Energy & Environmental Science
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2024
·Vol. 17
·期 11
·3807-3818
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IF 32.4
Shenyang Xu,Zhefeng Chen,Wenguang Zhao,Wenju Ren,Chenxin Hou,Jiajie Liu,Wu Wang,Chong Yin,Xinghua Tan,Xiaobing Lou,Xiangming Yao,Zhihai Gao,Hao Liu,Lu Wang,Zuwei Yin,Bao Qiu,Bingwen Hu,Tianyi Li,Cheng Dong,Feng Pan,Mingjian Zhang
As commercial cathodes with the highest practical capacity, the structural nature of Li-rich Mn-based (LMR) cathodes, composite or solid solution, is still under debate. Due to the extreme structural similarity of two layered-phase components, namely, the monoclinic phase (C2/m) and rhombohedral phase (Rm), no single tool can resolve this concern alone. Herein, we combined multiple advanced techniques to comprehensively study the structural changes during synthesis of LMR cathodes from different aspects such as the elemental distribution, local structure, long-range structure, and short-range structure, revealing a clear process from the formation of two phases to the gradual phase fusion and eventually to a nearly solid solution. Particularly, X-ray pair distribution function (PDF) analysis combined with theoretical simulations reveals for the first time that the transition metal (TM)–TM distance increases with the progress of the phase fusion, which makes the short-range structural change in TM–TM atomic pairs an effective parameter for judging the extent of phase fusion. Eventually, excellent electrochemical performance was achieved by balancing capacity and cycling stability through adjusting the phase fusion to a medium extent in lithium and sodium two layered-phase components. This study establishes an approach to investigate the structural evolution in the complicated multiple-phase system and provides valuable insights into the design and optimization of cathodes by tuning the phase fusion extent.
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 Communications
·
2025
·Vol. 16
·期 1
·1-11
·
IF 15.7
Lai Guojun,Zhao Zequan,Zhang Hao,Hu Xueting,Lu Bingan,Liang Shuquan,Zhou Jiang
Engineering the formulation of an Mn-based positive electrode is a viable strategy for producing an efficient aqueous zinc-ion battery. However, Mn dissolution and the byproducts result in capacity fading, thus limiting its electrochemical performances. To solve the undesirable issues, the concept of in-situ forming the positive electrode/electrolyte interface on the commercial MnO 2 is designed, with the help of introducing the Dioctyl Phthalate into the ZS-based electrolyte (2 M ZnSO 4 + 0.2 M MnSO 4 ), designated as ZS-DOP electrolyte. An advanced three-dimensional chemical and imaging analysis on a model material reveals the dynamic formation of positive electrode/electrolyte interface. The formed organic interface effectively suppresses the corrosion of the electrolytes with its hydrophobicity, and adjusts the pH value according to Le Chatelier’s Principle to inhibit the production of by-products. Specifically, the pouch cell assembled with the ZS-DOP electrolyte attains a reversible capacity of ~2.5 Ah and powers the unmanned aerial vehicle. Furthermore, photovoltaic energy storage applications deliver a stable capacity of 0.5 Ah and realize the power supply for mobile phones and other electronic devices. Our results facilitate the development of in-situ surface protection on the positive electrode in aqueous zinc-ion battery, providing insights into its practical application.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Zhaojin Li,Jialin Ren,Huilan Sun,Di Zhang,Qiujun Wang,Qujiang Sun,Bo Wang
Lithium-rich manganese-based cathode materials (LNCM) have garnered tremendous attention for the superior reversible capacity. However, the inherently unstable structure and low diffusion kinetics of Li + hamper their commercialization process. Recent studies have shown that void defects within grains are the main cause of oxygen release and voltage drop during cycling. Therefore, highly crystallinity small particles are the ideal structure for high power density and cycling stability of LNCM. However, improving the crystallinity of materials often means increasing the sintering temperature, which can easily cause material aggregation and grain growth. In this paper, by adopting the electrostatic spinning technology, nanowire shaped precursor are constructed, which facilitates the direct contact between the hot gas flow and the precursor during sintering, thus promoting ion diffusion and material crystallinity. Besides, the electronic and chemical environment in the modified LNCM sample have regulated simultaneously, accompanying with a significant increase in O vacancies, Mn 4+ and Ni 3+ ions. Adjustments from morphology to molecular structure increased the contact area between the material and electrolyte, improved the diffusion ability of Li + , and enhanced structural stability of the material, resulting in improved rate performance and cycling stability. This study expands our understanding of adopting electrospinning technology to prepare high-performance materials.
