Energy & Environmental Materials最新文献

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Harvesting Energy Via Water Movement and Surface Ionics in Microfibrous Ceramic Wools 通过微纤维陶瓷羊毛中的水运动和表面离子收集能量
IF 13 2区 材料科学
Energy & Environmental Materials Pub Date : 2024-05-26 DOI: 10.1002/eem2.12760
Manpreet Kaur, Avinash Alagumalai, Omid Mahian, Sameh M. Osman, Tadaaki Nagao, Zhonglin Wang
{"title":"Harvesting Energy Via Water Movement and Surface Ionics in Microfibrous Ceramic Wools","authors":"Manpreet Kaur,&nbsp;Avinash Alagumalai,&nbsp;Omid Mahian,&nbsp;Sameh M. Osman,&nbsp;Tadaaki Nagao,&nbsp;Zhonglin Wang","doi":"10.1002/eem2.12760","DOIUrl":"10.1002/eem2.12760","url":null,"abstract":"<p>Due to the push for carbon neutrality in various human activities, the development of methods for producing electricity without relying on chemical reaction processes or heat sources has become highly significant. Also, the challenge lies in achieving microwatt-scale outputs due to the inherent conductivity of the materials and diverting electric currents. To address this challenge, our research has concentrated on utilizing nonconductive mediums for water-based low-cost microfibrous ceramic wools in conjunction with a NaCl aqueous solution for power generation. The main source of electricity originates from the directed movement of water molecules and surface ions through densely packed microfibrous ceramic wools due to the effect of dynamic electric double layer. This occurrence bears resemblance to the natural water transpiration in plants, thereby presenting a fresh and straightforward approach for producing electricity in an ecofriendly manner. The generator module demonstrated in this study, measuring 12 × 6 cm<sup>2</sup>, exhibited a noteworthy open-circuit voltage of 0.35 V, coupled with a short-circuit current of 0.51 mA. Such low-cost ceramic wools are suitable for ubiquitous, permanent energy sources and hold potential for use as self-powered sensors and systems, eliminating the requirement for external energy sources such as sunlight or heat.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"7 6","pages":""},"PeriodicalIF":13.0,"publicationDate":"2024-05-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12760","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141173052","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Multistage Microstructured Ionic Skin for Real-Time Vital Signs Monitoring and Human-Machine Interaction 用于实时生命体征监测和人机交互的多级微结构离子皮肤
IF 13 2区 材料科学
Energy & Environmental Materials Pub Date : 2024-05-26 DOI: 10.1002/eem2.12767
Xueke Wang, Jinyu Zi, Yi Chen, Qiang Wu, Zhimin Xiang, Yongqiang Tu, Peng Yang, Yanfen Wan
{"title":"Multistage Microstructured Ionic Skin for Real-Time Vital Signs Monitoring and Human-Machine Interaction","authors":"Xueke Wang,&nbsp;Jinyu Zi,&nbsp;Yi Chen,&nbsp;Qiang Wu,&nbsp;Zhimin Xiang,&nbsp;Yongqiang Tu,&nbsp;Peng Yang,&nbsp;Yanfen Wan","doi":"10.1002/eem2.12767","DOIUrl":"10.1002/eem2.12767","url":null,"abstract":"<p>Skin-like electronics research aiming to mimic even surpass human-like specific tactile cognition by operating perception-to-cognition-to-feedback of stimulus to build intelligent cognition systems for certain imperceptible or inappreciable signals was so attractive. Herein, we constructed an all-in-one tri-modal pressure sensing wearable device to address the issue of power supply by integrating multistage microstructured ionic skin (MM i-skin) and thermoelectric self-power staffs, which exhibits high sensitivity simultaneously. The MM i-skin with multi-stage “interlocked” configurations achieved precise recognition of subtle signals, where the sensitivity reached up to 3.95 kPa<sup>−1</sup>, as well as response time of 46 ms, cyclic stability (over 1500 cycles), a wide detection range of 0–200 kPa. Furthermore, we developed the thermoelectricity nanogenerator, piezoelectricity nanogenerator, and piezocapacitive sensing as an integrated tri-modal pressure sensing, denoted as P-iskin, T-iskin, and C-iskin, respectively. This multifunctional ionic skin enables real-time monitoring of weak body signals, rehab guidance, and robotic motion recognition, demonstrating potential for Internet of things (IoT) applications involving the artificial intelligence-motivated sapiential healthcare Internet (SHI) and widely distributed human-machine interaction (HMI).</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"7 6","pages":""},"PeriodicalIF":13.0,"publicationDate":"2024-05-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12767","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141173008","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A Tri-Salt Composite Electrolyte with Temperature Switch Function for Intelligently Temperature-Controlled Lithium Batteries 用于智能温控锂电池的具有温度开关功能的三盐复合电解质
