Energy Storage Materials最新文献_第6页

Ion-selective gel polymer electrolyte and cathode binder derived from a shared polyether to synergistically mitigate polysulfides shuttling in lithium sulfur batteries 离子选择性凝胶聚合物电解质和正极粘合剂源自共用聚醚，可协同缓解锂硫电池中的多硫化物穿梭现象

IF 18.9 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2024-11-01 DOI: 10.1016/j.ensm.2024.103870

Mingjia Lu , Kai Chen , Zhenyu Jia , Jianguo Ren , Peng He , Shengyuan Yang , Roohollah Bagherzadeh , Feili Lai , Yue-E Miao , Tianxi Liu

As one kind of the most promising candidates for next-generation batteries, lithium-sulfur (Li-S) batteries with high theoretical energy density are still faced with the severe shuttle effect of polysulfides (PS) and safety issues caused by the flammable liquid electrolytes. To overcome the above challenges, an enhanced ion-selective strategy is proposed by collaboratively crosslinking a polyether containing epoxy groups with negatively charged aminated sodium lignosulfonate (ASL) and polar phytic acid (PA), respectively, to prepare a PS-repelling gel polymer electrolyte (AGPE) and a PS-anchoring cathode binder (PMG-PA) for Li-S batteries. The synergistically suppressed shuttle effect of PS makes the Li-S battery deliver a high capacity of 749.7 mAh g^-1 over 200 cycles at 1 C with a super low capacity decay of 0.11 % per cycle, compared to the poor cycling performance (329.1 mAh g^-1 over 200 cycles with a capacity decay of 0.26 % per cycle) of the conventional liquid electrolyte-based battery using polyvinylidene difluoride as the cathode binder. Furthermore, AGPE confines the liquid electrolyte within the polymer network, while ASL quenches free radicals during potential ignition events, thereby significantly enhancing the battery safety during operation. Therefore, the co-design strategy of ion-selective AGPE and PMG-PA cathode binder derived from a shared polyether offers a new way to mitigate polysulfides shuttling for safe and reliable Li-S batteries.

锂硫（Li-S）电池作为下一代电池最有前途的候选材料之一，具有很高的理论能量密度，但仍然面临着多硫化物（PS）的严重穿梭效应和易燃液态电解质带来的安全问题。为了克服上述挑战，我们提出了一种增强离子选择性的策略，通过将含有环氧基团的聚醚分别与带负电荷的胺化木质素磺酸钠（ASL）和极性植酸（PA）协同交联，制备出用于锂-S电池的PS排斥凝胶聚合物电解质（AGPE）和PS锚定阴极粘结剂（PMG-PA）。与使用聚偏二氟乙烯作为阴极粘合剂的传统液态电解质电池循环性能较差（200 次循环为 329.1 mAh g-1，每次循环容量衰减 0.26%）相比，PS 的协同抑制穿梭效应使得锂-S 电池在 1 C 下循环 200 次可输出 749.7 mAh g-1 的高容量，且每次循环容量衰减 0.11% 的超低容量。此外，AGPE 可将液态电解质限制在聚合物网络中，而 ASL 可在潜在点火事件中熄灭自由基，从而显著提高电池在运行期间的安全性。因此，离子选择性 AGPE 和源自共用聚醚的 PMG-PA 阴极粘合剂的协同设计策略为减轻多硫化物穿梭提供了一种新方法，可用于制造安全可靠的锂-S 电池。

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引用次数: 0

Copper-induced lattice distortion in Na4Fe3(PO4)2(P2O7) cathode enabling high power density Na-ion batteries with good cycling stability Na4Fe3(PO4)2(P2O7)阴极中铜诱导的晶格畸变可实现具有良好循环稳定性的高功率密度钠离子电池

IF 18.9 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2024-11-01 DOI: 10.1016/j.ensm.2024.103861

Xinran Qi , Qingyu Dong , Hanghang Dong , Baoxiu Hou , Haiyan Liu , Ningzhao Shang , Shuaihua Zhang , Longgang Wang , Hui Shao , Yanbin Shen , Shuangqiang Chen , Xiaoxian Zhao

