Pub Date : 2024-08-31DOI: 10.1016/j.mtchem.2024.102265
Changhui Fu, Li Yao, Zhiguang Guo
The pollution of oily wastewater and the frequent occurrence of oil spills seriously affect human economy, safety, and environment. So far, researchers have developed a series of strategies and materials to solve the oil pollution, but the development of green, efficient, sustainably separated, environmentally stable, and low-cost materials for oil-water separation remains a challenge. Biomass materials such as chitosan, gelatin, cellulose, alginate, and lignin have been widely used in the preparation of oil-water separation materials for environmental remediation due to their wide sources, environmental friendliness, and abundant active functional groups. Herein, this paper mainly reviews the recent research progress of chitosan-based oil-water separation materials. Firstly, the research background and wettability theory are introduced in Chapter 1 and Chapter 2, and then the design ideas, preparation methods, modified materials, separation principles and oil-water separation properties of two-dimensional chitosan-based membranes, including chitosan hydrogel membranes, and three-dimensional chitosan-based aerogels are highlighted in the subsequent chapters.
{"title":"Biomass chitosan-based complexes with superwettability for oil-water separation","authors":"Changhui Fu, Li Yao, Zhiguang Guo","doi":"10.1016/j.mtchem.2024.102265","DOIUrl":"https://doi.org/10.1016/j.mtchem.2024.102265","url":null,"abstract":"The pollution of oily wastewater and the frequent occurrence of oil spills seriously affect human economy, safety, and environment. So far, researchers have developed a series of strategies and materials to solve the oil pollution, but the development of green, efficient, sustainably separated, environmentally stable, and low-cost materials for oil-water separation remains a challenge. Biomass materials such as chitosan, gelatin, cellulose, alginate, and lignin have been widely used in the preparation of oil-water separation materials for environmental remediation due to their wide sources, environmental friendliness, and abundant active functional groups. Herein, this paper mainly reviews the recent research progress of chitosan-based oil-water separation materials. Firstly, the research background and wettability theory are introduced in Chapter 1 and Chapter 2, and then the design ideas, preparation methods, modified materials, separation principles and oil-water separation properties of two-dimensional chitosan-based membranes, including chitosan hydrogel membranes, and three-dimensional chitosan-based aerogels are highlighted in the subsequent chapters.","PeriodicalId":18353,"journal":{"name":"Materials Today Chemistry","volume":null,"pages":null},"PeriodicalIF":7.3,"publicationDate":"2024-08-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142204467","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 : 2024-08-30DOI: 10.1016/j.mtchem.2024.102278
Xinliang Guo, Hongyi Jin, Zejun Ye, Zhimin Yu, Yang Yang, Jiaming Sun
The GaO/MgO/ErO nanolaminates are fabricated by atomic layer deposition and crystallized into Er-doped MgGaO spinel (MGS:Er) nanofilms after annealing, with their electroluminescence (EL) performance characterized. The annealing above 600 °C achieves the polycrystalline spinel nanofilm, and the crystallization is promoted by the higher annealing temperature and GaO/MgO ratio. The dopant Er ions preferably substitute into the octahedron sites occupied by Ga ions in ordinary spinel and Mg in anti-spinel lattice, while the inversion degree is confirmed to increase with the reduction of GaO/MgO ratio and annealing temperature, resulting the relatively enhanced secondary EL at 1542 nm. This perturbation by Er-substitution into anti-spinel sites improves the emission intensity and excitation efficiencies, the main EL emission peaking at 1531 nm from the optimal MGS:Er device exhibits the excitation efficiency reaching 5.8 %, with the enhanced electrical injection realizing the maximum EL intensity above 17.3 mW/cm. The fluorescence lifetime of these MGS:Er devices is established in the range of 371–760 μs, which decreases mainly with the Er concentrations. The prototype device using the near-stoichiometric GaO/MgO ratio shows the operation time of 1.12 × 10 s. This work explores the fabrication of Si-based spinel nanofilms with designed composition and special microstructure, and their practical application in optoelectronics.