IF 13 2区 材料科学
Energy & Environmental Materials Pub Date : 2024-05-26 DOI: 10.1002/eem2.12745
Ende Fu, Huimin Wang, Yating Zhang, Zhenxue Xiao, Xiu Zheng, Shuai Hao, Xueping Gao
{"title":"A Tri-Salt Composite Electrolyte with Temperature Switch Function for Intelligently Temperature-Controlled Lithium Batteries","authors":"Ende Fu,&nbsp;Huimin Wang,&nbsp;Yating Zhang,&nbsp;Zhenxue Xiao,&nbsp;Xiu Zheng,&nbsp;Shuai Hao,&nbsp;Xueping Gao","doi":"10.1002/eem2.12745","DOIUrl":"10.1002/eem2.12745","url":null,"abstract":"<p>The intense research of lithium-ion batteries has been motivated by their successful applications in mobile devices and electronic vehicles. The emerging of intelligent control in kinds of devices brings new requirements for battery systems. The high-energy lithium batteries are expected to respond or react under different environmental conditions. In this work, a tri-salt composite electrolyte is designed with a temperature switch function for intelligently temperature-controlled lithium batteries. Specifically, the halide Li<sub>3</sub>YBr<sub>6</sub> together with LiTFSI and LiNO<sub>3</sub> works as active fillers in a low-melting-point polymer matrix (polyethyleneglycol dimethyl ether (PEGDME) and polyethylene oxide (PEO)), which is further filled into the pre-lithiated alumina fiber skeleton. Above 60 °C, the composite electrolyte exists in the liquid state and fully contacts with the working electrodes on the liquid–solid interface, effectively minimizing the interfacial resistance and leading to high discharge capacity in the cell. The electrolyte is changed into a solid state below 30 °C so that the ionic conductivity is significantly reduced and the interface resistance is increased dramatically on the solid–solid interface. Therefore, by simply adjusting the temperature, the cell can be turned “ON” or “OFF” intentionally. This novel function of the composite electrolyte has enlightening significance in developing intelligently temperature-controlled lithium batteries.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"7 6","pages":""},"PeriodicalIF":13.0,"publicationDate":"2024-05-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12745","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141172972","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Effects of Rattling Behavior of K and Cd Atoms along Different Directions in Anisotropic KCdAs on Lattice Thermal Transport and Thermoelectric Properties 各向异性 KCdAs 中 K 原子和镉原子沿不同方向的响动行为对晶格热传输和热电性能的影响
IF 13 2区 材料科学
Energy & Environmental Materials Pub Date : 2024-05-26 DOI: 10.1002/eem2.12764
Yue Wang, Yinchang Zhao, Jun Ni, Zhenhong Dai
{"title":"Effects of Rattling Behavior of K and Cd Atoms along Different Directions in Anisotropic KCdAs on Lattice Thermal Transport and Thermoelectric Properties","authors":"Yue Wang,&nbsp;Yinchang Zhao,&nbsp;Jun Ni,&nbsp;Zhenhong Dai","doi":"10.1002/eem2.12764","DOIUrl":"10.1002/eem2.12764","url":null,"abstract":"<p>We employ advanced first principles methodology, merging self-consistent phonon theory and the Boltzmann transport equation, to comprehensively explore the thermal transport and thermoelectric properties of KCdAs. Notably, the study accounts for the impact of quartic anharmonicity on phonon group velocities in the pursuit of lattice thermal conductivity and investigates 3ph and 4ph scattering processes on phonon lifetimes. Through various methodologies, including examining atomic vibrational modes and analyzing 3ph and 4ph scattering processes, the article unveils microphysical mechanisms contributing to the low κ<sub>L</sub> within KCdAs. Key features include significant anisotropy in Cd atoms, pronounced anharmonicity in K atoms, and relative vibrations in non-equivalent As atomic layers. Cd atoms, situated between As layers, exhibit rattling modes and strong lattice anharmonicity, contributing to the observed low κ<sub>L</sub>. Remarkably flat bands near the valence band maximum translate into high PF, aligning with ultralow κ<sub>L</sub> for exceptional thermoelectric performance. Under optimal temperature and carrier concentration doping, outstanding <i>ZT</i> values are achieved: 4.25 (<i>a</i>(<i>b</i>)-axis, p-type, 3 × 10<sup>19</sup> cm<sup>−3</sup>, 500 K), 0.90 (<i>c</i>-axis, p-type, 5 × 10<sup>20</sup> cm<sup>−3</sup>, 700 K), 1.61 (<i>a</i>(<i>b</i>)-axis, n-type, 2 × 10<sup>18</sup> cm<sup>−3</sup>, 700 K), and 3.06 (<i>c</i>-axis, n-type, 9 × 10<sup>17</sup> cm<sup>−3</sup>, 700 K).</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"7 6","pages":""},"PeriodicalIF":13.0,"publicationDate":"2024-05-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12764","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141173040","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
