Energy Storage Materials
·
2024
·
IF 18.9
Yuhang Xin,Yingshuai Wang,Qingbo Zhou,Hexiao Zhang,Ziye Wang,Lei Liu,Kunyu Zhao,Feng Wu,Hongcai Gao
Due to the uniform distribution of sodium in the crust, the increasing demand for high specific energy and long life in terms of energy storage is placing higher requests on sodium-ion battery technology. The activation of multi-electron reactions in NASICON sodium-ion battery cathode materials can not only reduce the use of vanadium, but also effectively increase the specific energy, therefore, it has received enormous attention from researchers. In this report, the importance of the covalent proportion of metal-oxygen bond in activating the V 4+ /V 5+ redox with higher discharge voltage in Na 3 V 2 (PO 4 ) 3 has been extensively studied. Advanced characterization methods and theoretical calculations comprehensively explain the effects of Zn 2+ , Mg 2+ , and Cu 2+ on V 3+ substitution and the corresponding electrochemical behavior and structural change behavior. Moreover, a complete two-phase reaction in the high voltage reaction region (3.88 V) was observed in Na 3 V 1.5 Cu 0.5 (PO 4 ) 3 . Our results highlight the importance of the covalent proportion of metal-oxygen bonds in activating multi-electron reactions in NASICON structures.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2020
·Vol. 31
·期 8
·2008033
·
IF 16.836
Ying Liu,Yue Jiang,Zhe Hu,Jian Peng,Weihong Lai,Dianlun Wu,Shouwei Zuo,Jing Zhang,Bin Chen,Ziwen Dai,Yingguo Yang,Yang Huang,Wei Zhang,Wei Zhao,Wang Zhang,Lei Wang,Shulei Chou
Vanadium-based materials are fascinating potential cathodes for high energy density Zn-ion batteries (ZIBs), due to their high capacity arising from multi-electron redox chemistry. Most vanadium-based materials suffer from poor rate capability, however, owing to their low conductivity and large dimension. Here, we propose the application of V 2 C MXene (V 2 CT x ), a conductive 2D nanomaterial, for achieving high energy density ZIBs with superior rate capability. Through an initial charging activation, the valence of surface vanadium in V 2 CT x cathode is raised significantly from V 2+ /V 3+ to V 4+ /V 5+ , forming a nanoscale vanadium oxide (VO x ) coating that effectively undergoes multi-electron reactions, whereas the inner V-C-V 2D multi-layers of V 2 CT x are intentionally preserved, providing abundant nanochannels with intrinsic high conductivity. Owing to the synergistic effects between the outer high-valence VO x and inner conductive V-C-V, the activated V 2 CT x presents an ultrahigh rate performance, reaching 358 mAh g −1 at 30 A g −1 , together with remarkable energy and power density (318 Wh kg −1 /22.5 kW kg −1 ). The structural advantages of activated V 2 CT x are maintained after 2000 cycles, offering excellent stability with nearly 100% Coulombic efficiency. This work provides key insights into the design of high-performance cathode materials for advanced ZIBs.
