Liver diseases have become a great burden to human health because of their high morbidity and mortality rates. Orthotopic liver transplantation, which has always been considered the primary treatment for end-stage liver disease, has limitations in clinical practice. The development of cell therapy, especially induced pluripotent stem cells (iPSCs), holds promise in treating liver diseases. It has been reported that hepatocyte-like cells and liver organoids derived from iPSCs can be applied to establish disease models, test drug hepatotoxicity or directly perform specific functions as grafts. In this article, we systematically reviewed two differentiated derivants of iPSCs and show the prospective application of differentiated products in order to provide an experimental and theoretical basis for clinical treatment.
{"title":"Hepatocyte-like cells and liver organoids: the application of iPSCs and their derivants for treating liver diseases","authors":"Ruobing Ju, Siyuan Tian, Yulong Shang, Shuoyi Ma, Miao Zhang, Jingyi Liu, Keshuai Sun, Lina Cui, Xia Zhou and Ying Han","doi":"10.1039/D4MA00373J","DOIUrl":"https://doi.org/10.1039/D4MA00373J","url":null,"abstract":"<p >Liver diseases have become a great burden to human health because of their high morbidity and mortality rates. Orthotopic liver transplantation, which has always been considered the primary treatment for end-stage liver disease, has limitations in clinical practice. The development of cell therapy, especially induced pluripotent stem cells (iPSCs), holds promise in treating liver diseases. It has been reported that hepatocyte-like cells and liver organoids derived from iPSCs can be applied to establish disease models, test drug hepatotoxicity or directly perform specific functions as grafts. In this article, we systematically reviewed two differentiated derivants of iPSCs and show the prospective application of differentiated products in order to provide an experimental and theoretical basis for clinical treatment.</p>","PeriodicalId":18242,"journal":{"name":"Materials Advances","volume":null,"pages":null},"PeriodicalIF":5.2,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ma/d4ma00373j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142524360","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Shuai Li, Ruhul Quddus, Sree Sourav Das, Haobo Wang, Jerrold A. Floro and Mona Zebarjadi
Metallic thermoelectric materials with a high thermoelectric power factor and high thermal conductivity are favorable for transient dynamic active thermal management of microelectronics. Among these, several ytterbium intermetallic compounds demonstrate sharp peaks in their density of states due to contributions from ytterbium f-orbitals. YbZn11 is one of these compounds with a Gaussian-like density of states close to its Fermi level, an advantageous shape to achieve a high thermoelectric power factor. If the Fermi-level can be adjusted, high Seebeck coefficient values are expected following the Wiedemann–Franz law. Here we present YbZn11, a rarely made and studied sample, and for the first time, we report its thermoelectric and transport properties. Band structure calculations confirm the Gaussian function shape of the density of states. However, Seebeck calculations show that the Fermi level is not well positioned and ideally should be shifted by 200 meV. Al substitution for Zn (YbZn11−xAlx) and Zn-deficiency (YbZn11−x) are applied to modify the band structure and to shift the Fermi level to adjust the Seebeck coefficient.
具有高热电功率因数和高热导率的金属热电材料有利于微电子的瞬态动态主动热管理。在这些材料中,有几种镱金属间化合物由于镱 f 轨道的贡献而在其状态密度中显示出尖锐的峰值。YbZn11 是这些化合物中的一种,其状态密度接近费米级,呈高斯状,是实现高热电功率因数的有利形状。如果费米级可以调整,那么根据维德曼-弗兰茨定律,就有望获得较高的塞贝克系数。在此,我们介绍了很少制作和研究的样品 YbZn11,并首次报告了其热电和传输特性。带状结构计算证实了状态密度的高斯函数形状。然而,塞贝克计算显示费米级的位置并不理想,理想情况下应偏移 200 meV。用铝代替锌(YbZn11-xAlx)和缺锌(YbZn11-x)可以改变带状结构,移动费米级以调整塞贝克系数。
{"title":"Thermoelectric properties of YbZn11−xAlx†","authors":"Shuai Li, Ruhul Quddus, Sree Sourav Das, Haobo Wang, Jerrold A. Floro and Mona Zebarjadi","doi":"10.1039/D4MA00626G","DOIUrl":"https://doi.org/10.1039/D4MA00626G","url":null,"abstract":"<p >Metallic thermoelectric materials with a high thermoelectric power factor and high thermal conductivity are favorable for transient dynamic active thermal management of microelectronics. Among these, several ytterbium intermetallic compounds demonstrate sharp peaks in their density of states due to contributions from ytterbium f-orbitals. YbZn<small><sub>11</sub></small> is one of these compounds with a Gaussian-like density of states close to its Fermi level, an advantageous shape to achieve a high thermoelectric power factor. If the Fermi-level can be adjusted, high Seebeck coefficient values are expected following the Wiedemann–Franz law. Here we present YbZn<small><sub>11</sub></small>, a rarely made and studied sample, and for the first time, we report its thermoelectric and transport properties. Band structure calculations confirm the Gaussian function shape of the density of states. However, Seebeck calculations show that the Fermi level is not well positioned and ideally should be shifted by 200 meV. Al substitution for Zn (YbZn<small><sub>11−<em>x</em></sub></small>Al<small><sub><em>x</em></sub></small>) and Zn-deficiency (YbZn<small><sub>11−<em>x</em></sub></small>) are applied to modify the band structure and to shift the Fermi level to adjust the Seebeck coefficient.</p>","PeriodicalId":18242,"journal":{"name":"Materials Advances","volume":null,"pages":null},"PeriodicalIF":5.2,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ma/d4ma00626g?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142430910","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
