Journal of Materials Chemistry A最新文献

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Electrocatalysts work better in lean-electrolyte lithium‒sulfur batteries 电催化剂在贫电解质锂硫电池中效果更佳
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2024-07-13 DOI: 10.1039/d4ta01997k
Jia-Jia Zhao, Zi-Xian Chen, Qian Cheng, Meng Zhao, Xinzhi Ma, Xue-Qiang Zhang, Jia-Qi Huang, Bo-Quan Li
{"title":"Electrocatalysts work better in lean-electrolyte lithium‒sulfur batteries","authors":"Jia-Jia Zhao, Zi-Xian Chen, Qian Cheng, Meng Zhao, Xinzhi Ma, Xue-Qiang Zhang, Jia-Qi Huang, Bo-Quan Li","doi":"10.1039/d4ta01997k","DOIUrl":"https://doi.org/10.1039/d4ta01997k","url":null,"abstract":"Reducing electrolyte usage constitutes the prerequisite to construct high-energy-density lithium‒sulfur (Li‒S) batteries. However, the cathode kinetics is severely blocked under lean-electrolyte conditions. Electrocatalysts have been widely employed to boost the cathode kinetics, yet their effectiveness under lean-electrolyte conditions remains unclear. Herein, the cathode kinetics promotion effectiveness of electrocatalysts is systematically evaluated in lean-electrolyte Li‒S batteries. The kinetics promotion effects on both liquid‒liquid and liquid‒solid conversions are more prominent at higher sulfur concentrations using the titanium nitride (TiN) electrocatalyst. Similarly, discharge capacity increment and cell polarization decrease afforded by the TiN electrocatalyst are more significant in lean-electrolyte Li‒S batteries than the flooded-electrolyte ones. Polarization decoupling analysis further identifies activation polarization as the main challenge under lean-electrolyte conditions, which can be effectively overcome by the TiN electrocatalyst. Moreover, the energy density of 2 Ah Li–S pouch cells increases by 19% using TiN electrocatalyst. This work elucidates electrocatalysts are more effective in lean-electrolyte Li–S batteries and highlights advanced electrocatalyst design for high-energy-density Li–S batteries.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-07-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141602672","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
F-coordinated Single-atom Ru Species: Efficient and Durable Catalysts for Photo-Thermal Synergistic Catalytic CO2 Hydrogenation to Methane F 配位单原子 Ru 物种:光热协同催化 CO2 加氢制甲烷的高效持久催化剂
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2024-07-13 DOI: 10.1039/d4ta02984d
Yunxiang Tang, Hao Wang, Chan Guo, Lige Wang, Tingting Zhao, Zhengyi Yang, Shikang Xiao, Jiurong Liu, Yanyan Jiang, Yufei Zhao, Xiaodong Wen, Fenglong Wang
{"title":"F-coordinated Single-atom Ru Species: Efficient and Durable Catalysts for Photo-Thermal Synergistic Catalytic CO2 Hydrogenation to Methane","authors":"Yunxiang Tang, Hao Wang, Chan Guo, Lige Wang, Tingting Zhao, Zhengyi Yang, Shikang Xiao, Jiurong Liu, Yanyan Jiang, Yufei Zhao, Xiaodong Wen, Fenglong Wang","doi":"10.1039/d4ta02984d","DOIUrl":"https://doi.org/10.1039/d4ta02984d","url":null,"abstract":"Elucidating the correlation between coordination structures and catalytic performances of single-atom active site is imperative for the precise design of highly efficient catalysts; however, the feasible regulation of coordination environment in single-atom catalysts presents a formidable challenge. Herein, we fabricate single-atom Ru-based catalysts with Ru-F4 and Ru-O4 configurations (named as Ru-F4 SAs/PA and Ru-O4 SAs/PA, respectively), showcasing fine-tuning of the coordination structure of Ru sites can significantly enhance performances for CO2 hydrogenation to methane under mild conditions in a photo-thermal synergistic catalytic process. Comparative studies reveal that Ru-F4 SAs/PA outperformed Ru-O4 SAs/PA counterparts, giving a superior CO2 methanation performances with CH4 production rate of 47.4 mmol gcat−1 h−1 and CH4 selectivity of 93.8% at 200 ℃ in the presence of light irradiation (200-1100 nm, 1.9 W cm−2) under atmospheric pressure. Theoretical investigations unravel that the transition from Ru-O4 to Ru-F4 coordination environments optimizes the electronic states, thereby enhancing the adsorption of reactants and intermediates. Moreover, the optimized electronic structure promotes the production and transformation of key intermediate species, lowers the energy barrier for CO2 conversion, and thus elevates the catalytic activity. This comprehensive study not only clarifies the relationship between the coordination structures of active sites and catalytic performance at atomic-level but also offers a novel paradigm for the design of efficient CO2 conversion catalysts.