INORGANIC CHEMISTRY COMMUNICATIONS
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2024
·
IF 4.4
Shuailiang Xu,Mingqiang Li,Haochen Weng,Jingwen Li
Because of the high capacity, natural abundance, and safety of aluminum (Al), the Al–Li alloy formed by combining it with lithium (Li) is an attractive anode material. In this paper, we propose a new type of lithium battery that works in an open system and does not require sealing, the “Lithium-Aluminum” soft pack battery (LAB). Al foil is applied to the anode of the LAB, LiCl is used for the electrolyte, and LiFePO 4 is used as the cathode. LAB incorporated Al–Li alloy into lithium batteries in a new way. During charging, lithium deposits in the anode undergo an electrochemical synthesis reaction with Al to produce Al–Li alloys, which decompose during discharge. The LAB has a discharge voltage plateau of about 2.8 V and a discharge capacity of 0.48 mAh/cm 2 (145.5 mAh/g), with the Coulombic efficiency remaining above 90 %. The capacity retention rate is 95.9 % after 600 cycles and still reaches 65.2 % after 800 cycles. Notably, the battery remains functional when bent at will and in a broken or punctured state. Compared to traditional lithium metal batteries (LMBs), our work demonstrates superior cycle stability, a safer operational environment, increased versatility in application scenarios, and reduced costs.
研究领域:
材料科学
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电化学
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能源技术
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Jun Cheng,Wenjie Lin,Jingrong Hou,Yaqi Liao,Yunhui Huang
As the classic cathode material, lithium cobalt oxide (LiCoO2, LCO) suffers from severe structural and interfacial degradation at voltage >4.5 V, which induces fast capacity decay of the cells. Herein, we adopt a simple and effective method, doping aluminum (Al) cations in precursors, to improve the structural stability of LCO and systematically investigate the effect of Al doping on the electrochemical performances. Doping in precursors rather than bulk particles is beneficial to realize uniform Al ions distribution. Even at 4.5 V charging voltage, the LCO/graphite pouch cells with high Al doping levels (8500 ppm) deliver initial and reversible discharge capacities of 386 and 369 mAh after 500 cycles, respectively. The capacity retention is as high as 95.5%. When the cutoff voltage reaches 4.55 V, the pouch cell maintains 79.0% of the first-cycle discharge capacity after 500 cycles. With optimized electrolyte, the pouch cell realizes 87.3% of the initial discharge capacity after 500 cycles at 45 °C. Moreover, the thermal safety performance of the pouch cells with Al doping is promising. Our work displays an excellent inspiration for developing high-voltage, long-cycle, and safe LCO cathode for commercial lithium-ion batteries.
研究领域:
材料科学
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电化学
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能源存储
✓ 已验证
DOI
高影响因子
NATURE
·
2025
·
IF 48.5
Huang He,Hu Yitao,Hou Yajun,Wang Xingkai,Dong Qiujiang,Zhao Zhixin,Ji Mingfang,Zhang Wanxing,Li Jinyang,Xie Jianping,Guo Hao,Han Xiaopeng,Ouyang Xiaoping,Hu Wenbin
The development of high-energy lithium metal batteries (LMBs) is essential for advances in next-generation energy storage and electric vehicle technologies 1 , 2 , 3 . Nevertheless, the practical applications of LMBs are constrained by current electrolyte designs that inherently rely on dominant solvation structures, preventing transformative progress in performance optimization 4 , 5 . Here, we address this limitation through a delocalized electrolyte design that fosters a more disordered solvation microenvironment, thereby mitigating dynamic barriers and stabilizing interphases. The resulting delocalized electrolyte delivers notable energy densities of 604.2 Wh kg −1 in a 5.5-Ah LiNi 0.9 Co 0.05 Mn 0.05 O 2 (Ni90)||Li pouch cell with a lean electrolyte design (1.0 g Ah −1 ) and 618.2 Wh kg −1 in a 5.2-Ah Ni90||Li pouch cell with an ultralean electrolyte design (0.9 g Ah −1 ), maintaining significant cycle stability over 100 and 90 cycles, respectively. In addition, the 70–104 V NCM811||Li battery pack (3,904 Wh) exhibits a high energy density of 480.9 Wh kg −1 and stable cycling over 25 cycles. These results demonstrate the need to circumvent inherent reliance on dominant solvation structures in electrolyte design to achieve the high-energy Battery600 and scalable Pack480 targets.
