Journal of Energy Chemistry最新文献_第5页

Deposition and etching of (101)Zn facet exposed zinc electrode induced by trace COS achieving ultra-long cycle stability in zinc batteries 微量 COS 诱导的 (101)Zn 面暴露锌电极的沉积和蚀刻，实现锌电池的超长循环稳定性

IF 13.1 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2024-10-30 DOI: 10.1016/j.jechem.2024.10.025

Keren Lu , Haiyan Jing , Qiubo Guo, Cai Liu, Boyuan Liu, Xifeng Xia, Fengyun Wang, Wu Lei, Mingzhu Xia, Qingli Hao

Rechargeable aqueous zinc-based batteries (RZBs) often suffer from poor cycling stability due to the instability of zinc deposition and etching processes. This work achieves dendrite-free zinc deposition with a smaller nucleation radius and rapid completion of the nucleation stage by a “triple regulation strategy” with trace chitosan oligosaccharide (COS) in ZnSO₄ electrolyte (2 g L⁻¹ COS). Theoretical and experimental results indicate that COS, with hydroxyl and amino functional groups, exhibits a high affinity for the (002)_Zn and (100)_Zn facets. Under the influence of a small amount of COS, the selective exposure of the (101)_Zn facet is facilitated. The extensively exposed (101)_Zn facet is protected by COS, which inhibits the occurrence of side reactions. Moreover, the presence of trace COS-02 changes the etching mode from three-dimensional (3D) to two-dimensional (2D), ensuring a uniform distribution of Zn²⁺ in the electric field during the deposition process. The unique 3D deposition and 2D etching mechanism induced by the COS additive result in exceptional cycling stability, exceeding 3800 h (1 mA cm⁻²) and 430 h (5 mA cm⁻²) in zinc symmetrical cells. Additionally, COS acts as a “molecular pillar” to stabilize VS₂, enabling the Zn||VS₂ full cell to achieve 1000 stable cycles with 89.6% capacity retention and an average coulombic efficiency of 99.95%. This work reveals a novel multiple regulation mechanism by using trace COS in RZBs, and provides a new approach for the development of long-term stable RZBs with preferential exposure facets.

由于锌沉积和蚀刻过程的不稳定性，可充电锌基水溶液电池（RZB）的循环稳定性通常较差。这项研究通过在 ZnSO4 电解液（2 g L-1 COS）中添加微量壳聚糖低聚糖（COS）的 "三重调节策略"，实现了无树枝状晶核的锌沉积，且成核半径更小，成核阶段快速完成。理论和实验结果表明，带有羟基和氨基官能团的 COS 对 (002)Zn 和 (100)Zn 面具有很高的亲和力。在少量 COS 的影响下，(101)Zn 面的选择性暴露得到了促进。广泛暴露的 (101)Zn 面受到 COS 的保护，从而抑制了副反应的发生。此外，痕量 COS-02 的存在将蚀刻模式从三维（3D）转变为二维（2D），确保了在沉积过程中 Zn2+ 在电场中的均匀分布。COS 添加剂诱导的独特三维沉积和二维蚀刻机制带来了卓越的循环稳定性，在锌对称电池中超过 3800 小时（1 mA cm-2）和 430 小时（5 mA cm-2）。此外，COS 还是稳定 VS2 的 "分子支柱"，使 Zn||VS2 全电池实现了 1000 次稳定循环，容量保持率达到 89.6%，平均库仑效率达到 99.95%。这项工作揭示了在 RZB 中使用痕量 COS 的新型多重调节机制，为开发具有优先暴露面的长期稳定 RZB 提供了一种新方法。

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引用次数: 0

Improving redox reactions of Spiro-OMeTAD via p-type molecular scaffold to reduce energy loss at Ag-electrode in perovskite solar cells 通过 p 型分子支架改善螺-OMeTAD 的氧化还原反应，减少过氧化物太阳能电池中 Ag-电极的能量损失

