Shi-Ming Wang, Kai-Hua Wang, Lu Zhou, Tianyang Lu, Eunkyoung Kim, Zhengbo Han, Jun Liang Lin, Lin Liu, Guodong Li
{"title":"Room-Temperature Spin-Coatable Polyoxometalate Composites for High-Contrast, Large-Area Electrochromic Capacitive Films","authors":"Shi-Ming Wang, Kai-Hua Wang, Lu Zhou, Tianyang Lu, Eunkyoung Kim, Zhengbo Han, Jun Liang Lin, Lin Liu, Guodong Li","doi":"10.1039/d4ta06915c","DOIUrl":"https://doi.org/10.1039/d4ta06915c","url":null,"abstract":"Room-temperature spin-coatable polyoxometalate based composite is explored for low cost electrochromic capacitive film. Transparent stable K6P2W18O64 -polyvinyl alcohol (P2W18-PVA) solution was developed which suit for rigid and flexible substrates. The electrodeposited HKUST-1 particles were employed to create the pore structure in the film leading facile ion transportation. The excellent EC performance of P2W18 was fully expressed in this thin film with the thickness of 500 nm. The state-of-the-art record of 95% optical contrast and 1600 stable EC cycles are achieved. Electrochromic energy storage device with the capacity of 7.89 mF cm-2 was realized with MnO2 as counter electrode. This strategy for the preparation of highly stable and transparent POMs coating at room temperature is a general and simple solution that is not limited to the preparation of electrochromic films.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"6 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673726","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Ultra-Sensitive Covalent Organic Frameworks based Smoldering Sensor for Early Warning of Granary Fire","authors":"Yunlu Luan, Jing Zhan, Xiaojuan Ye, Xiaowei Mu","doi":"10.1039/d4ta06517d","DOIUrl":"https://doi.org/10.1039/d4ta06517d","url":null,"abstract":"The rice, as an important strategic material, is stored in the granary every year. Typically, the rice nearly fills the entire granary, making it difficult to detect smoldering in time. Once the smoldering of rice begins, it will be difficult to extinguish. To prevent granary fires, this paper analyzes the pyrolysis products of rice and proposes a novel granary smoldering early warning method based on the color reaction between furfural (the main product during rice smoldering) and aniline hydrochloride, and the excellent gas adsorption performance of three-dimensional covalent organic frameworks (COFs). A small-scale smoldering model of rice storage granary is built. The smoldering of rice in small-scale granary is detected successfully by the designed rice smoldering sensor (RSS). RSS shows good flexibility and ultra-sensitivity for rice smoldering. The minimum monitoring concentration of furfural produced during rice smoldering is 0.03 ug/mL. The early warning mechanism of RSS has also been revealed. This work provides a new method for early warning of grain fires.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"14 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142678460","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Recent Advances and Future Prospectives of Flexible and Wearable Applications Based on Liquid Metals Demands","authors":"Yifei Li, Sunwu Xu, Pengyu Zhu, Shuai Zhang, Yuntao Sun, Shuye Zhang, Peng He","doi":"10.1039/d4ta06879c","DOIUrl":"https://doi.org/10.1039/d4ta06879c","url":null,"abstract":"Liquid metals have garnered significant attention from researchers in recent years, which possess fascinating characteristics originating from their simultaneous metallic and liquid qualities. The great fluidity and conductivity make liquid metals promising for broad prospects in many fields, such as composites, aerospace, flexible electronics, biomedical devices. However, the study of liquid metals still not forming integrated research system nowadays, neglected by the wider research community. The question of “how to improve the basic performance of flexible electronic products and endow them with more unique functions” has emerged. In this review, we provide an overview of the processing methods for liquid metal based flexible devices, with a particular emphasis on various applications based on the conductivity, such as wearable sensors, controllable switches, flexible circuits, devices based on magnetic effect, joule heater, electromagnetic shielding devices. This work comprehensively introduces the application directions of liquid metals in conductivity and aims to offer innovation insights and inspiration for future research endeavors in liquid metal based flexible devices and systems.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"10 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673734","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ahmed N Mahfouz, Andrew Z Haddad, Jordan D Kocher, Akanksha K Menon