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-07-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141602671","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
Ferrocene-modified polymer-SWCNT composite films for high-performance flexible thermoelectric generators 用于高性能柔性热电发电机的二茂铁改性聚合物-SWCNT 复合薄膜
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2024-07-13 DOI: 10.1039/d4ta02037e
Zelin Sun, Zhifeng Ma, Xuan Zhou, Yanzhao Wang, Jie Zhang, Wai-Yeung Raymond Wong
{"title":"Ferrocene-modified polymer-SWCNT composite films for high-performance flexible thermoelectric generators","authors":"Zelin Sun, Zhifeng Ma, Xuan Zhou, Yanzhao Wang, Jie Zhang, Wai-Yeung Raymond Wong","doi":"10.1039/d4ta02037e","DOIUrl":"https://doi.org/10.1039/d4ta02037e","url":null,"abstract":"In this study, we explore a new design strategy for enhancing the thermoelectric performance of composites between poly(Fc-CPT)-based metallopolymers (Fc-P1, Fc-P2, and Fc-P3) and single-walled carbon nanotubes (SWCNTs) by modifying CPT-based polymer backbones with pendant redox ferrocene groups and thiophene functional groups. After optimizing the conditions, all three one-dimensional (1D) conjugated metallopolymers exhibit excellent thermoelectric performance by interacting well with SWCNT. The study provides insights into polymer-SWCNT composites through morphological analysis and theoretical calculations. The flexible OTEG incorporating Fc-P3-SWCNT composites achieves an impressive output power of 1.18 μW at T is 72 K, underscoring the potential of these materials in advancing organic thermoelectric technologies. These findings are expected to stimulate further interest and research in high-performance OTE materials.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-07-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141602677","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
Template-Directed In-situ Grown Bimetallic Nanoarchitectures with Hydroxide Active Sites Enriched Multi-Charge Transfer Routes for Energy Storage 具有氢氧化物活性位点的模板导向原位生长双金属纳米结构丰富了用于储能的多电荷转移途径
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2024-07-13 DOI: 10.1039/d4ta03412k
Dennyson Savariraj Antonysamy, Thondaiman Pugalenthiyar, Periyasamy Sivakumar, Manikandan Ramu, John D Rodney, Byung Chul Kim, Hyun Jung
{"title":"Template-Directed In-situ Grown Bimetallic Nanoarchitectures with Hydroxide Active Sites Enriched Multi-Charge Transfer Routes for Energy Storage","authors":"Dennyson Savariraj Antonysamy, Thondaiman Pugalenthiyar, Periyasamy Sivakumar, Manikandan Ramu, John D Rodney, Byung Chul Kim, Hyun Jung","doi":"10.1039/d4ta03412k","DOIUrl":"https://doi.org/10.1039/d4ta03412k","url":null,"abstract":"Cobalt metal-organic frameworks were used as templates to obtain densely stacked two-dimensional ultrathin nanosheets of nickel/cobalt metal-organic frameworks on carbon cloth via in situ deposition at room temperature. The freestanding electrodes made of ultra-thin nanosheets and quasi-one-dimensional pores exhibited a unique electronic structure with Ni(OH)2 anchoring to the surface. With the distinctive structural superiority, multiple charge transfer routes, and Ni(OH)2 entities as active sites, the electrode showcased a towering areal capacity (Ca) of 2041 mC cm-2 (2 mA cm-2), a specific capacity of (Cs) 671 C g-1 and a volumetric capacitance (Cvc) of 1033 F cm-3 (2 A g-1) and a prolonged cycling life of 5000 cycles with an appreciable capacity retention of 91.5% in 6 M KOH. The asymmetric supercapacitor device assembled (CC/CoNi-MOF@Ni(OH)2//CC/O,N,S@AC) delivered a thumping specific capacity (Cs) of 284 C g-1, a specific capacitance (Csp) of 189 F g-1, a volumetric capacitance (Cvc) of 128 F cm-3, a maximum specific energy (Es) of 75.0 W h kg-1, an excellent specific power (Ps) of 17.13 kW kg-1, and withstood 10,000 charge/discharge cycles with a decline of 11.3% in the initial capacity. The proposed method with DFT analysis underpins a strategy to custom-design economically viable freestanding electrodes with a large surface area per volume/mass, synergy effect at the interface, and multiple charge transfer pathways for potential application in energy storage. KEYWORDS: Organic frameworks, multiple charge transfer, freestanding electrode, large surface area, synergy effect.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-07-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141602684","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
Efficient and Stable Inorganic Perovskite Solar Cells Enabled by Lead Silicate Glass Layer 利用硅酸铅玻璃层实现高效、稳定的无机过氧化物太阳能电池
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2024-07-12 DOI: 10.1039/d4ta04018j
Wanpeng Yang, Haixuan Yu, Zhiguo Zhang, Haodan Shi, Yong Hu, Junyi Huang, Zhirong Liu, Yan Shen, Mingkui Wang
{"title":"Efficient and Stable Inorganic Perovskite Solar Cells Enabled by Lead Silicate Glass Layer","authors":"Wanpeng Yang, Haixuan Yu, Zhiguo Zhang, Haodan Shi, Yong Hu, Junyi Huang, Zhirong Liu, Yan Shen, Mingkui Wang","doi":"10.1039/d4ta04018j","DOIUrl":"https://doi.org/10.1039/d4ta04018j","url":null,"abstract":"Inorganic cesium lead triiodide perovskite (CsPbI3) exhibits remarkable potential in photovoltaic application due to its exemplary thermal stability. However, CsPbI3 is extremely sensitive to moisture which hinders its practical application in stable and high-efficiency photovoltaic devices. Here we show an effective method to enhance water resistance of CsPbI3 via an ultrathin hydrophobic lead silicate (PbSiO3) glass layer. The resulted CsPbI3 inorganic perovskite solar cells achieved a remarkably efficiency of 20.59% under standard test condition. More importantly, the unencapsulated devices possess outstanding moisture resilience which maintain about 92% of their initial efficiency even after being stored under 25±5% relative humidity (RH) for 600 hours.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141602810","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
Impact of intermolecular packing on separation of chlorinated cyclic hydrocarbons by flexible hydrogen-bonded organic frameworks 分子间填料对柔性氢键有机框架分离氯化环烃的影响
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2024-07-12 DOI: 10.1039/d4ta03910f
Peng Chong Xue, Siwen Hu, He Zhao, Meng Liang, Rui Wang, Jingjun Hao
{"title":"Impact of intermolecular packing on separation of chlorinated cyclic hydrocarbons by flexible hydrogen-bonded organic frameworks","authors":"Peng Chong Xue, Siwen Hu, He Zhao, Meng Liang, Rui Wang, Jingjun Hao","doi":"10.1039/d4ta03910f","DOIUrl":"https://doi.org/10.1039/d4ta03910f","url":null,"abstract":"The nonplanar phenothiazine derivative (PTTCN) was synthesized to construct adsorption hydrogen-bonded organic frameworks for separation of chlorinated cyclic hydrocarbons, chlorobenzene (ClBz) and chlorocyclohexane (ClCy). PTTCN can form two distinct organic frameworks in ClBz and ClCy through intermolecular hydrogen bonding. These frameworks exhibit different fluorescence colors, which can be attributed to variations in molecular conformations and packing patterns. Upon heating, both frameworks are capable of releasing the guests; however, their separation performances towards the ClBz/ClCy mixture differ significantly. Specifically, X-HOF-6a derived from ClBz selectively reabsorbs ClBz from the equimolar mixture accompanying with a gate-opening process and asmall change in intermolecular arrangement, resulting in a purity of 99.4%. Moreover, X-HOF-6a demonstrates excellent reusability. On the other hand, the intermolecular stacking type in X-HOF-7a derived from ClCy is very different from those in X-HOF-a and X-HOF-7, and then X-HOF-7a exhibits non-selective adsorption by capturing both ClCy and ClBz molecules simultaneously. The investigations suggest that selectivity is determined by the extent of alteration in intermolecular stacking upon guest adsorption, with higher selectivity observed for smaller changes.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141602757","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
