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The Analysis of Electron Densities: From Basics to Emergent Applications 电子密度分析:从基础知识到新兴应用
IF 62.1 1区 化学
Chemical Reviews Pub Date : 2024-11-15 DOI: 10.1021/acs.chemrev.4c00297
Daniel Koch, Michele Pavanello, Xuecheng Shao, Manabu Ihara, Paul W. Ayers, Chérif F. Matta, Samantha Jenkins, Sergei Manzhos
{"title":"The Analysis of Electron Densities: From Basics to Emergent Applications","authors":"Daniel Koch, Michele Pavanello, Xuecheng Shao, Manabu Ihara, Paul W. Ayers, Chérif F. Matta, Samantha Jenkins, Sergei Manzhos","doi":"10.1021/acs.chemrev.4c00297","DOIUrl":"https://doi.org/10.1021/acs.chemrev.4c00297","url":null,"abstract":"The electron density determines all properties of a system of nuclei and electrons. It is both computable and observable. Its topology allows gaining insight into the mechanisms of bonding and other phenomena in a way that is complementary to and beyond that available from the molecular orbital picture and the formal oxidation state (FOS) formalism. The ability to derive mechanistic insight from electron density is also important with methods where orbitals are not available, such as orbital-free density functional theory (OF-DFT). While density topology-based analyses such as QTAIM (quantum theory of atoms-in-molecules) have been widely used, novel, vector-based techniques recently emerged such as next-generation (NG) QTAIM. Density-dependent quantities are also actively used in machine learning (ML)-based methods, in particular, for ML DFT functional development, including machine-learnt kinetic energy functionals. We review QTAIM and its recent extensions such as NG-QTAIM and localization-delocalization matrices (LDM) and their uses in the analysis of bonding, conformations, mechanisms of redox reactions excitations, as well as ultrafast phenomena. We review recent research showing that direct density analysis can circumvent certain pitfalls of the FOS formalism, in particular in the description of anionic redox, and of the widely used (spherically) projected density of states analysis. We discuss uses of density-based quantities for the construction of DFT functionals and prospects of applications of analyses of density topology to get mechanistic insight with OF-DFT and recently developed time-dependent OF-DFT.","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"10 1","pages":""},"PeriodicalIF":62.1,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142637820","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Noncanonical Amino Acid Incorporation in Animals and Animal Cells. 动物和动物细胞中的非顺式氨基酸结合
IF 51.4 1区 化学
Chemical Reviews Pub Date : 2024-11-14 DOI: 10.1021/acs.chemrev.3c00955
Joo-Chan Kim, YouJin Kim, Suho Cho, Hee-Sung Park
{"title":"Noncanonical Amino Acid Incorporation in Animals and Animal Cells.","authors":"Joo-Chan Kim, YouJin Kim, Suho Cho, Hee-Sung Park","doi":"10.1021/acs.chemrev.3c00955","DOIUrl":"https://doi.org/10.1021/acs.chemrev.3c00955","url":null,"abstract":"<p><p>Noncanonical amino acids (ncAAs) are synthetic building blocks that, when incorporated into proteins, confer novel functions and enable precise control over biological processes. These small yet powerful tools offer unprecedented opportunities to investigate and manipulate various complex life forms. In particular, ncAA incorporation technology has garnered significant attention in the study of animals and their constituent cells, which serve as invaluable model organisms for gaining insights into human physiology, genetics, and diseases. This review will provide a comprehensive discussion on the applications of ncAA incorporation technology in animals and animal cells, covering past achievements, current developments, and future perspectives.</p>","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":" ","pages":""},"PeriodicalIF":51.4,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142612700","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Asymmetric Orbital Hybridization at MXene-VO2-x Interface Stabilizes Oxygen Vacancies for Enhanced Reversibility in Aqueous Zinc-ion Battery MXene-VO2-x 界面的不对称轨道杂化可稳定氧空位,从而提高锌离子水电池的可逆性
IF 32.5 1区 化学
Chemical Reviews Pub Date : 2024-11-14 DOI: 10.1039/d4ee04466e
Yuan Fang, Chunhong Qi, Weichao Bao, Fangfang Xu, Wei Sun, Bin Liu, Xiqian Yu, Wan Jiang, Peng Peng Qiu, Lianjun Wang, Wei Luo