H. Samet Varol, Dila Kaya, Emma Contini, Chiara Gualandi and Damiano Genovese
Single- and multi-nanoporous (1–100 nm pore size) solid-state membranes (SSNMs) receive significant attention in various fields, spanning from biosensing to water purification. Their finely tunable nanopore geometry and chemistry, combined with the large selection of materials that they can be made of, such as polymers, inorganic materials (e.g., silicon, silica, and alumina), and hydrogels, provide an excellent platform to control their mass transport and sensing capabilities for different cargoes from Å scale ions up to macromolecular biomaterials. The critical requirement to merge these nanoporous membranes’ advanced structural and chemical features with their applications is to find the most suitable analytical techniques that permit macro- and micro-scale and real-time probing of different nanopore activities. Luminescence-based detection of various physico-chemical processes in nanoporous membranes has recently received great attention: it permits rapid, non-invasive, and dynamic probing of nanoporous materials, yielding information on mass transport and sensing both (i) macroscopically, such as from an array of nanopores, and (ii) micro-nanoscopically, with ultra-high (e.g., single molecule) sensitivity and high resolution in time and space. Quantitative information arising from luminescence experiments on membrane-analyte interactions has uncovered the effects of nanoconfinement, membrane stability, and performance. This review article aims to provide the reader with a handbook of fluorescent methods–from the simplest to implement to the most advanced–helpful in studying different kinds of SSNMs for a specific application or function. To this end, we include examples from the literature published in the last ten years. At the end of our article, we also discuss limitations of the current state of fluorescence probing techniques and their future prospects.
{"title":"Fluorescence methods to probe mass transport and sensing in solid-state nanoporous membranes","authors":"H. Samet Varol, Dila Kaya, Emma Contini, Chiara Gualandi and Damiano Genovese","doi":"10.1039/D4MA00705K","DOIUrl":"https://doi.org/10.1039/D4MA00705K","url":null,"abstract":"<p >Single- and multi-nanoporous (1–100 nm pore size) solid-state membranes (SSNMs) receive significant attention in various fields, spanning from biosensing to water purification. Their finely tunable nanopore geometry and chemistry, combined with the large selection of materials that they can be made of, such as polymers, inorganic materials (<em>e.g.</em>, silicon, silica, and alumina), and hydrogels, provide an excellent platform to control their mass transport and sensing capabilities for different cargoes from Å scale ions up to macromolecular biomaterials. The critical requirement to merge these nanoporous membranes’ advanced structural and chemical features with their applications is to find the most suitable analytical techniques that permit macro- and micro-scale and real-time probing of different nanopore activities. Luminescence-based detection of various physico-chemical processes in nanoporous membranes has recently received great attention: it permits rapid, non-invasive, and dynamic probing of nanoporous materials, yielding information on mass transport and sensing both (i) macroscopically, such as from an array of nanopores, and (ii) micro-nanoscopically, with ultra-high (<em>e.g.</em>, single molecule) sensitivity and high resolution in time and space. Quantitative information arising from luminescence experiments on membrane-analyte interactions has uncovered the effects of nanoconfinement, membrane stability, and performance. This review article aims to provide the reader with a handbook of fluorescent methods–from the simplest to implement to the most advanced–helpful in studying different kinds of SSNMs for a specific application or function. To this end, we include examples from the literature published in the last ten years. At the end of our article, we also discuss limitations of the current state of fluorescence probing techniques and their future prospects.</p>","PeriodicalId":18242,"journal":{"name":"Materials Advances","volume":null,"pages":null},"PeriodicalIF":5.2,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ma/d4ma00705k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142524349","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Sepide Taleb, Wiebren M. van Lingen and Mónica Acuautla
In this research, ZnO/P(VDF-TrFE) piezoelectric composites are fabricated in different concentrations by two methods, spray coating and casting. Crystallinity, surface morphology, and piezoelectric performance of such films were analyzed and resulted in the optimal properties of 20 wt% ZnO in casted films (d33 = 48.93 pm V−1). The high sensitivity (18.5 mV N−1) of such piezoelectric films as tactile sensors was observed by performing two experiments, as a sensor in a gripping robot, and as a wearable device, monitoring the movement in the human arm. The research highlights the intricate relationship between crystallinity, β-phase content, piezoelectric coefficient, and sensor performance, underscoring the role of factors like stress distribution and mechanical behavior in determining overall efficacy.