研究领域:
储能
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电化学
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电池技术
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nano Energy
·
2025
·
IF 17.1
Zhaowen Hu,Ling Che,Zezhou Lin,Chao Shen,Haitao Huang,Nan Li,Ting Jin,Keyu Xie
Graphite-based Li-ion batteries (LIBs) can pose safety risks under harsh conditions due to undesired Li plating, involving sluggish Li + desolvation and diffusion through SEI, which is strongly determined by interfacial solvation structure. Here, we develop a kilogram-level preparation of lithium-plating suppressed graphite (LPSG) by incorporating a defective N and Co-doped carbon layer, which can induce low-solvent coordination Li + solvation structure in the inner Helmholtz plane. The underlying nanoscale interfacial solvation structure and interface chemistry regulation mechanism is revealed. The Co and N in the coating layer can generate local electron deviation, thus preferentially absorbing anions and making more anions participate in the first solvation sheath. Combined with facilitating P-F bond breaking, an inorganic-rich SEI is prompted to form, which enhances ion transport and achieves lithium-plating suppressed. Notably, the 5 Ah LFP||LPSG pouch cell demonstrates an extremely fast-charging capability (10C-rate constant current charging for 90.4 % of the 1C-rate capacity in less than 6 min). When charging at −20℃ and 0.5 C, the capacity retention of the pouch cell with LPSG improves nearly 20 times more than pristine graphite. More impressively, the LPSG enables the cell to exhibit a significant increase in thermal runaway trigger temperature (195.3℃ vs. 152.3℃) after being charged fully at 10 C. This work provides a novel insight into regulating the interfacial solvation structure and interface chemistry based on the electrode surface structure for high-safety LIBs.
研究领域:
储能材料
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电化学
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电池技术
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表面化学
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纳米技术
✓ 已验证
产品关联
DOI
高影响因子
Small Methods
·
2021
·Vol. 6
·期 2
·2101402
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IF 14.188
Hao Guo,Jing Hu,Huimin Yuan,Ningning Wu,Yingzhi Li,Guiyu Liu,Ning Qin,Kemeng Liao,Zhiqiang Li,Wen Luo,Shuai Gu,Weihua Wan,Bin Shi,Xusheng Xu,Qinghua Yang,Jiayuan Shi,Zhouguang Lu
Fabrication of a highly porous sulfur host and using excess electrolyte is a common strategy to enhance sulfur utilization. However, flooded electrolyte limits the practical energy density of Li–S pouch cells. In this study, a novel Fe 0.34 Co 0.33 Ni 0.33 S 2 (FCN) is proposed as host for sulfur to realize Ah-level Li–S full cells demonstrating excellent electrochemical performances under 2 µL mg −1 lean electrolyte conditions. Moreover, Kelvin probe force microscopy shows that the FCN surface contains positive charge with a potential of ≈70 mV, improving the binding of polysulfides through Lewis acid base interaction. In particular, the FCN@S possesses inherent electrochemical activity of simultaneous anionic and cationic redox for lithium storage in the voltage window of 1.8–2.1 V, which additionally contributes to the specific capacity. Due to the low carbon content (≈10 wt%), the sulfur loading is as high as ≈6 mg cm −2 , approaching an outstanding energy density of 394.9 and 267.2 Wh kg −1 at the current density of 1.5 and 4 mA cm −2 , respectively. Moreover, after 60 cycles at 1.5 mA cm −2 , the pouch cell still retains an energy of 300.2 Wh kg −1 . This study represents a milestone in the practical applications of high-energy Li–S batteries.
研究领域:
材料科学
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电化学
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能源存储
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纳米材料
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固态离子学
✓ 已验证
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-14
·
IF 15.7
Zou Zhijuan,Liu Pengfei,Dou Ruiyang,Liu Kaijun,Wang Yunlong,Song Lixian,Tong Liping,Yin Guolu,Kang Wenbin,Cai Wenlong,Zhang Yaping,Chen Hongbing,Song Yingze
Binders are essential for maintaining positive electrode integrity in Li||S batteries and significantly affect their performance. However, commercial linear binders often have disordered networks, poor binding efficiency, and insufficient mechanical strength. To address these challenges, three-dimensional covalent binders offer a promising solution. Traditional methods for producing cross-linked binders require additives and result in poorly controlled polymer networks due to the stochastic nature of liquid-phase polymerization. Moreover, the mechanisms by which reticulated binders stabilize the positive electrode remain unclear, requiring investigation under operando conditions. Herein, we present an approach to tailor cross-linked polyacrylamide networks using solid-state operando γ-ray irradiation chemistry, which eliminates additives and produces a pure, ordered network with remarkable binding capabilities. By integrating in situ high-resolution optical frequency domain reflectometry, multiscale synchrotron radiation characterization, and virtual simulations, this study reveals the role of binders in dynamically encaging and confining sulfur. Specifically, γ-ray-enabled polyacrylamide networks enhance battery performance through mechanical strengthening, optimized sulfur regeneration, and improved re-occupancy. Consequently, the well-designed composite positive electrode structure with only 5.0 wt% binder improves soft-packaged Li||S battery performance across various scenarios. Notably, a 1.2-Ah pouch cell achieves 410.1 Wh kg −1 specific energy with a low electrolyte/sulfur ratio of 3.0 µL mg –1 .
