ELECTROCHIMICA ACTA
·
2020
·
IF 6.215
Ce Qiu,Xiaohui Zhu,Liang Xue,Mingzhu Ni,Yang Zhao,Bo Liu,Hui Xia
Adding Mn 2+ in aqueous electrolyte is a well adopted approach to improve cycle performance for Zn/MnO 2 batteries. The function of Mn 2+ additive in aqueous electrolyte, however, is not well understood, which could affect revealing the real performance of the MnO 2 cathode itself. In this work, a battery system with Zn anode and birnessite MnO 2 cathode is constructed and systematically investigated by using MnSO 4 additive in the electrolyte with different concentrations. The function of Mn 2+ in the electrolyte, the structural evolution of the electrode, the reaction mechanism, and the cause for capacity fading are comprehensively investigated in this system. It is found that Mn 2+ can be continuously electro-oxidized at the cathode and form ε-MnO 2 when the charge voltage is above 1.7 V during cycling, leading to successive capacity increase up to hundreds of cycles. The capacity increase, however, stops after certain cycle numbers, and is followed by fast capacity fading, which is correlated to the competition between ε-MnO 2 formation and phase transition from birnessite to spinel ZnMn 2 O 4 . It is suggested that addition of Mn 2+ in the electrolyte cannot stabilize the MnO 2 cathode and the improved cycle performance is achieved at the expense of consuming the Mn 2+ in the electrolyte.
研究领域:
电化学
·
材料科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Cong Chen,Minjie Shi,Yue Zhao,Cheng Yang,Liping Zhao,Chao Yan
Although manganese dioxide (MnO 2 ) is of great promise as the cathode material for aqueous Zn-ion batteries (ZIBs), its capacity decreases sharply during cycles due to the irreversible phase transition and Mn dissolution, consequently hindering the large-scale practical application. Herein, for the first time, a novel Al-intercalation engineering of MnO 2 cathode has been proposed for aqueous ZIBs, in which the structural regulation and Zn 2+ storage performance of Al-intercalated MnO 2 (denoted as AMO) cathode are deeply investigated. Electrochemical testing results indicate significant improvement in specific capacity (401.7 mAh g −1 ) and cycling retention (~94.5% over 2000 cycles) of the AMO cathode, which is owing to the effective Al-intercalation that result in the formation of strong Al-O bonds in tunnel-type MnO 2 framework. This reasonable configuration not only optimizes charge/ion state and electronic bandgap, but also ensures reversible phase transition and alleviates the Mn dissolution of AMO cathode, which are further demonstrated by the density functional theory (DFT) calculations and in-situ Raman investigation upon charging-discharging. As a proof of concept, coin-type and flexible aqueous ZIBs based on such AMO cathode are effectively fabricated, and they both achieve excellent electrochemical behaviors, revealing the great potential applications in energy technologies and portable/wearable electronics.
研究领域:
材料科学
·
电化学
✓ 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
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Xin Ren,Fanjue Wen,Shuai Cao,Fei Xu
Rechargeable magnesium batteries (RMBs) attract special interests as a low-cost and reliable energy-storage technology, but the development is hindered by the low capacities and sluggish Mg 2+ diffusion kinetics of the traditional inorganic cathode materials. Organic polymers break the hindrance of inorganic lattice and deliver plenty of candidates for RMB cathodes with the flexible and designable frameworks. Herein, three organic polyanthraquinonyl sulfides (PAQSs) are fabricated and investigated comparatively as RMB cathodes to reveal the effect of structure on the electrochemical magnesium-storage performance. It is demonstrated that the capacity decay is primarily owing to the dissolution of the discharge products (magnesiation state) in the electrolyte. The degree of polymerization is an important factor for the cycling stability. Prominently, poly(2,6-anthraquinonyl sulfide) shows an outstanding comprehensive performance, providing a high capacity (145 mAh g −1 at 50 mA g −1 ), an outstanding rate capability (74 mAh/g at 10C) and an excellent cyclability (99 % capacity retained after 1000 cycles at 5C). Significantly, poly(2,6-anthraquinonyl sulfide) store Mg 2+ rather than MgCl + , and exhibits a considerable specific energy density of 185 Wh kg −1 . The present work would assist the rational design of advanced organic RMB electrode materials, and highlights the advantages of organic polymers based on enolization chemistry for high-performance magnesium-storage.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-14