通过原子层沉积制备了 GaO/MgO/ErO 纳米层压板，并在退火后结晶成掺铒 MgGaO 尖晶石（MGS:Er）纳米薄膜，其电致发光（EL）性能得到了表征。600 °C 以上的退火温度可获得多晶尖晶石纳米薄膜，较高的退火温度和 GaO/MgO 比率可促进结晶。掺杂剂 Er 离子优先取代了普通尖晶石中 Ga 离子和反尖晶石晶格中 Mg 离子占据的八面体位点，而反转程度则随着 GaO/MgO 比率和退火温度的降低而增加，从而导致 1542 纳米波长的二次电致发光相对增强。Er 取代反尖晶石位点的扰动提高了发射强度和激发效率，最佳 MGS:Er 器件在 1531 nm 处的主要 EL 发射峰值的激发效率达到 5.8%，增强的电注入实现了 17.3 mW/cm 以上的最大 EL 强度。这些 MGS:Er 器件的荧光寿命为 371-760 μs，主要随 Er 浓度的增加而降低。这项研究探索了具有设计成分和特殊微观结构的硅基尖晶石纳米薄膜的制备及其在光电子领域的实际应用。
{"title":"Increase the inversion degree in Er-doped MgGa2O4 spinel nanofilms to obtain strong electroluminescence","authors":"Xinliang Guo, Hongyi Jin, Zejun Ye, Zhimin Yu, Yang Yang, Jiaming Sun","doi":"10.1016/j.mtchem.2024.102278","DOIUrl":"https://doi.org/10.1016/j.mtchem.2024.102278","url":null,"abstract":"The GaO/MgO/ErO nanolaminates are fabricated by atomic layer deposition and crystallized into Er-doped MgGaO spinel (MGS:Er) nanofilms after annealing, with their electroluminescence (EL) performance characterized. The annealing above 600 °C achieves the polycrystalline spinel nanofilm, and the crystallization is promoted by the higher annealing temperature and GaO/MgO ratio. The dopant Er ions preferably substitute into the octahedron sites occupied by Ga ions in ordinary spinel and Mg in anti-spinel lattice, while the inversion degree is confirmed to increase with the reduction of GaO/MgO ratio and annealing temperature, resulting the relatively enhanced secondary EL at 1542 nm. This perturbation by Er-substitution into anti-spinel sites improves the emission intensity and excitation efficiencies, the main EL emission peaking at 1531 nm from the optimal MGS:Er device exhibits the excitation efficiency reaching 5.8 %, with the enhanced electrical injection realizing the maximum EL intensity above 17.3 mW/cm. The fluorescence lifetime of these MGS:Er devices is established in the range of 371–760 μs, which decreases mainly with the Er concentrations. The prototype device using the near-stoichiometric GaO/MgO ratio shows the operation time of 1.12 × 10 s. This work explores the fabrication of Si-based spinel nanofilms with designed composition and special microstructure, and their practical application in optoelectronics.","PeriodicalId":18353,"journal":{"name":"Materials Today Chemistry","volume":null,"pages":null},"PeriodicalIF":7.3,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142204468","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}
Non-centrosymmetric structure is the prerequisite to symmetry-dependent properties for functional materials. The inherent tendency of crystallization toward centrosymmetric arrangements has posed a great challenge in nonlinear optical crystals that requires non-centrosymmetric structure. Here we discovered two new hydroxyborates A[C(NH)][BO(OH)]·HO (A = K, Rb; = 3, 1.5), which have high similarity in cationic and anionic frameworks but clearly differ in terms of symmetry, such as non-centrosymmetric versus centrosymmetric. Variations in the hydrogen bonds of water molecules in the lattice are confirmed to be the origin of the symmetry breaking and transformation. The effectiveness of hydrogen bond-derived molecular engineering in producing non-centrosymmetric structure and opening up new avenues in the nonlinear optical crystal sector is demonstrated in this work.