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-11
·
IF 14.7
Li Wei,Zhang Menghang,Sun Xinyi,Sheng Chuanchao,Mu Xiaowei,Wang Lei,He Ping,Zhou Haoshen
Li-CO 2 batteries offer a promising avenue for converting greenhouse gases into electricity. However, the inherent challenge of direct electrocatalytic reduction of inert CO 2 often results in the formation of Li 2 CO 3 , causing a dip in output voltage and energy efficiency. Our innovative approach involves solid redox mediators, affixed to the cathode via a Cu(II) coordination compound of benzene-1,3,5-tricarboxylic acid. This technique effectively circumvents the shuttle effect and sluggish kinetics associated with soluble redox mediators. Results show that the electrochemically reduced Cu(I) solid redox mediator efficiently captures CO 2 , facilitating Li 2 C 2 O 4 formation through a dimerization reaction involving a dimeric oxalate intermediate. The Li-CO 2 battery employing the Cu(II) solid redox mediator boasts a higher discharge voltage of 2.8 V, a lower charge potential of 3.7 V, and superior cycling performance over 400 cycles. Simultaneously, the successful development of a Li-CO 2 pouch battery propels metal-CO 2 batteries closer to practical application.
研究领域:
电化学
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材料科学
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能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Nano
·
2020
·
IF 14.588
Zhipeng Jiang,Hui-Juan Guo,Ziqi Zeng,Zhilong Han,Wei Hu,Rui Wen,Jia Xie
An ultrathick lithium metal anode (LMA) is a prerequisite for developing practical lithium–sulfur (Li–S) batteries that simultaneously meet the requirements of high areal capacity, lean electrolyte, and limited excess Li. Inspired by the electrochemical process for an organosulfur cathode, herein, we reconfigure such a sulfur cathode by using an overlithiation strategy to enable the formation of a high performance LMA. Specifically, an applicable ultrathick LMA is successfully constructed by overlithiating a well-known organosulfur cathode material, sulfurized polyacrylonitrile (SPAN). SPAN contains a polymeric pyridine structure with an outstanding lithium-ion affinity, so that it can act as a lithiophilic matrix. More importantly, a Li2S-rich solid electrolyte interphase (SEI) can be generated on the surface of SPAN during the overlithiation process. The synergistic effect of the lithiophilic matrix and a robust SEI leads to a dense deposition of lithium, which enables one to form an ultrathick LMA (159 μm, 30 mAh cm–2) with high Coulombic efficiency (99.7%). Such an LMA paired with a sulfur cathode of high areal capacity (up to 16 mAh cm–2) shows stable cycling under practical conditions of a lean electrolyte (2.2 μL mgS–1) and a negative-to-positive capacity (N/P) ratio as low as 1.3. The applicability of the ultrathick LMA was further verified with Li–S pouch cells, indicating a highly prospective route toward realization of practical Li–S batteries.
研究领域:
储能技术
·
电化学
·
材料科学
·
纳米技术
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电池技术
✓ 已验证
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-9
·
IF 14.7
Chen Ze,Wang Tairan,Wu Zhuoxi,Hou Yue,Chen Ao,Wang Yanbo,Huang Zhaodong,Schmidt Oliver G.,Zhu Minshen,Fan Jun,Zhi Chunyi
The high redox potential of Zn 0/2+ leads to low voltage of Zn batteries and therefore low energy density, plaguing deployment of Zn batteries in many energy-demanding applications. Though employing high-voltage cathode like spinel LiNi 0.5 Mn 1.5 O 4 can increase the voltages of Zn batteries, Zn 2+ ions will be immobilized in LiNi 0.5 Mn 1.5 O 4 once intercalated, resulting in irreversibility. Here, we design a polymer hetero-electrolyte consisting of an anode layer with Zn 2+ ions as charge carriers and a cathode layer that blocks the Zn 2+ ion shuttle, which allows separated Zn and Li reversibility. As such, the Zn ‖ LNMO cell exhibits up to 2.4 V discharge voltage and 450 stable cycles with high reversible capacity, which are also attained in a scale-up pouch cell. The pouch cell shows a low self-discharge after resting for 28 days. The designed electrolyte paves the way to develop high-voltage Zn batteries based on reversible lithiated cathodes.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2022
·Vol. 13
·期 1
·1-12
·
IF 17.694
Ou Xing,Liu Tongchao,Zhong Wentao,Fan Xinming,Guo Xueyi,Huang Xiaojing,Cao Liang,Hu Junhua,Zhang Bao,Chu Yong S.,Hu Guorong,Lin Zhang,Dahbi Mouad,Alami Jones,Amine Khalil,Yang Chenghao,Lu Jun