Conjugated microporous polytriphenylamine as high-performance anion-capture electrode for hybrid capacitive deionization with ultrahigh areal adsorption capacity 共轭微孔聚三苯胺作为高性能阴离子捕获电极,用于具有超高吸附容量的混合电容式去离子法
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2024-07-12 DOI: 10.1039/d4ta04010d
Weiqing Kong, Xiaoyuan Lu, Xu Ge, Qingao Zhang, Xiaoyu Jin, Meng Zhang, Yuan-Yuan Feng
{"title":"Conjugated microporous polytriphenylamine as high-performance anion-capture electrode for hybrid capacitive deionization with ultrahigh areal adsorption capacity","authors":"Weiqing Kong, Xiaoyuan Lu, Xu Ge, Qingao Zhang, Xiaoyu Jin, Meng Zhang, Yuan-Yuan Feng","doi":"10.1039/d4ta04010d","DOIUrl":"https://doi.org/10.1039/d4ta04010d","url":null,"abstract":"Conducting polymers with good electron conductivity and rich redox functional groups have attracted enormous attention as anode material for capacitive deionization (CDI) towards the relief of global freshwater scarcity. However, because of their intrinsically poor porosity and severe particle aggregation natures, previously used conducting polymers for CDI desalination have suffered from the disadvantage of rather low specific surface areas (&lt;50 m<small><sup>2</sup></small>g<small><sup>−1</sup></small>), sluggish ion diffusion kinetics, limited desalination capacities, and low mass loadings (~1 mg cm<small><sup>−2</sup></small>) on electrodes. Herein, we synthesized an amino group-rich conjugated microporous polytriphenylamine (m-PTPA) and demonstrated for the first time its great potential as a high-performance anion-capture electrode material in CDI applications. m-PTPA possesses reversible redox property, predominant &lt;2 nm microporous characteristics, and ultrahigh specific surface area (506 m<small><sup>2</sup></small>g<small><sup>−1</sup></small>), which ensured the fast ion transport within interconnected porous network, and maximized the exposure of electrochemical active sites to saline solution. Owing these novel features, the m-PTPA-based CDI device, with m-PTPA as anode at a high mass loading of 8.7 mg cm<small><sup>−2</sup></small>and activated carbon as cathode, exhibited high gravimetric/areal/volumetric-normalized salt adsorption capacities (47.21 mg g<small><sup>−1</sup></small>, 0.41 mg cm<small><sup>−2</sup></small>, 10.92 mg cm<small><sup>−3</sup></small>), fast adsorption rate (2.83 mg g<small><sup>−1</sup></small>min<small><sup>−1</sup></small>), low energy consumption, and excellent cycling stability. Besides, we also evaluated the competitive adsorption of some common anions existing in water, and probed the mechanism for Cl<small><sup>−</sup></small>adsorption on m-PTPA. We believe that this work paves a new way for the usage of conjugated microporous polymers as a new kind of CDI electrode materials.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141602699","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
In-depth understanding of the electrochemical energy storage efficiency between a series of new 3d-4d mixed metal polyoxometalates: Experimental and Theoretical Investigations 深入了解一系列新型 3d-4d 混合金属多氧甲基盐的电化学储能效率:实验与理论研究
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2024-07-12 DOI: 10.1039/d4ta03188a
Kalyankumar S. Morla, Dewendra Thakre, Tushar B. Deshmukh, Sunanda Malo, Subuhan Ahamed, R. K. Aparna, Subham Sahoo, Debajit Sarma, Kartik Chandra Mondal, Babasaheb R. Sankapal, Abhishek Banerjee
