Journal of Materials Chemistry A最新文献

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Vertical Macroporous Chitosan Aerogel Adsorbents for Simple and Efficient Enhancement of Atmospheric Water Harvesting and Air Dehumidification 立式大孔壳聚糖气凝胶吸附剂用于简单高效地提高大气集水和空气除湿能力
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2024-11-12 DOI: 10.1039/d4ta07005d
Zhiguang Guo, Changhui Fu, Yuxuan He, Anhui Yu, Guangyi Tian, Danyan Zhan, Huimin Zhang
{"title":"Vertical Macroporous Chitosan Aerogel Adsorbents for Simple and Efficient Enhancement of Atmospheric Water Harvesting and Air Dehumidification","authors":"Zhiguang Guo, Changhui Fu, Yuxuan He, Anhui Yu, Guangyi Tian, Danyan Zhan, Huimin Zhang","doi":"10.1039/d4ta07005d","DOIUrl":"https://doi.org/10.1039/d4ta07005d","url":null,"abstract":"Adsorption-based atmospheric water harvesting (SAWH) has become one of the effective methods to extract water from the air in arid regions due to its high efficiency and low energy consumption. Hygroscopic salts have high water absorption rates but their disadvantages such as easy leakage and slow kinetics limit their further application. Most of the reported aerogel porous materials loaded with hygroscopic salts can effectively solve the leakage problem, but the disordered pores limit the water vapour transport. It is therefore necessary to develop a simple method to further improve the adsorption kinetics and increase the rate of water vapour adsorption. In this paper, a low-cost, green, and high water absorption LCSC-MC aerogel adsorbent is reported. The composite adsorbent is based on biomass chitosan and photoresponsive material nanocarbon as the aerogel skeleton structure, and the introduction of lithium chloride enables it to obtain excellent water-absorption performance. In addition, inspired by the pump effect of wood in nature, we constructed a large number of vertical macroporous channel structures on the hygroscopic aerogel by a simple needle array template. Benefiting from the vertical macroporous channel structure, the diffusion resistance of water vapour in the aerogel is reduced, resulting in more efficient and faster water absorption. The water absorption rates of LCSC-MC after 12 h of moisture absorption at 20% RH and 90% RH are as high as 0.75 g g-1 and 3.85 g g-1, respectively. In addition, LCSC-MC has excellent air dehumidification performance, reducing humidity from 75% RH to less than 30% RH in 50 minutes, which is superior to commercial desiccants such as silica gel, calcium chloride and 4A molecular sieve. Meanwhile, our prepared LCSC-MC showed good cyclic stability in both long-term atmospheric water collection and air passive dehumidification practical applications. Moreover, we further improved the water adsorption efficiency of the aerogel adsorbent with a simple strategy, which is expected to be extended on other aerogel adsorbents.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"72 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142600071","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}
引用次数: 0
Pre-lithiation carbon anodes mitigating potassium loss toward for high-performance potassium-ion energy storage devices 用于高性能钾离子储能设备的预硫化碳阳极可减少钾损耗
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2024-11-12 DOI: 10.1039/d4ta06451h
Danni Du, Qingyuan Liu, Jing Gao, Yuying Qin, Xiaobo Jiang, Yuanchang Shi, Minghao Hua, Xiaohang Lin, Zhiwei Zhang, Chengxiang Wang, Long-Wei Yin, Rutao Wang
{"title":"Pre-lithiation carbon anodes mitigating potassium loss toward for high-performance potassium-ion energy storage devices","authors":"Danni Du, Qingyuan Liu, Jing Gao, Yuying Qin, Xiaobo Jiang, Yuanchang Shi, Minghao Hua, Xiaohang Lin, Zhiwei Zhang, Chengxiang Wang, Long-Wei Yin, Rutao Wang","doi":"10.1039/d4ta06451h","DOIUrl":"https://doi.org/10.1039/d4ta06451h","url":null,"abstract":"Pre-potassiation technologies with the functions of providing additional potassium sources and/or mitigating potassium loss during cycling, make them capable of enhancing the energy density and cycling life of potassium-ion capacitors (PICs) and potassium-ion batteries (PIBs). However, many reported pre-potassiation strategies involve using high chemical reactivity potassium sources such as metallic potassium or K-containing additives, thereby increasing cost and risk in production. Herein, we propose a novel potassium-ion compensation strategy to fulfil the demand for high-performance potassium-ion full cells without using any high chemical reactivity potassium sources. This strategy is based on the foundation of that the pre-lithiation carbon anode with the preformed solid-electrolyte-interphase (SEI) layer can effectively mitigate potassium loss and not hinder the K+ diffusion from electrolyte to electrode during cell operation. PICs based on pre-lithiation carbon anodes including soft carbon, hard carbon, and graphite, show better capacitive performance than which based on pre-potassiation carbon counterparts. This versatile strategy is also applicable for high-performance PIBs. We believe that this design principle of implanting the mature pre-lithiation technologies into potassium-ion energy storage systems possesses far-reaching potential of resolving the scientific bottleneck of the immature pre-potassium technologies.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"32 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142600070","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}