Na₄Fe₃(PO₄)₂P₂O₇ (NFPP) has attracted attention due to its high theoretical capacity, low cost, and good structure stability for Na-ion batteries. However, its practical application is limited by the low intrinsic electronic conductivity and sluggish ion diffusion kinetics. To tackle those problems, lattice strain engineering by heteroatom doping is applied to tune the local molecular structure and optimize the electrochemical properties of electrode materials. Copper cation (+2) with a smaller ionic radius was chosen to dope at Fe-site in NFPP, and the doping amount was also optimized, illustrating the optimized sample of Na₄Fe_2.7Cu_0.3(PO₄)₂P₂O₇ (NFPP-0.3Cu) delivered a high capacity of 119.01 mAh g^-1 at 1 C (1 C = 129 mA g^-1) and a high capacity retention of 82.76 % after 3000 cycles at 20 C. Notably, full cells with NFPP-0.3 Cu as cathode and hard carbon as anode delivered a high energy density of 230 Wh kg^-1 and a power density of 2280 W kg^-1. The exceptional electrochemical performances are attributed to the modulated electronic structure and abundant lattice defects by Cu-doping. Furthermore, in-situ X-ray diffraction technique and theoretical calculation have jointly proved that the lattice distortions originated from Cu-doping have reduced the band gap of the NFPP-0.3Cu and altered the coordination environment of Fe, shortening the Fe-O and Cu-O bond lengths, significantly enhancing the intrinsic ionic conductivity and the diffusion kinetics of Na⁺. This work provides new point of views on lattice strain engineering and reaction kinetics of cathode materials in promoting high energy and power density sodium-ion batteries.

Na4Fe3(PO4)2P2O7（NFPP）因其理论容量高、成本低、结构稳定性好而备受关注。然而，由于其内在电子电导率低和离子扩散动力学缓慢，其实际应用受到了限制。为了解决这些问题，人们采用杂原子掺杂的晶格应变工程来调整局部分子结构，优化电极材料的电化学性能。选择离子半径较小的铜阳离子（+2）掺杂到 NFPP 中的 Fe 位上，并优化了掺杂量，结果表明，Na4Fe2.7Cu0.3(PO4)2P2O7（NFPP-0.3Cu）的优化样品在 1°C 时的电容量高达 119.值得注意的是，以 NFPP-0.3Cu 为阴极、硬质碳为阳极的全电池可提供 230 Wh kg-1 的高能量密度和 2280 W kg-1 的功率密度。优异的电化学性能归功于铜掺杂调制的电子结构和丰富的晶格缺陷。此外，原位 X 射线衍射技术和理论计算共同证明，掺杂 Cu 所产生的晶格畸变降低了 NFPP-0.3Cu 的带隙，改变了 Fe 的配位环境，缩短了 Fe-O 和 Cu-O 键长，显著提高了本征离子电导率和 Na+ 扩散动力学。这项工作为晶格应变工程和正极材料的反应动力学提供了新的视角，有助于促进高能量和高功率密度钠离子电池的发展。

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引用次数: 0

Artificial intelligence in rechargeable battery: Advancements and prospects 可充电电池中的人工智能：进步与前景

IF 18.9 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2024-11-01 DOI: 10.1016/j.ensm.2024.103860

Yige Xiong , Die Zhang , Xiaorong Ruan , Shanbao Jiang , Xueqin Zou , Wei Yuan , Xiuxue Liu , Yapeng Zhang , Zeqi Nie , Donghai Wei , Yubin Zeng , Peng Cao , Guanhua Zhang

Advanced rechargeable battery technologies are the primary source of energy storage, which hold significant promise for tackling energy challenges. However, the progress of these technologies is affected by various factors, including technical and capital investment challenges. The technical challenges primarily involve performance optimization. Artificial intelligence (AI), with its robust data processing and decision-making capabilities, is poised to promote the high-quality and rapid development of rechargeable battery research. This paper begins by elucidating the key techniques and fundamental framework of AI, then summarizes applications of AI in advanced battery research. Subsequently, critical applications and exemplary research advancements of AI techniques in various batteries are presented. Finally, potential issues and future development directions of AI technologies in facilitating the development of batteries are discussed. This review offers guidance for applications of AI techniques in future research on advanced batteries.

