Wang Peng, Rongrong Zhu, Qianqiu Ni, Junqing Zhao, Xuanchen Zhu, Qingsong Mei, Chi Zhang, Lingyi Liao
In the era of Internet of Things (IoT) and Artificial Intelligence (AI), sensors have become an integral part of intelligent systems. Although the traditional sensing technology is very mature in long-term development, there are remaining defects and limitations that make it difficult to meet the growing demands of current applications, such as high-sensitivity detection and self-supplied sensing. As a new type of sensor, array triboelectric nanogenerators (TENG)-based tactile sensors can respond to wide dynamic range of mechanical stimuli in the surrounding environment and converting them into quantifiable electrical signals, thus realizing real-time self-supplied tactile sensing. The array structure allows for fine delineation of the sensing area and improved spatial resolution, resulting in accurate localization and quantification of the detected tactile signals, and have been widely used in wearable devices, smart interaction, medical and health detection, and other fields. In this paper, the latest research progress of functional tactile sensors based on arrayed triboelectric nanogenerators is systematically reviewed from the aspects of working mechanism, material selection, material processing, structural design, functional integration, and application. Finally, the challenges faced by arrayed triboelectric tactile sensors are summarized with a view to providing inspiration and guidance for the future development of tactile sensors.
{"title":"Functional Tactile Sensor Based on Arrayed Triboelectric Nanogenerators","authors":"Wang Peng, Rongrong Zhu, Qianqiu Ni, Junqing Zhao, Xuanchen Zhu, Qingsong Mei, Chi Zhang, Lingyi Liao","doi":"10.1002/aenm.202403289","DOIUrl":"https://doi.org/10.1002/aenm.202403289","url":null,"abstract":"In the era of Internet of Things (IoT) and Artificial Intelligence (AI), sensors have become an integral part of intelligent systems. Although the traditional sensing technology is very mature in long-term development, there are remaining defects and limitations that make it difficult to meet the growing demands of current applications, such as high-sensitivity detection and self-supplied sensing. As a new type of sensor, array triboelectric nanogenerators (TENG)-based tactile sensors can respond to wide dynamic range of mechanical stimuli in the surrounding environment and converting them into quantifiable electrical signals, thus realizing real-time self-supplied tactile sensing. The array structure allows for fine delineation of the sensing area and improved spatial resolution, resulting in accurate localization and quantification of the detected tactile signals, and have been widely used in wearable devices, smart interaction, medical and health detection, and other fields. In this paper, the latest research progress of functional tactile sensors based on arrayed triboelectric nanogenerators is systematically reviewed from the aspects of working mechanism, material selection, material processing, structural design, functional integration, and application. Finally, the challenges faced by arrayed triboelectric tactile sensors are summarized with a view to providing inspiration and guidance for the future development of tactile sensors.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142161181","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Zheming Liu, Jordi Llusar, Hiba H. Karakkal, Dongxu Zhu, Yurii P. Ivanov, Mirko Prato, Giorgio Divitini, Sergio Brovelli, Ivan Infante, Luca De Trizio, Liberato Manna
A colloidal synthesis protocol is demonstrated for InAs@InP core@shell quantum dots (QDs) with a tunable InP shell thickness (ranging from 3 to 8 monolayers), utilizing tris(diethylamino)-arsine and -phosphine. Structural analysis reveals that the InP shell preferentially grows onto the tetrahedral InAs cores along the <-1-1-1> directions, forming tetrapodal-shaped InAs@InP QDs. Growth of the InP shell causes a red shift in the absorption spectrum of the QDs. This is explained by considering that electrons are delocalized throughout the whole core@shell QDs, while holes preferentially leak along the <-1-1-1> directions, as indicated by the density functional theory calculations. This means such heterostructures cannot be described as type-I or quasi type-II, contrary to earlier assumptions. The overlap of carrier wavefunctions throughout the entire InAs@InP QD structure results in no significant reduction of the Auger recombination rate, which remains as fast as in InAs QDs. However, the InP shell enhances photoluminescence (PL) efficiency (up to ≈13%) by passivating surface trap states of the InAs QDs (mainly located close to the top of the valence band). The overgrowth of a ZnSe shell endows the QDs with a high PL efficiency (≈55%) and good stability upon air exposure (≈80% PL intensity retention after 14 days).