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
Nano Energy
·
2021
·
IF 17.881
Shiqi Ding,Xin Dai,Yuxin Tian,Bo Song,Lei Wang,Guicun Li,Shaoxiang Li,Jianfeng Huang,Zhenjiang Li,Alan Meng
Multi-electron reaction as the appealing alternative can offer higher specific capacity, however, it delivers a tendency to collapse the structure causing cycling instability. Herein, K + pre-intercalation strategy is applied to modify VS 4 /N-TG as cathode for MIBs . As opposed to the structural breakdown caused by multi-electron reaction, pre-intercalated K + not only modulate electronic state, making V 2+ present as instead of partial V 4+ achieving multi-electron reaction, but also act as pillar ions for coordinating the interaction of guest-ions with adjacent host ions to strengthen the framework to maintain structural stability, therefore, K 0.20 VS 4 /N-TG delivers high specific capacity of 190 mAh g –1 , and excellent cycling stability with about near 100% capacity retention after 2000 cycles. This finding gives insights into enabling multi-electron transfer reaction while achieving high structural stability via K + pre-intercalation, shed light on designing viable multi-electron reaction in intercalation type cathode without destroying stable structure for high performance magnesium ions batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2020
·Vol. 25
·期 4
·1000
·
IF 3.267
Rui Liu,Ziteng Liang,Yuxuan Xiang,Weimin Zhao,Haodong Liu,Yan Chen,Ke An,Yong Yang
Na3V(PO4)2was reported recently as a novel cathode material with high theoretical energy density for Sodium-ion batteries (SIBs). However, whether V3+/V4+/V5+multielectron reactions can be realized during the charging process is still an open question. In this work, Na3V(PO4)2is synthesized by using a solid-state method. Its atomic composition and crystal structure are verified by X-ray diffraction (XRD) and neutron diffraction (ND) joint refinement. The electrochemical performance of Na3V(PO4)2is evaluated in two different voltage windows, namely 2.5–3.8 and 2.5–4.3 V.51V solid-state NMR (ssNMR) results disclose the presence of V5+in Na2−xV(PO4)2when charging Na3V(PO4)2to 4.3 V, confirming Na3V(PO4)2is a potential high energy density cathode through realization of V3+/V4+/V5+multielectron reactions.Keywords:polyanion;energy density;multielectron reaction;solid-state NMR
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 Nano
·
2024
·
IF 15.8
Zhiqiang Hao,Xiaoyan Shi,Wenqing Zhu,Zhuo Yang,Xunzhu Zhou,Chenchen Wang,Lin Li,Weibo Hua,Chang-Qi Ma,Shulei Chou
Na3V2(PO4)3 (NVP) based on the multielectron reactions between V2+ and V5+ has been considered a promising cathode for sodium-ion batteries (SIBs). However, it still suffers from unsatisfactory stability, caused by the poor reversibility of the V5+/V4+ redox couple and structure evolution. Herein, we propos a strategy that combines high-entropy substitution and electrolyte optimization to boost the reversible multielectron reactions of NVP. The high reversibility of the V5+/V4+ redox couple and crystalline structure evolution are disclosed by in situ X-ray absorption near-edge structure spectra and in situ X-ray diffraction. Meanwhile, the electrochemical reaction kinetics of high-entropy substitution NVP (HE-NVP) can be further improved in the diglyme-based electrolyte. These enable HE-NVP to deliver a superior electrochemical performance (capacity retention of 93.1% after 2000 cycles; a large reversible capacity of 120 mAh g–1 even at 5.0 A g–1). Besides, the long cycle life and high power density of the HE-NVP∥natural graphite full-cell configuration demonstrated the superiority of HE-NVP cathode in SIBs. This work highlights that the synergism of high-entropy substitution and electrolyte optimization is a powerful strategy to enhance the sodium-storage performance of polyanionic cathodes for SIBs.
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
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Zhuo Chen,Qiming Wang,Shuai Bai,Xi Wang,Wenlie Lin,Yining Zhang
Pseudocapacitive material can achieve rapid charge and discharge response. In this study, a vanadium-based conductive network hydrate (Na 0.13 Mg 0.02 )V 2 O 5 ·0.98H 2 O (NMVO) was designed. The Na + and Mg 2+ in NMVO are sandwiched between two layers of vacancy-ordered prisms and monoclinic nanonetwork V 3 O 7 (VO 2 :V 2 O 5 = 1:1) to form a conductive network with a layer spacing of up to 11.67 Å, this structure facilitates rapid interlayer diffusion of cations and enhanced conductivity. Reduction-NMVO (r-NMVO) with hierarchical heterostructures was prepared via an in-situ electrochemical process to generate interlayer vanadium-based active sites (LiV 3 O 8 , LiV 2 O 5 , Na 3 V 3 O 8 , MgVO 3 ) with multi-electron reaction, which enhanced the generation of surface redox pseudocapacitance. The interlayer heterostructure is integrated with the core of the precursor V 3 O 7 to form an active site-rich conductive network with strong pulse impact resistance, which promotes the generation of intercalated pseudocapacitance and increases the cycle stability of the electrode. This intercalation-surface redox pseudocapacitive mechanism was confirmed by first-principles, in-situ, and ex-situ characterization analysis. The r-NMVO|Li battery still maintains a capacity of 95.5 % after 65,500 cycles at a current density of 50 A g −1 . These results contribute directly to the realization of stable, fast charge and discharge material design.