·
IF 15.7
Zhang Hang,Li Jiayang,Liu Jinhang,Gao Yun,Fan Yameng,Liu Xiaohao,Guo Chaofei,Liu Haoxuan,Chen Xiudong,Wu Xingqiao,Liu Yang,Gu Qinfen,Li Li,Wang Jiazhao,Chou Shu-Lei
Low-cost Fe-based Prussian blue analogues often suffer from capacity degradation, resulting in continuous energy loss, impeding commercialization for practical sodium-ion batteries. The underlying cause of capacity decrease remains mysterious. Herein, we show that irreversible phase transitions, structural degradation, deactivation of surface redox centres, and dissolution of transition metal ions in Prussian blue analogues accumulate continuously during cycling. These undesirable changes are responsible for massive destruction of their morphology, leading to the capacity decay. A dual regulation strategy is applied to alleviate the above-mentioned problems of Prussian blue analogues. The designed 18650/33140 cylindrical cells using modified Prussian blue analogues and hard carbon display improved cycling stability and wide-temperature working performance (−40 o C–100 o C). The findings resolve the controversy over the origins of Prussian blue analogues cathode degradation, emphasize the necessity of eliminating irreversible crystal/structural changes to guarantee enhanced cycling stability, and demonstrate the potential of Prussian blue analogues cathode for commercial sodium-ion batteries.
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
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Binbin Zhang,Ruichao Lu,Yueli Cheng,Kamran Amin,Lijuan Mao,Zhixiang Wei
Drastic capacity decay as a result of active sulfur loss caused by the severe shuttle effect of dissolved polysulfides is the main obstacle in the commercial application of Li–S batteries. Various methods have been developed to suppress the active sulfur loss, but the results are far from ideal. Herein, we propose a facile sulfur compensation strategy to improve the cyclic stability of Li–S batteries. The strategy is to compensate sulfur to the cathode by chemical reactions between additional sulfur and lithium polysulfides diffusing away from the cathode. The compensatory sulfur can effectively mitigate the loss of active sulfur in the cathode side caused by the shuttle effect and thus maintain the high capacity of the battery during charging and discharging for long life cycle assessments. Using this strategy, the specific capacity of the assembled Li–S batteries was maintained at >700 mA h g–1 for more than 500 cycles at 1 C and >1000 mA h g–1 for ∼100 cycles at 0.1 C, while the capacity of control batteries rapidly decreased to <200 mA h g–1 under the same conditions.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-14
·
IF 15.7
Zhang Pengbo,Liu Yuzhu,Wei Jie,Wu Zuoao,Song Xinmei,Ding Guochun,Wang Huaizhu,Liang Junchuan,Tie Zuoxiu,Jin Zhong
Aqueous organic redox flow batteries offer promising prospects for large-scale, high-safety, and cost-effective energy storage systems with no reliance on scarce mineral resources. However, challenges such as limited water solubility and poor stability hinder the practical application of organic redox molecules in aqueous organic redox flow batteries. Herein, we report the design and synthesis of an artificial redox-active α-amino acid molecule by functionalizing 1,5-dihydroxyanthraquinone with natural cysteine side group, which exhibits enhanced aqueous solubility and redox reversibility in alkaline aqueous organic redox flow batteries. Owing to its unique zwitterionic structure and abundant hydrogen bonds, the negolyte based on artificial α-amino acid molecule exhibits a very low capacity decay rate of 0.00025% per cycle (equivalent to 0.011% per day) under 1 M electron transfer. Theoretical simulations and spectroscopic analyses underscore the importance of the symmetric distribution and abundant hydrogen-bonding interactions of amphipathic amino acid side chains in enhancing the stability of the anthraquinone redox core and reducing its dimerization, as well as enhancing its water solubility and redox reversibility. This study presents the promising potential of nature-inspired principles in designing electrochemically stable, redox-active organic molecules, contributing to the advancement of large-scale, biocompatible, and sustainable aqueous organic redox flow batteries.