{"title":"Toward high quality tactile sensors using ZnO/P(VDF-TrFE) flexible piezoelectric composite films","authors":"Sepide Taleb, Wiebren M. van Lingen and Mónica Acuautla","doi":"10.1039/D4MA00283K","DOIUrl":"https://doi.org/10.1039/D4MA00283K","url":null,"abstract":"<p >In this research, ZnO/P(VDF-TrFE) piezoelectric composites are fabricated in different concentrations by two methods, spray coating and casting. Crystallinity, surface morphology, and piezoelectric performance of such films were analyzed and resulted in the optimal properties of 20 wt% ZnO in casted films (<em>d</em><small><sub>33</sub></small> = 48.93 pm V<small><sup>−1</sup></small>). The high sensitivity (18.5 mV N<small><sup>−1</sup></small>) of such piezoelectric films as tactile sensors was observed by performing two experiments, as a sensor in a gripping robot, and as a wearable device, monitoring the movement in the human arm. The research highlights the intricate relationship between crystallinity, β-phase content, piezoelectric coefficient, and sensor performance, underscoring the role of factors like stress distribution and mechanical behavior in determining overall efficacy.</p>","PeriodicalId":18242,"journal":{"name":"Materials Advances","volume":null,"pages":null},"PeriodicalIF":5.2,"publicationDate":"2024-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ma/d4ma00283k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142329316","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Marcin W. Orzech, Francesco Mazzali, Arturas Adomkevicius, Mauro Coduri, Yubiao Niu, James D. McGettrick, Philip A. Chater, Laura Cabo-Fernandez, Laurence J. Hardwick, Lorenzo Malavasi and Serena Margadonna
Sodium-ion batteries represent a sustainable and cost-effective solution for grid-scale energy storage. However, the reliance on cathode materials containing scarce transition metals currently limits their wider adoption. Carbonaceous materials present an environmentally sustainable and economically viable alternative. This study investigates the application of reduced graphene oxide as a cathode active material. A detailed analysis of the storage mechanism and its dependence on the morphological and chemical structure revealed that it combines surface capacitance and faradaic reactions. The key factors responsible for high capacity and long cycle life are the open structure of graphene sheets and the presence of functional oxygen and nitrogen groups where Na+ ions are stored in the R–CO + Na+ + e− ↔ R–C–O–Na reaction. A good understanding of the mechanism allowed optimisation of cycling conditions in a proof-of-concept all-carbon full cell incorporating reduced graphene oxide and hard carbon as a cathode and an anode, respectively. The system displays good energy density (80 W h kg−1) and remarkable stability over 500 cycles. The gained insights will support the rational design of more efficient carbonaceous electrodes.
钠离子电池是电网规模能源存储的一种可持续且具有成本效益的解决方案。然而,目前对含有稀缺过渡金属的阴极材料的依赖限制了其更广泛的应用。碳质材料是一种环境可持续且经济可行的替代品。本研究调查了还原氧化石墨烯作为阴极活性材料的应用。通过详细分析其存储机制及其对形态和化学结构的依赖性,发现它结合了表面电容和法拉第反应。石墨烯薄片的开放式结构以及功能性氧和氮基团的存在是造成高容量和长循环寿命的关键因素,Na+离子在其中的R-CO + Na+ + e- ↔ R-C-O-Na反应中被储存起来。通过对这一机理的深入了解,可以优化概念验证型全碳电池的循环条件,将还原氧化石墨烯和硬碳分别作为阴极和阳极。该系统显示出良好的能量密度(80 W h kg-1)和超过 500 次循环的显著稳定性。所获得的见解将有助于合理设计更高效的碳质电极。
{"title":"Understanding the electrochemical behaviour of reduced graphene oxide cathodes in all-carbon Na-ion batteries†","authors":"Marcin W. Orzech, Francesco Mazzali, Arturas Adomkevicius, Mauro Coduri, Yubiao Niu, James D. McGettrick, Philip A. Chater, Laura Cabo-Fernandez, Laurence J. Hardwick, Lorenzo Malavasi and Serena Margadonna","doi":"10.1039/D4MA00605D","DOIUrl":"https://doi.org/10.1039/D4MA00605D","url":null,"abstract":"<p >Sodium-ion batteries represent a sustainable and cost-effective solution for grid-scale energy storage. However, the reliance on cathode materials containing scarce transition metals currently limits their wider adoption. Carbonaceous materials present an environmentally sustainable and economically viable alternative. This study investigates the application of reduced graphene oxide as a cathode active material. A detailed analysis of the storage mechanism and its dependence on the morphological and chemical structure revealed that it combines surface capacitance and faradaic reactions. The key factors responsible for high capacity and long cycle life are the open structure of graphene sheets and the presence of functional oxygen and nitrogen groups where Na+ ions are stored in the R–C<img>O + Na<small><sup>+</sup></small> + e<small><sup>−</sup></small> ↔ R–C–O–Na reaction. A good understanding of the mechanism allowed optimisation of cycling conditions in a proof-of-concept all-carbon full cell incorporating reduced graphene oxide and hard carbon as a cathode and an anode, respectively. The system displays good energy density (80 W h kg<small><sup>−1</sup></small>) and remarkable stability over 500 cycles. The gained insights will support the rational design of more efficient carbonaceous electrodes.