{"title":"Amino-Arsine and Amino-Phosphine Based Synthesis of InAs@InP@ZnSe core@shell@shell Quantum Dots","authors":"Zheming Liu, Jordi Llusar, Hiba H. Karakkal, Dongxu Zhu, Yurii P. Ivanov, Mirko Prato, Giorgio Divitini, Sergio Brovelli, Ivan Infante, Luca De Trizio, Liberato Manna","doi":"10.1002/aenm.202402246","DOIUrl":"https://doi.org/10.1002/aenm.202402246","url":null,"abstract":"A colloidal synthesis protocol is demonstrated for InAs@InP core@shell quantum dots (QDs) with a tunable InP shell thickness (ranging from 3 to 8 monolayers), utilizing tris(diethylamino)-arsine and -phosphine. Structural analysis reveals that the InP shell preferentially grows onto the tetrahedral InAs cores along the <-1-1-1> directions, forming tetrapodal-shaped InAs@InP QDs. Growth of the InP shell causes a red shift in the absorption spectrum of the QDs. This is explained by considering that electrons are delocalized throughout the whole core@shell QDs, while holes preferentially leak along the <-1-1-1> directions, as indicated by the density functional theory calculations. This means such heterostructures cannot be described as type-I or quasi type-II, contrary to earlier assumptions. The overlap of carrier wavefunctions throughout the entire InAs@InP QD structure results in no significant reduction of the Auger recombination rate, which remains as fast as in InAs QDs. However, the InP shell enhances photoluminescence (PL) efficiency (up to ≈13%) by passivating surface trap states of the InAs QDs (mainly located close to the top of the valence band). The overgrowth of a ZnSe shell endows the QDs with a high PL efficiency (≈55%) and good stability upon air exposure (≈80% PL intensity retention after 14 days).","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142161183","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
High-quality perovskite (PVK) films is essential for the fabrication of efficient and stable perovskite solar cells (PSCs). However, unstable colloidal particles in PVK suspensions often hinder the formation of crystalline films with low defect densities. Herein, ethylenediaminetetraacetic acid (EDTA) as a colloidal stabilizer into lead iodide (PbI2) is introduced colloidal solutions. EDTA forms chelated complexes with Pb2+, enhancing the electrostatic repulsion and steric hindrance between colloidal particles. This stabilizes the particles and inhibits disordered motion (Brownian motion) and excessive aggregation. As a result, PbI2 films with a uniform hole distribution are formed, providing ample pathways for subsequent PVK film growth and sufficient space. During the film formation process, the replacement of molecules by formamidinium iodide (FAI) and EDTA slows down crystallization, ultimately leading to PVK films with large grain sizes and low defect density. By using this approach, champion power conversion efficiencies (PCEs) of 24.05% for FA0.97Cs0.03PbI3 PSC, 11.08% for CsPbBr3 PSC, and 25.19% for FA0.945MA0.025Cs0.03Pb(I0.975Br0.025)3 PSC are achieved. Moreover, the EDTA-based FA0.97Cs0.03PbI3 device retains over 90% of its initial PCE after 1000 h at the maximum power point (MPP) under continuous illumination.