研究领域:
材料科学
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能源存储
✓ 已验证
产品关联
DOI
高影响因子
Journal of Cleaner Production
·
2018
·
IF 5.651
Yue Yang,Shaole Song,Feng Jiang,Jiahui Zhou,Wei Sun
Recovering metal values from spent Lithium ion batteries (LIBs) enjoys a great significance in environmental protection and sustainable development of resources. But the application of mixed-type cathode materials in PHEV and EV with high content of manganese brings new challenges for spent LIBs recycling. In this study, a facile approach for directly regenerating Mn-rich cathode material from mixed-type spent cathode materials was developed. The spent cathode materials were firstly tested by X-Ray Diffraction (XRD) and X-ray fluorescence (XRF) and then leached in H 2 SO 4 +H 2 O 2 system. The spherical Mn-rich cathode material was directly regenerated from leaching liquor through a facile co-precipitation method followed by solid-phase sintering. The regenerative cathode material was measured by XRD, scanning electron microscope (SEM) equipped with energy dispersive X-ray spectroscopy system (EDXS), inductively coupled plasma atomic emission spectrometry (ICP), laser particle size analyzer and electrochemical tests. According to the results, pure cathode material exhibits a uniform particle size distribution and a layered structure. Furthermore, the regenerative cathode material with high working voltage (>4.5 V) possesses excellent discharge capacity. Cleaner production analysis indicates that whole process can effectively reduce waste residue and water, and helps turn the solid waste into resource. Meanwhile, compared to traditional methods, the proposed process can simplify the recovery process, obtain high value added Mn-rich cathode material and maximize the recovery of manganese in the mixed-type spent cathode materials.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Nano
·
2021
·
IF 15.881
Xiaodong Zhu,Ziyi Cao,Wenjie Wang,Haijing Li,Juncai Dong,Shangpeng Gao,Dongxiao Xu,Lei Li,Jianfeng Shen,Mingxin Ye
Mn-based aqueous zinc-ion batteries (ZIBs) are promising candidate for large-scale rechargeable energy storage because of easy fabrication, low cost, and high safety. Nevertheless, the commercial application of Mn-based cathode is hindered by the challenging issues of low rate capability and poor cyclability. Herein, a manganese–vanadium hybrid, K–V2C@MnO2 cathode, featured with MnO2 nanosheets uniformly formed on a V2CTX MXene surface, is elaborately designed and synthesized by metal–cation intercalation and following in situ growth strategy. Benefiting from the hybrid structure with high conductivity, abundant active sites, and the synergistic reaction of Mn2+ electrodeposition and inhibited structural damage of MnO2, K–V2C@MnO2 shows excellent electrochemical performance for aqueous ZIBs. Specifically, it presents the high specific capacity of 408.1 mAh g–1 at 0.3 A g–1 and maintains the specific capacity of 119.2 mAh g–1 at a high current density of 10 A g–1 in a long-term cycle of up to 10000 cycles. It is superior to almost all reported Mn-based cathodes for ZIBs in the aqueous electrolyte. The superior electrochemical performance suggests that the Mn-based cathode materials designed in this work can be a rational approach to be applied for high-performance ZIBs cathodes.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2025
·
IF 5.6
Huihui Gan,Liang Li,Pengyuan Qiu,Mingyu Cui,Jiajun Sun,Ye Xia,Wen Zhu
Layered Li-rich Mn-based oxide cathode materials (LRMO) have attracted extensive attention because of their high energy density. However, the poor cyclic stability, rate capability, and rapidly decay in voltage impede the practical application. Herein, a novel strategy for designing LRMO modified by silica-coated silver nanowires (AgNWs@SiO 2 ) is reported. The AgNWs@SiO 2 can provide the faster Li + diffusion kinetics, increase oxygen vacancy, and facilitate the heat dissipation in LRMO. As a result, the AgNWs@SiO 2 modified LRMO delivers a higher capacity retention of 71.6 % (after 500 cycles at 25 °C) and 58.5 % (after 200 cycles at 60 °C) at 1C than that of the untreated LRMO (65.2 % after 500 cycles at 25 °C and 37.8 % after 110 cycles at 60 °C). Meanwhile, the AgNWs@SiO 2 modified LRMO also possesses high-rate discharge specific capacity of 105.4 mAh g -1 at 10C and capacity retention of 50.6 % after 1000 cycles at 3C (the untreated LRMO only remains 19.3 % after 600 cycles at 3C). Furthermore, the AgNWs@SiO 2 modified LRMO also exhibits good electrochemical performance in the cell assembled with Si@C anode. This work provides a promising strategy for the possibility practical application toward next-generation high energy density lithium-ion batteries.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Chao Wu,Shuang Cao,Heng Li,Zhi Li,Gairong Chen,Xiaowei Guo,Baobao Chang,Yansong Bai,Xianyou Wang