先进的可充电电池技术是能源储存的主要来源，在应对能源挑战方面大有可为。然而，这些技术的进展受到各种因素的影响，包括技术和资本投资方面的挑战。技术挑战主要涉及性能优化。人工智能（AI）具有强大的数据处理和决策能力，有望促进充电电池研究的高质量和快速发展。本文首先阐明了人工智能的关键技术和基本框架，然后总结了人工智能在先进电池研究中的应用。随后，介绍了人工智能技术在各种电池中的关键应用和示范性研究进展。最后，讨论了人工智能技术在促进电池发展方面的潜在问题和未来发展方向。本综述为人工智能技术在未来先进电池研究中的应用提供了指导。

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引用次数: 0

Turning crisis into opportunity: Intrinsically polarised low concentration eutectic electrolytes enable highly reversible zinc anodes 化危机为机遇：本征极化低浓度共晶电解质实现了锌阳极的高度可逆性

IF 18.9 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2024-11-01 DOI: 10.1016/j.ensm.2024.103866

Wenruo Li , Luzheng Zhao , Jiancong Guo, Haoyuan Zhu, Wei Liu, Weiqiang Kong, Farva Ilyas, Xu Han, Liying Cui, Zhongsheng Wen

Low-concentration electrolytes (LCEs) hold great promise for sustainable energy storage due to their low viscosity, excellent wettability, and cost-effectiveness. However, their intrinsic polarization issues often lead to side reactions and dendrite growth, hindering their broader application. Herein, we present an approach to convert the negative effects of intrinsic polarization in LCEs into advantages, overcoming these challenges. The experimental and theoretical analyses demonstrate that acetate-adsorbed zinc anodes can harness the intrinsic polarization of LCEs to direct the electrocrystallization process on their surfaces. This promotes the preferential orientation of Zn(002) plane with high stability, resulting in symmetric batteries loaded with low-concentration eutectic electrolytes (LCEE) that maintain surprisingly low voltage polarization during the dendrite-free growth of up to 3150 h. In addition, by forming an organic-inorganic composite film enriched with N and Cl, LCEE achieves rapid migration of Zn²⁺. This allows Zn//PANI full batteries with LCEE to demonstrate superior capacity and cycling stability compared to other Zn-based batteries with LCEs. This study not only achieves a divergent design in LCEs but also provides clear guidance for future electrolyte development.

低浓度电解质（LCE）具有低粘度、出色的润湿性和成本效益，因此在可持续能源储存方面大有可为。然而，其固有的极化问题往往会导致副反应和枝晶生长，从而阻碍其更广泛的应用。在此，我们提出了一种方法，将 LCE 固有极化的负面影响转化为优势，从而克服这些挑战。实验和理论分析表明，醋酸盐吸附锌阳极可以利用 LCE 的固有极化来引导其表面的电晶化过程。这促进了具有高稳定性的 Zn(002) 平面的优先取向，从而使装载了低浓度共晶电解质 (LCEE) 的对称电池在长达 3150 小时的无枝晶生长过程中保持了惊人的低电压极化。因此，与其他含有 LCE 的锌基电池相比，含有 LCEE 的 Zn//PANI 全电池具有更高的容量和循环稳定性。这项研究不仅实现了 LCE 的差异化设计，还为未来的电解质开发提供了明确的指导。

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引用次数: 0

Solvation and interface engineering for stable operation of lithium metal batteries under harsh conditions 溶解和界面工程技术促进锂金属电池在恶劣条件下稳定运行

IF 18.9 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2024-11-01 DOI: 10.1016/j.ensm.2024.103875

Yehui Wu , Xihao Wang , Kun Zhang , Hankun Wang , Xingyu Ma , Shengchuang Du , Tiansheng Bai , Jiawen Huang , Deping Li , Lijie Ci , Jingyu Lu