{"title":"Hydrogen bond-derived symmetry transformation in hydroxyborates: Converting the nonlinearity from null to active","authors":"Ziqi Chen, Changyou Liu, Junjie Li, Zhihua Yang, Shilie Pan, Miriding Mutailipu","doi":"10.1016/j.mtchem.2024.102277","DOIUrl":"https://doi.org/10.1016/j.mtchem.2024.102277","url":null,"abstract":"Non-centrosymmetric structure is the prerequisite to symmetry-dependent properties for functional materials. The inherent tendency of crystallization toward centrosymmetric arrangements has posed a great challenge in nonlinear optical crystals that requires non-centrosymmetric structure. Here we discovered two new hydroxyborates A[C(NH)][BO(OH)]·HO (A = K, Rb; = 3, 1.5), which have high similarity in cationic and anionic frameworks but clearly differ in terms of symmetry, such as non-centrosymmetric versus centrosymmetric. Variations in the hydrogen bonds of water molecules in the lattice are confirmed to be the origin of the symmetry breaking and transformation. The effectiveness of hydrogen bond-derived molecular engineering in producing non-centrosymmetric structure and opening up new avenues in the nonlinear optical crystal sector is demonstrated in this work.","PeriodicalId":18353,"journal":{"name":"Materials Today Chemistry","volume":null,"pages":null},"PeriodicalIF":7.3,"publicationDate":"2024-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142204470","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}
This study presents an innovative organic-inorganic hybrid transducer of poly(acrylic acid) (PAA), poly(3,4-ethylenedioxythiophene) (PEDOT) and Prussian blue (PB) nanocatalysts. The transducer demonstrated functionality conducive to enzyme conjugation and exhibited favorable electrochemical properties for biosensor signal transduction. Fabricated by a one-tube chemical redox method, the PAA:PEDOT-PB transducer showed long-term electrocatalytic and structural stability. The performance of the transducer was characterized by high transduction activity and low charge transfer resistance, particularly for HO reduction. It achieves a linear detection range from 1.0 μM to 4.0 mM, with a sensitivity of 494 ± 10 μA mM cm and a LOD of 0.34 μM. The PAA:PEDOT-PB transducer featured a high density of carboxyl groups (D = 14.64 ± 0.05 μmol cm) that promoted the immobilization of the HO-dependent oxidase enzyme lactate oxidase (LOx) with an EDC/S–NHS coupling agent. The LOx-PAA:PEDOT-PB transducer was developed for lactate biosensing. The transducer provided high LOx-enzyme affinity (K = 1.47 ± 0.05 mM), and a rapid response time (10 s) for lactate detection across a concentration range of 5.0 μM to 4.0 mM, showing a sensitivity of 223 ± 3 μA mM cm and an LOD of 1.45 μM. The LOx-PAA:PEDOT-PB transducer was integrated with a flexible screen-printed electrode, incorporating a wireless, battery-free near-field communication potentiostat module to measure lactate in artificial sweat on a skin model via smartphone. The PAA:PEDOT-PB transducer could enable connections with multiple bio-recognition molecules through polycarboxylic acid groups, providing potential avenues for the development of advanced biosensors.
{"title":"Bio-functionalized conductive poly(acrylic acid):poly(3,4-Ethylenedioxythiophene)-Prussian blue hybrid transducer for biosensors and bioelectronics interfaces","authors":"Kiattisak Promsuwan, Jenjira Saichanapan, Asamee Soleh, Kasrin Saisahas, Kritsada Samoson, Sangay Wangchuk, Warakorn Limbut","doi":"10.1016/j.mtchem.2024.102271","DOIUrl":"https://doi.org/10.1016/j.mtchem.2024.102271","url":null,"abstract":"This study presents an innovative organic-inorganic hybrid transducer of poly(acrylic acid) (PAA), poly(3,4-ethylenedioxythiophene) (PEDOT) and Prussian blue (PB) nanocatalysts. The transducer demonstrated functionality conducive to enzyme conjugation and exhibited favorable electrochemical properties for biosensor signal transduction. Fabricated by a one-tube chemical redox method, the PAA:PEDOT-PB transducer showed long-term electrocatalytic and structural stability. The performance of the transducer was characterized by high transduction activity and low charge transfer resistance, particularly for HO reduction. It achieves a linear detection range from 1.0 μM to 4.0 mM, with a sensitivity of 494 ± 10 μA mM cm and a LOD of 0.34 μM. The PAA:PEDOT-PB transducer featured a high density of carboxyl groups (D = 14.64 ± 0.05 μmol cm) that promoted the immobilization of the HO-dependent oxidase enzyme lactate oxidase (LOx) with an EDC/S–NHS coupling agent. The LOx-PAA:PEDOT-PB transducer was developed for lactate biosensing. The transducer provided high LOx-enzyme affinity (K = 1.47 ± 0.05 mM), and a rapid response time (10 s) for lactate detection across a concentration range of 5.0 μM to 4.0 mM, showing a sensitivity of 223 ± 3 μA mM cm and an LOD of 1.45 μM. The LOx-PAA:PEDOT-PB transducer was integrated with a flexible screen-printed electrode, incorporating a wireless, battery-free near-field communication potentiostat module to measure lactate in artificial sweat on a skin model via smartphone. The PAA:PEDOT-PB transducer could enable connections with multiple bio-recognition molecules through polycarboxylic acid groups, providing potential avenues for the development of advanced biosensors.","PeriodicalId":18353,"journal":{"name":"Materials Today Chemistry","volume":null,"pages":null},"PeriodicalIF":7.3,"publicationDate":"2024-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142204493","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}