IF 13.1 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2024-10-30 DOI: 10.1016/j.jechem.2024.10.027

Peng Wang , Shafidah Shafian , Feng Qiu , Xiao Zhang , Yuping Zhao , Bin Wu , Kyungkon Kim , Yong Hua , Lin Xie

2,2′,7,7′-Tetrakis(N,N-di(4-methoxyphenyl)amino)-9,9′-spirobifluorene (Spiro) is an essential hole-transport material used in perovskite solar cells (PSCs). However, the redox reaction of Spiro and its impact at the interface with the metal electrode are not yet fully understood. In this study, we introduced a crystalline additive (CA) to regulate the redox process of Spiro and its interface with an Ag electrode. Our findings indicate that CA functions as a molecular scaffold, improving the crystallinity and stability of radicals in Spiro throughout the entire redox reaction. This enhancement increases the hole mobility of Spiro and strengthens the internal electric field, thereby improving hole extraction and transport efficiency at both interfaces. Moreover, the optimized redox reaction of Spiro reduces energy loss at the Ag electrode, significantly boosting the power conversion efficiency to 25.21%. Furthermore, CA mitigates the aggregation of lithium salt and enhances the stability of the device. Our findings contribute to a deeper understanding of hole-transport mechanisms of Spiro and emphasize the importance of reducing energy loss at the Spiro/Ag electrode interface in PSCs.

2,2′,7,7′-四(N,N-二(4-甲氧基苯基)氨基)-9,9′-螺二芴（Spiro）是一种用于过氧化物太阳能电池（PSC）的重要空穴传输材料。然而，人们对斯派罗的氧化还原反应及其对金属电极界面的影响尚未完全了解。在这项研究中，我们引入了一种晶体添加剂（CA）来调节斯派罗的氧化还原过程及其与银电极的界面。我们的研究结果表明，CA 起着分子支架的作用，在整个氧化还原反应过程中提高了斯派罗中自由基的结晶度和稳定性。这种改善提高了螺的空穴迁移率，增强了内部电场，从而提高了两个界面的空穴萃取和传输效率。此外，经过优化的斯派罗氧化还原反应减少了银电极上的能量损失，从而将功率转换效率显著提高到 25.21%。此外，CA 还能减轻锂盐的聚集，提高器件的稳定性。我们的研究结果有助于加深对斯派罗空穴传输机制的理解，并强调了减少 PSC 中斯派罗/银电极界面能量损失的重要性。

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引用次数: 0

Energy harvesting and movement tracking by polypyrrole functionalized textile for wearable IoT applications 用于可穿戴物联网应用的聚吡咯功能化纺织品的能量收集和运动跟踪功能

IF 13.1 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2024-10-30 DOI: 10.1016/j.jechem.2024.10.028

Guilherme Ferreira , Shubham Das , Guilherme Coelho , Rafael R.A. Silva , Sumita Goswami , Rui N. Pereira , Luís Pereira , Elvira Fortunato , Rodrigo Martins , Suman Nandy

Textiles for health and sporting activity monitoring are on the rise with the advent of smart portable wearables. The intention of this work is to design wireless monitoring wearables, based on widely available textiles and low environmental impact production technologies. Herein we have developed a polymeric ink which is able to functionalize different types of textile fibers (including silver conducting fibers, cotton, and commercial textile) with polypyrrole. These fibers were weaved together with a thinner silver conducting fiber and carbon fiber to form a touch-sensitive energy harvesting system that would generate an electric output when mechanical pressure is applied to it. Different prototypes were manufactured with loom weaving accessories to simulate real textile cloths. By simple touch, the prototypes produced a maximum voltage of 244 V and a maximum power density of 2.29 W m⁻². The current generated is then transformed into a digital signal, which is further utilized for human motion or gesture monitorization. The system comprises a wireless block for the Internet of Things (IoT) applicability that will be eventually extended to future remote health and sports monitoring systems.