</p>","PeriodicalId":18242,"journal":{"name":"Materials Advances","volume":null,"pages":null},"PeriodicalIF":5.2,"publicationDate":"2024-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ma/d4ma00605d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142430917","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Emmanuel Santos Moraes, Luís Gustavo Teixeira Alves Duarte, Fabiano Severo Rodembusch, José Carlos Germino, Luiz Fernando Ribeiro Pereira and Teresa Dib Zambon Atvars
Organic light-emitting diodes (OLEDs) are one of the most studied and utilized optoelectronic components in display technology. However, their application in lighting remains limited due to materials costs and a guaranteed feasible deposition technique. To address this challenge, we explored the use of easily synthesized organic molecules capable of complexation with abundant transition metals to enhance their optoelectronic properties, coupled with low-cost wet processing protocols. Four zinc(II) coordination compounds were synthesized and the impact of incorporating two different ligands into a metal center was evaluated in terms of their optoelectronic properties. A photophysical investigation was made, encompassing emission and absorption analyses in both solid-state and thin film configurations. Förster resonance energy transfer (FRET) processes were performed using polyfluorene (PFO) and zinc(II) compounds in a host–guest system, revealing FRET efficiencies ranging from 10 to 68%, depending on the concentration of zinc(II) compounds in the PFO matrix. Subsequently, solution-processed OLEDs were fabricated using PFO:zinc(II) homo (ZnL11 and ZnL22) and heteroligand (ZnL13 and ZnL23) compounds as the emissive layer at a concentration of 1%, following a straightforward architecture, ITO|PEDOT:PSS|PVK|PFO:Zn(II)-compounds|TmPyPB|Ca|Al. The OLEDs achieved external quantum efficiencies (EQE) close to the theoretical limit of these active layers, ranging from 1.2% to 1.8%, with an applicable brightness value (L > 100 cd m−2), coupled with low roll-off in EQE values. Notably, the heteroligand coordination compounds exhibited superior device performance, attributed to their high electrical charge-carrier mobilities, trap-state profiles, and density of free carriers, as elucidated by space-charge shallow- (SCLC) and deep-trap (TCLC) transport models.
{"title":"Zinc(ii)-heteroligand compounds for wet processing OLEDs: a study on balancing charge carrier transport and energy transfer†","authors":"Emmanuel Santos Moraes, Luís Gustavo Teixeira Alves Duarte, Fabiano Severo Rodembusch, José Carlos Germino, Luiz Fernando Ribeiro Pereira and Teresa Dib Zambon Atvars","doi":"10.1039/D4MA00581C","DOIUrl":"https://doi.org/10.1039/D4MA00581C","url":null,"abstract":"<p >Organic light-emitting diodes (OLEDs) are one of the most studied and utilized optoelectronic components in display technology. However, their application in lighting remains limited due to materials costs and a guaranteed feasible deposition technique. To address this challenge, we explored the use of easily synthesized organic molecules capable of complexation with abundant transition metals to enhance their optoelectronic properties, coupled with low-cost wet processing protocols. Four zinc(<small>II</small>) coordination compounds were synthesized and the impact of incorporating two different ligands into a metal center was evaluated in terms of their optoelectronic properties. A photophysical investigation was made, encompassing emission and absorption analyses in both solid-state and thin film configurations. Förster resonance energy transfer (FRET) processes were performed using polyfluorene (PFO) and zinc(<small>II</small>) compounds in a host–guest system, revealing FRET efficiencies ranging from 10 to 68%, depending on the concentration of zinc(<small>II</small>) compounds in the PFO matrix. Subsequently, solution-processed OLEDs were fabricated using PFO:zinc(<small>II</small>) homo (<strong>ZnL11</strong> and <strong>ZnL22</strong>) and heteroligand (<strong>ZnL13</strong> and <strong>ZnL23</strong>) compounds as the emissive layer at a concentration of 1%, following a straightforward architecture, ITO|PEDOT:PSS|PVK|PFO:Zn(<small>II</small>)-compounds|TmPyPB|Ca|Al. The OLEDs achieved external quantum efficiencies (EQE) close to the theoretical limit of these active layers, ranging from 1.2% to 1.8%, with an applicable brightness value (<em>L</em> > 100 cd m<small><sup>−2</sup></small>), coupled with low roll-off in EQE values. Notably, the heteroligand coordination compounds exhibited superior device performance, attributed to their high electrical charge-carrier mobilities, trap-state profiles, and density of free carriers, as elucidated by space-charge shallow- (SCLC) and deep-trap (TCLC) transport models.