Flexible sensors have received increasing attention due to their various applications in health monitoring, artificial intelligence, and other fields. The simple fabrication of flexible sensing devices with high performances has been a research hotpot. In this work, an ionogel composite sensor combined with elastic knitted coil (EIC) is proposed as a wearable device to monitor human movement and related feature information. This sensor can be fabricated in a simple and easy protocol, which can work as a clothing accessary to track the wellness status parameters in daily life. After washing, the redundant gel originally embedded between the fibers was removed, improving the sensitivity of the sensor, which can provide accurate information about human joint movements and other physiological activities. The EIC sensor is in high sensitivity with superior working durability, which can provide continuous piezoresistive signals in detection mode. Other than the common joint bending movements (wrist, knee, elbow and finger) of human body, this sensor can also accurately output monitoring data on periocular, oral, and pharyngeal movements, providing information about human health status. Besides, a Morse codes transmission system can be constructed based on the piezoresistive outputs of this EIC sensor under different tapping modes, providing a new working platform in other related applications.
{"title":"A flexible sensor based on ionogel/knitted coil prepared by a simple method for accurate monitoring of human physiological signals","authors":"Yuejing Sun, Li Yang, Qiujin Li, Peiduan Zhang, Jixian Gong, Zheng Li, Xiuming Liu, Jianfei Zhang","doi":"10.1016/j.mtchem.2024.102273","DOIUrl":"https://doi.org/10.1016/j.mtchem.2024.102273","url":null,"abstract":"Flexible sensors have received increasing attention due to their various applications in health monitoring, artificial intelligence, and other fields. The simple fabrication of flexible sensing devices with high performances has been a research hotpot. In this work, an ionogel composite sensor combined with elastic knitted coil (EIC) is proposed as a wearable device to monitor human movement and related feature information. This sensor can be fabricated in a simple and easy protocol, which can work as a clothing accessary to track the wellness status parameters in daily life. After washing, the redundant gel originally embedded between the fibers was removed, improving the sensitivity of the sensor, which can provide accurate information about human joint movements and other physiological activities. The EIC sensor is in high sensitivity with superior working durability, which can provide continuous piezoresistive signals in detection mode. Other than the common joint bending movements (wrist, knee, elbow and finger) of human body, this sensor can also accurately output monitoring data on periocular, oral, and pharyngeal movements, providing information about human health status. Besides, a Morse codes transmission system can be constructed based on the piezoresistive outputs of this EIC sensor under different tapping modes, providing a new working platform in other related applications.","PeriodicalId":18353,"journal":{"name":"Materials Today Chemistry","volume":null,"pages":null},"PeriodicalIF":7.3,"publicationDate":"2024-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142204471","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}
Ionogels with broad temperature, environment, and long-term stability are desirable in intelligent flexible electronics. Herein, we have developed a novel ultra-stable ionogel through hydrogen bonding between the amphiphilic ionic liquid--1-ethyl-3-methylimidazolium bis[(trifluoromethyl)sulfonyl]imide ([EMIM][NTf]) and butyl acrylate (BA)-ethyl ethoxyethyl acrylate (EO) copolymer (P(BA-co-EO)). The ionogel demonstrates high decomposition voltage, strong adhesion stability, non-corrosive stability, and cyclic strain sensing stability (500 cycles at 120 % strain). Additionally, it exhibits broad temperature and environment adaptability, capable of stretching up to 7 times at −20 °C, maintaining consistent weight after 30 days of storage in extreme environments such as low/high temperatures (−20∼100 °C), high vacuum (6 × 10 Pa), and underwater (without additional sealed packaging), while also maintaining electrophysiological monitoring at −20 °C or 100 °C. Most importantly, the ionogel without sealing can self-adhere to the human skin for continuous and high-quality electrophysiological monitoring for 1 month under daily life conditions. We have utilized the ionogel to fabricate an ionic skin with multifunctional sensing capabilities for strain, pressure, and temperature, which has been successfully employed in human motion and pressure detection. It is believed that ionogels with long-term stability will pave the way for developing next-generation intelligent flexible electronics in future research endeavors.