Stable operation of lithium (Li) metal batteries (LMBs) under harsh conditions (e.g., at high rates, at extreme temperatures, and with water-containing electrolytes) has been suffering from the sluggish charge transfer kinetics at electrode-electrolyte interfaces, and limited thermodynamic stability in general carbonate electrolytes. Herein, lithium nitrate (LiNO₃) and N,N’-dimethylpropyleneure (DMPU) are incorporated into a commercial carbonate electrolyte to address these challenges, it significantly changed the electrolyte solvation chemistry to enhance the electrolyte's moisture tolerance and thermal stability, and lead to nitrided interfaces (including inorganic and organic nitrides) that boost interfacial kinetics and stability. Consequently, the excellent electrochemical performance is achieved with Li||Li symmetric cells, Li||Cu half cells, and Li||LiFePO₄ full cells, under harsh conditons. The Li||LiFePO₄ full cell shows a capacity retention of ∼86.0 % after 8100 cycles at 30C, and they could even cycle stably at temperatures as high as 60 °C and as low as −15 °C; besides, even if using the electrolyte containing 2 % water, the full cell delivers a capacity retention of ∼95.3 % after 5000 cycles at 10C. This work elucidates the correlations between electrolyte solvation chemistry, electrode interface composition, and battery performance, paving a way for realising stable LMBs under harsh conditions.

锂（Li）金属电池（LMB）在苛刻条件下（如高倍率、极端温度和含水电解质）的稳定运行一直受到电极-电解质界面电荷转移动力学迟缓和一般碳酸盐电解质热力学稳定性有限的影响。为了解决这些问题，我们在商用碳酸盐电解质中加入了硝酸锂（LiNO3）和N,N'-二甲基丙烯脲（DMPU），这极大地改变了电解质的溶解化学性质，增强了电解质的耐湿性和热稳定性，并形成了氮化界面（包括无机和有机氮化物），提高了界面动力学和稳定性。因此，在苛刻的条件下，锂||锂对称电池、锂||铜半电池和锂||锂铁PO4全电池都能实现优异的电化学性能。在 30C 温度下循环 8100 次后，||LiFePO4 全电池的容量保持率可达 86.0%，甚至可以在高达 60°C 和低至 -15°C 的温度下稳定循环；此外，即使使用含 2% 水的电解液，在 10C 温度下循环 5000 次后，全电池的容量保持率也可达 95.3%。这项工作阐明了电解质溶解化学、电极界面成分和电池性能之间的相关性，为在恶劣条件下实现稳定的 LMB 铺平了道路。

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引用次数: 0

In-situ construction of an alloy hybrid interface and ultrathin ZnS nanosheets catalyst for polysulfide by trifunctional ZnI2 electrolyte additive for Li-S batteries 利用三官能 ZnI2 电解质添加剂原位构建合金杂化界面和超薄 ZnS 纳米片催化剂用于锂-S 电池

IF 18.9 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2024-11-01 DOI: 10.1016/j.ensm.2024.103862

Zehua Zhao , Bezawit Z. Desalegn , Hye Jeong Joe , Seok Ki Kim , Jungho Yoo , Deyu Wang , Jeong Gil Seo

Lithium-sulfur batteries (LSBs) are considered promising candidates for next-generation energy storage devices owing to their ultrahigh theoretical energy density. However, LSBs are hindered by uncontrollable lithium dendrite growth, polysulfides shuttle effects, and sluggish sulfur kinetics. Herein, this work develops a multifunctional ZnI₂ electrolyte additive for LSB for local high concentration base electrolyte. At anode side, a Li_xZn alloy hybrid interface leading to planar deposited lithium is formed from the reaction between Li metal and the ZnI₂ additive and reduction products of Li⁺ solvation shell of the electrolyte. Moreover, planar deposited lithium was confirmed by in-situ liquid transmission electron microscopy (TEM). For cathode side, Zn²⁺ under the drive of electric field prior react with lithium polysulfide to form ultrathin ZnS nanosheets exposed with (100) miller index serving as a catalyst to accelerate sulfur redox kinetics and inhibit polysulfides shuttling. Consequently, the LSB with ZnI₂ additive exhibits a remarkable discharge capacity of 712 mA h g⁻¹ at 0.5 C after 300 cycles and a superior rate capability of 674.9 mA h g⁻¹ at 2 C. This work demonstrates that ZnI₂ serves as a multifunctional electrolyte additive to simultaneously facilitate the sulfur redox kinetics, reduce the shuttle effect, and promote smooth Li growth.

