Pub Date : 2024-04-27DOI: 10.1016/j.gee.2024.04.009
Qigao Han, Yaqing Guo, Fuhe Wang, Xuechun Lou, Fengqian Wang, Jun Zhong, Jinqiao Du, Jie Tian, Weixin Zhang, Shun Tang, Shijie Cheng, Yuancheng Cao
Solid-state batteries (SSBs) with high safety are promising for the energy fields, but the development has long been limited by machinability and interfacial problems. Hence, supporting, Nano LLZO CSEs are prepared with a at . The contents of Nano LLZO particles enable the Nano LLZO CSEs to maintain good while exhibiting a wide electrochemical window of and a . The mean modulus reaches 4376 MPa. Benefiting from the , the Li|Li symmetric batteries based on the Nano LLZO CSEs show benign at the current densities of , , and . In addition, the Li|LiFePO (LFP) SSBs achieve favorable he specific capacity reaches at rate, with a capacity retention of about . In the further tests of the LiNiCoMnO (NCM811) cathodes with higher energy density, the Nano LLZO CSEs also demonstrate good compatibility: the specific capacities of NCM811-based SSBs reach at rate, while the capacity retention is over . Furthermore, the verify the and the potential for application, which have a desirable prospect.
{"title":"Interfacial modulation of nano Li7La3Zr2O12 composite electrolytes prepared by solvent-free method","authors":"Qigao Han, Yaqing Guo, Fuhe Wang, Xuechun Lou, Fengqian Wang, Jun Zhong, Jinqiao Du, Jie Tian, Weixin Zhang, Shun Tang, Shijie Cheng, Yuancheng Cao","doi":"10.1016/j.gee.2024.04.009","DOIUrl":"https://doi.org/10.1016/j.gee.2024.04.009","url":null,"abstract":"Solid-state batteries (SSBs) with high safety are promising for the energy fields, but the development has long been limited by machinability and interfacial problems. Hence, supporting, Nano LLZO CSEs are prepared with a at . The contents of Nano LLZO particles enable the Nano LLZO CSEs to maintain good while exhibiting a wide electrochemical window of and a . The mean modulus reaches 4376 MPa. Benefiting from the , the Li|Li symmetric batteries based on the Nano LLZO CSEs show benign at the current densities of , , and . In addition, the Li|LiFePO (LFP) SSBs achieve favorable he specific capacity reaches at rate, with a capacity retention of about . In the further tests of the LiNiCoMnO (NCM811) cathodes with higher energy density, the Nano LLZO CSEs also demonstrate good compatibility: the specific capacities of NCM811-based SSBs reach at rate, while the capacity retention is over . Furthermore, the verify the and the potential for application, which have a desirable prospect.","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":null,"pages":null},"PeriodicalIF":13.3,"publicationDate":"2024-04-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140881772","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-04-11DOI: 10.1016/j.gee.2024.04.002
Wei Li, Shu Zhang, Xinya Bu, Jing Luo, Yi Zhang, Mengyu Yan, Ting Quan, Yanli Zhu
Garnet LiLaZrO (LLZO) electrolytes have been recognized as a promising candidate to replace liquid/molten-state electrolytes in battery applications due to their exceptional performance, particularly Ga-doped LLZO (LLZGO), which exhibits high ionic conductivity. However, the limited size of the Li transport bottleneck restricts its high-current discharging performance. The present study focuses on the synthesis of Ga and Ba co-doped LLZO (LLZGBO) and investigates the influence of doping contents on the morphology, crystal structure, Li transport bottleneck size, and ionic conductivity. In particular, GaBa exhibits the highest ionic conductivity (6.11E-2 S cm at 550 °C) in comparison with other compositions, which can be attributed to its higher-energy morphology, larger bottleneck and unique Li transport channel. In addition to Ba, Sr and Ca have been co-doped with Ga into LLZO, respectively, to study the effect of doping ion radius on crystal structures and the properties of electrolytes. The characterization results demonstrate that the easier Li transport and higher ionic conductivity can be obtained when the electrolyte is doped with larger-radius ions. As a result, the assembled thermal battery with GaBa-LLZO electrolyte exhibits a remarkable voltage platform of 1.81 V and a high specific capacity of 455.65 mA h g at an elevated temperature of 525 °C. The discharge specific capacity of the thermal cell at 500 mA amounts to 63% of that at 100 mA, showcasing exceptional high-current discharging performance. When assembled as prototypes with fourteen single cells connected in series, the thermal batteries deliver an activation time of 38 ms and a discharge time of 32 s with the current density of 100 mA cm. These findings suggest that Ga, Ba co-doped LLZO solid-state electrolytes with high ionic conductivities holds great potential for high-capacity, quick-initiating and high-current discharging thermal batteries.
