Conventional approaches for bacterial cell analysis are hindered by lengthy processing times and tedious protocols that rely on gene amplification and cell culture. Impedance spectroscopy has emerged as a promising tool for efficient real-time bacterial monitoring, owing to its simple, label-free nature and cost-effectiveness. However, its limited practical applications in real-world scenarios pose a significant challenge. In this review, we provide a comprehensive study of impedance spectroscopy and its practical utilization in bacterial system measurements. We begin by outlining the fundamentals of impedance theory and modeling, specific to bacterial systems. We then offer insights into various strategies for bacterial cell detection and discuss the role of impedance spectroscopy in antimicrobial susceptibility testing (AST) and single-cell analysis. Additionally, we explore key aspects of impedance system design, including the influence of electrodes, media, and cell enrichment techniques on the sensitivity, specificity, detection speed, concentration accuracy, and cost-effectiveness of current impedance biosensors. By combining different biosensor design parameters, impedance theory, and detection principles, we propose that impedance applications can be expanded to point-of-care diagnostics, enhancing their practical utility. This Perspective focuses exclusively on ideally polarizable (fully capacitive) electrodes, excluding any consideration of charge transfer resulting from Faradaic reactions.
{"title":"Impedance Spectroscopy for Bacterial Cell Monitoring, Analysis, and Antibiotic Susceptibility Testing.","authors":"Pragya Swami, Satyam Anand, Anurag Holani, Shalini Gupta","doi":"10.1021/acs.langmuir.4c01907","DOIUrl":"10.1021/acs.langmuir.4c01907","url":null,"abstract":"<p><p>Conventional approaches for bacterial cell analysis are hindered by lengthy processing times and tedious protocols that rely on gene amplification and cell culture. Impedance spectroscopy has emerged as a promising tool for efficient real-time bacterial monitoring, owing to its simple, label-free nature and cost-effectiveness. However, its limited practical applications in real-world scenarios pose a significant challenge. In this review, we provide a comprehensive study of impedance spectroscopy and its practical utilization in bacterial system measurements. We begin by outlining the fundamentals of impedance theory and modeling, specific to bacterial systems. We then offer insights into various strategies for bacterial cell detection and discuss the role of impedance spectroscopy in antimicrobial susceptibility testing (AST) and single-cell analysis. Additionally, we explore key aspects of impedance system design, including the influence of electrodes, media, and cell enrichment techniques on the sensitivity, specificity, detection speed, concentration accuracy, and cost-effectiveness of current impedance biosensors. By combining different biosensor design parameters, impedance theory, and detection principles, we propose that impedance applications can be expanded to point-of-care diagnostics, enhancing their practical utility. This Perspective focuses exclusively on ideally polarizable (fully capacitive) electrodes, excluding any consideration of charge transfer resulting from Faradaic reactions.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142386415","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-22DOI: 10.1021/acs.langmuir.4c02134
Jiayu Xin, Xi Zhao, Lihe Zhang, Changliu He, Shuai Li, Cui Li, Ce Liu, Jiahong Li, Yao Ji, Xu Zhang
Driven by renewable energy, using electrocatalysis to reduce carbon dioxide (CO2) to chemicals is a key technology. It could dim global carbon emissions and promote the carbon cycle. Here, we reported an approach to prepare a Br-doped Bi nanosphere (Br-doped Bi NSP) catalyst for the preparation of formate by electrochemical conversion of CO2. The synthesized Br-doped Bi NSP catalyst manifests high selectivity toward HCOOH. At the applied potential of −0.9 V versus reversible hydrogen electrode, it could achieve a maximum FEHCOOH of 98%. It can remain constant, and the degradation is negligible in continuous electrolysis for 9 h. The excellent CO2 reduction performance is due to the electron richness at the surface of Br-doped Bi NSP induced by the electron transfer between Bi and Br. Density functional theory calculations and in situ attenuated total reflectance–Fourier transform infrared measurements were used to predict the underlying catalyst action’s pathway. It can be concluded that the introduction of Br is advantageous to the *OCHO formation, which is conducive to the reduction of the determination step. This research could provide a meaningful view into anion-doping effects to enable effiective electrocatalytic material that selectively reduces carbon dioxide into valuable products.