{"title":"Performance enhancement of aqueous ionic liquids with lower critical solution temperature (LCST) behavior through ternary mixtures","authors":"Ahmed N Mahfouz, Andrew Z Haddad, Jordan D Kocher, Akanksha K Menon","doi":"10.1039/d4ta07575g","DOIUrl":"https://doi.org/10.1039/d4ta07575g","url":null,"abstract":"Thermally responsive ionic liquids (ILs) exhibit liquid-liquid phase separation when mixed with water and heated above a lower critical solution temperature (LCST), resulting in a water-rich (WR) and an IL-rich (ILR) phase. These binary IL-water mixtures can be employed in a variety of thermodynamic processes such as forward osmosis (FO) desalination, for which two solution properties are desirable: low phase separation temperature and high osmotic strength (osmolality). However, these two properties are interlinked, with ILs that exhibit higher osmotic strengths typically requiring higher phase separation temperatures. This behavior tends to arise from the hydrophilicity of the IL cations, which enhances osmotic strength while also elevating the phase separation temperature. In this work, we highlight a pathway to overcome this tradeoff by developing ternary IL mixtures (two ILs with varying cation hydrophilicity mixed with water), which lowers the phase separation temperature while maintaining and even enhancing the osmotic strength of the solution. We characterize the mixing behavior (osmolality, phase separation temperature, WR phase purity, and WR to ILR phase mass ratio) of four ILs as a function of their concentration in solution. We find that an enhancement of up to 81.6% in the osmolality with a concomitant reduction of up to 15.4% in the phase separation temperature can be achieved using this approach. The ternary mixture is also shown to improve the phase separation kinetics by nearly 95% compared to the binary mixture. Overall, this work highlights a new pathway to improve the performance of LCST ILs for water and energy applications.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"15 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673763","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Heterointerface engineering in Cr2GaC/C hybrids through bottom-up template synthesis for enhanced electromagnetic wave absorption","authors":"Feiyue Hu, Shengyu Xie, Fushuo Wu, Jian Liu, Peigen Zhang, Jianxiang Ding, Bingbing Fan, Wei Zheng, Longzhu Cai, Zhengming Sun","doi":"10.1039/d4ta07294d","DOIUrl":"https://doi.org/10.1039/d4ta07294d","url":null,"abstract":"MAX phases are emerging as efficient electromagnetic wave absorption (EMA) materials, favored for their outstanding conductivity, high-temperature stability, and corrosion resistance. However, the limitations of a singular energy loss mechanism and the need for a high filler ratio hinder their further development. Herein, a template method utilizing absorbent cotton as a carbon source was employed to synthesize 0D/1D Cr2GaC/C hybrid materials. The bottom-up preparation strategy maintains the size of the Cr2GaC MAX-phase particles at ~200 nm while ensuring their uniform distribution within the carbon fibers. The abundant heterointerfaces between Cr2GaC and carbon enhanced interfacial polarization, while the carbon fiber network improved conduction loss. Consequently, the Cr2GaC/C hybrid exhibits excellent EMA properties, achieving a minimum reflection loss value of -59.0 dB at a thickness of only 1.56 mm and an ultra-low filler content of 15 wt.%. Additionally, its maximum radar cross section reduction value is 17.78 dB m², showing excellent stealth capability. This research provides new insights into the nanoscale synthesis of MAX phases and offers promising pathways for optimizing their EMA performance.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"63 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673786","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jie Wu, Anqi Huang, Wen Cao, Xuehui Gao, Zhongwei Chen