MOF-Derived Iron-Cobalt Phosphide Nanoframe as Bifunctional Electrocatalysts for Overall Water Splitting MOF 衍生的磷化铁钴纳米框架作为整体水分离的双功能电催化剂
IF 13 2区 材料科学
Energy & Environmental Materials Pub Date : 2024-05-21 DOI: 10.1002/eem2.12747
Yanqi Yuan, Kun Wang, Boan Zhong, Dongkun Yu, Fei Ye, Jing Liu, Joydeep Dutta, Peng Zhang
{"title":"MOF-Derived Iron-Cobalt Phosphide Nanoframe as Bifunctional Electrocatalysts for Overall Water Splitting","authors":"Yanqi Yuan,&nbsp;Kun Wang,&nbsp;Boan Zhong,&nbsp;Dongkun Yu,&nbsp;Fei Ye,&nbsp;Jing Liu,&nbsp;Joydeep Dutta,&nbsp;Peng Zhang","doi":"10.1002/eem2.12747","DOIUrl":"10.1002/eem2.12747","url":null,"abstract":"<p>Transition metal phosphides (TMPs) have emerged as an alternative to precious metals as efficient and low-cost catalysts for water electrolysis. Elemental doping and morphology control are effective approaches to further improve the performance of TMPs. Herein, Fe-doped CoP nanoframes (Fe-CoP NFs) with specific open cage configuration were designed and synthesized. The unique nano-framework structured Fe-CoP material shows overpotentials of only 255 and 122 mV at 10 mA cm<sup>−2</sup> for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER), respectively, overwhelming most transition metal phosphides. For overall water splitting, the cell voltage is 1.65 V for Fe-CoP NFs at a current density of 10 mA cm<sup>−2</sup>, much superior to what is observed for the classical nanocubic structures. Fe-CoP NFs show no activity degradation up to 100 h which contrasts sharply with the rapidly decaying performance of noble metal catalyst reference. The superior electrocatalytic performance of Fe-CoP NFs due to abundant accessible active sites, reduced kinetic energy barrier, and preferable *O-containing intermediate adsorption is demonstrated through experimental observations and theoretical calculations. Our findings could provide a potential method for the preparation of multifunctional material with hollow structures and offer more hopeful prospects for obtaining efficient earth-abundant catalysts for water splitting.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"7 6","pages":""},"PeriodicalIF":13.0,"publicationDate":"2024-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12747","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141113773","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Mo2B2O2 MBene for Efficient Electrochemical CO Reduction to C2 Chemicals: Computational Exploration 用于高效电化学 CO 还原成 C2 化学品的 Mo2B2O2MBene:计算探索
IF 13 2区 材料科学
Energy & Environmental Materials Pub Date : 2024-05-16 DOI: 10.1002/eem2.12738
Bikun Zhang, Jianwen Jiang
{"title":"Mo2B2O2 MBene for Efficient Electrochemical CO Reduction to C2 Chemicals: Computational Exploration","authors":"Bikun Zhang,&nbsp;Jianwen Jiang","doi":"10.1002/eem2.12738","DOIUrl":"10.1002/eem2.12738","url":null,"abstract":"<p>Emerging as a new class of two-dimensional materials with atomically thin layers, MBenes have great potential for many important applications such as energy storage and electrocatalysis. Toward mitigating carbon footprint, there has been increasing interest in CO<sub>2</sub>/CO conversion on MBenes, but mostly focused on C<sub>1</sub> products. C<sub>2+</sub> chemicals generally possess higher energy densities and wider applications than C<sub>1</sub> counterparts. However, C–C coupling is technically challenging because of high energy requirement and currently few catalysts are suited for this process. Here, we explore electrochemical CO reduction reaction to C<sub>2</sub> chemicals on Mo<sub>2</sub>B<sub>2</sub>O<sub>2</sub> MBene via density-functional theory calculations. Remarkably, the most favorable CO–COH coupling is revealed to be a spontaneous and barrierless process, making Mo<sub>2</sub>B<sub>2</sub>O<sub>2</sub> an efficient catalyst for C–C coupling. Among C<sub>1</sub> and C<sub>2</sub> chemicals, ethanol is predicted to be the primary product. Furthermore, by charge and bond analysis, it is unraveled that there exist significantly more unbonded electrons in the C atom of intermediate *COH than other C<sub>1</sub> intermediates, which is responsible for the facile C–C coupling. From an atomic scale, this work provides microscopic insight into C–C coupling process and suggests Mo<sub>2</sub>B<sub>2</sub>O<sub>2</sub> a promising catalyst for electrochemical CO reduction to C<sub>2</sub> chemicals.