{"title":"Asymmetric Orbital Hybridization at MXene-VO2-x Interface Stabilizes Oxygen Vacancies for Enhanced Reversibility in Aqueous Zinc-ion Battery","authors":"Yuan Fang, Chunhong Qi, Weichao Bao, Fangfang Xu, Wei Sun, Bin Liu, Xiqian Yu, Wan Jiang, Peng Peng Qiu, Lianjun Wang, Wei Luo","doi":"10.1039/d4ee04466e","DOIUrl":"https://doi.org/10.1039/d4ee04466e","url":null,"abstract":"Modulating the storage kinetics of Zn2+ through oxygen vacancy (Ov) manipulation represents a promising approach for developing cathode materials in aqueous rechargeable zinc-ion batteries (ZIBs). However, recent studies have shown that these Ov can undergo migration and refilling during electrochemical cycling, leading to severe structural degradation and rapid capacity fading. Therefore, developing technologies to stabilize Ov is critical for maximizing their efficiency, although it presents a significant challenge. Herein, we demonstrate a covalent heterostructure design that pushes the cycling performance of a vanadium dioxide (VO2) cathode to an unprecedented level. The rational lies in the chemical growth of VO2 nanowall arrays on MXene nanosheets to form Ti-O-V asymmetric orbital hybridization (AOH) at the interface, which remarkably enhances the stability of Ov on VO2. Due to this advanced cathode design, the prepared ZIBs exhibit highly reversible aqueous Zn2+ storage capacities and maintain a robust structure over 30,000 cycles at 20 A g-1, without any significant capacity loss (1.4 %). Detailed experimental and theoretical analysis indicate that the Ti-O-V AOH facilitates a charge transfer pathway at the interface, allowing electrons to migrate from VO2 to MXene surface, thereby stabilizing the Ov both thermodynamically and kinetically. Our work offers an inspiring design principle for developing sustainable cathode materials for high-performance aqueous ZIBs and beyond, leveraging the synergistic effects of Ov and interfacial orbital engineering.","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"11 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609920","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Scalable electrified cementitious materials production and recycling 可扩展的电气化胶凝材料生产和回收利用
IF 32.5 1区 化学
Chemical Reviews Pub Date : 2024-11-13 DOI: 10.1039/d4ee03529a
Xiao Kun Lu, Wenxin Zhang, Brianna N. Ruggiero, Linsey C. Seitz, Jiaqi Li
{"title":"Scalable electrified cementitious materials production and recycling","authors":"Xiao Kun Lu, Wenxin Zhang, Brianna N. Ruggiero, Linsey C. Seitz, Jiaqi Li","doi":"10.1039/d4ee03529a","DOIUrl":"https://doi.org/10.1039/d4ee03529a","url":null,"abstract":"The production of Portland cement, the industry-standard cement, contributes ∼8% of global CO<small><sub>2</sub></small> emissions through fossil-fuel heating and decomposition of limestone (the primary cement raw material). Decarbonization, <em>e.g.</em>, <em>via</em> direct electrification, of this 200-year-old liming routine is extremely challenging at the industry scale. We propose a scalable electrochemical decarbonization approach to circumvent the limestone use by switching to carbon-free calcium silicates from abundant minerals and recycled concrete. Water electrolysis produces protons and hydroxides to drive a pH gradient that accelerates Ca<small><sup>2+</sup></small> ion leaching from calcium silicates and captures atmospheric CO<small><sub>2</sub></small> to form carbon-negative CaCO<small><sub>3</sub></small>, which serves as the feedstock for cement manufacturing or as the carbon-mineralized product for cement substitution with permanent carbon storage. Value-added co-products amorphous silica and green H<small><sub>2</sub></small> further enhance cement performance and supplant fossil fuels for net-zero transition, respectively. The products readily meet present-day regulatory standards and demands, and the approach readily synergizes with business-as-usual cement manufacturing and concrete construction, which are important for upscaling and structural safety, promising ready reception by the public and industries. Blended Portland cement produced through our approach with carbon-negative CaCO<small><sub>3</sub></small> and silica demonstrates enhanced resilience and achieves carbon neutrality or negativity when incorporating storage or circulation of CO<small><sub>2</sub></small> from cement plant flue gas, respectively. This low-cost, electrochemical cement production approach using abundant ubiquitous raw materials enables electrification, transition to clean fuel, and decarbonization at a gigaton scale.","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"14 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601559","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
High triboelectrification and charge collection efficiency of direct current triboelectric nanogenerator achieved by tri-synergistic enhancement strategy 通过三协同增强策略实现直流三电纳米发电机的高三电化和电荷收集效率
IF 32.5 1区 化学
Chemical Reviews Pub Date : 2024-11-13 DOI: 10.1039/d4ee03784g