锂硫电池（LSB）具有超高的理论能量密度，因此被认为是下一代储能设备的理想候选材料。然而，锂硫电池受制于无法控制的锂枝晶生长、多硫化物穿梭效应以及缓慢的硫动力学。为此，本研究开发了一种多功能 ZnI2 电解质添加剂，用于局部高浓度碱电解质的 LSB。在阳极侧，金属锂与 ZnI2 添加剂的反应以及电解液中 Li+ 溶解壳的还原产物形成了 LixZn 合金混合界面，从而导致锂的平面沉积。此外，原位液态透射电子显微镜（TEM）也证实了锂的平面沉积。在阴极侧，Zn2+ 在电场的驱动下先与多硫化锂发生反应，形成超薄的 ZnS 纳米片，其磨矿指数为（100），可作为催化剂加速硫氧化还原动力学并抑制多硫化物的穿梭。因此，添加了 ZnI2 添加剂的 LSB 在 0.5 C 条件下循环 300 次后，放电容量达到了 712 mA h g-1，在 2 C 条件下，放电速率达到了 674.9 mA h g-1。这项工作表明，ZnI2 是一种多功能电解质添加剂，可同时促进硫氧化还原动力学、降低穿梭效应并促进锂的顺利生长。

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引用次数: 0

Revealing stable organic cathode/solid electrolyte interface to promote all-solid-state sodium batteries using organic cathodes 揭示稳定的有机阴极/固体电解质界面，促进使用有机阴极的全固态钠电池的发展

IF 18.9 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2024-11-01 DOI: 10.1016/j.ensm.2024.103857

Shuaishuai Yang , Changxiang Shao , Xiong Xiao , Debao Fang , Na Li , Enyue Zhao , Chengzhi Wang , Lai Chen , Ning Li , Jingbo Li , Yuefeng Su , Haibo Jin

All-solid-state sodium batteries (ASSBs) offer an attractive low-cost and high-safety power source for vehicles and stationary power plants beyond of lithium-based batteries. Currently, their application is limited by the rigid solid electrolyte (SE)/electrode contact interface which causes large interfacial resistance and poor cycling stability. Here we reveal a soft perylene-3,4,9,10-tetracarboxylic dianhydride (PTCDA) as a representative organic cathode material shows good mechanical and electrochemical compatibility with a rigid inorganic Na₃Zr₂Si₂PO₁₂ SE, thus can promote the ASSBs using organic cathodes. Specifically, all-solid-state PTCDA/Na₃Zr₂Si₂PO₁₂/sodium batteries are assembled which show a smaller charge transfer resistance of 310 Ω cm² at 25 °C than that (460 Ω cm²) of the PTCDA//sodium batteries using a conventional liquid electrolyte. Moreover, the all-solid-state sodium battery delivers an initial capacity of 120.8 mAh g^-1, and achieves a retention of 73.4% over 500 cycles at 200 mA g^-1, while the liquid battery shows quick capacity decay after the 50th cycles. This work demonstrates an effective strategy by combining a soft cathode with a rigid solid electrolyte to overcome the interfacial issues of ASSBs, and will promote the development of ASSBs using diverse cathodes of low cost, high specific capacity, and long-term reliability.

全固态钠电池（ASSB）为车辆和固定发电厂提供了一种具有吸引力的低成本、高安全性的电源，超越了锂电池。目前，它们的应用受到刚性固体电解质（SE）/电极接触界面的限制，这导致了较大的界面电阻和较差的循环稳定性。在此，我们揭示了以软质过烯-3,4,9,10-四羧酸二酐（PTCDA）为代表的有机阴极材料与刚性无机 Na3Zr2Si2PO12 SE 之间良好的机械和电化学相容性，从而促进了使用有机阴极的 ASSB 的发展。具体来说，组装出的全固态 PTCDA/Na3Zr2Si2PO12 钠电池在 25 °C 时的电荷转移电阻为 310 Ω cm2，小于使用传统液态电解质的 PTCDA//钠电池的电荷转移电阻（460 Ω cm2）。此外，全固态钠电池的初始容量为 120.8 mAh g-1，在 200 mA g-1 的条件下循环 500 次后容量保持率达到 73.4%，而液态电池在循环 50 次后容量迅速衰减。这项工作展示了一种将软阴极与刚性固体电解质相结合的有效策略，从而克服了 ASSB 的界面问题，并将促进使用低成本、高比容量和长期可靠性的多样化阴极开发 ASSB。

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引用次数: 0

For elements-utilization regeneration of spent LiFePO4: Designed basic precursors for advanced polycrystal electrode materials 废旧磷酸铁锂的元素利用再生：先进多晶电极材料的基础前驱体设计