{"title":"Colloidal Stabilizer-Mediated Crystal Growth Regulation and Defect Healing for High-Quality Perovskite Solar Cells","authors":"Zhe Xin, Yang Ding, Yuanyuan Zhao, Yue Peng, Qing Zhang, Yusheng Cao, Qiyao Guo, Jialong Duan, Jie Dou, Liqing Sun, Qiang Zhang, Qunwei Tang","doi":"10.1002/aenm.202403018","DOIUrl":"https://doi.org/10.1002/aenm.202403018","url":null,"abstract":"High-quality perovskite (PVK) films is essential for the fabrication of efficient and stable perovskite solar cells (PSCs). However, unstable colloidal particles in PVK suspensions often hinder the formation of crystalline films with low defect densities. Herein, ethylenediaminetetraacetic acid (EDTA) as a colloidal stabilizer into lead iodide (PbI<sub>2</sub>) is introduced colloidal solutions. EDTA forms chelated complexes with Pb<sup>2+</sup>, enhancing the electrostatic repulsion and steric hindrance between colloidal particles. This stabilizes the particles and inhibits disordered motion (Brownian motion) and excessive aggregation. As a result, PbI<sub>2</sub> films with a uniform hole distribution are formed, providing ample pathways for subsequent PVK film growth and sufficient space. During the film formation process, the replacement of molecules by formamidinium iodide (FAI) and EDTA slows down crystallization, ultimately leading to PVK films with large grain sizes and low defect density. By using this approach, champion power conversion efficiencies (PCEs) of 24.05% for FA<sub>0.97</sub>Cs<sub>0.03</sub>PbI<sub>3</sub> PSC, 11.08% for CsPbBr<sub>3</sub> PSC, and 25.19% for FA<sub>0.945</sub>MA<sub>0.025</sub>Cs<sub>0.03</sub>Pb(I<sub>0.975</sub>Br<sub>0.025</sub>)<sub>3</sub> PSC are achieved. Moreover, the EDTA-based FA<sub>0.97</sub>Cs<sub>0.03</sub>PbI<sub>3</sub> device retains over 90% of its initial PCE after 1000 h at the maximum power point (MPP) under continuous illumination.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142161170","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Vanadate materials are promising for sodium-ion batteries (SIBs) due to their low cost, high capacity, and high power characteristics enabled by vanadium's multiple oxidation states. However, their development is hindered by poor conductivity, suboptimal high-rate performance, and limited cycle life. In this work, a layered structure modification strategy involving Ca/F co-doping in sodium vanadate Na2CaV2O6F (CVF) is proposed to address these issues. Through a combination of experiments and density functional theory calculations, it is demonstrated that Ca/F synergies enhance the Na layer spacing in CVF, resulting in reduced crystal water content and volume shrinkage compared to Na2V2O6 (NVO). Additionally, Ca/F incorporation significantly mitigates the diffusion potential of Na+ within the material framework. The unmodified CVF sample exhibits a high reversible capacity of 220 mAh g−1 at 10 mA g−1 and an excellent rate capacity of 65.78 mAh g−1 at 400 mA g−1. Furthermore, the cathode material maintains a capacity of up to 138 mAh g−1 at 200 mA g−1 and retains 104.88 mAh g−1 after 100 cycles within the voltage range of 1.5−4.0 V. These findings enhance the understanding of the crystal structure of NVO cathode materials and pave the way for the rational design of high-quality vanadate cathodes for SIBs.
钒酸盐材料因其低成本、高容量和钒的多种氧化态带来的高功率特性，在钠离子电池（SIB）中大有可为。然而，由于导电性差、高倍率性能不理想以及循环寿命有限，钒酸盐材料的发展受到了阻碍。本研究提出了一种在钒酸钠 Na2CaV2O6F (CVF) 中掺杂 Ca/F 的分层结构改性策略，以解决这些问题。通过实验和密度泛函理论计算相结合的方法，证明了 Ca/F 协同作用增强了 CVF 中的 Na 层间距，从而与 Na2V2O6 (NVO) 相比降低了晶体含水量和体积收缩。此外，Ca/F 的加入大大减轻了 Na+ 在材料框架内的扩散潜力。未经改性的 CVF 样品在 10 mA g-1 的条件下显示出 220 mAh g-1 的高可逆容量，在 400 mA g-1 的条件下显示出 65.78 mAh g-1 的出色速率容量。此外，该阴极材料在 200 mA g-1 时可保持高达 138 mAh g-1 的容量，在 1.5-4.0 V 的电压范围内循环 100 次后可保持 104.88 mAh g-1 的容量。这些发现加深了人们对 NVO 阴极材料晶体结构的理解，为合理设计用于 SIB 的高质量钒酸盐阴极铺平了道路。