{"title":"Construction of Cobalt-doped Ni3S2@NiFe-LDH Heterojunction with Enhanced Local Electric Field for Efficient Oxygen Evolution Reaction","authors":"Jie Wu, Anqi Huang, Wen Cao, Xuehui Gao, Zhongwei Chen","doi":"10.1039/d4ta06830k","DOIUrl":"https://doi.org/10.1039/d4ta06830k","url":null,"abstract":"Alkaline oxygen evolution reaction (OER), involving a four-electron transfer process, is characterized by high overpotential and extremely sluggish reaction kinetics, posing a significant challenge for catalyst design. Herein, a strategy is proposed to modulate the electronic structure of electrocatalyst by constructing cobalt-doped Ni3S2@NiFe-LDH (Co-Ni3S2@NiFe-LDH) hierarchical hollow heterojunction with enhanced local electric fields (ELEF). The ELEF in the heterojunction induces band bending of the components, expediting electron transfer and accelerating OER kinetics. Furthermore, the hierarchical hollow structure offers a large specific surface area that ensures full exposure of adsorption and active sites. Benefiting from these synergetic advantages, Co-Ni3S2@NiFe-LDH shows remarkable performance and stability with low overpotential of only 217 mV at 50 mA cm-2. Density functional theory (DFT) calculations further confirms that the ELEF can optimize the adsorption energy of intermediate reaction species, reduce reaction energy barriers, and modulate the d-band center of active sites, thereby improving the inherent catalyst activity.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"197 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673723","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Structural Rule of Heteroatom-Modified Single-Atom Catalysts for CO2 Electroreduction Reaction","authors":"Xinyuan Sui, Haiyang Yuan, Yu Hou","doi":"10.1039/d4ta06604a","DOIUrl":"https://doi.org/10.1039/d4ta06604a","url":null,"abstract":"Carbon dioxide electroreduction reaction (CO2RR) has emerged as a viable strategy to address pressing energy and environmental challenges. Single-atom catalysts (SACs) are of particular interest for CO2RR due to their maximized atom utilization. The incorporation of heteroatoms as ligands is a common strategy to modify the geometric and electronic structures of metal centers to enhance performance. Here, we employed density functional theory study to investigate nitrogen-coordinated SACs with various heteroatom ligands, and elucidated the structural rule of SACs on CO2RR. The results show that the planar structural SACs exhibit relatively better stabilities than the raised ones, and their stabilities exhibit a volcano-shaped trend as a function of the ligand radius, with both excessively large and small radius compromising stability. Although the raised structural SACs have the better ability to activate CO2 for the tip effect, they also hinder the CO desorption and facilitate the H+ adsorption, leading to relatively poor CO2RR activity and selectivity (vs HER). In contrast, the planar-structured SACs generally show better activity and CO2RR selectivity, where promoting the CO2 activation/hydrogenation step is necessary. This work provides fundamental insights into the structure-dependence of SACs, and offers guidance for designing SACs for CO2RR or other reactions.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"14 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673724","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Dong Han Ha, Gichang Noh, Hakseong Kim, Dong Hwan Kim, Jeongho Kim, Suyong Jung, Chanyong Hwang, Ha Young Lee, Yong Ju Yun, Joon Young Kwak, Kibum Kang, Sam Nyung Yi
{"title":"Raman spectroscopy study of K-birnessite single crystals","authors":"Dong Han Ha, Gichang Noh, Hakseong Kim, Dong Hwan Kim, Jeongho Kim, Suyong Jung, Chanyong Hwang, Ha Young Lee, Yong Ju Yun, Joon Young Kwak, Kibum Kang, Sam Nyung Yi","doi":"10.1039/d4ta06118g","DOIUrl":"https://doi.org/10.1039/d4ta06118g","url":null,"abstract":"Raman studies of manganese dioxide (MnO<small><sub>2</sub></small>), a crucial material for sustainable and innovative solutions in energy storage and environmental remediation, have predominantly been conducted on fine-grained aggregates, leaving the identification of Raman peaks open to debate. To address this, in this study the Raman spectra of potassium (K)-birnessite single crystals with varying crystal thickness, temperature, and polarization configuration are measured. An acoustic phonon mode of birnessite is identified, which is found to be sensitive to both crystal thickness and interlayer spacing, with its frequency increasing by approximately 35% when the c-axis lattice parameter is reduced from 0.70 to 0.65 nm by the removal of interlayer water. In contrast, the dependence of the optical phonon modes on crystal thickness and interlayer spacing is not particularly noticeable. It is demonstrated that the characteristic Raman peak of K-birnessite, observed at approximately 559 cm<small><sup>–1</sup></small>, originates from a two-dimensional hexagonal configuration of cations and water molecules within the interlayer space, rather than from the MnO<small><sub>6</sub></small> octahedra. Additionally, the doubly degenerate vibrational mode of MnO<small><sub>6</sub></small> octahedra, corresponding to the motion of oxygen atoms in the basal plane, splits into two, confirming that the MnO6 octahedra are distorted by the Jahn–Teller effect.