引用次数: 0
Scalable Synthesis of N–Doped Graphene–Oxide–Supported FeCo(OH)x Nanosheets for Efficient Co–Doped Fe3O4 Nanoparticle-Based Oxygen Reduction Reaction Electrocatalysis 可扩展地合成 N 掺杂氧化石墨烯支撑的 FeCo(OH)x 纳米片,用于基于共掺 Fe3O4 纳米粒子的高效氧还原反应电催化
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2024-11-12 DOI: 10.1039/d4ta06684g
Sunglun Kwon, Jong Hyeon Lee
{"title":"Scalable Synthesis of N–Doped Graphene–Oxide–Supported FeCo(OH)x Nanosheets for Efficient Co–Doped Fe3O4 Nanoparticle-Based Oxygen Reduction Reaction Electrocatalysis","authors":"Sunglun Kwon, Jong Hyeon Lee","doi":"10.1039/d4ta06684g","DOIUrl":"https://doi.org/10.1039/d4ta06684g","url":null,"abstract":"Developing efficient and cost-effective materials is crucial for advancing electrochemical oxygen reduction reaction (ORR). This study presents a synthesis route for high-performance spinel Fe and Co oxide nanoparticles on N-doped reduced graphene oxide (NRGO). This solvothermal synthesis in formamide yields well-dispersed, ultrafine FeCo(OH)x nanoparticles (∼5 nm) anchored on NRGO. These nanoparticles can be employed for the formation of spinel FexCo3-xO4 oxide nanoparticles, potentially because of their high surface area and intense interaction with the NRGO support. By introducing Co2+ ions into formamide, our method prevents rapid Fe2+ oxidation to Fe3+, promoting the formation of well-defined Fe3O4 nanoparticles, not Fe2O3. This, in turn, facilitates the successful decoration of highly dispersed spinel FexCo3-xO4 oxide nanoparticles (∼30 nm) onto the NRGO support, even after calcination at 900°C, which represents the critical temperature for conventional graphitization. This unique approach results in significantly reduced particle aggregation compared with that of conventional methods. The (Co)Fe3O4–NRGO nanocomposite exhibits remarkable ORR activity, achieving an electron number of ∼3.7 and a current density of 5.01 mA·cm−2 at E = 0.75 VRHE, comparable to those of commercial Pt/C catalysts. Furthermore, the catalyst exhibits remarkable stability, maintaining a reducing current density that is 42% lower after 40,000 s of uninterrupted operation at 0.75 VRHE compared with a 75% reduction observed with Pt/C. This exceptional performance is attributed to the strong interaction between the (Co)Fe3O4 nanoparticles and NRGO, facilitated by the Co ion precursor during annealing.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"15 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142600080","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}
引用次数: 0
Machine learning aided design of high performance copper-based sulfide photocathodes 机器学习辅助设计高性能硫化铜光电阴极
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2024-11-12 DOI: 10.1039/d4ta06128d
Yuxi Cao, Kaijie Shen, Yuanfei Li, Fumei Lan, Zeyu Guo, Kelu Zhang, Kang Wang, Feng Jiang
{"title":"Machine learning aided design of high performance copper-based sulfide photocathodes","authors":"Yuxi Cao, Kaijie Shen, Yuanfei Li, Fumei Lan, Zeyu Guo, Kelu Zhang, Kang Wang, Feng Jiang","doi":"10.1039/d4ta06128d","DOIUrl":"https://doi.org/10.1039/d4ta06128d","url":null,"abstract":"Copper-based sulfide photocathodes have shown impressive performance in solar water splitting applications due to their narrow bandgaps, high absorption coefficients, and good carrier transport properties. Several factors, such as composition, thickness, and doping, have a direct influence on the onset potential, photocurrent density, and solar-to-hydrogen efficiency. Screening for the optimal combination in the presence of multiple variables is undoubtedly a challenging task. However, constructing a comprehensive database, developing photocathode models, and utilizing machine learning to derive the best results clearly save a significant amount of experimental effort. This approach efficiently reduces the experimental workload, streamlines the process, and expedites the development of high-performance materials for photoelectrochemical water splitting applications. Here, we introduce a comprehensive machine learning process to guide the preparation of copper-based sulfide photocathodes. The random forest model was selected to train and capture the complex relationship between different layers of copper-based sulfide photocathodes and electrolytes to predict unstudied conditions, and the accuracy of the test set reached 96.7%. Through SHAP interpretability analysis, we provide heuristic rules to deepen the understanding of the influence of different factors on the performance of the catalytic system. We also developed a prediction platform to share our prediction models.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"15 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142600075","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}
