhao Ma, Yun Fan, Xinyi Xu, Hongxia Li, Ruoyu Liu, Chaojun Liu","doi":"10.1021/acsomega.4c02099","DOIUrl":"https://doi.org/10.1021/acsomega.4c02099","url":null,"abstract":"As a photostabilizing agent for cyanine dye, methyl-β-cyclodextrin (MβCD) was investigated as a possible antifading agent for cyanine dye-labeled proteins. Cyanine-3 (Cy3)-labeled streptavidin (SA-Cy3) solutions containing MβCD exhibited improved resistance against photobleaching. Further research revealed that MβCD can be used as a coating material on the surface of gene chips. Chips loaded with cyanine dye (Cy3 and Cyanine-5 (Cy5))-conjugated model microbeads exhibited resistance against photobleaching with MβCD coatings. MβCD coatings improved the imaging quality of model chips and resulted in higher discrimination ratios (DR) of single base recognition by a set of control beads (NP68). In a whole genome genotyping assay for human samples, the MβCD-coated samples were found to have a better clustering performance than the noncoated ones for a group of randomly picked single nucleotide polymorphisms (SNPs).","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":null,"pages":null},"PeriodicalIF":4.1,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141524147","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}
Pub Date : 2024-06-27DOI: 10.1021/acsomega.4c02772
Mrinmoy Karmakar, Somya Sadaf, Chinmay Ghoroi
The elevated accumulation of electronic wastes, especially containing Dysprosium ion [i.e., Dy(III)], is emerging as a potential environmental threat. To overcome the deleterious effects of Dy(III), detection and removal of Dy(III) is crucial. Moreover, recovery of high-value Dy(III) is economically beneficial. However, the availability of a single material, capable of sensing Dy(III) in nanomolar concentration and simultaneously adsorbing it with high adsorption capacity (AC), is rare. Therefore, to solve this problem, a pH-responsive fluorescent amino graphene oxide-impregnated-engineered polymer hydrogel (AGO-EPH) has been synthesized, suitable for selective sensing of Dy(III) in nanomolar concentration and adsorbing it from wastewater at ambient temperature. This terpolymeric hydrogel is synthesized from two nonfluorescent monomers, propenoic acid (PNA) and prop-2-enamide (PEAM), along with an in situ generated comonomer (3-acrylamidopropanoic acid/AAPPA) through N–H activation during polymerization. Surface properties and structural details of AGO-EPH are established using NMR, FTIR, XRD, TEM, SEM, EDX, Raman, MALDI-mass, and DLS studies. The AGO-EPH exhibits blue fluorescence with selective turn-off sensing of Dy(III) with the detection limit of 1.88 × 10–7 (M). The maximum AC of AGO-EPH is 41.97 ± 0.39 mg g–1. The developed AGO-EPH shows consistent adsorption–desorption property over five cycles, with more than 90% desorption efficiency per cycle, confirming significant recovery of the valuable Dy(III). From Logic gate calculations, complexation of Dy(III) and AGO-EPH may be the reason behind fluorescence quenching. The AGO-EPH also shows antibacterial action against ∼3 × 108 cells mL–1 of E. coli solution. Overall, the developed pH-responsive engineered hydrogel can be used as a potential low-cost sensing device and reusable adsorbent for Dy(III).