{"title":"Ultra-stable ionogels based on hydrogen networks with broad temperature, environment, and long-term stability","authors":"Huiyuan Zhang, Tianhong Dong, Cancan Zheng, Hongxing Zhang, Yumin Xia, Yong He","doi":"10.1016/j.mtchem.2024.102275","DOIUrl":"https://doi.org/10.1016/j.mtchem.2024.102275","url":null,"abstract":"Ionogels with broad temperature, environment, and long-term stability are desirable in intelligent flexible electronics. Herein, we have developed a novel ultra-stable ionogel through hydrogen bonding between the amphiphilic ionic liquid--1-ethyl-3-methylimidazolium bis[(trifluoromethyl)sulfonyl]imide ([EMIM][NTf]) and butyl acrylate (BA)-ethyl ethoxyethyl acrylate (EO) copolymer (P(BA-co-EO)). The ionogel demonstrates high decomposition voltage, strong adhesion stability, non-corrosive stability, and cyclic strain sensing stability (500 cycles at 120 % strain). Additionally, it exhibits broad temperature and environment adaptability, capable of stretching up to 7 times at −20 °C, maintaining consistent weight after 30 days of storage in extreme environments such as low/high temperatures (−20∼100 °C), high vacuum (6 × 10 Pa), and underwater (without additional sealed packaging), while also maintaining electrophysiological monitoring at −20 °C or 100 °C. Most importantly, the ionogel without sealing can self-adhere to the human skin for continuous and high-quality electrophysiological monitoring for 1 month under daily life conditions. We have utilized the ionogel to fabricate an ionic skin with multifunctional sensing capabilities for strain, pressure, and temperature, which has been successfully employed in human motion and pressure detection. It is believed that ionogels with long-term stability will pave the way for developing next-generation intelligent flexible electronics in future research endeavors.","PeriodicalId":18353,"journal":{"name":"Materials Today Chemistry","volume":null,"pages":null},"PeriodicalIF":7.3,"publicationDate":"2024-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142204472","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 : 2024-08-29DOI: 10.1016/j.mtchem.2024.102279
Jiuna Zhao, Min Zheng
Bacterial contamination of medical devices and food poses critical threat to mankind's health. Although some antibiotics can kill bacteria, their mis/overuse in healthcare and agriculture has brought about serious bacterial antibiotic resistance. Thus, developing a convenient and rapid sterilization method becomes increasingly important. Herein, the nanocomposite NR@CDs was synthesized by the assembly of neutral red (NR) with carbon dots (CDs). Compared with NR, NR@CDs has stronger reactive oxygen species (ROS) generation ability. NR@CDs can photodynamically destroy both gram-positive and gram-negative bacteria efficiently, and the minimum inhibitory concentration (MIC) is 45 μg mL. NR@CDs spray is an eco-friendly sterilizing agent, with favorable biocompatibility and water-washability properties. Just 1 min of irradiation, NR@CDs spray can quickly and accurately kill the bacteria on the surface of the mouthguards (MGs). As the NR@CDs aqueous solution sprays on cherries, it can effectively prolong the quality guarantee period of perishable foods. The present work provides an innovative strategy to solve the global bacterial contamination and antibiotic resistance problems.
