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ACS Applied Materials & Interfaces · 2019 · IF 8.456

In Situ Electrochemical Synthesis of Novel Lithium-Rich Organic Cathodes for All-Organic Li-Ion Full Batteries

Yang Hu,Wu Tang,Qihang Yu,Chuluo Yang,Cong Fan

The lithium-rich organic cathodes are undoubtedly important for fabricating lithium-ion (Li-ion) full batteries. Currently, very few lithium-rich organic cathodes have been reported for their O2-sensitive characteristics. In this article, we initially propose a new electrochemical method to in situ synthesize a novel lithium-rich organic cathode, namely lithium anthracene-9,10-bis[2-benzene-1,4-bis(olate)] (ABB4OLi, CT = 256 mA h g–1), from its phenol precursor of anthracene-9,10-bis(2-benzene-1,4-diol). The addition of anthracene moiety as the linking bridge is to increase the molecular weight and simultaneously enhance the electronic conductivity for the designed organic molecule (ABB4OLi). In Li-ion half cells, ABB4OLi could deliver average specific capacities of 194 mA h g–1 during 250 cycles (50 mA g–1) and 100 mA h g–1 during 400 cycles (2 A g–1). In the all-organic Li-ion full cells with the working voltage above 1 V, the ABB4OLi electrode could realize the average capacities of 70 mA h g–1cathode during 200 cycles (50 mA g–1). This work has forwarded a significant step for the development of organic Li-ion full batteries.

研究领域: 电化学 · 材料科学 · 能源存储 · 锂离子电池 · 有机功能材料 · 电极材料
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ACS Nano · 2025 · IF 16

Fluorine-Free Ion-Selective Membrane with Enhanced Mg2+ Transport for Mg-Organic Batteries

Wen Ren,Migo Szeman Ng,Ye Zhang,Alae Eddine Lakraychi,Yanliang Liang,Dawei Feng,Michelle Lehmann,Guang Yang,Judith Jeevarajan,Wan Si Tang,Yan Yao

Magnesium batteries offer a safer alternative for next-generation battery technology due to their insusceptibility to dendrite deposition. Selective membranes tailored for magnesium-ion conduction will unlock further technological advancement. Herein, we demonstrate fluorine-free magnesiated sulfonated poly(ether ether ketone) (Mg-SPEEK) selective membranes capable of facilitating magnesium-ion conduction while effectively rejecting soluble organic species. These membranes demonstrate a reversible Mg plating and stripping Coulombic efficiency (CE) of 85.4% and an ionic conductivity of 3.3 × 10–4 S cm–1 at room temperature, surpassing those for a Mg-Nafion selective membrane. Theoretical density functional theory (DFT) calculations reveal that SPEEK possesses more localized charge centers along its backbone compared with Nafion, potentially facilitating enhanced ion conduction. Full cells assembled with Mg-SPEEK coupled with the organic cathode pyrene-4,5,9,10-tetraone (PTO) and Mg metal demonstrated significantly improved capacity retention as compared to those assembled with conventional nonselective separators.

CAS / MDL: 920-66-1
研究领域: 材料科学 · 电化学 · 理论计算
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JOURNAL OF POWER SOURCES · 2020 · IF 8.247

Electrolyte formulation to enable ultra-stable aqueous Zn-organic batteries

Kexian Huang,Zhenguo Yao,Ke Sun,Keyi Chen,Jiulin Hu,Dongguang Yin,Chilin Li

Aqueous zinc batteries (ZBs) possess great potential in energy storage due to their advantages in safety, low-cost and resource abundance. However, the commercialization of ZBs is plagued by the lacking of suitable cathode structures (or nano-textures) and their poor cycle life. The popular cathode materials of Mn or V based oxides suffer from the high solubility and toxicity of transition metals (TMs). It is highly required to develop robust TM-free organic cathodes with design flexibility and environmental benignity. Herein, 1,4,5,8-naphthalene diimide (NDI) layered molecules are proposed as cathode candidate for ZBs, and they are characterized by sufficient interconnection of nano-particles (for continuous electron transport) into porous network (for facilitated ion filtration). It enables the achievement of reversible redox of carbonyl function groups and a stable gravimetric capacity around 200 mAh g −1 . The superior cycling and rate performance (at least 5000 cycles under 3 A g −1 ) benefits from the electrolyte formulation. The blending of Na 2 SO 4 additive takes effect in terms of the cathode grain attenuation into ultrathin 2D nanosheets , pseudo-capacitance contribution enhancement and Zn anode smoothening.