{"title":"Layered Structure Modification of Sodium Vanadate through Ca/F Co-Doping for Enhanced Energy Storage Performance","authors":"Jiajia Han, Shuting Gao, Zhefei Sun, Zonghua Yang, Xingjun Liu, Cuiping Wang","doi":"10.1002/aenm.202401481","DOIUrl":"https://doi.org/10.1002/aenm.202401481","url":null,"abstract":"Vanadate materials are promising for sodium-ion batteries (SIBs) due to their low cost, high capacity, and high power characteristics enabled by vanadium's multiple oxidation states. However, their development is hindered by poor conductivity, suboptimal high-rate performance, and limited cycle life. In this work, a layered structure modification strategy involving Ca/F co-doping in sodium vanadate Na<sub>2</sub>CaV<sub>2</sub>O<sub>6</sub>F (CVF) is proposed to address these issues. Through a combination of experiments and density functional theory calculations, it is demonstrated that Ca/F synergies enhance the Na layer spacing in CVF, resulting in reduced crystal water content and volume shrinkage compared to Na<sub>2</sub>V<sub>2</sub>O<sub>6</sub> (NVO). Additionally, Ca/F incorporation significantly mitigates the diffusion potential of Na<sup>+</sup> within the material framework. The unmodified CVF sample exhibits a high reversible capacity of 220 mAh g<sup>−1</sup> at 10 mA g<sup>−1</sup> and an excellent rate capacity of 65.78 mAh g<sup>−1</sup> at 400 mA g<sup>−1</sup>. Furthermore, the cathode material maintains a capacity of up to 138 mAh g<sup>−1</sup> at 200 mA g<sup>−1</sup> and retains 104.88 mAh g<sup>−1</sup> after 100 cycles within the voltage range of 1.5−4.0 V. These findings enhance the understanding of the crystal structure of NVO cathode materials and pave the way for the rational design of high-quality vanadate cathodes for SIBs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142159030","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Sucheng Liu, Boyong Wu, Song Huang, Zitian Lin, Huiyu Song, Li Du, Zhenxing Liang, Zhiming Cui
In situ formed poly(1,3-dioxolane) (PDOL) electrolytes are of great interest due to the facile process and the improved interface contact. However, the practical application of in situ PDOL electrolytes is still plagued by fast solidification time (liquid state) and poor high-voltage stability (solid state). Herein, the slow-release carriers triglycidyl isocyanurate (TGIC), which play dual roles as initiator sustained-release and network confinement, can tune DOL curing time and cathode/electrolyte interface chemistry is demonstrated. Specifically, the electronegative C≐O and epoxy groups in TGIC have an affinity with BF3, the decomposition product of lithium bis(oxalate)borate (LiDFOB), delaying BF3 protonation reaction and thus extending DOL solidification time. In addition, the epoxy groups in TGIC serve as crosslinking sites to form in situ crosslinked polymer electrolytes (TPDOL@FEC). The corresponding network structure suppresses the contact reaction between high-fluidity organic components and cathodes, generating a uniform and thin cathode electrolyte interface layer. As a result, the TPDOL@FEC precursor solution can remain its liquid state even after resting 24 h at room temperature. The assembled LiNi0.6Co0.2Mn0.2O2||TPDOL@FEC||Li cells display an impressive capacity retention of 91.5% after 100 cycles at 4.4 V (0.5 C). This study is expected to be a leap in the pursuit of practically feasible in situ formed PDOL electrolytes.