随着智能便携式可穿戴设备的出现，用于健康和体育活动监测的纺织品也在不断增加。这项工作的目的是在广泛使用的纺织品和低环境影响生产技术的基础上，设计无线监测可穿戴设备。在此，我们开发了一种聚合墨水，能够将不同类型的纺织纤维（包括银导电纤维、棉花和商用纺织品）与聚吡咯功能化。我们将这些纤维与较细的银导电纤维和碳纤维编织在一起，形成了一个触敏能量采集系统，当机械压力施加在该系统上时，它就会产生电输出。我们用织布机编织配件制造了不同的原型，以模拟真实的纺织品。通过简单的触摸，原型产生的最大电压为 244 V，最大功率密度为 2.29 W m-2。产生的电流随后被转换成数字信号，进一步用于人体运动或手势监控。该系统包括一个适用于物联网（IoT）的无线模块，最终将扩展到未来的远程健康和运动监测系统。

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引用次数: 0

Defective wood-based chainmail electrocatalysts boost performances of seawater-medium Zn-air batteries 缺陷木质链状电催化剂提高了海水-中型锌-空气电池的性能

IF 13.1 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2024-10-30 DOI: 10.1016/j.jechem.2024.10.029

Zhonghao Chen , Hongjiao Chen , Teng Li , Xing Tian , Kewei Zhang , Yijun Miao , Changlei Xia , Liping Cai , Bin Hui , Chaoji Chen

A high-activity and stable bifunctional oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) electrocatalyst is critical for seawater-based Zn-air batteries (ZABs). Herein, we report a wood-derived chainmail electrocatalyst containing defective nitrogen-doped carbon nanotubes encapsulating cobalt nanoparticles (Co@D-NCNT/CW) to enhance the ORR/OER activity and stability in seawater medium. During the preparation process, the introduction and removal of Zn increased the defect sites and pyridine N content in the carbon material, modulating charge distribution and influencing the adsorption and activation processes. The highly ordered open channels in Co@D-NCNT/CW promoted mass transfer of reactants and accelerated gas diffusion. The resultant chainmail electrocatalyst exhibited impressive bifunctional ORR and OER activities with an ultra-low gap of 0.67 V in seawater-based alkaline electrolyte. The Co@D-NCNT/CW-assembled seawater-based rechargeable liquid ZABs demonstrated a maximum power density of 245.3 mW cm⁻² and a long-term cycling performance over 500 h. The seawater-based all-solid-state ZABs achieved the maximum power density of 48.2 mW cm⁻² and stabilized over 30 h. Density functional theory revealed that the presence of defects and pyridine nitrogen in Co@D-NCNT/CW modulated the electronic structure of Co, optimizing the binding affinity of the Co sites with intermediates and weakening Cl⁻ adsorption. This work provides a new approach to preparing high-activity and stable ORR/OER electrocatalyst utilizing wood nanostructures, boosting the development of seawater-based ZABs.

高活性、稳定的氧还原反应（ORR）和氧进化反应（OER）双功能电催化剂对于基于海水的锌空气电池（ZAB）至关重要。在此，我们报告了一种由木材衍生的链状电催化剂，该催化剂含有封装钴纳米颗粒的缺陷氮掺杂碳纳米管（Co@D-NCNT/CW），可提高海水介质中 ORR/OER 的活性和稳定性。在制备过程中，锌的引入和去除增加了碳材料中的缺陷位点和吡啶N含量，调节了电荷分布并影响了吸附和活化过程。Co@D-NCNT/CW 中高度有序的开放通道促进了反应物的传质并加速了气体扩散。由此产生的链锁电催化剂在海水碱性电解质中表现出令人印象深刻的 ORR 和 OER 双功能活性，并具有 0.67 V 的超低间隙。Co@D-NCNT/CW 组装的海水基可充电液体 ZABs 的最大功率密度为 245.3 mW cm-2，长期循环性能超过 500 h。密度泛函理论显示，Co@D-NCNT/CW 中缺陷和吡啶氮的存在调节了 Co 的电子结构，优化了 Co 位点与中间体的结合亲和力，削弱了对 Cl- 的吸附。这项工作为利用木质纳米结构制备高活性和稳定的 ORR/OER 电催化剂提供了一种新方法，推动了基于海水的 ZAB 的发展。