研究领域: 材料科学 · 电化学
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Energy & Environmental Science · 2022 ·Vol. 16 ·期 1 ·89-96 · IF 39.714

A semi-conductive organic cathode material enabled by extended conjugation for rechargeable aqueous zinc batteries

Lu Lin,Zirui Lin,Jiaqi Zhu,Kuo Wang,Wanlong Wu,Tong Qiu,Xiaoqi Sun

Quinone cathode materials show great promise for aqueous zinc batteries. However, the poor electrical conductivity of organic compounds calls for the addition of high percentages of conductive agents during electrode preparation, usually ≥30%. Herein, we synthesize a semi-conductive piperazine-linked quinone of 2,3,7,8-tetraamino-5,10-dihydrophenazine-1,4,6,9-tetraone (TDT) for zinc batteries. Theoretical calculations suggest the extended conjugation among the π-electrons on the quinone rings and p-electrons on nitrogen sites in the structure. This allows electron delocalization throughout the entire molecule, and a small band gap of 1.5 eV is revealed by theoretical calculations and solid-state UV-vis spectroscopy. Besides, electron paramagnetic resonance demonstrates the formation of cationic radicals on the nitrogen of the middle piperazine ring. The radical is also stabilized by the extended conjugated system and further enhances the electrical conductivity. Thanks to the above factors, TDT exhibits a good electrical conductivity on the order of 0.1–1 mS cm−1. In aqueous zinc batteries, the TDT cathode with 10% carbon delivers a high capacity of 369 mA h g−1 at 0.2 A g−1 and retains 182 mA h g−1 at 10 A g−1. In situ UV-vis analysis further reveals the insolubility of TDT at all charged/discharged states, which ensures stable cycling for 3000 cycles.

CAS / MDL: 1074-82-4 118-75-2
研究领域: 材料科学 · 电化学
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Novel low-cost, high-energy-density (>700 Wh kg−1) Li-rich organic cathodes for Li-ion batteries

Qihang Yu,Wu Tang,Yang Hu,Jian Gao,Ming Wang,Sihong Liu,Huanhuan Lai,Liang Xu,Cong Fan

For the first time, two novel air-sensitive Li-rich organic cathodes ( m -TP4OLi and p -TP4OLi) are designed and reported. The structure-performance relationship for the two organic cathodes is comparatively studied. Using organic anode of lithium terephthalate (Li 2 TP), the resulting Li 2 TP II p -TP4OLi all-organic Li-ion batteries can deliver the peak discharge capacity of 330 mAh g −1 cathode in 1–3.4 V, corresponding to the high energy density of ~574 Wh kg −1 cathode using the median voltage of 1.74 V. Furthermore, the fabricated graphite II p -TP4OLi Li-ion batteries can show the peak discharge capacity of 305 mAh g −1 cathode in 1.5–3.4 V with a high median voltage of 2.4 V, resulting in the peak energy density of ~732 Wh kg −1 cathode (2.4 V × 305 mAh g −1 ). Meanwhile, the graphite II p -TP4OLi Li-ion batteries exhibit impressive device stability over 20,000 cycles. To the best of our knowledge, the peak energy density of our p -TP4OLi is currently the world record among Li-rich organic cathodes in lab conditions, outperforms the energy density of inorganic LiFePO 4 (~476 Wh kg −1 ), comparable with that of inorganic LiCoO 2 (~760 Wh kg -1 ) under the same lab conditions.