Shuyan Xu, Jian Wang, Chuncai Shan, Kaixian Li, Huiyuan Wu, Gui Li, Shaoke Fu, Qionghua Zhao, Yi Xi, Chenguo Hu
{"title":"High triboelectrification and charge collection efficiency of direct current triboelectric nanogenerator achieved by tri-synergistic enhancement strategy","authors":"Shuyan Xu, Jian Wang, Chuncai Shan, Kaixian Li, Huiyuan Wu, Gui Li, Shaoke Fu, Qionghua Zhao, Yi Xi, Chenguo Hu","doi":"10.1039/d4ee03784g","DOIUrl":"https://doi.org/10.1039/d4ee03784g","url":null,"abstract":"Direct current triboelectric nanogenerator (DC-TENG) utilized air-breakdown effect to collect triboelectrification charges from dielectric tribo-layers, providing a new type of mechanical energy harvesting mode for TENGs, which has demonstrated its high efficiency in energy conversion process. However, boosting the output performance based on structure designs and material modifications still meets great challenges. Herein, we propose a ternary dual-DC-TENG (TDD-TENG) with a triple synergistic enhancement mechanism. The strategies include the space optimization using multiple-unit structure on slider by seamlessly arranging PTFE/PA/electrode to realize maximized space utilization, ternary dielectric material selection by adopting PTFE, PA and PU foam as the tribo-layers with the spontaneously introduced PTFE powder on PU foam to achieve a higher triboelectrification effect and surface lubrication, and bottom electrode design to collect charges unreached by charge collection electrodes (CCEs) on slider forming a dual-DC output. Consequently, TDD-TENG achieves the average power density of 18.37 W m-2, which is the highest in sliding mode DC-TENGs. In addition, the output charge density of rotary TDD-TENG reaches 7.3 mC m-2 at an ultra-low speed of 5 rpm. This work provides a new method to improve output power from structure design and material modification for DC-TENGs.","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"157 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601560","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Multifunctional zeolite film enables stable high-voltage operation of LiCoO2 cathode 多功能沸石薄膜实现了钴酸锂阴极的稳定高压运行
IF 32.5 1区 化学
Chemical Reviews Pub Date : 2024-11-13 DOI: 10.1039/d4ee04370g
Zezhou Lin, Yiran Ying, Zhihang Xu, Gao Chen, Xi Gong, Zehua Wang, Daqin Guan, Leqi Zhao, Mingyang Yang, Ke Fan, Tiancheng Liu, Hao LI, Honglei Zhang, Huangxu Li, Xi Zhang, Ye Zhu, Zhou-Guang Lu, Zongping Shao, Peiyu Hou, Haitao Huang
{"title":"Multifunctional zeolite film enables stable high-voltage operation of LiCoO2 cathode","authors":"Zezhou Lin, Yiran Ying, Zhihang Xu, Gao Chen, Xi Gong, Zehua Wang, Daqin Guan, Leqi Zhao, Mingyang Yang, Ke Fan, Tiancheng Liu, Hao LI, Honglei Zhang, Huangxu Li, Xi Zhang, Ye Zhu, Zhou-Guang Lu, Zongping Shao, Peiyu Hou, Haitao Huang","doi":"10.1039/d4ee04370g","DOIUrl":"https://doi.org/10.1039/d4ee04370g","url":null,"abstract":"Increasing upper cut-off voltage is a useful way for enhancing specific capacity of LiCoO<small><sub>2</sub></small> (LCO) cathode and the energy density of corresponding lithium-ion batteries (LIBs), while the main challenge is concurrent phase transition associated with oxygen evolution reaction that results in quick decay in electrochemical performance. Here, we report a significant improvement in both capacity and durability at high voltage by simply growing an AlPO<small><sub>4</sub></small>-5 zeolite protecting layer over LCO, with good crystallinity, ordered porous channels and full surface coverage. Such coating, realized by using triethylamine as a template, acts multifunctionally to remarkably alleviative phase transition via suppressing the oxygen release at high voltage, enable fast Li<small><sup>+</sup></small> diffusion through its nanoporous structure, accelerate the Li<small><sup>+</sup></small>-desolvation on the cathode/electrolyte interface, and boost the redox kinetics, as supported by various in-situ and ex-situ measurements of LCO@AlPO<small><sub>4</sub></small>-5 zeolite (LCO@Z) cathode under a high cut-off voltage of 4.6 V (vs. Li/Li<small><sup>+</sup></small>) and density functional theory (DFT) calculations. As a result, the surface engineered LCO@Z electrode exhibits outstanding cycling stability (capacity retention of 90.3% after 200 cycles) and high-rate capability (108.2 mAh g<small><sup>-1</sup></small> at 10C). Such zeolite coating strategy provides a new way for developing high-energy-density LIBs with great application potential.","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"6 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601557","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Efficient Fully Textured Perovskite Silicon Tandems with Thermally Evaporated Hole Transporting Materials 采用热蒸发空穴传输材料的高效全纹理包晶硅串联系统