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引用次数: 0

VP-VO core-shell heterostructure: Harmonizing adsorption and catalysis of polysulfides for high-performance Li-S batteries VP-VO 核壳异质结构：协调多硫化物的吸附和催化，实现高性能锂离子电池

IF 13.1 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2024-10-30 DOI: 10.1016/j.jechem.2024.10.026

Tao Ren , Xinji Dong , Xiaolan Li , Haojie Zhu , Cheng Yang , Jinliang Zhu

引用次数: 0

Catalytic production of high-energy-density spiro polycyclic jet fuel with biomass derivatives 用生物质衍生物催化生产高能量密度螺多环喷气燃料

IF 13.1 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2024-10-30 DOI: 10.1016/j.jechem.2024.10.024

Wen-Jing Zhang , Yan-Cheng Hu , Yan-Hong Tan , Jia Li , Ning Li , Jing-Pei Cao

High-energy-density (HED) fuel (e.g. widely used JP-10 and RJ-4), featuring compact 3D polycyclic structure with high strain, is of critical importance for volume-limited military aircraft, since their high density and combustion heat can provide more propulsion energy. To reduce the reliance on petroleum source, it is highly desirable to develop renewable alternatives for the production of strained polycyclic HED fuel, but which remains a big challenge because of the inaccessibility caused by the high strain. We herein demonstrate a three-step catalytic route towards highly strained C₁₇ and C₁₈ spirofuel with biomass feedstocks. The process includes catalytic aldol condensation of renewable cyclohexanone/cyclopentanone with benzaldehyde, catalytic spiro Diels-Alder (D-A) reaction of aldol adduct with isoprene, and catalytic hydrodeoxygenation. The key spiro D-A reaction is enabled by the catalysis of heterogeneous Lewis acidic ionic liquid. The chloroaluminate IL, formed by benign urea and AlCl₃, exhibits good catalytic performance and reusability for this step. An eventual hydrodeoxygenation (HDO) over Pd/C and H-Y produces strained tricyclic spirofuel with density >0.93 g/mL, combustion heat >41 MJ/L and freezing point < −40 °C, which are better than the properties of tactical fuel RJ-4. Therefore, it is anticipated that the as-prepared renewable fuels have the potential to replace traditional petroleum-derived HED fuels.

高能量密度（HED）燃料（如广泛使用的 JP-10 和 RJ-4）具有高应变的紧凑三维多环结构，对体积有限的军用飞机至关重要，因为其高密度和燃烧热可提供更多推进能量。为了减少对石油资源的依赖，开发生产应变多环 HED 燃料的可再生替代品是非常可取的，但由于高应变造成的不可获取性，这仍然是一个巨大的挑战。在此，我们展示了利用生物质原料生产高应变 C17 和 C18 螺烷燃料的三步催化路线。该工艺包括可再生环己酮/环戊酮与苯甲醛的催化醛缩合反应、醛加合物与异戊二烯的催化螺 Diels-Alder (D-A) 反应以及催化加氢脱氧反应。关键的螺 D-A 反应是由异相路易斯酸离子液体催化实现的。由良性脲和 AlCl3 生成的氯铝酸盐离子液体在这一步骤中表现出良好的催化性能和重复使用性。最终在 Pd/C 和 H-Y 上进行加氢脱氧（HDO）生成了拉伸三环螺环燃料，其密度为 0.93 g/mL，燃烧热为 41 MJ/L，凝固点为 -40 °C，优于战术燃料 RJ-4。因此，预计制备的可再生燃料具有替代传统石油衍生 HED 燃料的潜力。