在可再生能源的推动下,利用电催化技术将二氧化碳(CO2)还原成化学品是一项关键技术。它可以减少全球碳排放,促进碳循环。在此,我们报告了一种制备掺杂溴的生物纳米球(Br-doped Bi NSP)催化剂的方法,用于通过二氧化碳的电化学转化制备甲酸盐。合成的掺杂溴的 Bi NSP 催化剂对 HCOOH 具有高选择性。在对可逆氢电极施加 -0.9 V 的电位时,其 FEHCOOH 的最大值可达 98%。优异的 CO2 还原性能得益于掺杂 Br 的 Bi NSP 表面由 Bi 和 Br 之间的电子转移引起的电子富集。密度泛函理论计算和原位衰减全反射-傅立叶变换红外测量被用来预测催化剂的基本作用途径。结果表明,Br 的引入有利于 *OCHO 的形成,从而有利于测定步骤的还原。这项研究为阴离子掺杂效应提供了一个有意义的视角,使高效的电催化材料能够选择性地将二氧化碳还原成有价值的产品。
{"title":"Remarkable Enhancement of Bismuth Nanosphere Catalyst Activity for the Conversion of Electrocatalytic CO2 to Formate by Bromine Doping","authors":"Jiayu Xin, Xi Zhao, Lihe Zhang, Changliu He, Shuai Li, Cui Li, Ce Liu, Jiahong Li, Yao Ji, Xu Zhang","doi":"10.1021/acs.langmuir.4c02134","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c02134","url":null,"abstract":"Driven by renewable energy, using electrocatalysis to reduce carbon dioxide (CO<sub>2</sub>) to chemicals is a key technology. It could dim global carbon emissions and promote the carbon cycle. Here, we reported an approach to prepare a Br-doped Bi nanosphere (Br-doped Bi NSP) catalyst for the preparation of formate by electrochemical conversion of CO<sub>2</sub>. The synthesized Br-doped Bi NSP catalyst manifests high selectivity toward HCOOH. At the applied potential of −0.9 V versus reversible hydrogen electrode, it could achieve a maximum FE<sub>HCOOH</sub> of 98%. It can remain constant, and the degradation is negligible in continuous electrolysis for 9 h. The excellent CO<sub>2</sub> reduction performance is due to the electron richness at the surface of Br-doped Bi NSP induced by the electron transfer between Bi and Br. Density functional theory calculations and <i>in situ</i> attenuated total reflectance–Fourier transform infrared measurements were used to predict the underlying catalyst action’s pathway. It can be concluded that the introduction of Br is advantageous to the *OCHO formation, which is conducive to the reduction of the determination step. This research could provide a meaningful view into anion-doping effects to enable effiective electrocatalytic material that selectively reduces carbon dioxide into valuable products.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142486591","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-22Epub Date: 2024-10-10DOI: 10.1021/acs.langmuir.4c03422
Xin-Yu Liu, Wei-Bin Zhang, Xia-Yue Yuan, Bi Chen, Fan Yang, Kang Yang, Xue-Jing Ma
Salinity gradient energy is a chemical potential energy between two solutions with different ionic concentrations, which is also an ocean energy at the junction of rivers and seas. In our original work, the device "activated carbon//(0.083 M Na2SO4, 0.5 M Na2SO4)//vanadium pentoxide" for the conversion of salinity gradient energy was designed, and the conversion value of 6.29 J g-1 was obtained. However, the low specific surface area of the original V2O5 inevitably resulted in limited active sites and slow ionic transport rates, and the inherent lower conductivity and narrower layer spacing of the original V2O5 also resulted in poor electrode kinetic performance and cycle stability, hindering its practical application. To solve the above problems, the present work provides a strategy of using polyaniline (PANI) molecule chain intercalation to regulate the layer spacing of the original V2O5, and through the expansion and traction of the layer spacing, the composite PANI/V2O5 (PVO) with high specific surface area is prepared and used as an anode material for electrochemical conversion of salinity gradient energy application. The significantly increased layer spacing of the crystal plane (001) corresponding to the original V2O5 was confirmed with the PANI by the hydrogen bonding and the van der Waals force. The high specific surface area of the composite provides more electrochemical active sites to realize a fast Na+ migration rate and high specific capacitance. Meanwhile, the inserted PANI molecule chain, which acts not only as a pillar enlarging the Na+ diffusion channel but also as an anchor locking the gap between V2O5 bilayers, improves the structural stability of the V2O5 electrode during the electrochemical conversion process. The proposed insertion strategy for the conductive polymer PANI has created a new way to improve the cycle stability performance of the salinity gradient energy conversion device.