引用次数: 0
PEO/cysteine composite nanofiber-based triboelectric nanogenerator for tiny mechanical energy harvesting 基于 PEO/半胱氨酸复合纳米纤维的微型机械能采集三电纳米发电机
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2024-11-12 DOI: 10.1039/d4ta06845a
Yijun Hao, Jia Yang, Xiaopeng Zhu, Keke Hong, Jiayu Su, Yong Qin, Wei Su, Hongke Zhang, Chuguo Zhang, Xiuhan Li
{"title":"PEO/cysteine composite nanofiber-based triboelectric nanogenerator for tiny mechanical energy harvesting","authors":"Yijun Hao, Jia Yang, Xiaopeng Zhu, Keke Hong, Jiayu Su, Yong Qin, Wei Su, Hongke Zhang, Chuguo Zhang, Xiuhan Li","doi":"10.1039/d4ta06845a","DOIUrl":"https://doi.org/10.1039/d4ta06845a","url":null,"abstract":"Triboelectric nanogenerator (TENG) has acted as a promising method for capturing mechanical energy. However, traditional polymer triboelectric materials result burden to environment, the natural/biodegradable tribo-materials have the disadvantages of poor output performance. For this purpose, we proposed a polyethylene oxide (PEO) /cysteine composite nanofiber film (PCF) which prepared from biodegradable polymer PEO and natural cysteine. Thanks to the superior tribo-positive properties of PEO and cysteine, the electrical performance of PCF-based TENG (PC-TENG) with 4 wt% cysteine is several times than that of pure PEO nanofiber film. In addition, PC-TENG obtain better power density (6.6 W/m2), which is 3-110 times more than that of studies using related eco-friendly materials as tribo-layer. Importantly, we designed multi-layer funnel-shaped TENG (MF-TENG) which constructed by 4 layers of PC-TENG, which can effectively harvest a variety of tiny mechanical energy to built self-powered electronics devices by integrating the power management circuit. This research offers an efficient approach for the practical application of natural and environmental-friendly material-based TENGs in energy harvesting and power supply in Internet of Things.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"34 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142600081","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}
引用次数: 0
Enhancing the Thermoelectric Figure of Merit of BiN via Polymorphism, Pressure, and Nanostructuring 通过多态性、压力和纳米结构增强 BiN 的热电特性
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2024-11-11 DOI: 10.1039/d4ta05891g
Elena R. Remesal, Victor Posligua, Miguel Mahillo-Paniagua, Konstantin Glazyrin, Javier Fernández Sanz, Antonio Márquez, Jose Javier Plata Ramos
{"title":"Enhancing the Thermoelectric Figure of Merit of BiN via Polymorphism, Pressure, and Nanostructuring","authors":"Elena R. Remesal, Victor Posligua, Miguel Mahillo-Paniagua, Konstantin Glazyrin, Javier Fernández Sanz, Antonio Márquez, Jose Javier Plata Ramos","doi":"10.1039/d4ta05891g","DOIUrl":"https://doi.org/10.1039/d4ta05891g","url":null,"abstract":"Materials discovery extends beyond the synthesis of new compounds. Detailed characterization is essential to understand the potential applications of novel materials. However, experimental characterization can be challenging due to the vast chemical and physical spaces, as well as the specific conditions required for certain techniques. Computational high-throughput methods can overcome these challenges. In this work, the transport and thermoelectric properties of the recently synthesized BiN are explored, including the effects of temperature, pressure, carrier concentration, polymorphism and polycrystalline grain size. We find that the band structure is strongly dependent on pressure and the polymorph studied. Both polymorphs exhibit low thermal conductivity at 0 GPa, which rapidly increases when pressure is applied. Electronic transport properties can be finely tuned based on the effects of pressure and polymorph type on the band gap, carrier mobilities, and presence of secondary pockets. The thermoelectric figure of merit can reach values around 0.85 for both p- and n-type BiN if the power factor and lattice thermal conductivity are optimized at 600 K, making this material competitive with other well-known thermoelectric families, such as Bi<small><sub>2</sub></small>Te<small><sub>3</sub></small> or PbX, in the low-to-medium temperature range.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"95 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601598","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}