IF 32.5 1区 化学
Chemical Reviews Pub Date : 2024-11-13 DOI: 10.1039/d4ee03899a
Bhushan Kore, Oussama Er-raji, Oliver Fischer, Adrian Callies, Oliver Schultz-Wittmann, Patricia Samia Cerian Schulze, Martin Bivour, Stefaan De Wolf, Stefan W Glunz, Juliane Borchert
{"title":"Efficient Fully Textured Perovskite Silicon Tandems with Thermally Evaporated Hole Transporting Materials","authors":"Bhushan Kore, Oussama Er-raji, Oliver Fischer, Adrian Callies, Oliver Schultz-Wittmann, Patricia Samia Cerian Schulze, Martin Bivour, Stefaan De Wolf, Stefan W Glunz, Juliane Borchert","doi":"10.1039/d4ee03899a","DOIUrl":"https://doi.org/10.1039/d4ee03899a","url":null,"abstract":"Fully textured perovskite silicon tandem solar cells effectively minimize the reflection losses and are compatible with industrial silicon production lines. To facilitate scalability and industrial deployment of perovskite silicon tandems all functional layers including perovskite need to be deposited with scalable techniques. Currently, self-assembling molecules (SAM), polymeric and low-molecular-weight organic semiconductors, are widely used as hole transport layers (HTLs) in p-i-n structured perovskite solar cells. Usually, SAMs are deposited via spin coating method, but use of this method could be challenging on large area textured silicon substrates, leading to inhomogeneous SAM layers and lossy HTL/perovskite interfaces. To address this issue, we have investigated thermal evaporation of SAMs (2PACz and Me-4PACz) and some other HTLs like TaTm and Spiro-TTB. We examined the effect of varying HTL thickness on the device performance and showed that the thickness of the thermally evaporated HTLs significantly affects the open circuit voltage (VOC) and fill factor (FF) of the solar cells. Furthermore, using ultraviolet photoemission spectroscopy and Suns-VOC measurements we correlate the changes observed in the VOC and FF with HTL thickness variations to the changes in the energy band positions (loss in the hole selectivity) and effective resistance losses, respectively. With the optimized HTL thickness we obtained ~30% efficiency on 1 cm2 area and ~26% on 4 cm2 area tandem devices.","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"19 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601558","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A self-adsorption molecule passivated interface enables efficient and stable lithium metal batteries 自吸附分子钝化界面可实现高效稳定的锂金属电池
IF 32.5 1区 化学
Chemical Reviews Pub Date : 2024-11-13 DOI: 10.1039/d4ee02903h
Gongxun Lu, Xinru Wu, Miaofei Huang, Mengtian Zhang, Zhihong Piao, Xiongwei Zhong, Chuang Li, Yanze Song, Chengshuai Chang, Kuang Yu, Guangmin Zhou
{"title":"A self-adsorption molecule passivated interface enables efficient and stable lithium metal batteries","authors":"Gongxun Lu, Xinru Wu, Miaofei Huang, Mengtian Zhang, Zhihong Piao, Xiongwei Zhong, Chuang Li, Yanze Song, Chengshuai Chang, Kuang Yu, Guangmin Zhou","doi":"10.1039/d4ee02903h","DOIUrl":"https://doi.org/10.1039/d4ee02903h","url":null,"abstract":"Despite the theoretical promise of attaining high energy densities, practical applications of lithium metal batteries (LMBs) remain hindered by the inadequacies of the electrode/electrolyte interface and unsatisfied cycling stability. Herein, a self-adsorption molecule with polar groups was designed and introduced in ether electrolyte, aiming to form a high-density and ordered molecular layer occupying active sites on the electrode surface, while restricting electrolyte molecule penetration into the interface. This self-adsorption molecule favors the formation of a robust anion-rich cathode/anode electrolyte interphase due to the change of the interfacial solvation structure, thus inhibiting solvent decomposition and enhancing interfacial stability. Consequently, the addition of this molecule into low-concentration ether electrolytes notably upgrades the electrochemical performance of the LiNi<small><sub>0.8</sub></small>Co<small><sub>0.1</sub></small>Mn<small><sub>0.1</sub></small>O<small><sub>2</sub></small> (NCM811)||Li battery, which enables a high capacity retention of 87.2% after 250 cycles at 4.5 V. Moreover, the NMC811||Li pouch cells achieve stable cycling over 150 cycles with a capacity retention of 92.9% at a low negative/positive capacity ratio of 2.7 with a lean electrolyte. This interface passivation design strategy provides a promising path toward high-energy, durable, and safe rechargeable LMBs.","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"1 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601562","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Advancing high-temperature electrostatic energy storage via linker engineering of metal–organic frameworks in polymer nanocomposites 通过聚合物纳米复合材料中金属有机框架的链接工程推进高温静电储能