盐度梯度能是两种离子浓度不同的溶液之间的化学势能,也是江海交界处的海洋能。在我们最初的工作中,设计了 "活性炭//(0.083 M Na2SO4,0.5 M Na2SO4)//五氧化二钒 "的盐度梯度能转换装置,并获得了 6.29 J g-1 的转换值。然而,原 V2O5 的低比表面积不可避免地导致活性位点有限和离子传输速率缓慢,而原 V2O5 本身较低的电导率和较窄的层间距也导致电极动力学性能和循环稳定性较差,阻碍了其实际应用。为解决上述问题,本研究提供了一种利用聚苯胺(PANI)分子链插层调节原 V2O5 层间距的策略,通过层间距的扩展和牵引,制备出具有高比表面积的 PANI/V2O5 复合材料(PVO),并将其作为电化学转换盐度梯度能量应用的阳极材料。与原始 V2O5 相对应的晶面(001)层间距明显增大,通过氢键和范德华力证实了 PANI 的作用。复合材料的高比表面积提供了更多的电化学活性位点,实现了快速的 Na+ 迁移速率和高比电容。同时,插入的 PANI 分子链既是扩大 Na+ 扩散通道的支柱,又是锁定 V2O5 双层之间空隙的锚,提高了 V2O5 电极在电化学转换过程中的结构稳定性。导电聚合物 PANI 的插入策略为提高盐度梯度能量转换装置的循环稳定性能开辟了一条新途径。
{"title":"Regulating V<sub>2</sub>O<sub>5</sub> Layer Spacing by a Polyaniline Molecule Chain to Improve Electrochemical Performance in Salinity Gradient Energy Conversion.","authors":"Xin-Yu Liu, Wei-Bin Zhang, Xia-Yue Yuan, Bi Chen, Fan Yang, Kang Yang, Xue-Jing Ma","doi":"10.1021/acs.langmuir.4c03422","DOIUrl":"10.1021/acs.langmuir.4c03422","url":null,"abstract":"<p><p>Salinity gradient energy is a chemical potential energy between two solutions with different ionic concentrations, which is also an ocean energy at the junction of rivers and seas. In our original work, the device \"activated carbon//(0.083 M Na<sub>2</sub>SO<sub>4</sub>, 0.5 M Na<sub>2</sub>SO<sub>4</sub>)//vanadium pentoxide\" for the conversion of salinity gradient energy was designed, and the conversion value of 6.29 J g<sup>-1</sup> was obtained. However, the low specific surface area of the original V<sub>2</sub>O<sub>5</sub> inevitably resulted in limited active sites and slow ionic transport rates, and the inherent lower conductivity and narrower layer spacing of the original V<sub>2</sub>O<sub>5</sub> also resulted in poor electrode kinetic performance and cycle stability, hindering its practical application. To solve the above problems, the present work provides a strategy of using polyaniline (PANI) molecule chain intercalation to regulate the layer spacing of the original V<sub>2</sub>O<sub>5</sub>, and through the expansion and traction of the layer spacing, the composite PANI/V<sub>2</sub>O<sub>5</sub> (PVO) with high specific surface area is prepared and used as an anode material for electrochemical conversion of salinity gradient energy application. The significantly increased layer spacing of the crystal plane (001) corresponding to the original V<sub>2</sub>O<sub>5</sub> was confirmed with the PANI by the hydrogen bonding and the van der Waals force. The high specific surface area of the composite provides more electrochemical active sites to realize a fast Na<sup>+</sup> migration rate and high specific capacitance. Meanwhile, the inserted PANI molecule chain, which acts not only as a pillar enlarging the Na<sup>+</sup> diffusion channel but also as an anchor locking the gap between V<sub>2</sub>O<sub>5</sub> bilayers, improves the structural stability of the V<sub>2</sub>O<sub>5</sub> electrode during the electrochemical conversion process. The proposed insertion strategy for the conductive polymer PANI has created a new way to improve the cycle stability performance of the salinity gradient energy conversion device.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142386417","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-22Epub Date: 2024-10-11DOI: 10.1021/acs.langmuir.4c01937
Leila T Thieghi, Sarah I P M N Alves
This research studied the role of DMSO in a binary system of Triton X and water in the hexagonal mesophase. One effect of DMSO addition, determined using polarized optical microscopy and small-angle X-ray scattering measurements, is to promote a decrease in the hexagonal to isotropic phase transition temperature, TH-ISO, decreasing the range of temperatures of the hexagonal phase until the hexagonal phase completely disappears when DMSO is added up to 5.0 mol %. The periodicity and the lattice parameter of the hexagonal arrangement, calculated as a function of DMSO concentration, slight increased due to the insertion of DMSO molecules in the water region, causing a greater distance between the cylindrical micelles, while the radius of the apolar domains kept constant at 22 (1) Å.