{"title":"Neutral red/carbon dots photodynamic disinfectant spray for sports mouthguards cleaning and perishable foods preservation","authors":"Jiuna Zhao, Min Zheng","doi":"10.1016/j.mtchem.2024.102279","DOIUrl":"https://doi.org/10.1016/j.mtchem.2024.102279","url":null,"abstract":"Bacterial contamination of medical devices and food poses critical threat to mankind's health. Although some antibiotics can kill bacteria, their mis/overuse in healthcare and agriculture has brought about serious bacterial antibiotic resistance. Thus, developing a convenient and rapid sterilization method becomes increasingly important. Herein, the nanocomposite NR@CDs was synthesized by the assembly of neutral red (NR) with carbon dots (CDs). Compared with NR, NR@CDs has stronger reactive oxygen species (ROS) generation ability. NR@CDs can photodynamically destroy both gram-positive and gram-negative bacteria efficiently, and the minimum inhibitory concentration (MIC) is 45 μg mL. NR@CDs spray is an eco-friendly sterilizing agent, with favorable biocompatibility and water-washability properties. Just 1 min of irradiation, NR@CDs spray can quickly and accurately kill the bacteria on the surface of the mouthguards (MGs). As the NR@CDs aqueous solution sprays on cherries, it can effectively prolong the quality guarantee period of perishable foods. The present work provides an innovative strategy to solve the global bacterial contamination and antibiotic resistance problems.","PeriodicalId":18353,"journal":{"name":"Materials Today Chemistry","volume":null,"pages":null},"PeriodicalIF":7.3,"publicationDate":"2024-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142204469","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 : 2024-08-28DOI: 10.1016/j.mtchem.2024.102267
N. Baaalla, H. Absike, F. Mezzat, E.K. Hlil, R. Masrour, A. Benyoussef, A. El Kenz
The theoretical investigation of the newly discovered quadruple perovskite Ag₂Mo₃SeO was conducted using density functional theory (DFT) with the generalized gradient approximation (GGA-PBE) for the structural properties. This study examined the compound's structural, electronic, optical, and thermoelectric properties, utilizing the Tran Blaha modified Becke-Johnson exchange potential (mBJ) for accurate band gap measurement to overcome the bandgap underestimation by GGA-PBE. The stable structure was confirmed through energy-volume optimization and fitted with the Birch-Murnaghan equation of state, using PBE-GGA exchange correlation functional. The findings revealed a band structure with direct transition under the TB-mBJ approach with an energy gap of 1.45 eV. Detailed analyses were conducted, including the density of states and charge density distribution maps. Various optical parameters such as the dielectric function, absorption coefficient, refractive index, and reflectivity were computed, with the static dielectric constant measured at 6.3. Notably, a significant evolution of the absorption coefficient in the visible region highlights the potential of Ag₂Mo₃SeO₁₂ for solar cell and optoelectronic applications. These results pave the way for new photovoltaic material designs. Furthermore, the material demonstrates promising thermoelectric properties with an appropriate figure of merit, Seebeck coefficient, and electrical and thermal conductivity evolution under different temperature conditions, indicating its potential for photovoltaic and optoelectronic applications.
{"title":"Insights into Ag2Mo3SeO12 for photovoltaic and optoelectronic applications: A theoretical exploration of its structural, electronic, and thermoelectric behavior","authors":"N. Baaalla, H. Absike, F. Mezzat, E.K. Hlil, R. Masrour, A. Benyoussef, A. El Kenz","doi":"10.1016/j.mtchem.2024.102267","DOIUrl":"https://doi.org/10.1016/j.mtchem.2024.102267","url":null,"abstract":"The theoretical investigation of the newly discovered quadruple perovskite Ag₂Mo₃SeO was conducted using density functional theory (DFT) with the generalized gradient approximation (GGA-PBE) for the structural properties. This study examined the compound's structural, electronic, optical, and thermoelectric properties, utilizing the Tran Blaha modified Becke-Johnson exchange potential (mBJ) for accurate band gap measurement to overcome the bandgap underestimation by GGA-PBE. The stable structure was confirmed through energy-volume optimization and fitted with the Birch-Murnaghan equation of state, using PBE-GGA exchange correlation functional. The findings revealed a band structure with direct transition under the TB-mBJ approach with an energy gap of 1.45 eV. Detailed analyses were conducted, including the density of states and charge density distribution