{"title":"In-depth understanding of the electrochemical energy storage efficiency between a series of new 3d-4d mixed metal polyoxometalates: Experimental and Theoretical Investigations","authors":"Kalyankumar S. Morla, Dewendra Thakre, Tushar B. Deshmukh, Sunanda Malo, Subuhan Ahamed, R. K. Aparna, Subham Sahoo, Debajit Sarma, Kartik Chandra Mondal, Babasaheb R. Sankapal, Abhishek Banerjee","doi":"10.1039/d4ta03188a","DOIUrl":"https://doi.org/10.1039/d4ta03188a","url":null,"abstract":"Transition-metal complexes, with their reversible redox properties, are the basis for electrochemical energy storage devices, such as rechargeable batteries and supercapacitors. In order to comprehend the variation in the electronic properties and electrochemical activity of concurrent transition elements existing in identical coordination environments, we have pursued extensive multi-method spectroscopic and electrochemical studies of three new isostructural 3d-4d mixed metal polyoxometalate complexes, viz. the vanado-molybdate Na2(NH4)5[(MoVI2O5)2(VIIIO2){O3PC(O)(CH2-4-C5NH4)PO32]•10H2O (1a), the chromo-molybdate (NH4)5[H2(MoVI2O5)2(CrIIIO2){O3P-C(O)(CH2-4-C5H4N)-PO3}2]•10H2O (2a) and the mangano-molybdate Na(NH4)6[H(MoVI2O5)2(MnIIIO2){O3P-C(O)(CH2-4-C5H4N)-PO3}2]•9H2O (3a). The structure of the polyanions have been determined using single-crystal X-ray diffraction studies, with all three polyanionic complexes having identical connectivity and arrangement in the solid-state. The electronic properties of the complexes have been analyzed thoroughly with electronic paramagnetic resonance (EPR) and X-ray photoelectronic spectroscopic (XPS) methods. EPR measurements for all three complexes are characterized by Δms = ±2 signals (forbidden half-field transition) at 77 K in solid state, confirming the existence of V(III), S = 1 for 1a; Cr(III), S = 3/2 for 2a; Mn(III), S = 2 for 3a. Using our original and novel binder-free approach to prepare supercapacitor electrodes, thorough comparative electrochemical energy storage studies have been performed on the three compounds using cyclic voltammetry, galvanostatic charge-discharge, electrochemical impedance spectroscopy, and cyclic stability tests. The oxo-vanado-molybdate complex has shown superior electrochemical performance, with respect to specific capacitances, energy density, power density, and electrochemical stability, followed by the oxo-chromo-molybdate and the oxo-mangano-molybdate complexes. The electrochemical performance trend has been corroborated from DFT calculations at B3LYP-D3(BJ)/Def2-SVP level of theory in a polar medium, with the same order of promptness of undergoing oxidation of the polyanionic species [M2+ to M3+; M = V (1') &gt; Cr (2') &gt; Mn (3'); ΔG(M3+-M2+) = +48 (1'), +58 (2'), +81 (3') kcal/mol], corroborating with experimental observations. The oxidation of these anionic species from 8- (MII) to 7- (MIII) has thus been computed to be highly favourable in the gas phase [~ -328 (1'), -311 (2'), -309 (3') kcal/mol]. The studies on the HOMO-LUMO structures of the complexes also corroborate the trend of the electrochemical behavior.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141602673","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-Assisted 3D Printing of Thermoelectric Materials of Ultrahigh Performances at Room Temperature 机器学习辅助三维打印室温下的超高性能热电材料
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2024-07-12 DOI: 10.1039/d4ta03062a
Kaidong Song, Guoyue Xu, ANM Tanvir, Ke Wang, Md Omarsany Bappy, Haijiang Yang, Wenjie Shang, Le Zhou, Alexander William Dowling, Tengfei Luo, Yanliang Zhang
{"title":"Machine Learning-Assisted 3D Printing of Thermoelectric Materials of Ultrahigh Performances at Room Temperature","authors":"Kaidong Song, Guoyue Xu, ANM Tanvir, Ke Wang, Md Omarsany Bappy, Haijiang Yang, Wenjie Shang, Le Zhou, Alexander William Dowling, Tengfei Luo, Yanliang Zhang","doi":"10.1039/d4ta03062a","DOIUrl":"https://doi.org/10.1039/d4ta03062a","url":null,"abstract":"Thermoelectric energy conversion is an attractive technology for generating electricity from waste heat and using electricity for solid-state cooling. However, conventional manufacturing processes for thermoelectric devices are costly and limited to simple device geometries. This work reports an extrusion printing method