{"title":"Effect of DMSO Addition on the Hexagonal Phase of the System Triton X/Water.","authors":"Leila T Thieghi, Sarah I P M N Alves","doi":"10.1021/acs.langmuir.4c01937","DOIUrl":"10.1021/acs.langmuir.4c01937","url":null,"abstract":"<p><p>This research studied the role of DMSO in a binary system of Triton X and water in the hexagonal mesophase. One effect of DMSO addition, determined using polarized optical microscopy and small-angle X-ray scattering measurements, is to promote a decrease in the hexagonal to isotropic phase transition temperature, <i>T</i><sub>H-ISO</sub>, decreasing the range of temperatures of the hexagonal phase until the hexagonal phase completely disappears when DMSO is added up to 5.0 mol %. The periodicity and the lattice parameter of the hexagonal arrangement, calculated as a function of DMSO concentration, slight increased due to the insertion of DMSO molecules in the water region, causing a greater distance between the cylindrical micelles, while the radius of the apolar domains kept constant at 22 (1) Å.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142398637","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Economic synthesis of amine-modified solid adsorbents is pivotal for the global-scale direct air capture (DAC) technologies required to realize net-zero emissions. To address the problems of the traditional reflux method using excessively costly amino silane, we propose introducing silane by impregnation into mesoporous silica with interconnected three-dimensional pores. X-ray diffraction, Fourier transform infrared spectroscopy, N2 adsorption-desorption, transmission electron and scanning electron microscopies, magic-angle spinning nuclear magnetic resonance, and elemental analysis identified the spatial distribution of amino silane in the materials with different loading levels. The results of structure characterization and a comparison with a reference experiment (using a porous support with one-dimensional pores and/or the conventional reflux method) revealed that the proposed strategy provided a uniform amine distribution, together with a high utilization efficiency of the amino silane. We also demonstrate that the obtained material has a high adsorption capacity and good recycling stability comparable to those of the previously reported amino silane modified adsorbents under simulated DAC conditions.
{"title":"High-Efficiency Silane Utilization in Amine-Modified Adsorbents for Direct Air Capture through Interconnected Three-Dimensional Pores.","authors":"Jin-Rui Li, Nao Tsunoji, Mahuya Bandyopadhyay, Masahiro Sadakane","doi":"10.1021/acs.langmuir.4c02931","DOIUrl":"10.1021/acs.langmuir.4c02931","url":null,"abstract":"<p><p>Economic synthesis of amine-modified solid adsorbents is pivotal for the global-scale direct air capture (DAC) technologies required to realize net-zero emissions. To address the problems of the traditional reflux method using excessively costly amino silane, we propose introducing silane by impregnation into mesoporous silica with interconnected three-dimensional pores. X-ray diffraction, Fourier transform infrared spectroscopy, N<sub>2</sub> adsorption-desorption, transmission electron and scanning electron microscopies, magic-angle spinning nuclear magnetic resonance, and elemental analysis identified the spatial distribution of amino silane in the materials with different loading levels. The results of structure characterization and a comparison with a reference experiment (using a porous support with one-dimensional pores and/or the conventional reflux method) revealed that the proposed strategy provided a uniform amine distribution, together with a high utilization efficiency of the amino silane. We also demonstrate that the obtained material has a high adsorption capacity and good recycling stability comparable to those of the previously reported amino silane modified adsorbents under simulated DAC conditions.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142379436","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The limited active sites and faster photogenerated electron-hole pair recombination rate of g-C3N4 restrict its application in photocatalytic H2 production. Constructing heterojunctions has been shown to improve the spatial (directional) separation of photogenerated electrons and holes. However, due to interface mismatch in traditional heterojunction structures and a lack of precise electron transport channels, the photocatalytic efficiency is limited. Here, we developed a two-step calcination approach to create an Fe2N/g-C3N4 heterojunction linked by Fe-O bonds (named as Fe-OCN). The newly formed Fe-O bonds within the heterojunction can act as atomic-level interface electron transfer channels, directly transferring the photogenerated electrons of g-C3N4 to the reactive center Fe2N, significantly improving the charge transfer rate and utilization, thus promoting visible-light-driven photocatalytic H2 production. The optimal Fe-OCN achieved a H2 production rate of 5986.29 μmol g-1 h-1 under visible light, 13.44 times higher than that of the OCN due to efficient charge separation and transfer capabilities. This work provides a constructive reference for the design and synthesis of organic-inorganic heterojunction with chemically bonded interfaces, establishing quick electron transfer channels, and achieving targeted electron transfer.