研究领域: 材料科学 · 能源技术
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Journal of Energy Storage · 2024 · IF 8.9

In-situ electropolymerization of bipolar organic cathodes for highly efficient Li-ion batteries

Meichen Guo,Wu Tang,Chenbin Tang,Xuesong He,Cong Fan

Organic cathodes face the challenge of dissolution problem, which severely hinders their electrochemical performances in lithium-ion batteries (LIBs). Herein, a bipolar organic cathode namely [ N , N ′-bis(4-(9H-carbazol-9-yl)phenyl)]-perylene-3,4,9,10-tetracarboxydiimide (PTCDI-DPC, 4-electron C T  = 123 mAh g −1 ) is optimized by in-situ electropolymerization to eliminate its dissolution problem, and thus the good cathode performance of the electropolymerized PTCDI-DPC can be fully released in LIBs. In half cells, PTCDI-DPC delivers a peak specific capacity of 164 mAh g −1 and the good retention of 96 % over 450 cycles. Meanwhile, PTCDI-DPC still remains 121 mAh g −1 after 2000 cycles at 1 A g −1 , and a superior rate performance of 98 mAh g −1 at 8 A g −1 . Furthermore, the fabricated 2PF 6 -PTCDI-DPC||LiC 6 Li-ion full cells can possess the peak discharge capacity of 157 mAh g −1 cathode and a high energy density of 385 Wh kg −1 cathode in 1.4–4.3 V, with 90 % capacity retention during 2000 cycles at 1 A g −1 . As far as we know, the cathode performance of the improved PTCDI-DPC is one of the best among bipolar organic cathodes reported for LIBs.

研究领域: 材料科学 · 电化学 · 能源存储
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Journal of Materiomics · 2025 · IF 9.6

PTCDA/CuS cathode enabling stable sulfide-based all-solid-state batteries

Zhixing Wan,Shuo Wang,Yahao Mu,Ruihua Zhou,Hang Liu,Tingwu Jin,Di Wu,Jianlong Xia,Ce-Wen Nan

Organic cathode materials have garnered significant attention for their potential application in lithium-ion batteries due to their lightweight nature, tunable structures, high energy density, and environmental friendliness. However, the dissolution of organic cathodes in liquid electrolytes often leads to poor cycling stability, which limits their practical application. In this study, a composite cathode was prepared by ball milling the PTCDA/CuS (perylene-3,4,9,10-tetracarboxylic dianhydride, PTCDA) with a sulfide-based electrolyte and carbon nanotubes. By optimizing the component ratios, the assembled all-solid-state batteries (ASSBs) show a high discharge capacity of 210 mA⸱h/g after 200 cycles without any capacity degradation at a current density of 33.0 mA/g. Through comprehensive characterization techniques including X-ray diffraction (XRD), Raman spectroscopy, Fourier-transform infrared spectroscopy (FTIR), and X-ray photoelectron spectroscopy (XPS), the coordination of Cu 2+ and the formation of sulfur-linked polymers during the charge-discharge processes are elucidated, and the reversibility of the electrochemical reactions has been confirmed. This work highlights the excellent compatibility between organic cathodes and sulfide-based electrolytes, providing a new way for the development of high-performance ASSBs with high energy density and extended lifespan.

研究领域: 材料科学 · 电化学 · 能源存储
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IONICS · 2016 ·Vol. 22 ·期 8 ·1377-1385 · IF 2.119

A novel nitroxide radical polymer-containing conductive polyaniline as molecular skeleton: its synthesis and electrochemical properties as organic cathode

Xu Lihuan,Ji Lvlv,Wang Guosheng,Zhang Cheng,Su Chang

A novel nitroxide radical-containing aniline, 4-(6-(2-amino-phenol-9 H -yl)hexanoyloxy)-2,2,6,6-tetramethylpiperidin-1-yloxy (AnT), was synthesized, and the copolymers of AnT and aniline (P (An-co-AnT)) were then prepared by chemical oxidative polymerization. The introduction of polyaniline (PAn) skeleton in copolymers improved the charge migration along polymer backbone, and the increased ratio of An/AnT monomer makes PAn’s anodic peak in copolymers shift to negative potential and the redox peaks for the nitroxide radical shift to the positive potential. Also, P (An-co-AnT) exhibited a gradually increased charged specific capacity from 120.1 to 141.0 mAh g −1 with increasing the feeding ratio of AnT/An, while the discharge specific capacity presented an opposite result. Specially, P (An-co-AnT) exhibited an obvious charge voltage platform and an even improved cycling stability than that of PAn in the high feeding ratio of AnT/An, and after 20 cycles, the discharge capacity of P (An-co-AnT) (1:1 ([An]/[AnT])) still maintained 82.7 % of the capacity obtained at the initial cycle.