石榴石态 LiLaZrO（LLZO）电解质因其优异的性能，尤其是掺镓 LLZO（LLZGO）表现出的高离子电导率，已被公认为有望在电池应用中取代液态/熔融态电解质的候选材料。然而，锂传输瓶颈的有限尺寸限制了其大电流放电性能。本研究重点研究了镓和钡共掺杂 LLZO（LLZGBO）的合成，并考察了掺杂量对其形貌、晶体结构、锂传输瓶颈尺寸和离子电导率的影响。与其他成分相比，GaBa 尤其表现出最高的离子电导率（550 ℃ 时为 6.11E-2 S cm），这可归因于其较高能量的形貌、较大的瓶颈和独特的锂传输通道。除了 Ba 之外，LLZO 中还分别掺杂了 Sr 和 Ca，以研究掺杂离子半径对晶体结构和电解质性质的影响。表征结果表明，电解质中掺入较大半径的离子时，锂的传输更容易，离子电导率更高。因此，使用 GaBa-LLZO 电解质组装的热电池在 525 °C 的高温下显示出 1.81 V 的显著电压平台和 455.65 mA h g 的高比容量。热电池在 500 mA 时的放电比容量是 100 mA 时的 63%，显示出卓越的大电流放电性能。当把 14 个单体电池串联组装成原型时，热电池的激活时间为 38 毫秒，放电时间为 32 秒，电流密度为 100 毫安厘米。这些研究结果表明，具有高离子导电率的镓、钡共掺杂 LLZO 固态电解质在高容量、快速启动和大电流放电热电池方面具有巨大潜力。
{"title":"Preparation and performance of highly-conductive dual-doped Li7La3Zr2O12 solid electrolytes for thermal batteries","authors":"Wei Li, Shu Zhang, Xinya Bu, Jing Luo, Yi Zhang, Mengyu Yan, Ting Quan, Yanli Zhu","doi":"10.1016/j.gee.2024.04.002","DOIUrl":"https://doi.org/10.1016/j.gee.2024.04.002","url":null,"abstract":"Garnet LiLaZrO (LLZO) electrolytes have been recognized as a promising candidate to replace liquid/molten-state electrolytes in battery applications due to their exceptional performance, particularly Ga-doped LLZO (LLZGO), which exhibits high ionic conductivity. However, the limited size of the Li transport bottleneck restricts its high-current discharging performance. The present study focuses on the synthesis of Ga and Ba co-doped LLZO (LLZGBO) and investigates the influence of doping contents on the morphology, crystal structure, Li transport bottleneck size, and ionic conductivity. In particular, GaBa exhibits the highest ionic conductivity (6.11E-2 S cm at 550 °C) in comparison with other compositions, which can be attributed to its higher-energy morphology, larger bottleneck and unique Li transport channel. In addition to Ba, Sr and Ca have been co-doped with Ga into LLZO, respectively, to study the effect of doping ion radius on crystal structures and the properties of electrolytes. The characterization results demonstrate that the easier Li transport and higher ionic conductivity can be obtained when the electrolyte is doped with larger-radius ions. As a result, the assembled thermal battery with GaBa-LLZO electrolyte exhibits a remarkable voltage platform of 1.81 V and a high specific capacity of 455.65 mA h g at an elevated temperature of 525 °C. The discharge specific capacity of the thermal cell at 500 mA amounts to 63% of that at 100 mA, showcasing exceptional high-current discharging performance. When assembled as prototypes with fourteen single cells connected in series, the thermal batteries deliver an activation time of 38 ms and a discharge time of 32 s with the current density of 100 mA cm. These findings suggest that Ga, Ba co-doped LLZO solid-state electrolytes with high ionic conductivities holds great potential for high-capacity, quick-initiating and high-current discharging thermal batteries.","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":null,"pages":null},"PeriodicalIF":13.3,"publicationDate":"2024-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140595787","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-04-10DOI: 10.1016/j.gee.2024.04.001
Miaojie Yu, Weiwei Zhang, Xueyan Liu, Guohui Zhao, Jun Du, Yongzhen Wu, Wei-Hong Zhu
Organic nanophotocatalysts are promising candidates for solar fuels production, but they still face the challenge of unfavorable geminate recombination due to the limited exciton diffusion lengths. Here, we introduce a binary nanophotocatalyst fabricated by blending two polymers, PS-PEG5 (PS) and PBT-PEG5 (PBT), with matched absorption and emission spectra, enabling a Förster resonance energy transfer (FRET) process for enhanced photocatalysis. These heterostructure nanophotocatalysts are processed using a facile and scalable flash nanoprecipitation (FNP) technique with precious kinetic control over binary nanoparticle formation. The resulting nanoparticles exhibits an exceptional photocatalytic hydrogen evolution rate up to 65 mmol g h, 2.5 times higher than that single component nanoparticle. Characterizations through fluorescence spectra and transient absorption spectra confirm the hetero-energy transfer within the binary nanoparticles, which prolongs the excited-state lifetime and extends the namely “effective exciton diffusion length”. Our finding opens new avenues for designing efficient organic photocatalysts by improving exciton migration.