</p>","PeriodicalId":18242,"journal":{"name":"Materials Advances","volume":null,"pages":null},"PeriodicalIF":5.2,"publicationDate":"2024-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ma/d4ma00581c?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142329366","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Raju Ram Puniya, Priyanka Takhar, Monika Chhapoliya, Rinki Deka, Dhruba Jyoti Kalita and Devendra Singh
<p >The significance of hydrogen-bonding interactions in improving the chemical and physical properties of functional materials related to sustainable energy, gas absorption, catalysis, and pharmaceuticals has gained considerable research attention. In this report, some unprecedented hydrogen bond motifs between the –COOH group and the solvents capable of forming multiple hydrogen bonds with –COOH are studied. The effects of such diverse motifs on the construction of 3D supramolecular architectures of hydrogen-bonded host–guest frameworks and their optical properties are elucidated. For this purpose, structural studies on seven solvates, namely, <strong>1a</strong> (<strong>1</strong>:2DMF), <strong>1b</strong> (<strong>1</strong>:2pyridine), <strong>1c</strong> (<strong>1</strong>:2quinoline), <strong>2a</strong> (<strong>1</strong>:2DMF), <strong>2b</strong> (<strong>1</strong>:2pyridine), <strong>2c</strong> (<strong>1</strong>:2quinoline), and <strong>2d</strong> (<strong>1</strong>:1quinoline:2piperidine), of two isomeric pyromellitic diimide hosts <strong>1</strong> and <strong>2</strong> were carried out. Single crystal X-ray diffraction (SCXRD) analyses revealed that solvates <strong>1a</strong>, <strong>2a</strong>, and <strong>2b</strong> show 3D non-porous supramolecular host–guest networks, whereas solvates <strong>1b</strong>, <strong>1c</strong>, <strong>2c</strong>, and <strong>2d</strong> show 3D supramolecular host–guest channelled architectures accommodating guest solvent molecules within the cavities of different dimensions. Formation of different hydrogen bond motifs, either cyclic/ring (R) or discrete (D) or a combination of both, between the –COOH groups of isomeric hosts and identical guest molecules is analysed through density functional theory (DFT) calculations. Minor differences in the interaction energies of different motifs of isomeric hosts with the same guest suggest that the formation of either motif depends on the steric orientations of hosts and other weak host–guest interactions in the crystal lattices. Solid state fluorescence emission properties of solvates <strong>1a</strong>, <strong>2a</strong>, and <strong>2b</strong> are found to be similar to their respective hosts, whereas those of solvates <strong>1b</strong>, <strong>1c</strong>, <strong>2c</strong>, and <strong>2d</strong> are different from their hosts. Along with the diversity of supramolecular synthons, frontier molecular orbital (FMO) analysis of hydrogen-bonded model structures explained well the different emission behaviours of solvates. Thermal analyses for the solvates are in good agreement for the association of the numbers of guest solvent molecules with both the isomeric hosts. Overall, this research is focused on establishing the phenomena for the formation of distinct hydrogen bond patterns between the two similar host–guest binding groups together with the effect of supramolecular states on the photophysical properties of such hydrogen-
{"title":"Development of photoluminescent hydrogen-bonded frameworks based on pyromellitic diimide-tethered carboxylic acid hosts and multi-bonding solvent guests†","authors":"Raju Ram Puniya, Priyanka Takhar, Monika Chhapoliya, Rinki Deka, Dhruba Jyoti Kalita and Devendra Singh","doi":"10.1039/D4MA00634H","DOIUrl":"https://doi.org/10.1039/D4MA00634H","url":null,"abstract":"<p >The significance of hydrogen-bonding interactions in improving the chemical and physical properties of functional materials related to sustainable energy, gas absorption, catalysis, and pharmaceuticals has gained considerable research attention. In this report, some unprecedented hydrogen bond motifs between the –COOH group and the solvents capable of forming multiple hydrogen bonds with –COOH are