{"title":"pH-Responsive Biocompatible Fluorescent Hydrogel for Selective Sensing and Adsorptive Recovery of Dysprosium","authors":"Mrinmoy Karmakar, Somya Sadaf, Chinmay Ghoroi","doi":"10.1021/acsomega.4c02772","DOIUrl":"https://doi.org/10.1021/acsomega.4c02772","url":null,"abstract":"The elevated accumulation of electronic wastes, especially containing Dysprosium ion [i.e., Dy(III)], is emerging as a potential environmental threat. To overcome the deleterious effects of Dy(III), detection and removal of Dy(III) is crucial. Moreover, recovery of high-value Dy(III) is economically beneficial. However, the availability of a single material, capable of sensing Dy(III) in nanomolar concentration and simultaneously adsorbing it with high adsorption capacity (AC), is rare. Therefore, to solve this problem, a pH-responsive fluorescent amino graphene oxide-impregnated-engineered polymer hydrogel (<b>AGO-EPH</b>) has been synthesized, suitable for selective sensing of Dy(III) in nanomolar concentration and adsorbing it from wastewater at ambient temperature. This terpolymeric hydrogel is synthesized from two nonfluorescent monomers, propenoic acid (PNA) and prop-2-enamide (PEAM), along with an in situ generated comonomer (3-acrylamidopropanoic acid/AAPPA) through N–<i>H</i> activation during polymerization. Surface properties and structural details of <b>AGO-EPH</b> are established using NMR, FTIR, XRD, TEM, SEM, EDX, Raman, MALDI-mass, and DLS studies. The <b>AGO-EPH</b> exhibits blue fluorescence with <i>selective</i> turn-off sensing of Dy(III) with the detection limit of 1.88 × 10<sup>–7</sup> (M). The maximum AC of <b>AGO-EPH</b> is 41.97 ± 0.39 mg g<sup>–1</sup>. The developed <b>AGO-EPH</b> shows consistent adsorption–desorption property over five cycles, with more than 90% desorption efficiency per cycle, confirming significant recovery of the valuable Dy(III). From Logic gate calculations, complexation of Dy(III) and <b>AGO-EPH</b> may be the reason behind fluorescence quenching. The <b>AGO-EPH</b> also shows antibacterial action against ∼3 × 10<sup>8</sup> cells mL<sup>–1</sup> of <i>E. coli</i> solution. Overall, the developed pH-responsive engineered hydrogel can be used as a potential low-cost sensing device and reusable adsorbent for Dy(III).","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":null,"pages":null},"PeriodicalIF":4.1,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141524148","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}
Pub Date : 2024-06-27DOI: 10.1021/acsomega.3c09715
Andrea Degl’Innocenti, Clarissa Braccia, Giada Graziana Genchi, Nicoletta di Leo, Luca Leoncino, Federico Catalano, Andrea Armirotti, Gianni Ciofani
Oxidative stress is a widespread causative agent of disease. Together with its general relevance for biomedicine, such a dynamic is recognizably detrimental to space exploration. Among other solutions, cerium oxide nanoparticles (or nanoceria, NC) display a long-lasting, self-renewable antioxidant activity. In a previous experiment, we evaluated oxidative imbalance in rat myoblasts in space, aboard the International Space Station, and unveiled possible protective effects from NC through RNA sequencing. Here, we focus on the myoblast response to NC on land by means of proteomics, defining a list of proteins that putatively react to NC and confirming nucleosomes/histones as likely mediators of its molecular action. The proteomics data set we present here and its counterpart from the space study share four factors. These are coherently either up- (Hist1h4b) or down-regulated (Gnl3, Mtdh, Trip12) upon NC exposure.
{"title":"Proteome Alterations and Nucleosome Activation in Rat Myoblasts Treated with Cerium Oxide Nanoparticles","authors":"Andrea Degl’Innocenti, Clarissa Braccia, Giada Graziana Genchi, Nicoletta di Leo, Luca Leoncino, Federico Catalano, Andrea Armirotti, Gianni Ciofani","doi":"10.1021/acsomega.3c09715","DOIUrl":"https://doi.org/10.1021/acsomega.3c09715","url":null,"abstract":"Oxidative stress is a widespread causative agent of disease. Together with its general relevance for biomedicine, such a dynamic is recognizably detrimental to space exploration. Among other solutions, cerium oxide nanoparticles (or <i>nanoceria</i>, NC) display a long-lasting, self-renewable antioxidant activity. In a previous experiment, we evaluated oxidative imbalance in rat myoblasts in space, aboard the International Space Station, and unveiled possible protective effects from NC through RNA sequencing. Here, we focus on the myoblast response to NC on land by means of proteomics, defining a list of proteins that putatively react to NC and confirming nucleosomes/histones as likely mediators of its molecular action. The proteomics data set we present here and its counterpart from the space study share four factors. These are coherently either up- (<i>Hist1h4b</i>) or down-regulated (<i>Gnl3</i>, <i>Mtdh</i>, <i>Trip12</i>) upon NC exposure.","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":null,"pages":null},"PeriodicalIF":4.1,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141524141","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}
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