Herein, we put forward a feasible interfacial modification strategy in virtue of Mn 3 O 4 surface coating to construct protective shell and alleviate Jahn-Teller distortion during the charge/discharge process. It has been found that the increase of the oxygen vacancy on the surface of Li 1.2 Ni 0.27 Mn 0.54 O 2 of (LRNMO) after Mn 3 O 4 protective layer modification can effectively restrain the release of oxygen and enhancing rate capability, and thus improving its comprehensive electrochemical performances. In particular, the initial coulombic efficiency of the optimized LRNMO-1 electrode is improved from 72.3% to 84.3%. The capacity retention rate is up to 95.6% at 250 mA g −1 (1C) after 200 cycles. In addition, the LRNMO-1 electrode also has a good capacity retention rate (96.4% after 100 cycles) at a high current density of 5C. Moreover, the designed LRNMO@Mn 3 O 4 cathode exhibits higher ionic conductivity and better interface stability. As a result, this work offers a practicable and valuable exploration for the development and industrialization of Co-free Li-rich Mn-based cathode materials with high energy density .
研究领域:
材料科学
·
能源存储技术
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Hang Xu,Kezhu Jiang,Xueping Zhang,Xiaoyu Zhang,Shaohua Guo,Haoshen Zhou
Sodium-ion batteries (SIBs) are promising candidates applied to large-scale energy storage systems owing to abundant sodium resources and high economic efficiency. Layered manganese-based oxides as a prevailing cathode for sodium-ion batteries have been extensively studied, where doping or coating has been demonstrated to improve the electrochemical performance. However, the binder that tends to be the popular poly(vinylidene difluoride), is revealed to generate swellability upon cycling, leading to electrode material cracks and disconnection with current collectors. For the above issues, in this work, environmentally friendly sodium alginate is utilized as the aqueous binder in a conventional layered transition-metal oxide cathode P2-Na2/3MnO2 for SIBs. Through credible comparative experiments, sodium alginate is testified to play an essential role in suppressing cracks on the surface of materials, preventing surge in charge-transfer resistance and restraining detachment between electrode and current collector. Therefore, sodium alginate is proved to be an ideal binder to match with P2-Na2/3MnO2, where some issues existed before, as a promising cathode material with excellent performance and low cost. This study displays that improving battery performance by exploring suitable binder systems can equal or even exceed the performance improvement through modification of the material itself, and this perspective of enhancement should not be ignored.
研究领域:
材料科学
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能源存储技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Jingdong Guo,Weibing Ma,Zhiyuan Sang,Xueqi Zhang,Ji Liang,Feng Hou,Wenping Si,Song Wang,De'an Yang
Aqueous zinc‐ion batteries (ZIBs) have become a promising alternative to lithium-ion batteries (LIBs) for grid‐scale energy storage. However, the bivalent nature and large radius of zinc hydrated ions commonly lead to a strong electrostatic interaction with the host lattice and a huge strain feature during zinc-ion insertion, which results in slow diffusion kinetics and poor cycling stability. Herein, a lattice-water-rich V-based polyanionic cathode, named Mn 0.25 (VO) 0.75 PO 4 ·2.25H 2 O (MnVP), is mass-producible and in which the sufficient lattice water weakens the electrostatic interactions and facilitates the rapid Zn 2+ migration kinetics. The introduced Mn 3+ ions partially replaced the V elements, which made the crystal structure more stable during the cycle. Besides, the doping of inactive Mn 3+ can introduce the crystal water, which lower the stress and strain of the host lattice during zinc-ion insertion. Thus, the MnVP cathode delivers a high specific capacity (207.7 mAh g −1 at 0.1 A g −1 ), excellent rate capability (93.5% retention at 5 A g −1 ) and long cycle durability (after 700 cycles with a capacity retention of 88.4 %). Furthermore, the simple preparation and low cost make this cathode expect to be used in large‐scale energy storage systems.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Energy Materials
·
2024
·
IF 5.4