{"title":"Controllable In situ Polymerization of 1,3-Dioxolane via Sustained-Release Effect for Solid-State Lithium Metal Batteries","authors":"Sucheng Liu, Boyong Wu, Song Huang, Zitian Lin, Huiyu Song, Li Du, Zhenxing Liang, Zhiming Cui","doi":"10.1002/aenm.202402848","DOIUrl":"https://doi.org/10.1002/aenm.202402848","url":null,"abstract":"In situ formed poly(1,3-dioxolane) (PDOL) electrolytes are of great interest due to the facile process and the improved interface contact. However, the practical application of in situ PDOL electrolytes is still plagued by fast solidification time (liquid state) and poor high-voltage stability (solid state). Herein, the slow-release carriers triglycidyl isocyanurate (TGIC), which play dual roles as initiator sustained-release and network confinement, can tune DOL curing time and cathode/electrolyte interface chemistry is demonstrated. Specifically, the electronegative C≐O and epoxy groups in TGIC have an affinity with BF<sub>3</sub>, the decomposition product of lithium bis(oxalate)borate (LiDFOB), delaying BF<sub>3</sub> protonation reaction and thus extending DOL solidification time. In addition, the epoxy groups in TGIC serve as crosslinking sites to form in situ crosslinked polymer electrolytes (TPDOL@FEC). The corresponding network structure suppresses the contact reaction between high-fluidity organic components and cathodes, generating a uniform and thin cathode electrolyte interface layer. As a result, the TPDOL@FEC precursor solution can remain its liquid state even after resting 24 h at room temperature. The assembled LiNi<sub>0.6</sub>Co<sub>0.2</sub>Mn<sub>0.2</sub>O<sub>2</sub>||TPDOL@FEC||Li cells display an impressive capacity retention of 91.5% after 100 cycles at 4.4 V (0.5 C). This study is expected to be a leap in the pursuit of practically feasible in situ formed PDOL electrolytes.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142159033","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
In article number 2401479, Bolong Huang, Guo Hong, Wenjun Zhang, and co-workers designed a nanodiamond interfacial layer with rich nucleation sites to uniformize zinc ion flux and electric field distribution and realized smooth and dendrite-free zinc deposition. Furthermore, the zinc ion batteries and zinc ion hybrid capacitors comprising such nanodiamond layer protected Zn anode were developed and exhibited an ultra-long cycling performance.
锌离子电池
{"title":"Multifunctional Nanodiamond Interfacial Layer for Ultra-Stable Zinc-Metal Anodes (Adv. Energy Mater. 33/2024)","authors":"Kai Liu, Mingzi Sun, Shuo Yang, Guoqiang Gan, Shuyu Bu, Anquan Zhu, Dewu Lin, Tian Zhang, Chuhao Luan, Chunyi Zhi, Pengfei Wang, Bolong Huang, Guo Hong, Wenjun Zhang","doi":"10.1002/aenm.202470138","DOIUrl":"10.1002/aenm.202470138","url":null,"abstract":"<p><b>Zinc-Ion Batteries</b></p><p>In article number 2401479, Bolong Huang, Guo Hong, Wenjun Zhang, and co-workers designed a nanodiamond interfacial layer with rich nucleation sites to uniformize zinc ion flux and electric field distribution and realized smooth and dendrite-free zinc deposition. Furthermore, the zinc ion batteries and zinc ion hybrid capacitors comprising such nanodiamond layer protected Zn anode were developed and exhibited an ultra-long cycling performance.\u0000\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure></p>","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":24.4,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/aenm.202470138","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142161167","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Masthead: (Adv. Energy Mater. 33/2024)","authors":"","doi":"10.1002/aenm.202470137","DOIUrl":"https://doi.org/10.1002/aenm.202470137","url":null,"abstract":"","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":24.4,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/aenm.202470137","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142165607","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Lihong Su, Jin Chen, Jianzhong Zhou, Junjie Liu, Zhongli Hu, Sha Li, Xuebu Hu, Liang liang Xu, Li Zhang
Small molecule organic materials are widely used as anode materials for lithium-ion batteries (LIBs) due to their high reversible capacity, designable structure, and environmental friendliness. However, they suffer from poor intrinsic electronic conductivity, severe dissolution, and low initial coulombic efficiency. Recently, metal–organic frameworks (MOFs) have demonstrated in metal-ion batteries, outperforming some small molecule organic materials in terms of both cycling stability and rate capability. Herein, the first rational design and synthesis of a new cobalt-based MOF (CoBPDCA), are reported employing cobalt(II) nitrate as the metal source and small organic molecules (2,2-bipyridyl-4,4-dicarboxylic acid, BPDCA) as the ligands, which shows exceptional chemical stability and impressive electron conductivity. Most importantly, CoBPDCA electrodes deliver a high reversible capacity of 1112.9 mAh g−1 at 0.05 C (1 C = 1000 mA g−1) and outstanding high-rate durability (166.3 mAh g−1 after 2500 cycles at 10 C). Employing a series of spectroscopic and morphological characterizations and density functional theory (DFT) calculations, it is revealed that these impressively electrochemical performances are contributed to the dual active redox centers of Co cations and BPDCA ligands (CN and CO groups), and the superb electron conductivity. This work might provide a new strategy and a deeper understanding of the other MOFs' development for LIBs.