有机纳米光催化剂是太阳能燃料生产的理想候选材料，但由于激子扩散长度有限，它们仍然面临着不利的宝石化重组挑战。在这里，我们介绍了一种二元纳米光催化剂，它是由两种聚合物（PS-PEG5（PS）和 PBT-PEG5（PBT））混合制成的，这两种聚合物的吸收光谱和发射光谱相匹配，从而实现了弗斯特共振能量转移（FRET）过程，增强了光催化功能。这些异质结构纳米光催化剂是利用一种简便、可扩展的闪速纳米沉淀（FNP）技术加工而成的，对二元纳米粒子的形成具有珍贵的动力学控制。所得到的纳米粒子具有优异的光催化氢进化率，高达 65 mmol g h，是单组分纳米粒子的 2.5 倍。通过荧光光谱和瞬态吸收光谱进行的表征证实了二元纳米粒子内部的异能传递，这延长了激发态的寿命，并延长了 "有效激子扩散长度"。我们的发现为通过改善激子迁移设计高效有机光催化剂开辟了新途径。
{"title":"Energy transfer enhanced photocatalytic hydrogen evolution in organic heterostructure nanoparticles via flash nanoprecipitation processing","authors":"Miaojie Yu, Weiwei Zhang, Xueyan Liu, Guohui Zhao, Jun Du, Yongzhen Wu, Wei-Hong Zhu","doi":"10.1016/j.gee.2024.04.001","DOIUrl":"https://doi.org/10.1016/j.gee.2024.04.001","url":null,"abstract":"Organic nanophotocatalysts are promising candidates for solar fuels production, but they still face the challenge of unfavorable geminate recombination due to the limited exciton diffusion lengths. Here, we introduce a binary nanophotocatalyst fabricated by blending two polymers, PS-PEG5 (PS) and PBT-PEG5 (PBT), with matched absorption and emission spectra, enabling a Förster resonance energy transfer (FRET) process for enhanced photocatalysis. These heterostructure nanophotocatalysts are processed using a facile and scalable flash nanoprecipitation (FNP) technique with precious kinetic control over binary nanoparticle formation. The resulting nanoparticles exhibits an exceptional photocatalytic hydrogen evolution rate up to 65 mmol g h, 2.5 times higher than that single component nanoparticle. Characterizations through fluorescence spectra and transient absorption spectra confirm the hetero-energy transfer within the binary nanoparticles, which prolongs the excited-state lifetime and extends the namely “effective exciton diffusion length”. Our finding opens new avenues for designing efficient organic photocatalysts by improving exciton migration.","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":null,"pages":null},"PeriodicalIF":13.3,"publicationDate":"2024-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140595597","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-04-04DOI: 10.1016/j.gee.2024.03.006
Long Jiang, Yizhao Chai, Dongdong Ji, Liwei Li, Le Li, Bingan Lu, Dongmin Li, Jiang Zhou
Aqueous zinc-ion batteries (AZIBs) present a promising option for next-generation batteries given their high safety, eco-friendliness, and resource sustainability. Nonetheless, the practical application of zinc anodes is hindered by inevitable parasitic reactions and dendrite growth. Here, zinc alloy layers (i.e., ZnCo and ZnFe alloys) were rationally constructed on the zinc surface by chemical displacement reactions. The alloying process exposes more (002) planes of the ZnCo anode to guide the preferential and dendrite-free zinc deposition. Furthermore, the ZnCo alloy layer not only effectively inhibits water-induced side reactions but also accelerates electrode kinetics, enabling highly reversible zinc plating/stripping. As a result, the ZnCo anode achieves a Coulombic efficiency of 99.2% over 1300 cycles, and the ZnCo symmetric cell exhibits a long cycle life of over 2000 h at 4.4 mA cm. Importantly, the ZnCo//NHVO full cell retains a high discharge capacity of 218.4 mAh g after 800 cycles. Meanwhile, the ZnFe-based symmetric cell also displays excellent cycling stability over 2500 h at 1.77 mA cm. This strategy provides a facile anode modification approach toward high-performance AZIBs.