to fabricate high-performance thermoelectric materials with complex 3D architectures. By integrating high-throughput experimentation and Bayesian optimization (BO), our approach significantly accelerates the simultaneous search for the optimal ink formulation and printing parameters that deliver high thermoelectric performances while maintaining desired shape fidelity. A Gaussian process regression (GPR)-based machine learning model is employed to expeditiously predict thermoelectric power factor as a function of ink formulation and printing parameters. The printed bismuth antimony telluride (BiSbTe)-based thermoelectric materials under the optimized conditions exhibit an ultrahigh room temperature zT of 1.3, which is by far the highest in the printed thermoelectric materials. The machine learning-guided ink-based printing strategy can be highly generalizable to a wide range of functional materials and devices for broad technological applications.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141602758","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
Enhanced Photoelectrochemical Nitrogen Reduction to Ammonia by a Plasmon-Active Au Grating Decorated with gC3N4@MoS2 Heterosystem and Plasmon-Active Nanoparticles 用 gC3N4@MoS2 异源系统和等离子体活性纳米粒子装饰的等离子体活性金光栅增强氮还原成氨的光电化学作用
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2024-07-11 DOI: 10.1039/d4ta03350g
Denis Zabelin, Anastasiia Tulupova, Anna Zabelina, Andrea Tosovska, Rashid Valiev, Ruslan Ramazanov, David Mareš, Vitezslav Jerabek, Vasilii Burtsev, Mariia Erzina, Alena Michalcova, Anastasiia Skvortsova, Václav Švorčík, Oleksiy Lyutakov
{"title":"Enhanced Photoelectrochemical Nitrogen Reduction to Ammonia by a Plasmon-Active Au Grating Decorated with gC3N4@MoS2 Heterosystem and Plasmon-Active Nanoparticles","authors":"Denis Zabelin, Anastasiia Tulupova, Anna Zabelina, Andrea Tosovska, Rashid Valiev, Ruslan Ramazanov, David Mareš, Vitezslav Jerabek, Vasilii Burtsev, Mariia Erzina, Alena Michalcova, Anastasiia Skvortsova, Václav Švorčík, Oleksiy Lyutakov","doi":"10.1039/d4ta03350g","DOIUrl":"https://doi.org/10.1039/d4ta03350g","url":null,"abstract":"The electrochemical production of ammonia from nitrogen (so-called nitrogen reduction reaction - NRR) is one of the key tasks of modern electrochemistry. The use of photo-electrochemical approaches in NRR allows the involvement of renewable sunlight energy and partially reduces process energy demands and increases its efficiency. For efficient photoelectrochemical NRR realization, a rational design of the photoelectrode used is required. In this work, we propose the design, creation, and optimization of a hybrid electrode, based on utilization of coupled 2D semiconductors and plasmonic hot spots. In our approach the gC3N4@MoS2 semiconductors (in the form of 2D flakes), with high catalytic activity towards NRR are used as a redox-active material. For the involvement of the sunlight energy, the plasmon triggering is used in two modes: simple plasmonic triggering using a periodic Au grating and coupled plasmon triggering through the sandwiching of 2D gC3N4@MoS2 flakes between the Au grating and different plasmon active nanoparticles (gold and silver nanoparticles with different shapes). We also carried out a series of calculations (including finite difference time domain estimation of plasmon energy distribution and density functional calculation) aimed at the estimation of the local value of plasmon energy and the NRR process under conditions of plasmon triggering. As a result of careful design and the photoelectrode optimization, we were able to achieve 882.1 mg h-1 mg-1cat ammonia yield and 22.1 % Faradic efficiency. The proposed photoelectrode design makes it possible to effectively use both the catalytic properties of the coupled semiconductors and the strengths of the plasmon-assisted triggering.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-07-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141584556","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}
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