CAS / MDL: 62-53-3 872-50-4 88-75-5
研究领域: 材料科学 · 电化学
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Journal of Materials Chemistry A · 2022 ·Vol. 10 ·期 26 ·14111-14120 · IF 14.511

Organic-conjugated polyanthraquinonylimide cathodes for rechargeable magnesium batteries

Yiyuan Ding,Dong Chen,Xin Ren,Yuliang Cao,Fei Xu

Rechargeable Mg batteries (RMBs) are advantageous for large-scale energy storage because of the abundant reserves of Mg and high safety, but inorganic cathodes suffer from the availability of few species, low capacities, and sluggish Mg2+-diffusion kinetics. Organic materials provide more selections for RMB cathodes with designable structures. However, the open framework of organic RMB cathodes tends to store MgCl+ ions, largely affecting the energy density by making a certain amount of chlorine-containing electrolyte indispensable. Herein, three polyanthraquinonylimides (PAQIs; N14, N26 and P26) were synthesized and investigated as organic RMB cathodes. The large conjugated structure favors high capacities (122 mA h g−1 for N26 and 164 mA h g−1 for P26) and good cycling stabilities (115 mA h g−1 for N26 and 111 mA h g−1 for P26 maintained after 500 cycles), as well as good rate capabilities. More significantly, a comprehensive mechanism study demonstrated that the PAQIs stored Mg2+ rather than MgCl+ through carbonyl enolization, and N26 and P26 delivered high specific power densities of 2780 and 2431 W kg−1, respectively, at 2000 mA g−1. The present study developed high-performance organic PAQI cathodes for RMBs and demonstrated the Mg2+-storage mechanism, and suggests that organic materials based on the enolization chemistry of multi-electron transfer could be potential candidates for high-power RMB cathode materials.

研究领域: 材料科学 · 电化学 · 能源存储
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JOURNAL OF POWER SOURCES · 2019 · IF 7.467

Synthesis of 1,4-benzoquinone dimer as a high-capacity (501 mA h g−1) and high-energy-density (>1000 Wh kg−1) organic cathode for organic Li-Ion full batteries

Zeyi Yao,Wu Tang,Xinxin Wang,Chuan Wang,Chuluo Yang,Cong Fan

The organic cathodes with high specific capacity are highly desirable to fabricate high-specific-energy-density organic Li-ion full cells. Herein, we initially propose the long-term plan for the systematic synthesis of the oligomer family of 1,4-benzoquinone (BQ), which can possess theoretical specific capacity above 500 mA h g −1 . As a start, the dimer of 1,4-benzoquinone (2,2′-bis-(1,4-benzoquinone), BBQ) is synthesized, which can realize the specific capacity of 501 mA h g −1 and the average discharge potential of ~2.5 V (vs. Li + /Li). Even facing the dissolution problem, BBQ can deliver average specific capacities of ~190 mA h g −1 during 3000 cycles at 500 mA g −1 and ~120 mA h g −1 during 8000 cycles at 2 A g −1 in Li-ion half cells. Afterwards, the all-organic Li-ion full cells are fabricated by using the reduced state (Li 4 TP) of lithium terephthalate (Li 2 TP) as the starting anode and BBQ as the starting cathode. Delightfully, the resulting Li 4 TP-BBQ Li-ion full cells can realize the specific capacity of 316 mA h g −1 cathode in the 1st cycle (500 mA g −1 ). Meanwhile, average specific capacities of ~98 mA h g −1 during 1000 cycles can be fulfilled (500 mA g −1 ). The results of the Li 4 TP-BBQ Li-ion full cells are among the best all-organic Li-ion full batteries reported to date.