引用次数: 0
Unlocking recent progress in niobium and vanadium carbide-based MXenes for sodium-ion batteries 揭示钠离子电池用碳化铌和碳化钒基 MXenes 的最新进展
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2024-11-11 DOI: 10.1039/d4ta05669h
K. Karuppasamy, Ganesh Kumar Veerasubramani, Vishwanath Hiremath, Dhanasekaran Vikraman, Palanisamy Santhoshkumar, Georgios N. Karanikolos, Ali Abdulkareem Alhammadi, Hyun-Seok Kim, Akram Alfantazi
{"title":"Unlocking recent progress in niobium and vanadium carbide-based MXenes for sodium-ion batteries","authors":"K. Karuppasamy, Ganesh Kumar Veerasubramani, Vishwanath Hiremath, Dhanasekaran Vikraman, Palanisamy Santhoshkumar, Georgios N. Karanikolos, Ali Abdulkareem Alhammadi, Hyun-Seok Kim, Akram Alfantazi","doi":"10.1039/d4ta05669h","DOIUrl":"https://doi.org/10.1039/d4ta05669h","url":null,"abstract":"The performance of electrochemical energy storage (EES) devices is determined by the inherent characteristics of electrode materials such as anodes and cathodes. 2D materials are increasingly being studied for their unique structural and electrochemical properties. Various materials, including transition metal oxides, metal sulfides, phosphides, and metal-organic framework (MOF) compounds, have been explored as potential anodes for sodium storage. However, challenges include significant volume and conductivity changes, cyclability, low capacity, and hindered overall rate performance in sodium-ion batteries (SIBs). Employing 2D-layered transition metal carbides and nitrides (MXenes) and their functionalized/surface-modified composites provides a promising strategy for minimizing volume expansion during charge-discharge, mass-transport properties, and enhancing conductivity, thereby improving the specific capacity, rate capability, and cycling stability of SIBs. This review examines the ability of two specific MXene compounds, namely niobium carbide (Nb-C) and vanadium carbide (VC), to be advanced electrode materials for enhancing the performance of SIBs. Furthermore, it comprehensively analyses recent developments in SIB anodes based on Nb-C and VC hybrid materials, shedding light on their electrochemical and structural properties. Last, the crucial challenges of Nb-C and VC electrodes employed in SIBs are explained, and future insights into the SIB application of these electrodes are elaborated.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"127 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142598379","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}
引用次数: 0
A robust and adhesive anti-swelling hydrophobic ionogel with prolonged stability for strain and temperature sensors 用于应变和温度传感器的具有长期稳定性的坚固粘合型抗膨胀疏水离子凝胶
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2024-11-11 DOI: 10.1039/d4ta06181k
Yu Zhang, Yuanna Sun, Jiahang Yang, Ruobing Tian, Jiahao Liu, Xueming Tang, junbo wang, Qingshan Li
{"title":"A robust and adhesive anti-swelling hydrophobic ionogel with prolonged stability for strain and temperature sensors","authors":"Yu Zhang, Yuanna Sun, Jiahang Yang, Ruobing Tian, Jiahao Liu, Xueming Tang, junbo wang, Qingshan Li","doi":"10.1039/d4ta06181k","DOIUrl":"https://doi.org/10.1039/d4ta06181k","url":null,"abstract":"With the growing attention brought by wearable electronic devices, flexible sensors, as a fundamental component, are emerging as the focal point. However, achieving long-term stability and precise sensing underwater remain two significant challenges that urgently need to be addressed for sensors. In this study, we designed a hydrophobic ionogel (MCS) with good stretchability (720%), excellent wet adhesion, prolonged stability and anti-swelling capability. These remarkable advantages make ionogels stand out as strain sensors. The ionogels exhibit extraordinary signal sensing abilities. In specific, they can capture subtle physiological activities of the human body with precision and sensitivity both in air or underwater. Besides, the satisfactory thermosensitivity (-2.02%/ºC), high resolution (0.1 ºC) and fast response (14 s) ensure that the ionogel becomes a qualified temperature sensor. By integrating with a wireless Bluetooth transmission system, the real-time body temperature can be monitored by a smart cellphone. This work demonstrates great potential of MCS ionogel in marine exploitation and wearable health monitoring.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"153 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142598383","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}
引用次数: 0
Structural and thermodynamic properties of the Li6PS5Cl solid electrolyte using first-principles calculations 利用第一原理计算 Li6PS5Cl 固体电解质的结构和热力学性质