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"7 6","pages":""},"PeriodicalIF":13.0,"publicationDate":"2024-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12738","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140969166","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
High-Safety Anode Materials for Advanced Lithium-Ion Batteries 用于先进锂离子电池的高安全性阳极材料
IF 13 2区 材料科学
Energy & Environmental Materials Pub Date : 2024-05-16 DOI: 10.1002/eem2.12759
Kai Yuan, Yu Lin, Xiang Li, Yufeng Ding, Peng Yu, Jian Peng, Jiazhao Wang, HuaKun Liu, Shixue Dou
{"title":"High-Safety Anode Materials for Advanced Lithium-Ion Batteries","authors":"Kai Yuan,&nbsp;Yu Lin,&nbsp;Xiang Li,&nbsp;Yufeng Ding,&nbsp;Peng Yu,&nbsp;Jian Peng,&nbsp;Jiazhao Wang,&nbsp;HuaKun Liu,&nbsp;Shixue Dou","doi":"10.1002/eem2.12759","DOIUrl":"10.1002/eem2.12759","url":null,"abstract":"<p>Lithium-ion batteries (LIBs) play a pivotal role in today's society, with widespread applications in portable electronics, electric vehicles, and smart grids. Commercial LIBs predominantly utilize graphite anodes due to their high energy density and cost-effectiveness. Graphite anodes face challenges, however, in extreme safety-demanding situations, such as airplanes and passenger ships. The lithiation of graphite can potentially form lithium dendrites at low temperatures, causing short circuits. Additionally, the dissolution of the solid-electrolyte-interphase on graphite surfaces at high temperatures can lead to intense reactions with the electrolyte, initiating thermal runaway. This review introduces two promising high-safety anode materials, Li<sub>4</sub>Ti<sub>5</sub>O<sub>12</sub> and TiNb<sub>2</sub>O<sub>7</sub>. Both materials exhibit low tendencies towards lithium dendrite formation and have high onset temperatures for reactions with the electrolyte, resulting in reduced heat generation and significantly lower probabilities of thermal runaway. Li<sub>4</sub>Ti<sub>5</sub>O<sub>12</sub> and TiNb<sub>2</sub>O<sub>7</sub> offer enhanced safety characteristics compared to graphite, making them suitable for applications with stringent safety requirements. This review provides a comprehensive overview of Li<sub>4</sub>Ti<sub>5</sub>O<sub>12</sub> and TiNb<sub>2</sub>O<sub>7</sub>, focusing on their material properties and practical applicability. It aims to contribute to the understanding and development of high-safety anode materials for advanced LIBs, addressing the challenges and opportunities associated with their implementation in real-world applications.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"7 5","pages":""},"PeriodicalIF":13.0,"publicationDate":"2024-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12759","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140967192","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Accelerating the Screening of Modified MA2Z4 Catalysts for Hydrogen Evolution Reaction by Deep Learning-Based Local Geometric Analysis 通过基于深度学习的局部几何分析加速筛选用于氢气进化反应的改良 MA2Z4 催化剂
IF 13 2区 材料科学
Energy & Environmental Materials Pub Date : 2024-05-15 DOI: 10.1002/eem2.12743
Jingnan Zheng, Shibin Wang, Shengwei Deng, Zihao Yao, Junhua Hu, Jianguo Wang
{"title":"Accelerating the Screening of Modified MA2Z4 Catalysts for Hydrogen Evolution Reaction by Deep Learning-Based Local Geometric Analysis","authors":"Jingnan Zheng,&nbsp;Shibin Wang,&nbsp;Shengwei Deng,&nbsp;Zihao Yao,&nbsp;Junhua Hu,&nbsp;Jianguo Wang","doi":"10.1002/eem2.12743","DOIUrl":"10.1002/eem2.12743","url":null,"abstract":"<p>Machine learning (ML) integrated with density functional theory (DFT) calculations have recently been used to accelerate the design and discovery of single-atom catalysts (SACs) by establishing deep structure–activity relationships. The traditional ML models are always difficult to identify the structural differences among the single-atom systems with different modification methods, leading to the limitation of the potential application range. Aiming to the structural properties of several typical