研究领域:
能源化学
·
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Mengting Chen,Wenbao Liu,Danyang Ren,Yunlin An,Chang Shu,Shengguang Zhang,Wenjun Liang,Jianchao Sun,Feiyu Kang,Fuyi Jiang
At present, aqueous rechargeable Zn–MnO 2 batteries have attracted widespread attention as green potential application for renewable energy storage devices. MnO 2 cathode has great potential for application, but its proton reaction results in side reactions of cathode, electrolyte consumption, and dramatic pH value changes, suffering from capacity degradation. To address the issues caused by proton deficit, a proton–limited domain strategy is proposed by integrating solid acids (Sulfonic acid type polystyrene–divinylbenzene, SATP) with proton exchange reactions into MnO 2 . SATP can act as a new proton source increasing the amount of H + and reducing the generation of zinc hydroxide sulfate, by–product of proton at the cathode interface, via proton exchange reactions of -HSO 3 – group. As a result, Zn–MnO 2 /SATP battery delivered with excellent rate performance (218.4 mAh g –1 at 2 A g –1 ) and high cycling stability (the retained capacity of 115.8 mAh g –1 after 500 cycles at a current density of 1 A g –1 . This work provides an innovative strategy for high performance aqueous Zn–MnO 2 batteries.
研究领域:
材料科学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
Advanced Energy Materials
·
2024
·Vol. 14
·期 46
·2402227
·
IF 24.4
Hua Jiang,Wendong Yang,Pei Liu,Linfeng Wang,Jintao Meng,Shuangyan Gui,Xue Long,Xuan Cai,Yilin Zeng,Yifan Zhang,Jinhua Guo,Jun Wang,Jun Zhou,Jiangjiang Duan
Alkaline all-iron flow batteries possess intrinsic safety and low cost, demonstrating great potential for large-scale and long-duration energy storage. However, their commercial application is hindered by the issue of capacity decay resulting from the decomposition of iron complexes and ligand crossovers. In this paper, an robust anolyte Fe(TEA-2S) is reported, which is formed by chelating iron ions with the sulfonate-enriched ligand (TEA-2S) in alkaline environment. By skillfully designing the ligands, the binding energy of the iron complexes increases and ligand crossovers are suppressed, making the iron complexes highly stable in the charge–discharge cycles. Alkaline all-iron flow batteries coupling with Fe(TEA-2S) and the typical iron-cyanide catholyte perform a minimal capacity decay rate (0.17% per day and 0.0014% per cycle), maintaining an average coulombic efficiency of close to 99.93% over 2000 cycles along with a high energy efficiency of 83.5% at a current density of 80 mA cm −2 . In addition, Fe(TEA-2S) exhibits high solubility of up to 1.85 м (with a theoretical capacity of up to 49.58 Ah L −1 ), even at low temperatures as extreme as −30 °C. This work demonstrates a promising pathway toward achieving long-duration and large-scale energy storage.
研究领域:
能源存储技术
·
电化学材料
✓ 已验证
产品关联
DOI
高影响因子
ACTA PHYSICO-CHIMICA SINICA
·
2023
·
IF 10.9
Chaolin Mi,Yuying Qin,Xinli Huang,Yijie Luo,Zhiwei Zhang,Chengxiang Wang,Yuanchang Shi,Longwei Yin,Rutao Wang
Sodium-ion energy storage devices are considered as an ideal substitute for popular lithium-ion counterparts because of its resource richness and environmental friendliness. Among the various sodium-ion energy storage devices, sodium-ion capacitors (SICs) have the combined advantages in high energy and power densities as well as long-term cycling stability in theory. Antimony (Sb) is considered as an attractive anode material for SICs due to its high theoretical capacity of 660 mAh·g −1 , low operating potential (0.5–0.8 V vs. Na/Na + ), and high density of 6.68 g·cm −3 . However, the large volume change of Sb during the Na + insertion leads to fast decay in capacity and poor rate capability, which becomes a fundamental issue greatly hindering the practical application. Herein, a facile galvanic replacement approach is proposed for the synthesis of an ultrafine amorphous Sb nanoparticles anchoring on carbon coated two-dimensional (2D) reduced graphene oxides (RGO). Half-cell test ( vs . metal Na) shows that as-prepared Sb-C@RGO anode delivers a high specific capacity of 521.5 mAh·g −1 at 0.1 A·g −1 . As the current density increases to 10 A·g −1 , Sb-C@RGO anode still maintains a specific capacity of 83.5 mAh·g −1 , suggesting its high-rate properties. The excellent Na + charge