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2024-11-11 DOI: 10.1039/d4ta05159a
Tarek Ayadi, Maylise Nastar, Fabien Bruneval
{"title":"Structural and thermodynamic properties of the Li6PS5Cl solid electrolyte using first-principles calculations","authors":"Tarek Ayadi, Maylise Nastar, Fabien Bruneval","doi":"10.1039/d4ta05159a","DOIUrl":"https://doi.org/10.1039/d4ta05159a","url":null,"abstract":"We perform static and dynamic ab initio simulations to investigate the structural and the thermodynamic properties of Li6PS5Cl, a solid electrolyte actively considered for solid-state batteries. Our simulations account for the disorder in the structure where the Li atoms can rotate either around sulfur or chlorine atoms. Li6PS5Cl presents a non-uniform distribution of Li ions around S and Cl atoms, which tends to become more homogeneous at higher temperature. This specific short-range order of Li has a significant impact on the stability of Li6PS5Cl. Comparing with recent X-Ray and neutron diffraction studies, we confirm one Li crystallographic site position (Li1) and amend the coordinates of a second one (Li2). We then address the calculation of the heat capacity Cp with a combination of ab initio trajectories and a so-called temperature remapping approximation. Indeed, the standard quasi-harmonic approximation is not able to capture the complex energy landscape experienced by the mobile lithium atoms. To the best of our knowledge, there exists no experimental or theoretical Cp value for Li6PS5Cl in the literature, despite the importance of this thermodynamic quantity. Finally we use this more reliable Cp to investigate the thermodynamic stability of Li6PS5Cl against the decomposition reaction leading to Li2S, Li3PS4 and LiCl. We show that Li6PS5Cl is stable above 700 K, which is consistent with the high synthesis temperatures.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"38 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601597","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}
引用次数: 0
Size-dependent electrocatalytic hydrogen evolution activity of arrays of edge-like defects in MoS2 crystals patterned by focused ion beam 聚焦离子束图案化的 MoS2 晶体边缘缺陷阵列的电催化氢气进化活性与尺寸有关
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2024-11-11 DOI: 10.1039/d4ta05885b
Cláudia de Lourenço, Ana Beatriz Sorana de Araujo, Leonardo Hideki Hasimoto, Isaque A.A. Feitosa, Matheus Felipe Fagundes das Neves, Jefferson Bettini, Tarcísio Micheli Perfecto, Tulio C. R. Rocha, Thiago J.A. Mori, Edson R. Leite, Murilo Santhiago
{"title":"Size-dependent electrocatalytic hydrogen evolution activity of arrays of edge-like defects in MoS2 crystals patterned by focused ion beam","authors":"Cláudia de Lourenço, Ana Beatriz Sorana de Araujo, Leonardo Hideki Hasimoto, Isaque A.A. Feitosa, Matheus Felipe Fagundes das Neves, Jefferson Bettini, Tarcísio Micheli Perfecto, Tulio C. R. Rocha, Thiago J.A. Mori, Edson R. Leite, Murilo Santhiago","doi":"10.1039/d4ta05885b","DOIUrl":"https://doi.org/10.1039/d4ta05885b","url":null,"abstract":"Introducing surface defects on molybdenum disulfide (MoS<small><sub>2</sub></small>) crystals plays a crucial role in enhancing the electrocatalytic activity toward the hydrogen evolution reaction (HER). Despite the remarkable progress in this area, the precise control of the size, distance, and defective areas with minimal surface contamination remains unachieved. Conventional microfabrication methods often leave organic residues on the surface that impair electrocatalytic activity and hinder interface elucidation by advanced characterization tools. In this study, we pattern for the first-time arrays of pillars in nanometer-thick MoS<small><sub>2</sub></small> flakes using a focused ion beam to enhance HER activity. We observe size-dependent stability of the edge-like defects under HER conditions with defective areas. The pillars undergo chemical and structural changes post-patterning due to an amorphization process, unambiguously confirmed by atomic force microscopy, Raman spectroscopy, and synchrotron X-ray photoelectron spectroscopy. Furthermore, the amorphization process is more pronounced in specific in-plane directions, as confirmed by transmission electron microscopy. The electrocatalytic activity of the pillars was measured using a recently reported fabrication method, allowing us to unequivocally correlate defects with HER activity. Microelectrodes with less pillars, i.e. less catalytic sites, demonstrate a lower overpotential of 349 mV at 10 mA cm-2 showcasing a groundbreaking advancement in their fabrication.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"12 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601596","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}
引用次数: 0
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