{"title":"In-Situ Construction of Atomic-Level Fe-O Bond Bridges within Fe<sub>2</sub>N/g-C<sub>3</sub>N<sub>4</sub> Heterojunction for Efficient Visible-Light-Driven Photocatalytic H<sub>2</sub> Production.","authors":"Qian Zheng, Jiajun Fu, Guanyu Wu, Xunhuai Huang, Jiafeng Fan, Baoting Tan, Zhilong Song, Yanhua Song, Jia Yan","doi":"10.1021/acs.langmuir.4c02777","DOIUrl":"10.1021/acs.langmuir.4c02777","url":null,"abstract":"<p><p>The limited active sites and faster photogenerated electron-hole pair recombination rate of g-C<sub>3</sub>N<sub>4</sub> restrict its application in photocatalytic H<sub>2</sub> production. Constructing heterojunctions has been shown to improve the spatial (directional) separation of photogenerated electrons and holes. However, due to interface mismatch in traditional heterojunction structures and a lack of precise electron transport channels, the photocatalytic efficiency is limited. Here, we developed a two-step calcination approach to create an Fe<sub>2</sub>N/g-C<sub>3</sub>N<sub>4</sub> heterojunction linked by Fe-O bonds (named as Fe-OCN). The newly formed Fe-O bonds within the heterojunction can act as atomic-level interface electron transfer channels, directly transferring the photogenerated electrons of g-C<sub>3</sub>N<sub>4</sub> to the reactive center Fe<sub>2</sub>N, significantly improving the charge transfer rate and utilization, thus promoting visible-light-driven photocatalytic H<sub>2</sub> production. The optimal Fe-OCN achieved a H<sub>2</sub> production rate of 5986.29 μmol g<sup>-1</sup> h<sup>-1</sup> under visible light, 13.44 times higher than that of the OCN due to efficient charge separation and transfer capabilities. This work provides a constructive reference for the design and synthesis of organic-inorganic heterojunction with chemically bonded interfaces, establishing quick electron transfer channels, and achieving targeted electron transfer.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142398639","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Shale contains numerous organic micropores with significant potential for CO2 storage. To precisely evaluate the CO2 storage potential of shale reservoirs, it is essential to accurately quantify the adsorption of CO2 within these pores. This study used Grand Canonical Monte Carlo (GCMC) molecular simulations to analyze the CO2 adsorption behavior in organic micropores of varying sizes. The study clarified the number and width of the CO2 adsorption layers in micropores of various sizes and proposed a method for segmenting the multilayer adsorption structure. Additionally, the classic Ono-Kondo lattice (OK) model was extended to characterize pore-filling adsorption, incorporating solid-gas and gas-gas interactions. Accurate characterization of CO2 multilayer adsorption and precise calculation of CO2 absolute adsorption in micropores were achieved. Results indicate that CO2 exhibits pore-filling adsorption behavior in organic micropores, forming a multilayer adsorption structure governed by the pore size. Following symmetry principles, the adsorption layer structure in organic micropores can be simplified to a maximum of three layers. When only one adsorption layer forms, its width equals the gas-accessible pore size. For two or more layers, the width of the original layer stabilizes as additional layers form. The stable adsorption layer widths, from nearest to farthest from the pore wall, are 0.33, 0.45, and 0.39 nm. The improved OK model accurately describes CO2 excess and absolute adsorption isotherms across different pore sizes and calculates the CO2 density in each adsorption layer, showing high consistency with GCMC simulation results. These findings highlight the importance of understanding the CO2 multilayer adsorption structure for accurately estimating CO2 adsorption in organic micropores.