two-dimensional MA<sub>2</sub>Z<sub>4</sub>-based single-atom systems (bare MA<sub>2</sub>Z<sub>4</sub> and metal single-atom doped/supported MA<sub>2</sub>Z<sub>4</sub>), an improved crystal graph convolutional neural network (CGCNN) classification model was employed, instead of the traditional machine learning regression model, to address the challenge of incompatibility in the studied systems. The CGCNN model was optimized using crystal graph representation in which the geometric configuration was divided into active layer, surface layer, and bulk layer (ASB-GCNN). Through ML and DFT calculations, five potential single-atom hydrogen evolution reaction (HER) catalysts were screened from chemical space of 600 MA<sub>2</sub>Z<sub>4</sub>-based materials, especially V<sub>1</sub>/HfSn<sub>2</sub>N<sub>4</sub>(S) with high stability and activity (Δ<i>G</i><sub><i>H</i>*</sub> is 0.06 eV). Further projected density of states (pDOS) analysis in combination with the wave function analysis of the SAC-H bond revealed that the SAC-<i>dz</i><sup>2</sup> orbital coincided with the H-<i>s</i> orbital around the energy level of −2.50 eV, and orbital analysis confirmed the formation of σ bonds. This study provides an efficient multistep screening design framework of metal single-atom catalyst for HER systems with similar two-dimensional supports but different geometric configurations.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"7 6","pages":""},"PeriodicalIF":13.0,"publicationDate":"2024-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12743","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140974087","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Understanding Bonding Nature of α-Keggin Polyoxometalates [XW12O40]n− (X = Al, Si, P, S): A Generalized Superatomic Perspective 了解 α-Keggin 聚氧化金属盐 [XW12O40]n- (X = Al、Si、P、S)的键合性质:广义超原子视角
IF 13 2区 材料科学
Energy & Environmental Materials Pub Date : 2024-05-15 DOI: 10.1002/eem2.12754
Rui Li, Yulei Shi, Famin Yu, Rui Wang, Haitao Yan, Boon K. Teo, Zhigang Wang
{"title":"Understanding Bonding Nature of α-Keggin Polyoxometalates [XW12O40]n− (X = Al, Si, P, S): A Generalized Superatomic Perspective","authors":"Rui Li,&nbsp;Yulei Shi,&nbsp;Famin Yu,&nbsp;Rui Wang,&nbsp;Haitao Yan,&nbsp;Boon K. Teo,&nbsp;Zhigang Wang","doi":"10.1002/eem2.12754","DOIUrl":"10.1002/eem2.12754","url":null,"abstract":"<p>α-Keggin polyoxometalates (POMs) [XW<sub>12</sub>O<sub>40</sub>]<sup>n−</sup> (X = Al, Si, P, S) are widely used in batteries owing to their remarkable redox activity. However, the mechanism underlying the applications appears inconsistent with the widely accepted covalent bonding nature. Here, first-principles calculations show that XW<sub>12</sub> are core–shell structures composed of a shell and an XO<sub>4</sub><sup>n−</sup> core, both are stabilized by covalent interactions. Interestingly, owing to the presence of a substantial number of electrons in W<sub>12</sub>O<sub>36</sub> shell, the frontier molecular orbitals of XW<sub>12</sub> are not only strongly delocalized but also exhibit superatomic properties with high-angular momentum electrons that do not conform to the Jellium model. Detailed analysis indicates that energetically high lying filled molecular orbitals (MOs) have reached unusually high-angular momentum characterized by quantum number K or higher, allowing for the accommodation of numerous electrons. This attribute confers strong electron acceptor ability and redox activity to XW<sub>12</sub>. Moreover, electrons added to XW<sub>12</sub> still occupy the K orbitals and will not cause rearrangement of the MOs, thereby maintaining the stability of these structures. Our findings highlight the structure–activity relationship and provide a direction for tailor-made POMs with specific properties at atomic level.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"7 6","pages":""},"PeriodicalIF":13.0,"publicationDate":"2024-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12754","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140975788","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Outstanding Lithium Storage Performance of a Copper-Coordinated Metal-Covalent Organic Framework as Anode Material for Lithium-Ion Batteries 铜配位金属共价有机框架作为锂离子电池负极材料的出色储锂性能
IF 13 2区 材料科学
Energy & Environmental Materials Pub Date : 2024-05-15 DOI: 10.1002/eem2.12732
Derong Luo, Huizi Zhao, Feng Liu, Hai Xu, Xiaoyu Dong, Bing Ding, Hui Dou, Xiaogang Zhang
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