studied. The effects of such diverse motifs on the construction of 3D supramolecular architectures of hydrogen-bonded host–guest frameworks and their optical properties are elucidated. For this purpose, structural studies on seven solvates, namely, <strong>1a</strong> (<strong>1</strong>:2DMF), <strong>1b</strong> (<strong>1</strong>:2pyridine), <strong>1c</strong> (<strong>1</strong>:2quinoline), <strong>2a</strong> (<strong>1</strong>:2DMF), <strong>2b</strong> (<strong>1</strong>:2pyridine), <strong>2c</strong> (<strong>1</strong>:2quinoline), and <strong>2d</strong> (<strong>1</strong>:1quinoline:2piperidine), of two isomeric pyromellitic diimide hosts <strong>1</strong> and <strong>2</strong> were carried out. Single crystal X-ray diffraction (SCXRD) analyses revealed that solvates <strong>1a</strong>, <strong>2a</strong>, and <strong>2b</strong> show 3D non-porous supramolecular host–guest networks, whereas solvates <strong>1b</strong>, <strong>1c</strong>, <strong>2c</strong>, and <strong>2d</strong> show 3D supramolecular host–guest channelled architectures accommodating guest solvent molecules within the cavities of different dimensions. Formation of different hydrogen bond motifs, either cyclic/ring (R) or discrete (D) or a combination of both, between the –COOH groups of isomeric hosts and identical guest molecules is analysed through density functional theory (DFT) calculations. Minor differences in the interaction energies of different motifs of isomeric hosts with the same guest suggest that the formation of either motif depends on the steric orientations of hosts and other weak host–guest interactions in the crystal lattices. Solid state fluorescence emission properties of solvates <strong>1a</strong>, <strong>2a</strong>, and <strong>2b</strong> are found to be similar to their respective hosts, whereas those of solvates <strong>1b</strong>, <strong>1c</strong>, <strong>2c</strong>, and <strong>2d</strong> are different from their hosts. Along with the diversity of supramolecular synthons, frontier molecular orbital (FMO) analysis of hydrogen-bonded model structures explained well the different emission behaviours of solvates. Thermal analyses for the solvates are in good agreement for the association of the numbers of guest solvent molecules with both the isomeric hosts. Overall, this research is focused on establishing the phenomena for the formation of distinct hydrogen bond patterns between the two similar host–guest binding groups together with the effect of supramolecular states on the photophysical properties of such hydrogen-","PeriodicalId":18242,"journal":{"name":"Materials Advances","volume":null,"pages":null},"PeriodicalIF":5.2,"publicationDate":"2024-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ma/d4ma00634h?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142329369","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Muhammad Ali Ehsan, Akilarasan Muthumariappan, Muhammad Ali, Abbas Saeed Hakeem and Wasif Farooq
The hydrogen evolution reaction (HER) plays a crucial role in realizing the ambitious objectives of renewable hydrogen (H2) production and CO2 neutrality. The efficacy of the HER process mainly relies on the electrocatalysts that are highly active, stable, and cost-effective, ensuring efficient and sustainable H2 generation. In this study, binary copper–palladium (CuPd) alloy thin film catalysts directly grown on graphite sheets via aerosol-assisted chemical vapor deposition were employed for the HER in 0.5 M H2SO4. A unique array of tower-like microstructures were fabricated by varying the deposition time from 1 to 2 hours, demonstrating excellent HER activity by achieving high current densities of 100 and 1000 mA cm−2 at low overpotentials of 64 and 137 mV, respectively. It also exhibited favorable Tafel kinetics (28 mV dec−1), a high electrochemical surface area (3046 cm2), and reasonable stability over 24 hours, surpassing the benchmark Pt, Pd, and other reputed noble metal-based catalysts. The synergy between transition and noble metals (Cu–Pd) and the array of tower structure in the alloy has been shown to enhance conductivity and offer abundant active sites, resulting in its superior performance in the HER. Furthermore, density functional theory simulations indicated a decrease in the Gibbs free energy value for the binary CuPd alloy (−0.12 eV) compared to that of metallic Pd and Cu in the HER process, thereby validating the experimental observations. This study presents a straightforward deposition technique to design robust and efficient thin film electrocatalysts and optimize electrochemically active sites to achieve faster HER rates with low overpotential.
