ADVANCED MATERIALS
·
2023
·Vol. 35
·期 17
·2210082
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IF 29.4
Longhai Zhang,Rui Wang,Zixiang Liu,Jiandong Wan,Shilin Zhang,Siming Wang,Kang Hua,Xiaohao Liu,Xunzhu Zhou,Xiansheng Luo,Xiaoyang Zhang,Mengge Cao,Hongwei Kang,Chaofeng Zhang,Zaiping Guo
Sustainable organic electrode materials, as promising alternatives to conventional inorganic electrode materials for sodium-ion batteries (SIBs), are still challenging to realize long-lifetime and high-rate batteries because of their poor conductivity, limited electroactivity, and severe dissolution. It is also urgent to deeply reveal their electrochemical mechanism and evolution processes. A porous organic polymer (POP) with a conjugated and hierarchical structure is designed and synthesized here. The unique molecule and structure endow the POP with electron delocalization, high ionic diffusivity, plentiful active sites, exceptional structure stability, and limited solubility in electrolytes. When evaluated as an anode for SIBs, the POP exhibits appealing electrochemical properties regarding reversible capacity, rate behaviors, and long-duration life. Importantly, using judiciously combined experiments and theoretical computation, including in situ transmission electron microscopy (TEM), and ex situ spectroscopy, we reveal the Na-storage mechanism and dynamic evolution processes of the POP, including 12-electron reaction process with Na, low volume expansion (125–106% vs the initial 100%), and stable composition and structure evolution during repeating sodiation/de-sodiation processes. This quantitative design for ultrafast and highly durable sodium storage in the POP could be of immediate benefit for the rational design of organic electrode materials with ideal electrochemical properties.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Qingjuan Ren,Jianzeng Yang,Peng Zhang,Liang He,Zhongyu Sun,Ruirui Hao,Zhiqiang Shi
Hard carbon (HC) stands as a leading anode candidate for sodium-ion batteries, yet the specific functions of its multiscale pore structure, especially ultramicropores (< 0.7 nm), have remained contentious. Herein, the distinct functions of different pores (open pores, sub-0.7 nm ultramicropores, and closed pores) are elucidated through the rational design of model HC materials derived from a homologous zinc gluconate. It is demonstrated that closed pores (2–3 nm) serve as the dominant contributor to the low-voltage plateau capacity via quasi-metallic sodium cluster formation. Ultramicropores significantly enhance the initial Coulombic efficiency (ICE, up to 93.5%) by enabling selective desolvated Na + access while restricting electrolyte ingress, though they contribute only secondarily to the plateau capacity via adsorption. In contrast, open pores exacerbate irreversible electrolyte decomposition, impairing ICE. The optimized material, ZHC600-1300, delivers a high reversible capacity of 414.8 mAh g −1 , an exceptional ICE of 93.1%, a superior plateau capacity (306 mAh g −1 ), and remarkable cycling stability. When configured in full cells, it delivers a high energy density of 321.5 Wh kg −1 , demonstrating great potential for practical applications. This work provides fundamental insights into pore-dependent sodium storage mechanisms and establishes a design principle for high-performance HC anodes.
研究领域:
材料科学
·
储能
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Advanced Energy Materials
·
2021
·Vol. 11
·期 11
·2003854
·
IF 29.368
Zhaohua Wang,Xin Feng,Ying Bai,Haoyi Yang,Ruiqi Dong,Xinran Wang,Huajie Xu,Qiyu Wang,Hong Li,Hongcai Gao,Chuan Wu
Hard carbon (HC) is the most promising anode material for sodium-ion batteries (SIBs), nevertheless, the understanding of sodium storage mechanism in HC is very limited. As an important aspect of storage mechanism, the steady state of sodium stored in HC has not been revealed clearly to date. Herein, the formation mechanism of quasi-metallic sodium and the quasi-ionic bond between sodium and carbon within the electrochemical reaction on the basis of theoretical calculations are disclosed. The presence of quasi-metallic sodium is further confirmed with the assistance of a specific reaction between the sodiated HC electrode and ethanol, by analyzing the reaction products with Fourier-transform infrared spectroscopy, gas chromatography, and nuclear magnetic resonance. Moreover, based on the specific chemical reaction, the composition of fully sodiated HC is estimated to be NaC 6.7 , and the corresponding capacity of sucrose-derived HC is calculated to be 333.4 mAh g −1 in SIBs, matching well with the experimental result. This work helps to reveal the steady state of sodium and improve the understanding of sodium storage behavior in HC from the aspect of charge transfer. In addition, the proposed method is also expected to pave the way to investigate sodium storage mechanisms in other electrode systems.