小分子有机材料因其高可逆容量、可设计结构和环境友好性而被广泛用作锂离子电池（LIB）的负极材料。然而，它们的固有电子导电性差、溶解性强、初始库仑效率低。最近，金属有机框架（MOFs）在金属离子电池中的应用得到了证实，其循环稳定性和速率能力均优于一些小分子有机材料。本文以硝酸钴（II）为金属源，以小分子有机物（2,2-联吡啶-4,4-二羧酸，BPDCA）为配体，首次报道了一种新型钴基 MOF（CoBPDCA）的合理设计与合成。最重要的是，CoBPDCA 电极在 0.05 C（1 C = 1000 mA g-1）条件下具有 1112.9 mAh g-1 的高可逆容量和出色的高速耐久性（10 C 条件下循环 2500 次后达到 166.3 mAh g-1）。通过一系列光谱和形态表征以及密度泛函理论（DFT）计算，我们发现这些令人印象深刻的电化学性能得益于钴阳离子和 BPDCA 配体（CN 和 CO 基团）的双活性氧化还原中心以及卓越的电子传导性。这项工作可能会为其他 MOFs 开发 LIB 提供新的策略和更深入的理解。
{"title":"Co-Based Metal–Organic Frameworks With Dual Redox Active Centers for Lithium-Ion Batteries With High Capacity and Excellent Rate Capability","authors":"Lihong Su, Jin Chen, Jianzhong Zhou, Junjie Liu, Zhongli Hu, Sha Li, Xuebu Hu, Liang liang Xu, Li Zhang","doi":"10.1002/aenm.202402489","DOIUrl":"https://doi.org/10.1002/aenm.202402489","url":null,"abstract":"Small molecule organic materials are widely used as anode materials for lithium-ion batteries (LIBs) due to their high reversible capacity, designable structure, and environmental friendliness. However, they suffer from poor intrinsic electronic conductivity, severe dissolution, and low initial coulombic efficiency. Recently, metal–organic frameworks (MOFs) have demonstrated in metal-ion batteries, outperforming some small molecule organic materials in terms of both cycling stability and rate capability. Herein, the first rational design and synthesis of a new cobalt-based MOF (CoBPDCA), are reported employing cobalt(II) nitrate as the metal source and small organic molecules (2,2-bipyridyl-4,4-dicarboxylic acid, BPDCA) as the ligands, which shows exceptional chemical stability and impressive electron conductivity. Most importantly, CoBPDCA electrodes deliver a high reversible capacity of 1112.9 mAh g<sup>−1</sup> at 0.05 C (1 C = 1000 mA g<sup>−1</sup>) and outstanding high-rate durability (166.3 mAh g<sup>−1</sup> after 2500 cycles at 10 C). Employing a series of spectroscopic and morphological characterizations and density functional theory (DFT) calculations, it is revealed that these impressively electrochemical performances are contributed to the dual active redox centers of Co cations and BPDCA ligands (<span></span>CN and <span></span>CO groups), and the superb electron conductivity. This work might provide a new strategy and a deeper understanding of the other MOFs' development for LIBs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142159036","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Sodium metal batteries (SMBs), the next-generation advanced secondary batteries, have attracted extensive attention due to their low cost and high energy density. However, the unavoidable interfacial side reactions and uncontrollable dendrite growth severely restrict their practical application. In this work, a Na (100)-textured composite anode embedded with antimony-doped tin oxide (ATO) nanoparticles (ATO-12Na) is innovatively designed via an accumulative roll bonding technique. It is observed that the Na (100) texture not only contributes to the formation of anion-derived inorganic-rich solid electrolyte interphase layer on the surface of ATO-12Na composite anode but also efficiently induces the uniform and horizontal Na deposition during the pre-deposition stage. Profiting from the intrinsic Na affinity of Na (100) texture and the high sodiophilicity of ATO active sites, the integrated composite anode exhibits enhanced interfacial compatibility and excellent Na plating/stripping stability. At 2 mA cm−2, the ATO-12Na symmetric cell can operate steadily for more than 1400 h. The full cell assembled by ATO-12Na anode and Na3V2(PO4)3 cathode delivers impressive long-term cycling stability over 4500 cycles at 500 mA g−1 with a high capacity retention of 80.7%. This study offers a new approach to designing ultra-stable, dendrite-free, and high-performance SMBs.