氢气进化反应(HER)在实现可再生氢气(H2)生产和二氧化碳中和的宏伟目标方面发挥着至关重要的作用。氢进化反应过程的有效性主要依赖于高活性、高稳定性和高成本效益的电催化剂,以确保高效和可持续的氢气生成。本研究采用气溶胶辅助化学气相沉积法在石墨片上直接生长二元铜钯(CuPd)合金薄膜催化剂,用于 0.5 M H2SO4 中的 HER。通过改变沉积时间(1 到 2 小时),制备出了独特的塔状微结构阵列,并在 64 和 137 mV 的低过电位下分别获得了 100 和 1000 mA cm-2 的高电流密度,显示出卓越的 HER 活性。它还表现出良好的塔菲尔动力学(28 mV dec-1)、高电化学表面积(3046 cm2)和 24 小时内的合理稳定性,超过了基准铂、钯和其他著名的贵金属基催化剂。研究表明,过渡金属和贵金属(铜-钯)之间的协同作用以及合金中的塔状结构阵列增强了导电性,并提供了丰富的活性位点,从而使其在 HER 中表现出色。此外,密度泛函理论模拟表明,与金属钯和铜相比,二元铜钯合金在 HER 过程中的吉布斯自由能值(-0.12 eV)有所降低,从而验证了实验观察结果。本研究提出了一种直接沉积技术,可用于设计稳健高效的薄膜电催化剂,并优化电化学活性位点,从而以较低的过电位实现更快的 HER 速率。
{"title":"Facile fabrication of binary copper–palladium alloy thin film catalysts for exceptional hydrogen evolution performance†","authors":"Muhammad Ali Ehsan, Akilarasan Muthumariappan, Muhammad Ali, Abbas Saeed Hakeem and Wasif Farooq","doi":"10.1039/D4MA00410H","DOIUrl":"https://doi.org/10.1039/D4MA00410H","url":null,"abstract":"<p >The hydrogen evolution reaction (HER) plays a crucial role in realizing the ambitious objectives of renewable hydrogen (H<small><sub>2</sub></small>) production and CO<small><sub>2</sub></small> neutrality. The efficacy of the HER process mainly relies on the electrocatalysts that are highly active, stable, and cost-effective, ensuring efficient and sustainable H<small><sub>2</sub></small> generation. In this study, binary copper–palladium (CuPd) alloy thin film catalysts directly grown on graphite sheets <em>via</em> aerosol-assisted chemical vapor deposition were employed for the HER in 0.5 M H<small><sub>2</sub></small>SO<small><sub>4</sub></small>. A unique array of tower-like microstructures were fabricated by varying the deposition time from 1 to 2 hours, demonstrating excellent HER activity by achieving high current densities of 100 and 1000 mA cm<small><sup>−2</sup></small> at low overpotentials of 64 and 137 mV, respectively. It also exhibited favorable Tafel kinetics (28 mV dec<small><sup>−1</sup></small>), a high electrochemical surface area (3046 cm<small><sup>2</sup></small>), and reasonable stability over 24 hours, surpassing the benchmark Pt, Pd, and other reputed noble metal-based catalysts. The synergy between transition and noble metals (Cu–Pd) and the array of tower structure in the alloy has been shown to enhance conductivity and offer abundant active sites, resulting in its superior performance in the HER. Furthermore, density functional theory simulations indicated a decrease in the Gibbs free energy value for the binary CuPd alloy (−0.12 eV) compared to that of metallic Pd and Cu in the HER process, thereby validating the experimental observations. This study presents a straightforward deposition technique to design robust and efficient thin film electrocatalysts and optimize electrochemically active sites to achieve faster HER rates with low overpotential.</p>","PeriodicalId":18242,"journal":{"name":"Materials Advances","volume":null,"pages":null},"PeriodicalIF":5.2,"publicationDate":"2024-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ma/d4ma00410h?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142430914","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Guangshu Liang, Yining Yang, Daofu Cheng, Yuyan Ma and Linping Yan
Managing glioma, a particularly aggressive form of brain cancer, poses significant challenges because of its inherent resistance and the intricate nature of the central nervous system. Photodynamic therapy (PDT), which uses photosensitizers to target and destroy cancer cells while minimizing damage to surrounding healthy tissues, has emerged as a novel and effective approach for glioma treatment. In this study, we designed and synthesized a novel photosensitizer, ITIC, for potential application in glioma therapy. By employing nanotechnology, we enhanced the water dispersibility of ITIC. ITIC nanoparticles (NPs) exhibit near-infrared absorbance and are light-activatable for generating reactive oxygen species (ROS), which allows for effective killing of cancer cells. Furthermore, the unique chemical structure of ITIC makes it easy to conjugate ITIC with targeting ligands to enable specific recognition and uptake by glioma cells in both in vitro and in vivo studies, thereby increasing the precision of glioma cell detection and engagement.