锌离子水电池（AZIBs）具有高度安全性、生态友好性和资源可持续性，是下一代电池的理想选择。然而，锌阳极的实际应用受到不可避免的寄生反应和枝晶生长的阻碍。在这里，我们通过化学置换反应在锌表面合理地构建了锌合金层（即锌钴合金和锌铁合金）。合金化过程暴露了锌钴阳极的更多 (002) 平面，从而引导了锌的优先和无枝晶沉积。此外，锌钴合金层不仅能有效抑制水引起的副反应，还能加速电极动力学，实现高度可逆的镀锌/剥离。因此，锌钴阳极在 1300 次循环中的库仑效率达到了 99.2%，锌钴对称电池在 4.4 mA cm 的条件下可实现超过 2000 小时的长循环寿命。重要的是，ZnCo//NHVO 全电池在 800 次循环后仍能保持 218.4 mAh g 的高放电容量。同时，基于锌钴的对称电池在 1.77 mA cm 的条件下也显示出了超过 2500 小时的卓越循环稳定性。这种策略为实现高性能 AZIB 提供了一种简便的阳极改性方法。
{"title":"Construction of an artificial zinc alloy layer toward stable zinc-metal anode","authors":"Long Jiang, Yizhao Chai, Dongdong Ji, Liwei Li, Le Li, Bingan Lu, Dongmin Li, Jiang Zhou","doi":"10.1016/j.gee.2024.03.006","DOIUrl":"https://doi.org/10.1016/j.gee.2024.03.006","url":null,"abstract":"Aqueous zinc-ion batteries (AZIBs) present a promising option for next-generation batteries given their high safety, eco-friendliness, and resource sustainability. Nonetheless, the practical application of zinc anodes is hindered by inevitable parasitic reactions and dendrite growth. Here, zinc alloy layers (i.e., ZnCo and ZnFe alloys) were rationally constructed on the zinc surface by chemical displacement reactions. The alloying process exposes more (002) planes of the ZnCo anode to guide the preferential and dendrite-free zinc deposition. Furthermore, the ZnCo alloy layer not only effectively inhibits water-induced side reactions but also accelerates electrode kinetics, enabling highly reversible zinc plating/stripping. As a result, the ZnCo anode achieves a Coulombic efficiency of 99.2% over 1300 cycles, and the ZnCo symmetric cell exhibits a long cycle life of over 2000 h at 4.4 mA cm. Importantly, the ZnCo//NHVO full cell retains a high discharge capacity of 218.4 mAh g after 800 cycles. Meanwhile, the ZnFe-based symmetric cell also displays excellent cycling stability over 2500 h at 1.77 mA cm. This strategy provides a facile anode modification approach toward high-performance AZIBs.","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":null,"pages":null},"PeriodicalIF":13.3,"publicationDate":"2024-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140595783","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-03-18DOI: 10.1016/j.gee.2024.03.003
Nan Song, Xingxing Li, Ebtihal Abograin, Wenyao Chen, Junbo Cao, Jing Zhang, De Chen, Xuezhi Duan, Xinggui Zhou
Essentially clearing the structure–activity relationship between iron carbide catalysts involving multiple active centers to understand the reaction mechanism of CO hydrogenation conversion process is still a great challenge. Here, two main micro-environment factors, namely electronic properties and geometrical effects were found to have an integrated effect on the mechanism of CO hydrogenation conversion, involving active sites on multiple crystal phases. The Bader charge of the surface Fe atoms on the active sites had a guiding effect on the CO activation pathway, while the spatial configuration of the active sites greatly affected the energy barriers of CO activation. Although the defective surfaces were more conducive to CO activation, the defective sites were not the only sites to dissociate CO, as CO always tended to dissociate in a wider area. This synergistic effect of the micro-environment also occurred during the CO conversion process. Surface C atoms on relatively flat configurations were more likely to form methane, while the electronic properties of the active sites could effectively describe the C-C coupling process, as well as distinguish the coupling mechanisms.