页岩含有大量有机微孔,具有巨大的二氧化碳封存潜力。要精确评估页岩储层的二氧化碳封存潜力,就必须准确量化这些孔隙中的二氧化碳吸附情况。本研究利用大卡农蒙特卡罗(GCMC)分子模拟分析了不同大小的有机微孔中的二氧化碳吸附行为。研究明确了不同尺寸微孔中二氧化碳吸附层的数量和宽度,并提出了一种分割多层吸附结构的方法。此外,研究还扩展了经典的小野-近藤晶格(OK)模型,以描述孔隙填充吸附,并将固气和气气相互作用纳入其中。该模型准确表征了二氧化碳的多层吸附,并精确计算了二氧化碳在微孔中的绝对吸附量。结果表明,二氧化碳在有机微孔中表现出孔隙填充吸附行为,形成受孔隙大小制约的多层吸附结构。根据对称性原理,有机微孔中的吸附层结构最多可简化为三层。当只形成一层吸附层时,其宽度等于气体可进入孔隙的大小。对于两层或更多吸附层,随着更多吸附层的形成,原始吸附层的宽度会趋于稳定。从离孔壁最近到最远,稳定的吸附层宽度分别为 0.33、0.45 和 0.39 纳米。改进后的 OK 模型准确地描述了不同孔隙大小的二氧化碳过量和绝对吸附等温线,并计算出了每个吸附层中的二氧化碳密度,与 GCMC 模拟结果具有很高的一致性。这些发现凸显了了解二氧化碳多层吸附结构对于准确估算有机微孔中二氧化碳吸附量的重要性。
{"title":"Multilayer Adsorption Characteristics of CO<sub>2</sub> in Organic Nanopores with Different Pore Sizes: Molecular Simulation and Ono-Kondo Lattice Model.","authors":"Xintong Chen, Di Wu, Feng Miao, Xiaochun Xiao, Xueying Liu, Wenbo Zhai","doi":"10.1021/acs.langmuir.4c02480","DOIUrl":"10.1021/acs.langmuir.4c02480","url":null,"abstract":"<p><p>Shale contains numerous organic micropores with significant potential for CO<sub>2</sub> storage. To precisely evaluate the CO<sub>2</sub> storage potential of shale reservoirs, it is essential to accurately quantify the adsorption of CO<sub>2</sub> within these pores. This study used Grand Canonical Monte Carlo (GCMC) molecular simulations to analyze the CO<sub>2</sub> adsorption behavior in organic micropores of varying sizes. The study clarified the number and width of the CO<sub>2</sub> adsorption layers in micropores of various sizes and proposed a method for segmenting the multilayer adsorption structure. Additionally, the classic Ono-Kondo lattice (OK) model was extended to characterize pore-filling adsorption, incorporating solid-gas and gas-gas interactions. Accurate characterization of CO<sub>2</sub> multilayer adsorption and precise calculation of CO<sub>2</sub> absolute adsorption in micropores were achieved. Results indicate that CO<sub>2</sub> exhibits pore-filling adsorption behavior in organic micropores, forming a multilayer adsorption structure governed by the pore size. Following symmetry principles, the adsorption layer structure in organic micropores can be simplified to a maximum of three layers. When only one adsorption layer forms, its width equals the gas-accessible pore size. For two or more layers, the width of the original layer stabilizes as additional layers form. The stable adsorption layer widths, from nearest to farthest from the pore wall, are 0.33, 0.45, and 0.39 nm. The improved OK model accurately describes CO<sub>2</sub> excess and absolute adsorption isotherms across different pore sizes and calculates the CO<sub>2</sub> density in each adsorption layer, showing high consistency with GCMC simulation results. These findings highlight the importance of understanding the CO<sub>2</sub> multilayer adsorption structure for accurately estimating CO<sub>2</sub> adsorption in organic micropores.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142386416","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-22Epub Date: 2024-10-11DOI: 10.1021/acs.langmuir.4c02142
Jingjing Ji, Advait D Shukla, Ratnakshi Mandal, Wafiq Ibsan Khondkar, Catilin R Mehl, Arindam Chakraborty, Shikha Nangia
Proteins exhibit diverse structures, including pockets, cavities, channels, and bumps, which are crucial in determining their functions. This diversity in topography also introduces significant chemical heterogeneity, with polar and charged domains often juxtaposed with nonpolar domains in proximity. Consequently, accurately assessing the hydropathy of amino acid residues within the intricate nanoscale topology of proteins is essential. This study presents quantitative hydropathy data for 277,877 amino acid residues, computed using the Protocol for Assigning a Residue's Character on a Hydropathy (PARCH) scale. Leveraging this data set comprising 1000 structurally diverse proteins sourced from the Protein Data Bank, we examined residues situated in various nanoscale environments and analyzed hydropathy in relation to protein topography. Our findings indicate that the hydropathy of a residue is intricately linked to both its individual characteristics and the geometric features of its neighboring residues in response to water. Changes in the number and chemical identity of the neighbors, as well as the nanoscale topography surrounding a residue, are mirrored in its hydropathy profile. Our calculations reveal the intricate interplay of hydrophilic, hydroneutral, and hydrophobic residues distributed across the surface and core of proteins. Notably, we observe that protein surfaces can be ten times more hydrophilic than their cores.