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"57 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673755","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Unveiling the performance of ultrathin bimetallic CoxNi1−x(OH)2 nanosheets for pseudocapacitors and oxygen evolution reaction","authors":"Pallavi Bhaktapralhad Jagdale, Sayali Ashok Patil, Arupjyoti Pathak, Mukaddar Sk, Ranjit Thapa, Amanda Sfeir, Sebastien Royer, Akshaya Kumar Samal, Manav Saxena","doi":"10.1039/d4ta06846g","DOIUrl":"https://doi.org/10.1039/d4ta06846g","url":null,"abstract":"The rational design of highly efficient and stable electrodes is necessary for energy storage and electrocatalysis. Herein, we developed a nanometre thin bimetallic ultrathin Co<small><sub><em>x</em></sub></small>Ni<small><sub>1−<em>x</em></sub></small>(OH)<small><sub>2</sub></small> nanosheet with a large lateral size by the ionic layer epitaxy (ILE) technique as an efficient bifunctional electrode material for pseudocapacitors and the oxygen evolution reaction. Its electrochemical performance was readily tuned by controlling the Co/Ni ratio. The nanosheet with a 1 : 3 Co : Ni ratio (termed Co<small><sub>1</sub></small>Ni<small><sub>3</sub></small>-NS) showed an excellent volumetric (areal) capacitance of 3783 F cm<small><sup>−3</sup></small> (3 mF cm<small><sup>−2</sup></small>) at 0.3 mA cm<small><sup>−2</sup></small> with 336 mW h cm<small><sup>−3</sup></small> energy density at 256 W cm<small><sup>−3</sup></small> power density and excellent stability, substantially outperforming other monometallic and bimetallic NSs. Moreover, as an electrocatalyst, Co<small><sub>1</sub></small>Ni<small><sub>3</sub></small>-NS delivered a lower overpotential (<em>η</em><small><sub>10</sub></small> = 318 mV) and Tafel slope (61 mV dec<small><sup>−1</sup></small>) in an alkaline environment. <em>In situ</em> Raman spectroscopy was employed to demonstrate the dynamic structural evolution of the catalyst during the OER process. Furthermore, DFT investigations further revealed that Co<small><sub>1</sub></small>Ni<small><sub>3</sub></small>-NS is a promising electrode with higher quantum capacitance and lower overpotential compared to other Co/Ni ratios. These findings pave a new way for controlled synthesis of highly efficient, bimetallic, and bifunctional electrode materials for pseudocapacitors and the OER.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"232 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142670777","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Exploring the Photoactive Properties of Promising MXenes for Water Splitting","authors":"Diego Ontiveros, Francesc Viñes, Carmen Sousa","doi":"10.1039/d4ta06852a","DOIUrl":"https://doi.org/10.1039/d4ta06852a","url":null,"abstract":"The photoactive properties and effectiveness of a selected group of ten terminated MXenes —Sc<small><sub>2</sub></small>CT<small><sub>2</sub></small>, Y<small><sub>2</sub></small>CT<small><sub>2</sub></small> (T = Cl, Br, S, and Se), Y<small><sub>2</sub></small>CI<small><sub>2</sub></small> and Zr<small><sub>2</sub></small>CO<small><sub>2</sub></small>— has been deeply studied by means of density functional theory (DFT). Here it is demonstrated that the studied MXenes exhibit robust energetic and dynamical stability, having all an indirect bandgap, while most of them with values within the visible spectrum, and also exhibiting suitable band alignment for the water splitting reaction. The charge density distribution of the valence band maximum (VBM) and conduction band minimum (CBM) is found to be separated across different layers with low overlaps, below 30%. Most MXenes present high charge carrier mobilities with favourable electron-hole disparities, with Sc<small><sub>2</sub></small>CBr<small><sub>2</sub></small> also presenting directional charge carrier transport. Additionally, these materials show strong optical absorption (~105 cm<small><sup>–1</sup></small>) in the visible spectrum, translating to promising solar-to-hydrogen (STH) efficiency theoretical limits, up to 23%. Overall, the combination of all these features positions MXenes among the optimal materials for efficient photocatalytic water splitting.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"25 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142670779","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}