IF 32.5 1区 化学
Chemical Reviews Pub Date : 2024-11-12 DOI: 10.1039/d4ee04085f
Zongliang Xie, Zhiyuan Huang, He Li, Tianlei Xu, Haoyu Zhao, Yunfei Wang, Pang Xi, Zhiqiang Cao, Virginia Altoe, Liana M Klivansky, Zaiyu Wang, Steven Shelton, Shiqi Lai, Peng Liu, Chenhui Zhu, Michael D. Connolly, Corie Y. Ralston, Xiaodan Gu, Zongren Peng, Jian Zhang, Yi Liu
{"title":"Advancing high-temperature electrostatic energy storage via linker engineering of metal–organic frameworks in polymer nanocomposites","authors":"Zongliang Xie, Zhiyuan Huang, He Li, Tianlei Xu, Haoyu Zhao, Yunfei Wang, Pang Xi, Zhiqiang Cao, Virginia Altoe, Liana M Klivansky, Zaiyu Wang, Steven Shelton, Shiqi Lai, Peng Liu, Chenhui Zhu, Michael D. Connolly, Corie Y. Ralston, Xiaodan Gu, Zongren Peng, Jian Zhang, Yi Liu","doi":"10.1039/d4ee04085f","DOIUrl":"https://doi.org/10.1039/d4ee04085f","url":null,"abstract":"High-performance, thermally resilient polymer dielectrics are essential for film capacitors used in advanced electronic devices and renewable energy systems, particularly at elevated temperatures where conventional polymers fail to perform. Compositing polymers with nanofillers is a well-established approach to enhancing energy storage performance, though there remains a strong need for fillers with broad structural tunability and a clear structure-property relationship to further improve performance at elevated temperatures. Herein, we unravel the untapped potential of UiO-66 metal–organic framework (MOF) derivatives as exceptional nanofillers for tuning the properties of the widely used polyetherimide (PEI). By systematically varying the linker structures, we create a series of isostructural MOF fillers that exhibit contrasting capabilities in regulating the charge transport and energy storage capacities of the resulting composite films. Notably, capacitors based on composite films using the electron-deficient UiO-66-F4 show remarkable long-term charge-discharge stability and achieve ultrahigh discharged energy densities of 9.87 J cm−3 at 150 °C and 9.21 J cm−3 at 200 °C, setting a new benchmark for high-temperature flexible polymer composites. Through comprehensive experimental and theoretical analyses, we establish an unprecedented correlation between the MOF fillers' electronic structures and the composites’ improved electrical breakdown strength and energy storage properties. These findings offer a rational pathway to harness the exceptional structural diversity of MOFs for the development of composite materials suitable for high-temperature electrostatic energy storage.","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"1 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142599996","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Expanding momentum bandgaps in photonic time crystals through resonances 通过共振扩大光子时间晶体的动量带隙
IF 35 1区 化学
Chemical Reviews Pub Date : 2024-11-12 DOI: 10.1038/s41566-024-01563-3
X. Wang, P. Garg, M. S. Mirmoosa, A. G. Lamprianidis, C. Rockstuhl, V. S. Asadchy
{"title":"Expanding momentum bandgaps in photonic time crystals through resonances","authors":"X. Wang, P. Garg, M. S. Mirmoosa, A. G. Lamprianidis, C. Rockstuhl, V. S. Asadchy","doi":"10.1038/s41566-024-01563-3","DOIUrl":"https://doi.org/10.1038/s41566-024-01563-3","url":null,"abstract":"<p>The realization of photonic time crystals is a major opportunity but also comes with considerable challenges. The most pressing one, potentially, is the requirement for a substantial modulation strength in the material properties to create a noticeable momentum bandgap. Reaching that noticeable bandgap in optics is highly demanding with current, and possibly also future materials platforms because their modulation strength is small by tendency. Here we demonstrate that by introducing temporal variations in a resonant material, the momentum bandgap can be drastically expanded with modulation strengths in reach with known low-loss materials and realistic laser pump powers. The resonance can emerge from an intrinsic material resonance or a suitably spatially structured material supporting a structural resonance. Our concept is validated for resonant bulk media and optical metasurfaces and paves the way towards the first experimental realizations of photonic time crystals.</p>","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"1 1","pages":""},"PeriodicalIF":35.0,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142599378","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","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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