{"title":"Nanoscale Topography Dictates Residue Hydropathy in Proteins.","authors":"Jingjing Ji, Advait D Shukla, Ratnakshi Mandal, Wafiq Ibsan Khondkar, Catilin R Mehl, Arindam Chakraborty, Shikha Nangia","doi":"10.1021/acs.langmuir.4c02142","DOIUrl":"10.1021/acs.langmuir.4c02142","url":null,"abstract":"<p><p>Proteins exhibit diverse structures, including pockets, cavities, channels, and bumps, which are crucial in determining their functions. This diversity in topography also introduces significant chemical heterogeneity, with polar and charged domains often juxtaposed with nonpolar domains in proximity. Consequently, accurately assessing the hydropathy of amino acid residues within the intricate nanoscale topology of proteins is essential. This study presents quantitative hydropathy data for 277,877 amino acid residues, computed using the Protocol for Assigning a Residue's Character on a Hydropathy (PARCH) scale. Leveraging this data set comprising 1000 structurally diverse proteins sourced from the Protein Data Bank, we examined residues situated in various nanoscale environments and analyzed hydropathy in relation to protein topography. Our findings indicate that the hydropathy of a residue is intricately linked to both its individual characteristics and the geometric features of its neighboring residues in response to water. Changes in the number and chemical identity of the neighbors, as well as the nanoscale topography surrounding a residue, are mirrored in its hydropathy profile. Our calculations reveal the intricate interplay of hydrophilic, hydroneutral, and hydrophobic residues distributed across the surface and core of proteins. Notably, we observe that protein surfaces can be ten times more hydrophilic than their cores.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142398641","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
In this work, silk was selected as the substrate, and formic acid was utilized to create a rough texture on the silk. The conductive fabrics made from AgNWs and silk were created by applying multiple layers of silver nanowire dispersion onto the textured silk fabrics (SFs). The silk was immersed in a dispersion containing polydopamine (PDA), sericin (SE), tannic acid (TA), and silver nanowire under specific temperature conditions. After being cured at 120 °C, the three silver nanowire/silk fabrics (AgNWs/SFs), PDA/AgNWs/SF, SE/AgNWs/SF, and TA/AgNWs/SF, exhibited square resistances of 7.37, 540, and 200 Ω/sq, respectively. The method used to prepare the AgNW conductive SF is straightforward, resulting in fabrics that possess excellent thermal stability and resistance to washing. These fabrics also exhibit a range of useful properties, including conductivity, electrothermal capabilities, electrochemical functionality, human body sensing, hydrophobicity, and antimicrobial properties. These characteristics make them highly promising for various applications, such as human body motion detection, electronic textiles, electrothermal textiles, and antimicrobial applications.