maps. Various optical parameters such as the dielectric function, absorption coefficient, refractive index, and reflectivity were computed, with the static dielectric constant measured at 6.3. Notably, a significant evolution of the absorption coefficient in the visible region highlights the potential of Ag₂Mo₃SeO₁₂ for solar cell and optoelectronic applications. These results pave the way for new photovoltaic material designs. Furthermore, the material demonstrates promising thermoelectric properties with an appropriate figure of merit, Seebeck coefficient, and electrical and thermal conductivity evolution under different temperature conditions, indicating its potential for photovoltaic and optoelectronic applications.","PeriodicalId":18353,"journal":{"name":"Materials Today Chemistry","volume":null,"pages":null},"PeriodicalIF":7.3,"publicationDate":"2024-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142204494","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 : 2024-08-28DOI: 10.1016/j.mtchem.2024.102240
Sara Alkhoori, Seba Alareeqi, Aasif A. Dabbawala, Georgios Siakavelas, Angeliki Latsiou, Dalaver H. Anjum, Messaoud Harfouche, Michalis A. Vasiliades, Steven J. Hinder, Mark A. Baker, Maryam Khaleel, Daniel Bahamon, Lourdes F. Vega, Maria A. Goula, Angelos M. Efstathiou, Kyriaki Polychronopoulou
The study presented herein examines the role of a series of alkaline earth metals (i.e. Mg, Ca, Sr, Ba) as promoters for Ni-supported zeolite beta catalysts to produce hydrocarbon fuels through hydrodeoxygenation (HDO) of palm oil. The properties of the catalytic systems were explored using XRD, HRTEM, N adsorption, H-TPR, CO-, NH-, and H-TPDs. The surface chemistry and coordination environment were analyzed using synchrotron XAFS and XPS. It is found that the chemical and structural composition of the support, as well as the use of alkaline earth promoters, significantly altered the interfacial charge distribution and consequently the electronic structure of the Ni-support interface and Ni surface sites. HDO of palm oil was conducted at 350 and 400 °C, at 30 bar; the highest conversion was attained over 10Ni/5Sr-Beta catalyst (44 %), which can be attributed to its features, such as low acidity (NH-TPD/DRIFTS), high Ni dispersion (H-TPD) and high amount of accessible Ni sites at reaction temperature (H-TPR). Product analysis, in general, demonstrated higher selectivity towards bio-gasoline (C–C) as a result of high acidity of zeolite beta (Si/Al = 12.5) that promoted cracking activity. While the effect of alkaline earth metal cation promoters was investigated experimentally, DFT was utilized to investigate the trend on the deoxygenation of palmitic acid (predominant component of palm oil) over Ni(111) surface. Results revealed that although the elongated COH bond lengths, adsorption energies, and enhanced charge transfer between the OH group and surface promoters can be linked to the periodicity of the adatom types, the thermodynamic –OH cleavage reaction energies well reflect the varying experimental deoxygenation performance of the Ni-promoted catalyst, ascribed to their varying C−O/promoter interactions subsequent to OH cleavage.
{"title":"Steering palm oil hydrodeoxygenation towards biofuel production: An experimental and theoretical approach to unveil periodic trends","authors":"Sara Alkhoori, Seba Alareeqi, Aasif A. Dabbawala, Georgios Siakavelas, Angeliki Latsiou, Dalaver H. Anjum, Messaoud Harfouche, Michalis A. Vasiliades, Steven J. Hinder, Mark A. Baker, Maryam Khaleel, Daniel Bahamon, Lourdes F. Vega, Maria A. Goula, Angelos M. Efstathiou, Kyriaki Polychronopoulou","doi":"10.1016/j.mtchem.2024.102240","DOIUrl":"https://doi.org/10.1016/j.mtchem.2024.102240","url":null,"abstract":"The study presented herein examines the role of a series of alkaline earth metals (i.e. Mg, Ca, Sr, Ba) as promoters for Ni-supported zeolite beta catalysts to produce hydrocarbon fuels through hydrodeoxygenation (HDO) of palm oil. The properties of the catalytic systems were explored using XRD, HRTEM, N adsorption, H-TPR, CO-, NH-, and H-TPDs. The surface chemistry and coordination environment were analyzed using synchrotron XAFS and XPS. It is found that the chemical and structural composition of the support, as well as the use of alkaline earth promoters, significantly altered the interfacial charge distribution and consequently the electronic structure of the Ni-support interface and Ni surface sites. HDO of palm oil was conducted at 350 and 400 °C, at 30 bar; the highest conversion was attained over 10Ni/5Sr-Beta catalyst (44 %), which can be attributed to its features, such as low acidity (NH-TPD/DRIFTS), high Ni dispersion (H-TPD) and