IF 18.9 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2024-10-30 DOI: 10.1016/j.ensm.2024.103863

Shuya Lei , Wenqing Zhao , Jiexiang Li , Shaole Song , Wei Sun , Peng Ge , Yue Yang

Spent lithium iron phosphate (LFP) is commonly recovered by hydrometallurgy to prepare Li₂CO₃ and FePO₄, but suffering from long process and low value-added products. Hydrothermal method avoids element separation and regenerates LFP materials directly from leaching solution of spent LFP. However, it requires three-time the theoretical amount of lithium. In this study, using LiFePO₄(OH) (LFPOH) as a medium, LFP materials were regenerated with theoretical amount of lithium in virtue of energetically favorable reaction of Li-ions into the internal structure. The formation mechanism of LFPOH and LFP materials were investigated, and advanced polycrystal LFP materials with fast ions-diffusion ability and high reversibility were obtained. The capacities of recovered LFP materials are 156.17 mAh g⁻¹, 148.51 mAh g⁻¹, 138.34 mAh g⁻¹, 124.1 mAh g⁻¹ at 0.2 C, 0.5 C, 1 C and 2 C, respectively and their capacity could be remained 139.92 mAh g⁻¹ at 1 C with retention of almost 100 % after 200 cycles. Moreover, with the assistance of economic analysis, the designed regenerated path displayed considerable recycling value-potential, especially the reducing of Li-resources (from three-time to one-time). This study sheds light on designing polycrystal recovered LFP with help of basic medium, whilst provides an effective strategy for preparing high-performance LFP materials.

废磷酸铁锂（LFP）通常通过湿法冶金回收制备 Li2CO3 和 FePO4，但工艺流程长，产品附加值低。水热法避免了元素分离，可直接从废磷酸铁锂电池的浸出液中再生出磷酸铁锂电池材料。然而，这种方法需要三倍于理论量的锂。本研究以 LiFePO4(OH)（LFPOH）为介质，利用锂离子进入内部结构的有利能量反应，以理论锂量再生 LFP 材料。研究了 LFPOH 和 LFP 材料的形成机理，获得了具有快速离子扩散能力和高可逆性的先进多晶 LFP 材料。回收的 LFP 材料在 0.2 C、0.5 C、1 C 和 2 C 下的容量分别为 156.17 mAh g-1、148.51 mAh g-1、138.34 mAh g-1、124.1 mAh g-1，在 1 C 下可保持 139.92 mAh g-1，循环 200 次后容量保持率接近 100%。这项研究揭示了如何借助基本介质设计多晶回收锂离子电池，同时为制备高性能锂离子电池材料提供了有效策略。

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引用次数: 0

Innovative synthesis and sodium storage enhancement of closed-pore hard carbon for sodium-ion batteries 用于钠离子电池的闭孔硬质碳的创新合成与钠存储增强技术

IF 18.9 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2024-10-28 DOI: 10.1016/j.ensm.2024.103867

Weining Li , Junfeng Li , Bernard Wiafe Biney , Yingchun Yan , Xiaping Lu , Heng Li , He Liu , Wei Xia , Dong Liu , Kun Chen , Aijun Guo

Hard carbon with abundant closed-pore structures holds significant promise as an anode material for sodium-ion batteries. In this work, a one-step process was pioneered to produce porous carbon with abundant open-pore structures from walnut shells. Subsequently, small aromatic compounds derived from the pyrolysis of polystyrene were deposited into the pores of the porous carbon, forming hard carbon material with abundant closed-pore structures. The resulting hard carbon anode (WS-PS-1200) demonstrated a high capacity of 385 mAh g⁻¹ at 50 mA g⁻¹, with a corresponding plateau capacity of 225 mAh g⁻¹. It also exhibited an impressive initial Coulombic efficiency (ICE) of 88 % and excellent rate performance, compared to an ICE of only 57.5 % in the anode obtained by direct carbonization. By utilizing 3D time-of-flight secondary-ion mass spectrometry (3D TOF-SIMS) and depth-profiling X-ray photoelectron spectroscopies (XPS) characterization methods to analyze the solid electrolyte interface (SEI), the results indicate that reducing the open-pore structure can minimize the decomposition of the electrolyte, leading to an SEI composition that tends towards inorganic phases. To verify the practical applicability of WS-PS-1200, it was assembled into a full cell with Na₃V₂(PO₄)₃, achieving a capacity of 305 mAh g⁻¹ (0.03 A g⁻¹) and excellent rate performance. Moreover, the assembled all-carbon sodium-ion hybrid capacitor exhibits an energy density of 101 Wh kg⁻¹. This study not only introduces a new strategy for preparing hard carbon with closed pores but also successfully converts waste polystyrene and walnut shells into high-value materials, offering an innovative method for synthesizing hybrid capacitor electrode materials.