从根本上理清涉及多个活性中心的碳化铁催化剂之间的结构-活性关系，以了解 CO 加氢转化过程的反应机理，仍然是一个巨大的挑战。本研究发现，电子特性和几何效应这两大微环境因素对涉及多个晶相上活性位点的 CO 加氢转化机理具有综合影响。活性位点表面铁原子的巴德电荷对一氧化碳活化途径具有引导作用，而活性位点的空间构型则极大地影响了一氧化碳活化的能垒。虽然有缺陷的表面更有利于一氧化碳的活化，但有缺陷的位点并不是解离一氧化碳的唯一位点，因为一氧化碳总是倾向于在更大的范围内解离。微环境的这种协同效应也发生在 CO 转化过程中。相对平坦构型的表面 C 原子更有可能形成甲烷，而活性位点的电子特性可以有效地描述 C-C 耦合过程，并区分耦合机制。
{"title":"CO hydrogenation conversion driven by micro-environments of active sites over iron carbide catalysts","authors":"Nan Song, Xingxing Li, Ebtihal Abograin, Wenyao Chen, Junbo Cao, Jing Zhang, De Chen, Xuezhi Duan, Xinggui Zhou","doi":"10.1016/j.gee.2024.03.003","DOIUrl":"https://doi.org/10.1016/j.gee.2024.03.003","url":null,"abstract":"Essentially clearing the structure–activity relationship between iron carbide catalysts involving multiple active centers to understand the reaction mechanism of CO hydrogenation conversion process is still a great challenge. Here, two main micro-environment factors, namely electronic properties and geometrical effects were found to have an integrated effect on the mechanism of CO hydrogenation conversion, involving active sites on multiple crystal phases. The Bader charge of the surface Fe atoms on the active sites had a guiding effect on the CO activation pathway, while the spatial configuration of the active sites greatly affected the energy barriers of CO activation. Although the defective surfaces were more conducive to CO activation, the defective sites were not the only sites to dissociate CO, as CO always tended to dissociate in a wider area. This synergistic effect of the micro-environment also occurred during the CO conversion process. Surface C atoms on relatively flat configurations were more likely to form methane, while the electronic properties of the active sites could effectively describe the C-C coupling process, as well as distinguish the coupling mechanisms.","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":null,"pages":null},"PeriodicalIF":13.3,"publicationDate":"2024-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140153643","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
TiNbO has been emerged as one of the most promising electrode materials for high-energy lithium-ion batteries. However, limited by the slow electron/ion transport kinetics, and insufficient active sites in the bulk structure, the TiNbO electrode still suffers from unsatisfactory lithium storage performance. Herein, we demonstrate a spatially confined strategy toward a novel TiNbO-NMC/MXene composite through a triblock copolymer-directed one-pot solvothermal route, where TiNbO quantum dots with a particle size of 2-3 nm are evenly embedded into N-doped mesoporous carbon (NMC) and TiCT MXene. Impressively, the as-prepared TiNbO-NMC/MXene anode exhibits a high reversible capacity (486.2 mAh g at 0.1 A g after 100 cycles) and long cycle lifespan (363.4 mAh g at 1 A g after 500 cycles). Both experimental and theorical results further demonstrate that such a superior lithium storage performance is mainly ascribed to the synergistic effect among 0D TiNbO quantum dots, 2D TiCT MXene nanosheets, and N-doped mesoporous carbon. The strategy presented also opens up new horizon for space-confined preparation of high-performance electrode materials.