钠金属电池（SMB）是下一代先进的二次电池，因其低成本和高能量密度而受到广泛关注。然而，不可避免的界面副反应和不可控制的枝晶生长严重限制了其实际应用。在这项工作中，通过累积滚动键合技术，创新性地设计了一种嵌入掺锑氧化锡（ATO）纳米颗粒（ATO-12Na）的 Na (100) 纹理复合阳极。研究发现，Na（100）纹理不仅有助于在 ATO-12Na 复合阳极表面形成阴离子衍生的富含无机固体电解质的相间层，还能在预沉积阶段有效地诱导 Na 的均匀水平沉积。利用 Na (100) 纹理固有的 Na 亲和性和 ATO 活性位点的高亲钠性，集成的复合阳极表现出更强的界面相容性和优异的 Na 电镀/剥离稳定性。由 ATO-12Na 阳极和 Na3V2(PO4)3 阴极组装而成的完整电池在 500 mA g-1 下循环 4500 次以上，具有令人印象深刻的长期循环稳定性，容量保持率高达 80.7%。这项研究为设计超稳定、无树枝状突起的高性能 SMB 提供了一种新方法。
{"title":"Na (100)-Textured Electrode Embedded with Sb-Doped SnO2 Nanoparticles for Dendrite-Free Sodium Metal Batteries","authors":"Zhaopeng Li, Licheng Miao, Guangliang Lin, Wenyue Tian, Shaohui Yuan, Yuchang Si, Qinglun Wang, Lifang Jiao","doi":"10.1002/aenm.202402284","DOIUrl":"https://doi.org/10.1002/aenm.202402284","url":null,"abstract":"Sodium metal batteries (SMBs), the next-generation advanced secondary batteries, have attracted extensive attention due to their low cost and high energy density. However, the unavoidable interfacial side reactions and uncontrollable dendrite growth severely restrict their practical application. In this work, a Na (100)-textured composite anode embedded with antimony-doped tin oxide (ATO) nanoparticles (ATO-12Na) is innovatively designed via an accumulative roll bonding technique. It is observed that the Na (100) texture not only contributes to the formation of anion-derived inorganic-rich solid electrolyte interphase layer on the surface of ATO-12Na composite anode but also efficiently induces the uniform and horizontal Na deposition during the pre-deposition stage. Profiting from the intrinsic Na affinity of Na (100) texture and the high sodiophilicity of ATO active sites, the integrated composite anode exhibits enhanced interfacial compatibility and excellent Na plating/stripping stability. At 2 mA cm<sup>−2</sup>, the ATO-12Na symmetric cell can operate steadily for more than 1400 h. The full cell assembled by ATO-12Na anode and Na<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub> cathode delivers impressive long-term cycling stability over 4500 cycles at 500 mA g<sup>−1</sup> with a high capacity retention of 80.7%. This study offers a new approach to designing ultra-stable, dendrite-free, and high-performance SMBs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142159032","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Sheng Feng, Wenbo Gao, Runze Wang, Yeqin Guan, Han Wu, Qianru Wang, Hujun Cao, Lin Liu, Jianping Guo, Ping Chen
Ammonia decomposition to H2 (ADH) is one of the key reactions in the ammonia-based energy system. Recent research has been focused on developing more active and affordable catalysts, however, few can operate below 500 °C and typically require the expensive metal ruthenium. Herein, a fundamentally different thermal ADH via a chemical looping process (CLADH) mediated by alkali metal and its amide pairs, which can work under lower temperatures than the catalytic process, is reported. This CLADH consists of two steps: 1) Ammoniation step ̶ NH3 reacts with Na or K to generate NaNH2 or KNH2, respectively, accompanied by releasing one-third of H2 in NH3 at room temperature; 2) Decomposition step ̶ NaNH2 or KNH2 decomposes to N2 and H2 with the regeneration of Na or K which can be performed above 275 °C. Additionally, due to the significant enthalpy change in the two-step reactions of this CLADH, −78.0 kJ mol−1 for the first step and 123.9 kJ mol−1 for the second, using the Na and NaNH2 pair—suggest potential for thermal energy storage. This work not only reports an alternative route to produce H2 from NH3, but also unravels the potential of chemical looping process for thermal energy storage.