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Peng-Xing Xie,Qing-Yuan Zhao,Haojie Dong,Tao Long,Meng-Sha Ding,Bin Xie,Xiao-Feng Wang,Wei Ling,Mengting Liu,Xiong-Wei Wu,Peng-Fei Wang,Xian-Xiang Zeng
Delivery of high energy density in polyanion compound-Na 3 V 2 (PO 4 ) 3 based on three-electron redox is still challenging because of their controversial multi-electron reaction mechanism and unsatisfactory electrochemical reversibility. Herein, the reversible V 4+ /V 5+ redox ( ca. 4.0 V) could be successfully activated in Na 4 VFe(PO 4 ) 3 cathode material through a Na-rich strategy, demonstrating a reversible specific capacity of 154.7mAh g −1 at 0.1C and 90.3mAh g −1 after 800 cycles at 20C, with 80 % of the initial capacity retained. The entire electrochemical reaction undergoes a highly recoverable phase transition by in-situ X-ray diffraction. Impressively, the Na-rich strategy could not only allow Na2 site to be occupied to activate the V 4+ /V 5+ redox pair confirmed by X-ray absorption near-edge structure spectroscopy, but also enable Na + transportation across the generated vacancies rather than synergistic Na + diffusion. This work provides rational design strategy of multi-electron transfer reaction in high-energy sodium-ion batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Lei Tan,Zhao Li,Lei Wang,Yu Shang,Zhiguo Wang,Zhengwang Tong,Yan Li,Xiangming Li
Layered vanadium oxide materials exhibit significant multielectron redox reactions and regulatable transfer channels for Zn 2+ insertion/extraction in rechargeable aqueous zinc-ion batteries (AZIBs). However, vanadium dissolution poses a severe challenge to achieving stable performance in AZIBs. In this work, we report an in-situ polymerization of polyaniline (PANI) on ZnV 2 O 4 (ZVO) materials, resulting in a cross-interlocked nanosheet morphology to inhibit vanadium dissolution. The high conductivity and unique π-conjugated structure of PANI effectively weaken the electrostatic interactions between Zn 2+ and the V-O layers, thereby enhancing the diffusion of Zn 2+ at the electrode material interface, suppressing the vanadium dissolution of ZnV 2 O 4 and stabilizing its structure framework. Concurrently, density functional theory (DFT) calculations further confirm that PANI can significantly modulate the electronic properties of the ZVO matrix. PANI forms robust hydrogen bonds with ZVO, resulting in an abundance of free Zn ions within the system, which accelerates electron/ion transfer kinetics, thereby enhancing the efficient storage performance of Zn 2+ and increasing specific capacity. The ZVO@PANI composite electrode exhibits high specific capacity (706.4 mAh g −1 at 0.1 A g −1 ), remarkable rate capability (350.2 mAh g −1 at 5 A g −1 ), and robust cycling performance. This study provides a reasonable strategy for designing high-performance cathode materials for aqueous zinc-ion batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2017
·
IF 4.798
Haijun Ye,Fangqing Jiang,Hongqin Li,Zheng Xu,Jiao Yin,Hui Zhu
The redox-active organic compounds show great potentials as anodes for high energy density Li-ion batteries (LIBs), comparing with the traditional transition metal-based inorganic compounds. However, the inevitable dissolution behaviors of these organics in organic electrolyte will arouse the recession in their cycling stabilities. To circumvent this problem, we successfully applied an electrochemically active imine group to connect the carbonyl compound to form conjugated polymer, where the occurrence of multi-electron reactions suppressed the dissolution of anthraquinone in the organic electrolyte with improved cycling stability and high capacity for LIBs. In detail, by virtue of a facile solid-phase reaction between 1, 4-diaminoanthraquinone (14DAAQ) and p-phthalaldehyde (PPD), a highly conjugated polymeric Schiff base (PSB) was synthesized. The obtained PSB exhibited a reversible specific capacity of 175 mAh g −1 at a current density of 10 mA g −1 . In addition, after 100 cycles, a cycling stability with 90% capacity retention can be maintained, manifesting a promising application of the organic material in high performance anodes for LIBs.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Rong Niu,Jie Ding,Jiajun Chen,Zhenxin Zhao,Xiaomin Wang