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引用次数: 0

Metallized polymer current collector as “stress acceptor” for stable micron-sized silicon anodes 金属化聚合物集流器作为稳定的微米级硅阳极的 "应力接收器

IF 13.1 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2024-10-29 DOI: 10.1016/j.jechem.2024.09.071

Ziyi Cao , Haoteng Sun , Yi Zhang , Lixia Yuan , Yaqi Liao , Haijin Ji , Shuaipeng Hao , Zhen Li , Long Qie , Yunhui Huang

Micron-sized silicon (μSi) is a promising anode material for next-generation lithium-ion batteries due to its high specific capacity, low cost, and abundant reserves. However, the volume expansion that occurs during cycling leads to the accumulation of undesirable stresses, resulting in pulverization of silicon microparticles and shortened lifespan of the batteries. Herein, a composite film of Cu-PET-Cu is proposed as the current collector (CC) for μSi anodes to replace the conventional Cu CC. Cu-PET-Cu CC is prepared by depositing Cu on both sides of a polyethylene terephthalate (PET) film. The PET layer promises good ductility of the film, permitting the Cu-PET-Cu CC to accommodate the volumetric changes of silicon microparticles and facilitates the stress release through ductile deformation. As a result, the μSi electrode with Cu-PET-Cu CC retains a high specific capacity of 2181 mA h g⁻¹, whereas the μSi electrode with Cu CC (μSi/Cu) exhibits a specific capacity of 1285 mA h g⁻¹ after 80 cycles. The stress relieving effect of Cu-PET-Cu was demonstrated by in-situ fiber optic stress monitoring and multi-physics simulations. This work proposes an effective stress relief strategy at the electrode level for the practical implementation of μSi anodes.

微米级硅 (μSi)具有比容量高、成本低和储量丰富等优点，是下一代锂离子电池的理想负极材料。然而，在循环过程中发生的体积膨胀会导致不良应力的积累，从而导致硅微颗粒的粉碎和电池寿命的缩短。本文提出了一种 Cu-PET-Cu 复合薄膜作为微硅阳极的集流器（CC），以取代传统的 Cu CC。Cu-PET-Cu CC 是通过在聚对苯二甲酸乙二醇酯（PET）薄膜的两面沉积铜来制备的。PET 层保证了薄膜的良好延展性，使 Cu-PET-Cu CC 能够适应硅微颗粒的体积变化，并通过延展变形促进应力释放。因此，带有 Cu-PET-Cu CC 的微硅电极在 80 个循环后仍能保持 2181 mA h g-1 的高比容量，而带有 Cu CC 的微硅电极（μSi/Cu）的比容量为 1285 mA h g-1。原位光纤应力监测和多物理场仿真证明了 Cu-PET-Cu 的应力消除效果。这项研究提出了一种有效的电极应力消除策略，可用于μSi 阳极的实际应用。

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引用次数: 0

Design principles of fluoroether solvents for lithium metal battery electrolytes unveiled by extensive molecular simulation and machine learning 通过大量分子模拟和机器学习揭示锂金属电池电解质氟醚溶剂的设计原理

IF 13.1 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2024-10-29 DOI: 10.1016/j.jechem.2024.10.021

Xueying Yuan , Xiupeng Chen , Yuanxin Zhou , Zhiao Yu , Xian Kong

Electrolyte engineering with fluoroethers as solvents offers promising potential for high-performance lithium metal batteries. Despite recent progresses achieved in designing and synthesizing novel fluoroether solvents, a systematic understanding of how fluorination patterns impact electrolyte performance is still lacking. We investigate the effects of fluorination patterns on properties of electrolytes using fluorinated 1,2-diethoxyethane (FDEE) as single solvents. By employing quantum calculations, molecular dynamics simulations, and interpretable machine learning, we establish significant correlations between fluorination patterns and electrolyte properties. Higher fluorination levels enhance FDEE stability but decrease conductivity. The symmetry of fluorination sites is critical for stability and viscosity, while exerting minimal influence on ionic conductivity. FDEEs with highly symmetric fluorination sites exhibit favorable viscosity, stability, and overall electrolyte performance. Conductivity primarily depends on lithium-anion dissociation or association. These findings provide design principles for rational fluoroether electrolyte design, emphasizing the trade-offs between stability, viscosity, and conductivity. Our work underscores the significance of considering fluorination patterns and molecular symmetry in the development of fluoroether-based electrolytes for advanced lithium batteries.