研究领域:
材料科学
·
电化学
·
储能
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Haikuo Lei,Bo Tao,Yipu Xu,Wenbo Hou,Xuan Xie,Hui Peng
Developing facile and diverse polymer-derived porous carbon sphere synthesis strategies for sodium-ion battery (SIB) anodes is of great attraction, but the straightforward and scalable synthesis of carbon nanospheres remains a challenge. Different from the traditional sol–gel synthesis of metal–phenolic coordination spheres, here, a solvent-free regulating micelle transformation approach is involved to generate tannic acid–formaldehyde (TAF) polymer nanospheres by condensation reaction of tannic acid and formaldehyde decomposed from hexamethylenetetramine without adding external solvent and using F127 as the structure-directing agent. Subsequently, the TAF nanospheres were carbonized to obtain nitrogen-doped hard carbon nanospheres (NHCNs). The morphology and porous structure (especially the closed pores) of NHCNs were significantly affected by F127. The optimized NHCNs-3 exhibits uniform nanosphere morphology with obvious rough surfaces and abundant closed-pore structures, which significantly enhanced sodium-ion storage performance, including high reversible capacity of 377 mAh g–1 at 0.05 A g–1 and excellent rate performance (277 mAh g–1 at 1 A g–1), as well as good cycling stability (84.4% capacity retention after 1000 cycles at 1 A g–1), outperforming most reported carbon nanosphere anodes. Series characterization confirmed that the sodium storage mechanism of NHCNs-3 includes defect adsorption, graphite intercalation, and pore-filling processes. Moreover, the SIB assembled with a Na3V2(PO4)3 cathode and NHCNs-3 anode exhibited high reversible capacity and retention at high current density, revealing its potential for practical application.
研究领域:
储能
·
材料科学
·
电化学
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纳米技术
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高分子化学
✓ 已验证
产品关联
DOI
高影响因子
IONICS
·
2020
·Vol. 26
·期 9
·4499-4510
·
IF 2.394
Liu Jian,Xu Ying-Ge,Kong Ling-Bin
Herein, molybdenum trisulfide/nickel disulfide-reduced graphene oxide (Mo 2 S 3 /NiS 2 -RGO) composites as anode material for sodium-ion batteries (SIBs) and sodium-ion capacitors (SICs) were synthesized by one-step facile hydrothermal method. Through electron microscopy analysis, it could be observed that the Mo 2 S 3 /NiS 2 nano-rods and nano-balls were dispersed uniformly over the two-dimensional RGO sheets. When tested as an anode material, Mo 2 S 3 /NiS 2 -RGO showed a considerable reversible capacity of 653.1 mA h g −1 at 100 mA g −1 after 50 cycles and capacity retention of 197.5 mA h g −1 at 5000 mA g −1 after 226 cycles. The sodium storage mechanism of Mo 2 S 3 /NiS 2 -RGO was explained by ex situ XPS. Furthermore, as-fabricated SICs delivered an excellent specific energy of 182.7 W h kg −1 (at 1120 W kg −1 ), and SIBs exhibited the discharge capacities of 85 mA h g −1 at 2 C. Overall, the superior electrochemical performances of Mo 2 S 3 /NiS 2 -RGO demonstrated that it was a promising anode materials to construct high-performance full cell.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子