Transition metal sulfide (TMs) offers ultra-high specific capacity through multi-electron transfer, showing promise for aqueous batteries. However, the poor cycling performance and the uncleared energy storage mechanism are restricted from further development. Herein, CoS 2 nanowire arrays grown on carbon cloth (CoS 2 /CC) are proposed as binder-free and self-supporting electrodes for aqueous copper-ion batteries. The energy storage mechanism is clarified by a series of ex-situ tests: a multi-electron electrode reaction through a three-step reaction of CoS 2 → CuS → Cu 7 S 4 → Cu 2 S. Electrochemical results suggest that the CoS 2 /CC cathode exhibits excellent long cycle stability (capacity retention of 99.7 % after 1000 cycles at 10 A/g) along with high specific capacity (762.3 mAh g −1 at 1 A/g). The carbon cloth with stable three-dimensional (3D) conductive structure can not only offer high-speed pathways to promote the transfer of electrons but also inhibit the volume change. Meanwhile, CoS 2 nanowire arrays with high surface-to-volume ratios can improve wettability of electrolyte and promote redox reactions. Furthermore, an advanced Zn-CoS 2 /CC hybrid ion aqueous battery reveals an energy density of 724 Wh kg −1 and an output voltage of 1.24 V, providing a promising strategy for the establishment of transition metal sulfide cathode in high-energy aqueous 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
Journal of Energy Storage
·
2024
·
IF 8.9
Congcong Meng,Ning An,Shengmiao Song,Ling Wang,Liangzhikun Xiao,Yi Zhou,Ruibin Qiang,Yuying Yang,Zhimin Li,Zhongai Hu
P-benzoquinone (BQ) and derivatives represent a novel class of supercapacitor electrode materials due to their environmental friendliness, design flexibility and significant potential for rapid multi-electron faradaic reactions. But at present, the progress in guiding the structure design of electrochemical organic molecules and understanding their redox properties is still limited in explaining certain experimental phenomena related to supercapacitors. In this study, we propose an effective strategy for accurately predicting the redox potential of the organic molecular electrode (OME) through first-principles density functional theory (DFT). Additionally, we systematically investigated the impact of different functional groups and quantities on the reduction potential of 14 type BQ derivatives. We have identified a key factor that significantly affects the redox potential of OME: the electron cloud density surrounding the quinone active site (C=O). The electron-donating group (-CH 3 ) and benzene ring structure can further increase the electron cloud density around the quinone group, reducing reactivity with protons (H + ), thereby leading to a decrease in redox potential. Conversely, electron-withdrawing groups (-NO 2 ) lead to decreased electron cloud density around C O resulting in an increase in electrode potential. Furthermore, calculation results using Pearson correlation coefficients show that electron affinity (EA) has best linear correlation with reduction potential. Finally, we employed four methyl-p-benzoquinone derivatives (MBQ) as the composite organic electrode materials and achieve rapid and continuous reactions among multi-electron active centers within the designated potential window. Due to the synergistic effect from multiple molecules, MBQ-4 demonstrates an impressive specific capacitance of 681 F g −1 in 1 M H 2 SO 4 electrolyte, which is comparable to the pseudocapacitive material RuO 2 but at one-twentieth cost only.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Nano Energy
·
2022
·
IF 19.069
Gabriel Sikukuu Nambafu,Ernest Pahuyo Delmo,Usman Bin Shahid,Cheng Zhang,Qing Chen,Tianshou Zhao,Ping Gao,Khalil Amine,Minhua Shao
Non-aqueous redox flow batteries based on total organic electrolytes, consisting of earth-abundant elements, i.e., C, H, N, O, are regarded as a promising technology for sustainable and large-scale energy storage. In particular, bipolar redox-active organic materials (BROMs) are distinctly fascinating as electroactive species because they have multiple oxidation states and can undergo multiple redox processes . By virtue of this unique characteristic, BROMs can be utilized as both anolyte and catholyte in symmetric flow batteries, consequently, helping alleviate cross-contamination issues. Herein we report an all-organic symmetric redox flow battery based on diimide molecule as a bipolar electroactive material. The potential interval between the cathodic peak and the inner and outer anodic peaks led to a promising cell voltage of 2.22 V. The symmetric battery can be operated at a current density of 20 mA cm −2 , with a coulombic efficiency of 90% for over 100 cycles. This work proposes an alternative approach to designing multi-electron organic redox active materials to facilitate the advancement of high-density symmetric flow batteries.
研究领域:
能源科学
·
电化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）