TiNbO 已成为高能锂离子电池最有前途的电极材料之一。然而，受限于缓慢的电子/离子传输动力学以及块体结构中活性位点的不足，TiNbO 电极的锂存储性能仍然不尽如人意。在本文中，我们通过三嵌段共聚物引导的一锅溶热路线，展示了一种新型 TiNbO-NMC/MXene 复合材料的空间限制策略，即将粒径为 2-3 纳米的 TiNbO 量子点均匀地嵌入 N 掺杂介孔碳（NMC）和 TiCT MXene 中。令人印象深刻的是，制备的 TiNbO-NMC/MXene 阳极具有高可逆容量（100 次循环后，0.1 A g 时为 486.2 mAh g）和长循环寿命（500 次循环后，1 A g 时为 363.4 mAh g）。实验和理论结果进一步证明，如此优异的锂存储性能主要归功于 0D TiNbO 量子点、2D TiCT MXene 纳米片和掺杂 N 的介孔碳之间的协同效应。所提出的策略也为高性能电极材料的空间封闭制备开辟了新天地。
{"title":"Spatially confined synthesis of TiNb2O7 quantum dots onto mesoporous carbon and Ti3C2TX MXene for boosting lithium storage","authors":"Daoguang Sun, Cheng Tang, Haitao Li, Xinlin Zhang, Guanjia Zhu, Zhen-Dong Huang, Aijun Du, Haijiao Zhang","doi":"10.1016/j.gee.2024.03.004","DOIUrl":"https://doi.org/10.1016/j.gee.2024.03.004","url":null,"abstract":"TiNbO has been emerged as one of the most promising electrode materials for high-energy lithium-ion batteries. However, limited by the slow electron/ion transport kinetics, and insufficient active sites in the bulk structure, the TiNbO electrode still suffers from unsatisfactory lithium storage performance. Herein, we demonstrate a spatially confined strategy toward a novel TiNbO-NMC/MXene composite through a triblock copolymer-directed one-pot solvothermal route, where TiNbO quantum dots with a particle size of 2-3 nm are evenly embedded into N-doped mesoporous carbon (NMC) and TiCT MXene. Impressively, the as-prepared TiNbO-NMC/MXene anode exhibits a high reversible capacity (486.2 mAh g at 0.1 A g after 100 cycles) and long cycle lifespan (363.4 mAh g at 1 A g after 500 cycles). Both experimental and theorical results further demonstrate that such a superior lithium storage performance is mainly ascribed to the synergistic effect among 0D TiNbO quantum dots, 2D TiCT MXene nanosheets, and N-doped mesoporous carbon. The strategy presented also opens up new horizon for space-confined preparation of high-performance electrode materials.","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":null,"pages":null},"PeriodicalIF":13.3,"publicationDate":"2024-03-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140153624","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Mixed matrix membranes (MMMs) have demonstrated significant promise in energy-intensive gas separations by amalgamating the unique properties of fillers with the facile processability of polymers. However, achieving a simultaneous enhancement of permeability and selectivity remains a formidable challenge, due to the difficulty of achieving an optimal match between polymers and fillers. In this study, we incorporate a porous carbon-based zinc oxide composite (C@ZnO) into high-permeability polymers of intrinsic microporosity (PIMs) to fabricate MMMs. The dipole–dipole interaction between C@ZnO and PIMs ensures their exceptional compatibility, mitigating the formation of non-selective voids in the resulting MMMs. Concurrently, C@ZnO with abundant interconnected pores can provide additional low-resistance pathways for gas transport in MMMs. As a result, the CO permeability of the optimized C@ZnO/PIM-1 MMMs is elevated to 13,215 barrer, while the CO/N and COCH selectivity reached 21.5 and 14.4, respectively, substantially surpassing the 2008 Robeson upper bound. Additionally, molecular simulation results further corroborate that the augmented membrane gas selectivity is attributed to the superior CO affinity of C@ZnO. In summary, we believe that this work not only expands the application of MMMs for gas separation but also heralds a paradigm shift in the application of porous carbon materials.
{"title":"Merging polymers of intrinsic microporosity and porous carbon-based zinc oxide composites in novel mixed matrix membranes for efficient gas separation","authors":"Muning Chen, Jiemei Zhou, Jing Ma, Weigang Zheng, Guanying Dong, Xin Li, Zhihong Tian, Yatao Zhang, Jing Wang, Yong Wang","doi":"10.1016/j.gee.2024.03.002","DOIUrl":"https://doi.org/10.1016/j.gee.2024.03.002","url":null,"abstract":"Mixed matrix membranes (MMMs) have demonstrated significant promise in energy-intensive gas separations by amalgamating the unique properties of fillers with the facile processability of polymers. However, achieving a simultaneous enhancement of permeability and selectivity remains a formidable challenge, due to the difficulty of achieving an optimal match between polymers and fillers. In this study, we incorporate a porous carbon-based zinc oxide composite (C@ZnO) into