{"title":"Synthesis of a new photosensitizer for laser-mediated photodynamic therapy to kill cancer cells in gliomas†","authors":"Guangshu Liang, Yining Yang, Daofu Cheng, Yuyan Ma and Linping Yan","doi":"10.1039/D4MA00637B","DOIUrl":"https://doi.org/10.1039/D4MA00637B","url":null,"abstract":"<p >Managing glioma, a particularly aggressive form of brain cancer, poses significant challenges because of its inherent resistance and the intricate nature of the central nervous system. Photodynamic therapy (PDT), which uses photosensitizers to target and destroy cancer cells while minimizing damage to surrounding healthy tissues, has emerged as a novel and effective approach for glioma treatment. In this study, we designed and synthesized a novel photosensitizer, ITIC, for potential application in glioma therapy. By employing nanotechnology, we enhanced the water dispersibility of ITIC. ITIC nanoparticles (NPs) exhibit near-infrared absorbance and are light-activatable for generating reactive oxygen species (ROS), which allows for effective killing of cancer cells. Furthermore, the unique chemical structure of ITIC makes it easy to conjugate ITIC with targeting ligands to enable specific recognition and uptake by glioma cells in both <em>in vitro</em> and <em>in vivo</em> studies, thereby increasing the precision of glioma cell detection and engagement.</p>","PeriodicalId":18242,"journal":{"name":"Materials Advances","volume":null,"pages":null},"PeriodicalIF":5.2,"publicationDate":"2024-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ma/d4ma00637b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142236037","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The continuous rise in atmospheric CO2 level is a major concern, demanding the development of low-cost, scalable porous sorbents with improved efficiency and recyclability. The current chemical adsorption methods are energy-intensive, creating a demand for low-energy CO2 capture/removal strategies. Physical adsorption of CO2 offers an efficient and low-energy alternative. This study explores the design and screening of porous carbon pellets for physical adsorption of CO2 from 15% CO2 in N2 at 30 °C. Various sizes of spherical pellets were designed and investigated for their effect on adsorption capacity and kinetics. Changing the shape from spherical to flakes increased the CO2 adsorption capacity to 2.2 wt% (0.5 mmol g−1). The pellets were also analysed for cyclic adsorption–desorption to access long-term stability and recyclability, showing approximately 80% selectivity for CO2 over N2 over 20 cycles.
大气中二氧化碳含量的持续上升是人们关注的一个主要问题,这就要求开发低成本、可扩展、高效率和可回收的多孔吸附剂。目前的化学吸附方法能耗高,因此需要低能耗的二氧化碳捕获/去除策略。二氧化碳的物理吸附提供了一种高效、低能耗的替代方法。本研究探索了多孔碳颗粒的设计和筛选,用于在 30 °C 下物理吸附 15% CO2 在 N2 中的二氧化碳。我们设计了各种尺寸的球形颗粒,并研究了它们对吸附容量和动力学的影响。将形状从球形改为片状后,二氧化碳的吸附容量增加到 2.2 wt%(0.5 mmol g-1)。还对颗粒进行了循环吸附-解吸分析,以了解其长期稳定性和可回收性,结果表明,在 20 个循环中,二氧化碳对 N2 的选择性约为 80%。
{"title":"Porous carbon pellets for physical adsorption of CO2: size and shape effect†","authors":"Baljeet Singh, Marianna Kemell and Timo Repo","doi":"10.1039/D4MA00703D","DOIUrl":"https://doi.org/10.1039/D4MA00703D","url":null,"abstract":"<p >The continuous rise in atmospheric CO<small><sub>2</sub></small> level is a major concern, demanding the development of low-cost, scalable porous sorbents with improved efficiency and recyclability. The current chemical adsorption methods are energy-intensive, creating a demand for low-energy CO<small><sub>2</sub></small> capture/removal strategies. Physical adsorption of CO<small><sub>2</sub></small> offers an efficient and low-energy alternative. This study explores the design and screening of porous carbon pellets for physical adsorption of CO<small><sub>2</sub></small> from 15% CO<small><sub>2</sub></small> in N<small><sub>2</sub></small> at 30 °C. Various sizes of spherical pellets were designed and investigated for their effect on adsorption capacity and kinetics. Changing the shape from spherical to flakes increased the CO<small><sub>2</sub></small> adsorption capacity to 2.2 wt% (0.5 mmol g<small><sup>−1</sup></small>). The pellets were also analysed for cyclic adsorption–desorption to access long-term stability and recyclability, showing approximately 80% selectivity for CO<small><sub>2</sub></small> over N<small><sub>2</sub></small> over 20 cycles.</p>","PeriodicalId":18242,"journal":{"name":"Materials Advances","volume":null,"pages":null},"PeriodicalIF":5.2,"publicationDate":"2024-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ma/d4ma00703d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142329418","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}