研究领域: 材料科学 · 电化学 · 能源存储
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY · 2021 ·Vol. 168 ·期 5 ·050548 · IF 4.316

Poly(arylamine-imide)s Cathode Materials for Lithium-Ion Batteries with High Average Voltage and Long Cycle Life

Chengjun Zhang,Sha Chen,Guangying Zhou,Qiong Hou,Suilian Luo,Yuhai Wang,Guang Shi

Two poly(arylamine-imide)s, poly(N,N,N',N'-tetraphenyl-1,4-benzenediamine naphthalenediimide) (PDDP-NI) and poly(N,N,N',N'-tetraphenyl-1,4-benzenediamine perylenediimide) (PDDP-PI), were successfully prepared by condensation polymerization of an amine monomer N,N,N',N'-tetraphenyl-1,4-benzenediamine (DDP) with dianhydride monomer 1,4,5,8-naphthalenetetracarboxylic dianhydride (NTCDA) or 3,4,9,10-perylenetetracarboxylic dianhydride (PTCDA). The DDP units in the polymer can reversibly dope/dedope the PF6− anion, while the naphthalenediimide (NI) unit or perylene diimide (PI) unit can reversibly insert/extract the lithium cation. The lithium ion half-cells based on the polymer cathode and the lithium anode are assembled and the electrochemical properties are tested. Due to the high voltage of the DDP unit in the polymer backbone, lithium-ion half-cells based on PDDP-NI and PDDP-PI cathodes provide a high average discharge voltage of about 3.2 V. Moreover, the as-prepared polymer materials exhibit long-cycle performance, PDDP-NI remains 89% capacity after 500 cycles at 10 C and PDDP-PI maintains 98% capacity after 1000 cycles at 10 C, furthermore, their coulombic efficiency close to 100% at all current rates tested, which shows that these organic cathode materials have potential applications in long-cycle lithium-ion batteries.

研究领域: 材料科学 · 电化学 · 能源存储
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ChemSusChem · 2023 ·Vol. 16 ·期 15 ·e202300343 · IF 8.4

Small-Molecule Organic Cathodes with Carbon Coating for Highly Efficient Potassium-ion Batteries

Meichen Guo,Wu Tang,Chenbin Tang,Xuesong He,Jiahui Hu,Cong Fan

Graphical Through a surface self-carbonization strategy, a carbon layer with controllable thickness can be built on the surface of [ N , N’ -bis(2-anthraquinone)]-1,4,5,8-naphthalenetetracarboxdiimide (NTCDI-DAQ) particles and significantly increase their insolubility in liquid electrolytes without affecting the electrochemical behavior of the bulk particles. The resulting NTCDI-DAQ@C samples indeed show the expectantly enhanced cathode performance when compared to the pristine NTCDI-DAQ in K-ion batteries. Small-molecule organic cathodes face dissolution in potassium-ion batteries (PIBs). For the first time, an interesting and effective strategy is unveiled to resolve this issue by designing a new soluble small-molecule organic compound namely [ N , N ’-bis(2-anthraquinone)]-1,4,5,8-naphthalenetetracarboxdiimide (NTCDI-DAQ, 237 mAh g −1 ): Through the precise manipulation of carbonization temperature and time, the molecules on the surface of NTCDI-DAQ particles can be transformed into amorphous carbon with controllable thickness. This strategy called surface self-carbonization can form a carbon protective layer on organic cathodes and significantly increase their insolubility against liquid electrolytes without affecting the electrochemical behavior of bulk particles. As a result, the as-obtained NTCDI-DAQ@C sample displays significantly improved cathode performance in PIBs. In half cells, NTCDI-DAQ@C shows superior capacity stability of 84 % compared to 35 % of NTCDI-DAQ during 30 cycles under the same conditions. In full cells with a KC 8 anode, NTCDI-DAQ@C delivers a peak discharge capacity of 236 mAh g −1 cathode and a high energy density of 255 Wh kg −1 cathode in 0.1–2.8 V, with 40 % capacity retention during 3000 cycles at 1 A g −1 . To the best of our knowledge, the integrated performance of NTCDI-DAQ@C is among the best of soluble organic cathodes reported in PIBs.

研究领域: 材料科学 · 能源存储技术
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