High-capacity Ni-rich layered oxides are promising cathode materials for secondary lithium-based battery systems. However, their structural instability detrimentally affects the battery performance during cell cycling. Here, we report an Al/Zr co-doped single-crystalline LiNi 0.88 Co 0.09 Mn 0.03 O 2 (SNCM) cathode material to circumvent the instability issue. We found that soluble Al ions are adequately incorporated in the SNCM lattice while the less soluble Zr ions are prone to aggregate in the outer SNCM surface layer. The synergistic effect of Al/Zr co-doping in SNCM lattice improve the Li-ion mobility, relief the internal strain, and suppress the Li/Ni cation mixing upon cycling at high cut-off voltage. These features improve the cathode rate capability and structural stabilization during prolonged cell cycling. In particular, the Zr-rich surface enables the formation of stable cathode-electrolyte interphase, which prevent SNCM from unwanted reactions with the non-aqueous fluorinated liquid electrolyte solution and avoid Ni dissolution. To prove the practical application of the Al/Zr co-doped SNCM, we assembled a 10.8 Ah pouch cell (using a 100 μm thick Li metal anode) capable of delivering initial specific energy of 504.5 Wh kg −1 at 0.1 C and 25 °C.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2025
·
IF 5.6
Xiangzhong Kong,Yanting Cai,Xinwei Dai,Ruibo Jiang,Liya Rong,Xi Chen,Zhongmin Wan,Zequan Zhao,Guozhao Fang
Aqueous zinc metal batteries (AZMBs) have triggered tremendous research interest in large-scale energy storage systems due to the advantages of resource abundance, low cost and environmentally friendly. Current collectors play significant roles in enhancing the electrochemical performance of AZMBs, especially aqueous zinc metal pouch cells (AZMPCs). However, the influence of the carbon or metal based current collectors on the performance of AZMPCs has rarely been investigated. This work comprehensively studies the chemical and electrochemical corrosion behaviors of graphite felt (GF), nickel foam (Ni) and stainless steel (SS) as current collectors in AZMPCs for the first time to identify the optimal candidate. The 3D porous GF collector with chemical inertness exhibits excellent chemical corrosion resistance under 2 M ZnSO 4 + 0.2 M MnSO 4 aqueous electrolyte by immersion testing for 30 days. In addition, linear sweep voltammetry and chronoamperometry results demonstrate that GF has high electrochemical stability, which is beneficial to the inhibition of swelling and active materials shedding in pouch cells. In contrast, 2D SS and Ni collectors displays severe structural damage along with surface corrosion after cycling for 100 cycles in AZMPCs. This phenomenon could be ascribed to the intrinsic high activity of metal and formation of corrosion layer under high electrolyte content. Lastly, the corrosion behavior of SS from button cells to pouch cells has been investigated to reveal the rigorous requirements of the latter on current collectors in terms of chemical/electrochemical corrosion resistance and electrochemical stability. This work provides guidance for the development of advanced current collectors for AZMPCs.
研究领域:
材料科学
·
电化学
·
储能技术
·
腐蚀科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-16
·
IF 14.7
Hao Baojiu,Zhou Jinqiu,Yang Hao,Zhu Changhao,Wang Zhenkang,Liu Jie,Yan Chenglin,Qian Tao
The breakthrough in electrolyte technology stands as a pivotal factor driving the battery revolution forward. The colloidal electrolytes, as one of the emerging electrolytes, will arise gushing research interest due to their complex colloidal behaviors and mechanistic actions at different conditions (aqueous/nonaqueous solvents, salt concentrations etc.). Herein, we show “beyond aqueous” colloidal electrolytes with ultralow salt concentration and inherent low freezing points to investigate its underlying mechanistic principles to stabilize cryogenic Zn metal batteries. Impressively, the “seemingly undesired” concentration polarization at the interface would disrupt the coalescence stability of the electrolyte, leading to a mechanically rigid interphase of colloidal particle-rich layer, positively inhibiting side reactions on either side of the electrodes. Importantly, the multi-layered pouch cells with cathode loading of 10 mg cm –2 exhibit undecayed capacity at various temperatures, and a relatively high capacity of 50 mAh g –1 could be well maintained at −80 °C.
研究领域:
电池技术
·
电化学
·
材料科学
·
胶体化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）