以氟醚为溶剂的电解质工程为高性能锂金属电池提供了广阔的发展前景。尽管最近在设计和合成新型氟醚溶剂方面取得了进展，但人们仍然缺乏对氟化模式如何影响电解质性能的系统了解。我们研究了氟化模式对使用氟化 1,2- 二乙氧基乙烷 (FDEE) 作为单一溶剂的电解质性能的影响。通过量子计算、分子动力学模拟和可解释的机器学习，我们在氟化模式和电解质性能之间建立了显著的相关性。氟化水平越高，FDEE 的稳定性就越高，但电导率却越低。氟化位点的对称性对稳定性和粘度至关重要，而对离子电导率的影响则微乎其微。氟化位点高度对称的 FDEE 具有良好的粘度、稳定性和整体电解质性能。电导率主要取决于锂离子的解离或结合。这些发现为合理设计氟醚电解质提供了设计原则，强调了稳定性、粘度和电导率之间的权衡。我们的工作强调了在为先进锂电池开发基于氟醚的电解质时考虑氟化模式和分子对称性的重要性。

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引用次数: 0

Microdynamic modulation through Pt–O–Ni proton and electron “superhighway” for pH-universal hydrogen evolution 通过铂-氧-镍质子和电子 "高速公路 "的微动力调制实现 pH 值通用氢进化

IF 13.1 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2024-10-29 DOI: 10.1016/j.jechem.2024.10.020

Dewen Wang , Yuting Chen , Bohan Yao , Tian Meng , Yanchao Xu , Dongxu Jiao , Zhicai Xing , Xiurong Yang

Optimizing the microdynamics in alkaline and neutral conditions is a significant but challenging task in developing pH-universal hydrogen evolution (HER) electrocatalysts. Herein, a unique Pt–O–Ni bridge has been constructed to alter the coordination and electronic environment between Pt nanoparticles (Pt_n) and nickel metaphosphate (NPO) substrate (Pt-NPO). Sufficient electron transfer from NPO to Pt_n to maintain an electron-rich environment and a low valence state of Pt_n. Furthermore, H* is produced from the H₂O dissociation on Ni site and then spillover toward Pt sites to bind into H₂, which makes up for the insufficient H₂O dissociation ability of Pt in Volmer step. Pt-NPO exhibits long-term stability and only need the overpotentials of 22.3, 33.0 and 30.5 mV to attain 10 mA cm⁻² in alkaline, neutral and acidic media, respectively. The anion-exchange membrane (AEM) water electrolyzer catalyzed by Pt-NPO shows high water electrolysis performance that a cell voltage of 1.73 V is needed to obtain the current density of 500 mA cm⁻² in 1 M KOH at 80 °C, at the same time maintains good stability for 350 h. The regulation strategy proposed in this work is helpful for the design and synthesis of highly efficient pH-universal HER electrocatalysts.

优化碱性和中性条件下的微动力学是开发 pH 值通用型氢进化（HER）电催化剂的一项重要而又具有挑战性的任务。在此，我们构建了一种独特的铂-氧-镍桥，以改变铂纳米粒子（Ptn）和偏磷酸镍（NPO）底物（Pt-NPO）之间的配位和电子环境。从 NPO 到 Ptn 的充分电子传递维持了 Ptn 的富电子环境和低价态。此外，镍位点解离出的 H2O 产生 H*，然后溢出到铂位点结合成 H2，这弥补了铂在 Volmer 步骤中解离 H2O 能力的不足。Pt-NPO 具有长期稳定性，在碱性、中性和酸性介质中分别只需 22.3、33.0 和 30.5 mV 的过电位即可达到 10 mA cm-2。由 Pt-NPO 催化的阴离子交换膜（AEM）水电解槽具有很高的水电解性能，在 80 °C 的 1 M KOH 溶液中，需要 1.73 V 的电池电压才能获得 500 mA cm-2 的电流密度，同时还能在 350 h 内保持良好的稳定性。