high amount of accessible Ni sites at reaction temperature (H-TPR). Product analysis, in general, demonstrated higher selectivity towards bio-gasoline (C–C) as a result of high acidity of zeolite beta (Si/Al = 12.5) that promoted cracking activity. While the effect of alkaline earth metal cation promoters was investigated experimentally, DFT was utilized to investigate the trend on the deoxygenation of palmitic acid (predominant component of palm oil) over Ni(111) surface. Results revealed that although the elongated COH bond lengths, adsorption energies, and enhanced charge transfer between the OH group and surface promoters can be linked to the periodicity of the adatom types, the thermodynamic –OH cleavage reaction energies well reflect the varying experimental deoxygenation performance of the Ni-promoted catalyst, ascribed to their varying C−O/promoter interactions subsequent to OH cleavage.","PeriodicalId":18353,"journal":{"name":"Materials Today Chemistry","volume":null,"pages":null},"PeriodicalIF":7.3,"publicationDate":"2024-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142204496","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 : 2024-08-28DOI: 10.1016/j.mtchem.2024.102280
Xixi Cheng, Bobo Yang, Shiliang Mei, Wenfang Peng, Yuanyuan Wang, Changran Zheng, Yang Li, Rongrong Hu, Jiang Li, Jun Zou
Zero-dimensional (0D) organic-inorganic hybrid metal halides (OIHMHs) have received extensive attention due to their excellent photoelectric properties. Herein, a new 0D OIHMH single crystal, (CHN)SbCl, has been synthesized by slow antisolvent diffusion. In this crystal structure, CHN (CHN = Cetyldimethylbenzylammonium cations) cations separated SbCl to form a 0D square pyramid structure. (CHN)SbCl single crystals (SCs) manifest bright orange-yellow dual-emission bands at 472 and 616 nm, while having a high photoluminescent quantum yield of 97.5 %. The lifetime of high energy (HE) emission and low energy (LE) emission at room temperature is 9.73 ns and 4.61 μs, respectively. Based on lifetime differences and temperature-dependent spectra, the HE emission band is ascribed to singlet self-trapped excitons (STEs), while the LE emission band with a broad full width at half maxima of 136 nm can be attributed to triplet STEs. (CHN)SbCl appeared anti-thermal quenching behavior. In accordance with the luminescence characteristics of (CHN)SbCl, a warm white light-emitting diode device was fabricated with the correlated color temperature of 3410 K, the relevant color coordinate of (0.41, 0.39) and the color rendering index of 95.1, demonstrating (CHN)SbCl a promising phosphor for solid-state light-emitting application.
{"title":"A new zero-dimensional hybrid antimony halide of (C25H46N)2SbCl5 with dual-emission and high quantum-efficiency for light-emitting application","authors":"Xixi Cheng, Bobo Yang, Shiliang Mei, Wenfang Peng, Yuanyuan Wang, Changran Zheng, Yang Li, Rongrong Hu, Jiang Li, Jun Zou","doi":"10.1016/j.mtchem.2024.102280","DOIUrl":"https://doi.org/10.1016/j.mtchem.2024.102280","url":null,"abstract":"Zero-dimensional (0D) organic-inorganic hybrid metal halides (OIHMHs) have received extensive attention due to their excellent photoelectric properties. Herein, a new 0D OIHMH single crystal, (CHN)SbCl, has been synthesized by slow antisolvent diffusion. In this crystal structure, CHN (CHN = Cetyldimethylbenzylammonium cations) cations separated SbCl to form a 0D square pyramid structure. (CHN)SbCl single crystals (SCs) manifest bright orange-yellow dual-emission bands at 472 and 616 nm, while having a high photoluminescent quantum yield of 97.5 %. The lifetime of high energy (HE) emission and low energy (LE) emission at room temperature is 9.73 ns and 4.61 μs, respectively. Based on lifetime differences and temperature-dependent spectra, the HE emission band is ascribed to singlet self-trapped excitons (STEs), while the LE emission band with a broad full width at half maxima of 136 nm can be attributed to triplet STEs. (CHN)SbCl appeared anti-thermal quenching behavior. In accordance with the luminescence characteristics of (CHN)SbCl, a warm white light-emitting diode device was fabricated with the correlated color temperature of 3410 K, the relevant color coordinate of (0.41, 0.39) and the color rendering index of 95.1, demonstrating (CHN)SbCl a promising phosphor for solid-state light-emitting application.","PeriodicalId":18353,"journal":{"name":"Materials Today Chemistry","volume":null,"pages":null},"PeriodicalIF":7.3,"publicationDate":"2024-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142204473","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}
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