Tiandong Chen,Luxiang Ma,Hongli Su,Wencheng Pan,Chunxi Hai,Shengde Dong,Yanxia Sun,Qi Xu,Xin He,Yan Zhao,Jitao Chen,Zhiqin Zheng,Yuan Zhou
Despite the high energy density of lithium-rich manganese-based (LR) cathode materials, the practical implementation in batteries has been impeded by the intrinsic issues regarding cycling. Herein, a coherent interface modification strategy is proposed. The LR materials are coated with a lattice-matched Li3BO3 (LBO) layer at the interface. The coating applied to the electrode has two impacts. (1) It reduces interfacial side reactions between the electrode materials and electrolyte, thereby improving structural stability. (2) It mitigates stress between solid particles, which enhances the cycling stability (83% after 500 cycles at 2C) of LR. Furthermore, the LBO coating promotes the development of a spinel-like structure on the electrode materials surface, eliminating unstable oxygen, increasing oxygen vacancy (Ov), consequently enhancing the initial Coulombic efficiency (ICE, 92.18%), and alleviating particle breakage (Young’s moduli of LR@S@LBO is 3.26 ± 1.6 GPa) after optimization. Theoretical calculations show that Ov and spinel can improve the diffusion of Li+ and the structural stability of LR materials. This work shows great potential for the rational design of high-energy-density electrode materials.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Science China-Chemistry
·
2024
·
IF 10.4
Liu Zheng,Qiu Zhipeng,Li Zhiyuan,Wei Tong,Fan Zhuangjun,Pang Huan
Due to the low cost, high theoretical capacity, and environmental friendliness, manganese-based cathodes are regarded as promising alternatives for aqueous zinc ion batteries (AZIBs). However, the practicality of the zinc-manganese system is faced with great challenges, such as the inevitable structural collapse of the cathode and controversial energy storage mechanisms. Herein, we propose a novel concept of spatial deposition mechanism through the addition of MnSO 4 additives in the MnO-pillared graphene blocks (G-MnO). The covalent interface between MnO nanoparticles and multilayered graphene nanosheets can construct an in-built micro-electric field, which is beneficial for consecutive electron transfer (in both horizontal and vertical directions). On this basis, the surficial activity of MnO confined in the interlayered nano-space is greatly enhanced and provides enough spatial deposition and subsequent reaction site for MnSO 4 additives, thus firstly extending the surficial controlled process to stereoscopic space, effectively improving the electrochemical performance of AZIBs. Therefore, the assembled Zn//G-MnO battery exhibits an excellent rate capability of 281.5 mAh g −1 at 0.1 A g −1 and 106 mAh g −1 at 20 A g −1 , and impressive cycling stability (93 mAh g −1 remaining after 5,000 cycles). This finding may provide a new opportunity for the rational design of surficial controlled energy storage and conversion devices.
研究领域:
材料科学
·
能源存储
✓ 已验证
DOI
高影响因子
Small
·
2025
·Vol. 21
·期 19
·2411490
·
IF 12.1
Yujia Zhang,Fuliang Guo,Ao Li,Zhixiong Li,Pengcheng Yuan,Jing Xu,Zhiwei Hu,Liang Yin,Huiling Zhao,Ying Bai,Hong Li
Heteroatoms doping would validly stabilize the structure of Li-rich material and elevate electrochemical performance. For the synthesized Li-rich material, the conventional ex situ doping strategy can only incorporate heteroatoms in the outer particles, diminishing benefits for the internal structure of secondary particles. Recently, in situ doping has been employed to influence topological lithiation and achieve well-distribution in the bulk structure. However, the mechanisms of in/ex situ doping on elevating electrochemical performance for Li-rich material are ambiguous. Herein, by introducing magnesium (Mg 2+ ) ions on the precursor and synthesized Li-rich material, the in situ Mg doping (LRO-Mg1) and the ex situ Mg doping (LRO-Mg2) samples are successfully designed. Characterizations shows that Mg ion tend to incorporate into the Li-rich bulk structure for in situ doping, while they enrich in the surface for ex situ doping. Electrochemical measurement manifest that the in situ Mg doping Li-rich cathode exhibits more elevated high-rate performance, while the ex situ doping Li-rich cathode exhibits more elevated specific capacity, illuminating that enhances bulk structure of Li-rich cathode through in situ doping strategy is more effective than the surface modification (ex situ doping). Ex situ doping may be more effective for surface treatment, contributing to specific capacity improvement.
研究领域:
材料科学
·
电化学
✓ 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）