具有丰富闭孔结构的硬碳有望成为钠离子电池的负极材料。在这项工作中，率先采用一步法工艺从核桃壳中生产出具有丰富开孔结构的多孔碳。随后，在多孔碳的孔隙中沉积了由聚苯乙烯热解产生的少量芳香族化合物，形成了具有丰富闭孔结构的硬碳材料。由此产生的硬碳阳极（WS-PS-1200）在 50 mA g-1 的条件下显示出 385 mAh g-1 的高容量，相应的高原容量为 225 mAh g-1。它还表现出令人印象深刻的 88% 的初始库仑效率（ICE）和出色的速率性能，而直接碳化获得的阳极的 ICE 仅为 57.5%。通过利用三维飞行时间二次离子质谱（3D ToF-SIMS）和深度剖析 X 射线光电子能谱（XPS）表征方法分析固体电解质界面（SEI），结果表明减少开孔结构可以最大限度地减少电解质的分解，从而使 SEI 成分趋向于无机相。为了验证 WS-PS-1200 的实际应用性，我们将其与 Na3V2(PO4)3 组装成了一个完整的电池，电池容量达到了 305 mAh g-1（0.03 A g-1），并且具有优异的速率性能。此外，组装后的全碳钠离子混合电容器的能量密度达到 101 Wh kg-1。这项研究不仅介绍了一种制备封闭孔隙硬碳的新策略，还成功地将废弃聚苯乙烯和核桃壳转化为高价值材料，为合成混合电容器电极材料提供了一种创新方法。

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引用次数: 0

Spatial confinement strategy modulated by kinetic diameters of gaseous molecules for sodium storage 利用气态分子的动力学直径调节空间限制策略，实现钠储存

IF 18.9 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2024-10-24 DOI: 10.1016/j.ensm.2024.103835

Jingqiang Zheng, Weigang Liu, Simin Li, Yanqing Lai, Jie Li, Zhian Zhang

Constructing closed pore structures is essential for improving the plateau capacity of high-capacity hard carbon (HC) anodes for sodium-ion batteries. However, the absence of a straightforward and efficient strategy for constructing closed pores has hindered the advancement of high-capacity HC anodes. Here, we have developed a spatial confinement strategy for constructing closed pore structures using pyrolytic carbon (PC) as substrate and pyrolysis gas as the carbon source for chemical vapor deposition. The deposition of pyrolysis gas effectively tightens the pore entrance, thereby preventing electrolyte infiltration and transforming the open pores in the PC into highly efficient sites for sodium storage. The obtained optimal anodes demonstrate a remarkable specific capacity of 324.6 mAh g^-1. More importantly, we calculate the kinetic diameters of the carbon source molecules from their iso-electron density surfaces and correlate them with the mechanism of closed pore formation, which will effectively guide the fabrication of closed pores for sodium storage.

构建闭孔结构对于提高钠离子电池高容量硬碳（HC）阳极的高原容量至关重要。然而，由于缺乏直接有效的闭孔构造策略，阻碍了高容量碳氢化合物阳极的发展。在此，我们开发了一种空间限制策略，利用热解碳（PC）作为基底，热解气体作为化学气相沉积的碳源，构建封闭孔隙结构。热分解气体的沉积可有效收紧孔隙入口，从而防止电解质渗入，并将 PC 中的开放孔隙转化为高效的钠储存场所。所获得的最佳阳极的比容量高达 324.6 mAh g-1。更重要的是，我们从碳源分子的等电子密度表面计算出了碳源分子的动力学直径，并将其与封闭孔隙的形成机制联系起来，这将有效地指导用于钠储存的封闭孔隙的制造。

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引用次数: 0