high-permeability polymers of intrinsic microporosity (PIMs) to fabricate MMMs. The dipole–dipole interaction between C@ZnO and PIMs ensures their exceptional compatibility, mitigating the formation of non-selective voids in the resulting MMMs. Concurrently, C@ZnO with abundant interconnected pores can provide additional low-resistance pathways for gas transport in MMMs. As a result, the CO permeability of the optimized C@ZnO/PIM-1 MMMs is elevated to 13,215 barrer, while the CO/N and COCH selectivity reached 21.5 and 14.4, respectively, substantially surpassing the 2008 Robeson upper bound. Additionally, molecular simulation results further corroborate that the augmented membrane gas selectivity is attributed to the superior CO affinity of C@ZnO. In summary, we believe that this work not only expands the application of MMMs for gas separation but also heralds a paradigm shift in the application of porous carbon materials.","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":null,"pages":null},"PeriodicalIF":13.3,"publicationDate":"2024-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140153570","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
High-energy-density lithium (Li)–air cells have been considered a promising energy-storage system, but the liquid electrolyte-related safety and side-reaction problems seriously hinder their development. To address these above issues, solid-state Li–air batteries have been widely developed. However, many commonly-used solid electrolytes generally face huge interface impedance in Li–air cells and also show poor stability towards ambient air/Li electrodes. Herein, we fabricate a differentiating surface-regulated ceramic-based composite electrolyte (DSCCE) by constructing disparately LiI-containing polymethyl methacrylate (PMMA) coating and Poly (vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) layer on both sides of LiAlGe(PO) (LAGP). The cathode-friendly LiI/PMMA layer displays excellent stability towards O and also greatly reduces the decomposition voltage of discharge products in Li–air system. Additionally, the anode-friendly PVDF-HFP coating shows low-resistance properties towards anodes. Moreover, Li dendrite/passivation derived from liquid electrolyte-induced side reactions and air/I-attacking can be obviously suppressed by the uniform and compact composite framework. As a result, the DSCCE-based Li–air batteries possess high capacity/low voltage polarization (11,836 mA h g/1.45 V under 500 mA g), good rate performance (capacity ratio under 1000 mA g/250 mA g is 68.2%) and long-term stable cell operation (300 cycles at 750 mA g with 750 mAh g) in ambient air.
高能量密度锂（Li）-空气电池一直被认为是一种前景广阔的储能系统，但与液态电解质相关的安全和副反应问题严重阻碍了其发展。为了解决上述问题，固态锂空气电池得到了广泛开发。然而，许多常用的固态电解质在锂空气电池中普遍面临着巨大的界面阻抗，而且对环境空气/锂电极的稳定性也很差。在此，我们通过在 LiAlGe(PO) (LAGP) 两面构建不同的含 LiI 的聚甲基丙烯酸甲酯 (PMMA) 涂层和聚（偏氟乙烯-共六氟丙烯）（PVDF-HFP）层，制备了一种差异化表面调控陶瓷基复合电解质 (DSCCE)。阴极友好型 LiI/PMMA 层对 O 具有极佳的稳定性，同时还大大降低了锂空气系统中放电产物的分解电压。此外，阳极友好型 PVDF-HFP 涂层显示出对阳极的低电阻特性。此外，均匀紧凑的复合框架还能明显抑制液态电解质引起的副反应和空气/I 侵蚀所导致的锂枝晶/钝化。因此，基于 DSCCE 的锂空气电池在环境空气中具有高容量/低压极化（500 mA g 下为 11,836 mA h g/1.45 V）、良好的速率性能（1000 mA g/250 mA g 下容量比为 68.2%）和长期稳定的电池运行（750 mA g 下循环 300 次，750 mAh g）。
{"title":"Design of Multifunctional Interfaces on Ceramic Solid Electrolytes for High-Performance Lithium-Air Batteries","authors":"Yunxin Shi, Ziyang Guo, Changhong Wang, Mingze Gao, Xiaoting Lin, Hui Duan, Yonggang Wang, Xueliang Sun","doi":"10.1016/j.gee.2024.02.010","DOIUrl":"https://doi.org/10.1016/j.gee.2024.02.010","url":null,"abstract":"High-energy-density lithium (Li)–air cells have been considered a promising energy-storage system, but the liquid electrolyte-related safety and side-reaction problems seriously hinder their development. To address these above issues, solid-state Li–air batteries have been widely developed. However, many commonly-used solid electrolytes generally face huge interface impedance in Li–air cells and also show poor stability towards ambient air/Li electrodes. Herein, we fabricate a differentiating surface-regulated ceramic-based composite electrolyte (DSCCE) by constructing disparately LiI-containing polymethyl methacrylate (PMMA) coating and Poly (vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) layer on both sides of LiAlGe(PO) (LAGP). The cathode-friendly LiI/PMMA layer displays excellent stability towards O and also greatly reduces the decomposition voltage of discharge products in