氨分解为 H2（ADH）是以氨为基础的能源系统中的关键反应之一。近期研究的重点是开发活性更强、价格更合理的催化剂，但能在 500 °C 以下运行的催化剂很少，而且通常需要昂贵的金属钌。本文报告了一种由碱金属及其酰胺对介导的根本不同的通过化学循环过程（CLADH）的热 ADH，它可以在比催化过程更低的温度下工作。这种 CLADH 包括两个步骤：1) 氨化步骤 ̶ NH3 与 Na 或 K 反应，分别生成 NaNH2 或 KNH2，同时在室温下释放出 NH3 中三分之一的 H2；2) 分解步骤 ̶ NaNH2 或 KNH2 分解为 N2 和 H2，Na 或 K 可以在 275 °C 以上再生。此外，由于这种 CLADH 两步反应的焓值变化很大（第一步为 -78.0 kJ mol-1，第二步为 123.9 kJ mol-1），因此使用 Na 和 NaNH2 对热能储存具有潜力。这项工作不仅报告了从 NH3 生产 H2 的另一条途径，还揭示了化学循环过程在热能储存方面的潜力。
{"title":"Chemical Looping Ammonia Decomposition Mediated by Alkali Metal and Amide Pairs for H2 Production and Thermal Energy Storage","authors":"Sheng Feng, Wenbo Gao, Runze Wang, Yeqin Guan, Han Wu, Qianru Wang, Hujun Cao, Lin Liu, Jianping Guo, Ping Chen","doi":"10.1002/aenm.202401252","DOIUrl":"https://doi.org/10.1002/aenm.202401252","url":null,"abstract":"Ammonia decomposition to H<sub>2</sub> (ADH) is one of the key reactions in the ammonia-based energy system. Recent research has been focused on developing more active and affordable catalysts, however, few can operate below 500 °C and typically require the expensive metal ruthenium. Herein, a fundamentally different thermal ADH via a chemical looping process (CLADH) mediated by alkali metal and its amide pairs, which can work under lower temperatures than the catalytic process, is reported. This CLADH consists of two steps: 1) Ammoniation step ̶ NH<sub>3</sub> reacts with Na or K to generate NaNH<sub>2</sub> or KNH<sub>2</sub>, respectively, accompanied by releasing one-third of H<sub>2</sub> in NH<sub>3</sub> at room temperature; 2) Decomposition step ̶ NaNH<sub>2</sub> or KNH<sub>2</sub> decomposes to N<sub>2</sub> and H<sub>2</sub> with the regeneration of Na or K which can be performed above 275 °C. Additionally, due to the significant enthalpy change in the two-step reactions of this CLADH, −78.0 kJ mol<sup>−1</sup> for the first step and 123.9 kJ mol<sup>−1</sup> for the second, using the Na and NaNH<sub>2</sub> pair—suggest potential for thermal energy storage. This work not only reports an alternative route to produce H<sub>2</sub> from NH<sub>3</sub>, but also unravels the potential of chemical looping process for thermal energy storage.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142159034","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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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