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引用次数: 0

High-areal-capacity and long-life sulfide-based all-solid-state lithium battery achieved by regulating surface-to-bulk oxygen activity 通过调节表层与内层之间的氧活度实现高铝容量和长寿命硫化物全固态锂电池

IF 13.1 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2024-10-29 DOI: 10.1016/j.jechem.2024.10.022

Yanchen Liu , Yang Lu , Zongliang Zhang , Bin Xu , Fangbo He , Yang Liu , Yongle Chen , Kun Zhang , Fangyang Liu

Sulfide-based all-solid-state lithium batteries (ASSLBs) with nickel-rich oxide cathodes are emerging as primary contenders for the next generation rechargeable batteries, owing to their superior safety and energy density. However, the all-solid-state batteries with nickel-rich oxide cathodes suffer from performance degradation due to the reactions between the highly reactive surface oxygen of the cathode and the electrolyte, as well as the instability of the bulk oxygen structure in the cathode. Herein, we propose a synergistic modification design scheme to adjust the oxygen activity from surface to bulk. The LiBO₂ coating inhibits the reactivity of surface lattice oxygen ions. Meanwhile, Zr doping in the bulk phase forms strong Zr–O covalent bonds that stabilize the bulk lattice oxygen structure. The synergistic effect of these modifications prevents the release of oxygen, thus avoiding the degradation of the cathode/SE interface. Additionally, the regulation of surface-to-bulk oxygen activity establishes a highly stable interface, thereby enhancing the lithium ion diffusion kinetics and mechanical stability of the cathode. Consequently, cathodes modified with this synergistic strategy exhibit outstanding performance in sulfide-based ASSLBs, including an ultra-long cycle life of 100,000 cycles, ultra-high rate capability at 45C, and 85% high active material content in the composite cathode. Additionally, ASSLB exhibits stable cycling under high loading conditions of 82.82 mg cm⁻², achieving an areal capacity of 17.90 mA h cm⁻². These encouraging results pave the way for practical applications of ASSLBs in fast charging, long cycle life, and high energy density in the future.

具有富氧化镍阴极的硫化物全固态锂电池（ASSLBs）因其卓越的安全性和能量密度，正在成为下一代可充电电池的主要竞争者。然而，由于阴极高活性表面氧与电解质之间的反应以及阴极中大量氧结构的不稳定性，采用富镍氧化物阴极的全固态电池存在性能下降的问题。在此，我们提出了一种协同改性设计方案，以调整从表面到体积的氧活性。LiBO2 涂层抑制了表面晶格氧离子的反应活性。同时，在体相中掺杂 Zr 可形成强 Zr-O 共价键，从而稳定体相晶格氧结构。这些改性的协同效应阻止了氧的释放，从而避免了阴极/SE 界面的降解。此外，通过调节表层到体层的氧活性，可建立一个高度稳定的界面，从而提高锂离子扩散动力学和阴极的机械稳定性。因此，采用这种协同策略改性的阴极在硫化物基 ASSLB 中表现出卓越的性能，包括 100,000 次的超长循环寿命、45℃ 时的超高速率能力以及复合阴极中 85% 的高活性材料含量。此外，ASSLB 还能在 82.82 mg cm-2 的高负载条件下稳定循环，实现 17.90 mA h cm-2 的等效容量。这些令人鼓舞的结果为 ASSLB 未来在快速充电、长循环寿命和高能量密度方面的实际应用铺平了道路。

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引用次数: 0