Li–air system. Additionally, the anode-friendly PVDF-HFP coating shows low-resistance properties towards anodes. Moreover, Li dendrite/passivation derived from liquid electrolyte-induced side reactions and air/I-attacking can be obviously suppressed by the uniform and compact composite framework. As a result, the DSCCE-based Li–air batteries possess high capacity/low voltage polarization (11,836 mA h g/1.45 V under 500 mA g), good rate performance (capacity ratio under 1000 mA g/250 mA g is 68.2%) and long-term stable cell operation (300 cycles at 750 mA g with 750 mAh g) in ambient air.","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":null,"pages":null},"PeriodicalIF":13.3,"publicationDate":"2024-03-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140037378","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-03-02DOI: 10.1016/j.gee.2024.02.009
Wei Wu, Zhenglin Hu, Zhengfei Zhao, Aoxuan Wang, Jiayan Luo
Hard carbon (HC) is widely used in sodium-ion batteries (SIBs), but its performance has always been limited by low initial Coulombic efficiency (ICE) and cycling stability. Cathode compensation agent is a favorable strategy to make up for the loss of active sodium ions consumed by HC anode. Yet it lacks agent that effectively decomposes to increase the active sodium ions as well as regulate carbon defects for decreasing the irreversible sodium ions consumption. Here, we propose 1,2-dihydroxybenzene Na salt (NaDB) as a cathode compensation agent with high specific capacity (347.9 mAh g), lower desodiation potential (2.4–2.8 V) and high utilization (99%). Meanwhile, its byproduct could functionalize HC with more CO groups and promotes its reversible capacity. Consequently, the presodiation hard carbon (pHC) anode exhibits highly reversible capacity of 204.7 mAh g with 98% retention at 5 C rate over 1000 cycles. Moreover, with 5 wt% NaDB initially coated on the NaV(PO) (NVP) cathode, the capacity retention of NVP + NaDB|HC cell could increase form 36%–89% after 1000 cycles at 1 C rate. This work provides a new avenue to improve SIBs reversible capacity and cycling performance through designing functional cathode compensation agent.
硬碳（HC）被广泛应用于钠离子电池（SIB），但其性能一直受到初始库仑效率（ICE）和循环稳定性较低的限制。阴极补偿剂是弥补碳氢化合物阳极消耗的活性钠离子损失的有利策略。然而，目前缺乏既能有效分解以增加活性钠离子，又能调节碳缺陷以减少不可逆钠离子消耗的药剂。在此，我们提出了 1,2-二羟基苯 Na 盐（NaDB）作为阴极补偿剂，它具有较高的比容量（347.9 mAh g）、较低的解碘电位（2.4-2.8 V）和较高的利用率（99%）。同时，其副产物可使碳氢化合物具有更多的 CO 基团，从而提高其可逆容量。因此，预阳极化硬碳（pHC）阳极在 5 C 速率下可在 1000 次循环中显示出 204.7 mAh g 的高可逆容量和 98% 的保持率。此外，在 NaV(PO)（NVP）阴极上涂覆 5 wt% 的 NaDB 后，NVP + NaDB|HC 电池在 1 C 速率下循环 1000 次后，容量保持率可提高 36%-89%。这项工作为通过设计功能性阴极补偿剂来提高 SIB 的可逆容量和循环性能提供了一条新途径。
{"title":"A Functional Cathode Sodium Compensation Agent for Stable Sodium-Ion Batteries","authors":"Wei Wu, Zhenglin Hu, Zhengfei Zhao, Aoxuan Wang, Jiayan Luo","doi":"10.1016/j.gee.2024.02.009","DOIUrl":"https://doi.org/10.1016/j.gee.2024.02.009","url":null,"abstract":"Hard carbon (HC) is widely used in sodium-ion batteries (SIBs), but its performance has always been limited by low initial Coulombic efficiency (ICE) and cycling stability. Cathode compensation agent is a favorable strategy to make up for the loss of active sodium ions consumed by HC anode. Yet it lacks agent that effectively decomposes to increase the active sodium ions as well as regulate carbon defects for decreasing the irreversible sodium ions consumption. Here, we propose 1,2-dihydroxybenzene Na salt (NaDB) as a cathode compensation agent with high specific capacity (347.9 mAh g), lower desodiation potential (2.4–2.8 V) and high utilization (99%). Meanwhile, its byproduct could functionalize HC with more CO groups and promotes its reversible capacity. Consequently, the presodiation hard carbon (pHC) anode exhibits highly reversible capacity of 204.7 mAh g with 98% retention at 5 C rate over 1000 cycles. Moreover, with 5 wt% NaDB initially coated on the NaV(PO) (NVP) cathode, the capacity retention of NVP + NaDB|HC cell could increase form 36%–89% after 1000 cycles at 1 C rate. This work provides a new avenue to improve SIBs reversible capacity and cycling performance through designing functional cathode compensation agent.","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":null,"pages":null},"PeriodicalIF":13.3,"publicationDate":"2024-03-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140036479","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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