这项研究选择蚕丝作为基材,并利用甲酸在蚕丝上形成粗糙的纹理。将多层银纳米线分散液涂在纹理蚕丝织物(SFs)上,就制成了由银纳米线和蚕丝制成的导电织物。在特定温度条件下,将蚕丝浸入含有聚多巴胺(PDA)、丝胶(SE)、单宁酸(TA)和纳米银线的分散液中。在 120 °C 固化后,PDA/AgNWs/SF、SE/AgNWs/SF 和 TA/AgNWs/SF 这三种银纳米线/丝织物(AgNWs/SFs)分别表现出 7.37、540 和 200 Ω/sq 的平方电阻。制备 AgNW 导电 SF 的方法简便易行,制成的织物具有出色的热稳定性和耐洗涤性。这些织物还表现出一系列有用的特性,包括导电性、电热能力、电化学功能、人体感应、疏水性和抗菌性。这些特性使它们在人体运动检测、电子纺织品、电热纺织品和抗菌应用等各种应用中大有可为。
{"title":"Fabrication and Performance of a Silver Nanowire Silk Conductive Fabric.","authors":"Xinpeng Chen, Jiazhuang Chen, Jin Cheng, Runshan Chu, Lili Xing, Yurong Sun, Jiabao Wu, Guoqiang Chen, Tieling Xing","doi":"10.1021/acs.langmuir.4c03120","DOIUrl":"10.1021/acs.langmuir.4c03120","url":null,"abstract":"<p><p>In this work, silk was selected as the substrate, and formic acid was utilized to create a rough texture on the silk. The conductive fabrics made from AgNWs and silk were created by applying multiple layers of silver nanowire dispersion onto the textured silk fabrics (SFs). The silk was immersed in a dispersion containing polydopamine (PDA), sericin (SE), tannic acid (TA), and silver nanowire under specific temperature conditions. After being cured at 120 °C, the three silver nanowire/silk fabrics (AgNWs/SFs), PDA/AgNWs/SF, SE/AgNWs/SF, and TA/AgNWs/SF, exhibited square resistances of 7.37, 540, and 200 Ω/sq, respectively. The method used to prepare the AgNW conductive SF is straightforward, resulting in fabrics that possess excellent thermal stability and resistance to washing. These fabrics also exhibit a range of useful properties, including conductivity, electrothermal capabilities, electrochemical functionality, human body sensing, hydrophobicity, and antimicrobial properties. These characteristics make them highly promising for various applications, such as human body motion detection, electronic textiles, electrothermal textiles, and antimicrobial applications.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142386414","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Superhydrophobic materials have been widely applied in oil-water separation, self-cleaning, antifouling, and drag reduction; however, their role in liquid evaporation and drying remains unexplored. Inspired by the microstructure of the nonwetting legs of water striders, we designed a low-adhesion superhydrophobic cylindrical barrel (CB) derived from stainless-steel mesh (SSM) to enhance liquid thermal evaporation and drying. The CB was created by hydrothermally depositing zinc oxide (ZnO) with multilevel morphologies onto metal wires, followed by modification with low-surface-energy stearic acid (SA). We investigated the impact of the SSMCB on water evaporation and analyzed the decline in the liquid levels under varying porosities and temperatures through numerical normalization. A functional relationship was established between decline height, porosity, and temperature, revealing that the drop height increased from 3.7 to 25 mm as porosity increased from 0 to 0.5263. Moreover, the superhydrophobic coating demonstrated excellent resistance to friction and peeling, indicating improved mechanical stability.
{"title":"Superhydrophobic Porous Cylindrical Barrel Founded on Stainless-Steel Mesh for Interfacial Water Evaporation.","authors":"Jingfang Zhu, Haizhou Huang, Haiyang Jia, Meng Dong, Xubing Tang, Wenbin Sun, Longyang Li, Litao Sun","doi":"10.1021/acs.langmuir.4c02911","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c02911","url":null,"abstract":"<p><p>Superhydrophobic materials have been widely applied in oil-water separation, self-cleaning, antifouling, and drag reduction; however, their role in liquid evaporation and drying remains unexplored. Inspired by the microstructure of the nonwetting legs of water striders, we designed a low-adhesion superhydrophobic cylindrical barrel (CB) derived from stainless-steel mesh (SSM) to enhance liquid thermal evaporation and drying. The CB was created by hydrothermally depositing zinc oxide (ZnO) with multilevel morphologies onto metal wires, followed by modification with low-surface-energy stearic acid (SA). We investigated the impact of the SSMCB on water evaporation and analyzed the decline in the liquid levels under varying porosities and temperatures through numerical normalization. A functional relationship was established between decline height, porosity, and temperature, revealing that the drop height increased from 3.7 to 25 mm as porosity increased from 0 to 0.5263. Moreover, the superhydrophobic coating demonstrated excellent resistance to friction and peeling, indicating improved mechanical stability.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142453454","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}