storage property of Sb-C@RGO anode is primarily due to its unique 2D hybrid architecture, which largely increases the atomic interface contact with Na + and shortens ion diffusion path, thus facilitating ion/electron transfer. To demonstrate the feasibility of Sb-C@RGO as the high-performance electrode for emerging energy-storage devices, a hybrid cell configuration (e.g., SIC) was fabricated by employing the Sb-C@RGO as the negative electrode (battery type) and home-made activated carbon (PDPC) as the positive electrode (capacitive type) in a Na + based organic electrolyte. This SIC is capable of operating at a high voltage of 4.0 V and exhibiting a high energy density of 140.75 Wh·kg −1 at a power density of 250.84 W·kg −1 . Even the power density is magnified ~50 times to 12.43 kW·kg −1 , this SIC still delivers a high energy density of 55 Wh·kg −1 . Within a short charge/discharge of ~3.2 min, this SIC can store/release quite a high energy density of 108.5 Wh·kg −1 , which represents the remarkable performance among the reported Sb-based capacitors. In addition, this SIC shows the good cycling stability with an acceptable capacity retention value of 66.27% after 1000 cycles at a current density of 2 A·g −1 . Our results may provide insight into the rational design and construction of high-capacity Sb-based anode materials for advanced sodium-ion based energy storage devices. Download: Download high-res image (131KB) Download: Download full-size image
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
APPLIED ENERGY
·
2024
·
IF 10.1
Min Wu,Mingjun Nan,Yujiao Ye,Mingjun Yang,Lin Qiao,Huamin Zhang,Xiangkun Ma
Iron‑chromium flow battery (ICFB) is the one of the most promising flow batteries due to its low cost. However, the serious capacity loss of ICFBs limit its further development. Herein, we analyze the capacity loss mechanism of ICFBs. The capacity loss is due to inactive Cr(H 2 O) 6 3+ ions result in the mismatched content of active ions in catholyte and anolyte. Thus, a simple method is proposed to raise the content of active Cr 3+ species (Cr(H 2 O) 5 Cl 2+ and Cr(H 2 O) 4 Cl 2 + ), achieving the match of Fe 2+ /Fe 3+ and Cr 3+ /Cr 2+ redox couples and reducing the capacity loss of ICFBs. Meanwhile, the increasing content of active Cr 3+ ions was proved by the quantitative analysis of the UV–vis absorption spectra. As a result, the ICFB with the improved electrolyte of 1 M FeCl 2 + 1.3 M CrCl 3 + 3 M HCl (E-1.3Cr) exhibits an energy efficiency (EE) of 84.51%, which is much higher than the original one of 1 M FeCl 2 + 1 M CrCl 3 + 3 M HCl (E-1Cr) (82.32%) at a current density of 80 mA cm −2 . Most importantly, the ICFB with E-1.3Cr (7.44 mAh/cycle) shows the much slower capacity decay rate than that with E-1Cr (9.16 mAh/cycle). This work provides an effective way to accelerate engineering applications of ICFBs.
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 Materials & Interfaces
·
2021
·
IF 9.229
Jianshun Feng,Dong Wang,Qian Zhang,Jie Liu,Yumin Wu,Lei Wang
Exploiting macromolecule binders has been demonstrated as an effective approach to stabilize a Si anode with a huge volume change. The macromolecule polymer binders with vast intra/intermolecular interactions lead to an inferior dispersion of binders on a Si active material. Herein, a potassium triphosphate (PTP) inorganic oligomer was exploited as a robust binder to alleviate the problem of capacity fading in Si-based electrodes. PTP has abundant P–O– bonds and P═O bonds, which can form strong ion–dipolar and dipolar–dipolar forces with a hydroxylated Si surface (Si–OH). Particularly, the PTP inorganic oligomer has a short-chain structure and high water solubility, resulting in a superior dispersion of the PTP binder on Si nanoparticles (nano-Si) to effectively enhance the mechanical stability of Si-based electrodes. Hence, the as-prepared Si-based anode exhibits obviously improved electrochemical performance, delivering a charge capacity of 1279.7 mAh g–1 after 300 cycles at 800 mA g–1 with a high capacity retention of 72.7%. Moreover, using the PTP binder, a dense Si anode can be achieved for high volumetric energy density. The success of this study shows that the PTP inorganic oligomer as a binder has great significance for future advanced binder research.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）