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ACS Applied Materials & Interfaces · 2025 · IF 8.2

Tri-chamber Polysulfide/Iodide-Based Redox Flow Batteries with Improved Coulombic Efficiency

Chao Deng,Xiaoxin Li,Mustafa Kemal Bayazit,Barun Kumar Chakrabarti,Guo-Ming Weng

The polysulfide/iodide flow battery is a promising candidate for large-scale energy storage systems, but the technology suffers from a notably low Coulombic efficiency. This phenomenon arises because the crossover of hydroxide ions triggers the disproportionation reaction of I3– ions in the posolyte. To mitigate these issues, a middle chamber filled with Na2SO4 solution is created between two cation-exchange membranes to separate the posolyte and negolyte chambers of the PSIFB, thereby constructing a trichamber reactor. This middle chamber can serve as a reservoir for the cross-transportation OH– ions during charge-discharge processes, thereby minimizing their adverse effects on the posolyte. Experimental results reveal that the introduction of the middle chamber leads to a 97.3% reduction in the concentration of OH– ions within the posolyte. Furthermore, finite element analysis demonstrates that the trichamber configuration significantly reduces the flux of OH– ions entering the posolyte, achieving levels even lower than half of those in the dual-chamber structure. This innovative architecture markedly enhances the Coulombic efficiency from approximately 78% in the dual-chamber structure to around 91% in the trichamber structure with a high-concentration electrolyte (4 M NaI and 3 M Na2S2), while concurrently sustaining a highly competitive energy density of 20.05 W h Lposolyte+negolyte–1 at 75% state-of-charge. These findings demonstrate an effective strategy for improving the performance of the polysulfide/iodide flow battery through OH– management, showing potential for developing more efficient flow battery systems for renewable energy storage applications

研究领域: 电化学能源存储 · 液流电池技术 · 电化学工程 · 可再生能源存储 · 材料科学
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Journal of Energy Chemistry · 2024 · IF 14

Enhancing Li-S battery performance via functional polymer binders for polysulfide inhibition

Jinpeng Jian,Qian Chen,Hao Sun,Rui Li,Yaolin Hou,Yulong Liu,Jia Liu,Haiming Xie,Jiefang Zhu

The commercialization of lithium-sulfur (Li-S) batteries faces several challenges, including poor conductivity, unexpected volume expansion, and continuous sulfur loss from the cathode due to redox shuttling. In this study, we introduce a novel polymer via a simple cross-linking between poly(ether-thioureas) (PETU) and poly(3,4-ethylenedioxythiophene)- poly(styrenesulfonate) (PEDOT:PSS) as a bifunctional binder for Li-S batteries (devotes as “PPTU”). Compared to polyvinylidene fluoride (PVDF), as-prepared PPTU exhibits significantly higher electrical conductivity, facilitating electrochemical reactions. Additionally, PPTU demonstrates effective adsorption of lithium polysulfides, leading to improved cycling stability by suppressing the shuttling effect. We investigate this behavior by monitoring morphological changes at the cell interface using synchrotron X-ray tomography. Cells with PPTU binders exhibit remarkable rate performance, desired reversibility, and excellent cycling stability even under stringent bending and twisting conditions. Our work represents promising progress in functional polymer binder development for Li-S batteries.

研究领域: 材料科学 · 能源存储技术
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APPLIED SURFACE SCIENCE · 2020 · IF 6.182

Electrocatalytic polysulfide transformation for suppressing the shuttle effect of Li-S batteries

Tiancheng Na,Yang Liu,Xiangcun Li,Wenji Zheng,Yan Dai,Zhijun Yan,Wei Kou,Gaohong He

We report a method based on 2,4-dihydroxybenzoic acid-formaldehyde (RF-COOH) microsphere hard templates to prepare core-shelled Fe 2 O 3 microspheres , which were then added to graphene oxide to obtain hierarchical reduced graphene oxide, ultimately dropping Fe 2 O 3 (Fe 2 O 3 @rGO) by Vitamin C reduction and freeze drying. When used as cathode materials for lithium-sulfur batteries, Fe 2 O 3 @rGO shows a high specific capacity of 400.5 mAh g −1 at 2 C after 500 cycles. The prominent performance is due to the collaborative assembly of rGO , which provides stable   structural support and favourable conductivity, and core-shelled Fe 2 O 3 microspheres, which are certified to have a strong interaction with polysulfides. The   loose and stable skeletons of highly electroconductive rGO can offer a conductive framework for rapid ion/electron transport. Meanwhile, the unique core-shelled structure of Fe 2 O 3 with the ample void space can anchor polysulfides through the strong chemical adsorption and buffer the mechanical stresses caused by volume expansion during the charge and discharge processes. Moreover, Fe 2 O 3 promotes the transformation of polysulfides to insoluble LiPSs during the discharging process, effectively   alleviating the shuttling of the polysulfides.

研究领域: 材料科学 · 能源存储 · 电化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

rGO@TiO2-x Schottky heterojunction for enhanced bidirectional catalysis in polysulfide conversion

Rongjie Zhe,Haoyun Dou,Xuanpan Xu,Ziwei Zhao,Long Chen,Qingye Zhao,Xinjun Bao,Guozhong Cao,Hong-En Wang

The shuttling and sluggish conversion kinetics of lithium polysulfides (LiPSs) lead to poor cycling performance and low energy efficiency in lithium-sulfur batteries (LSBs). In this work, a hierarchically structured nanocomposite, synthesized through a surfactant-directed hydrothermal growth following dopamine-protected pyrolysis, serves as a bidirectional catalyst for LSBs. This nanocomposite comprises N -doped reduced graphene oxide (rGO) nanosheets anchored with uniformly distributed TiO 2- x nanoparticles via interfacial N -Ti and C-Ti bonding, resulting in the formation of abundant 2D/0D Schottky heterojunctions (rGO/TiO 2- x ). Density functional theory (DFT) calculations and in situ Raman characterizations demonstrate that rGO/TiO 2- x effectively inhibits the shuttling of LiPSs with enhanced redox kinetics, achieving high utilization of the sulfur cathode and improving the overall reversibility. A high areal capacity is attained at a high sulfur loading and a low electrolyte/sulfur ratio. The initial specific capacity reaches 1010 mA h g −1 at a current density of 0.2C (1C = 1675 mA g −1 ), and a retention of 86.4 % is attained over 100 cycles. A light-emitting diode (LED) screen using two LSBs with rGO/TiO 2- x demonstrates their high potential for practical applications.

研究领域: 材料科学 · 电化学
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International Journal of Electrochemical Science · 2023 · IF 1.5

Effective Polysulfide Adsorption by Double Side Coated Separator in Lithium-Sulfur Batteries

Yulin Liu,Jing Li,Min Zeng,Xun Xu,Jianna Deng,Jianqiang Guo,Dan Zhao,Jianzhao Yang,Hongru Wang

Lithium-sulfur batteries have attracted much attention because of their high specific capacity and energy density. However, the commercialization of lithium-sulfur batteries is limited by low utilization of active materials and excessive capacity decay which caused by the shuttle effect of polysulfide in the practical applications. In this article, effective polysulfide adsorption method was applied via using modified PP separator coated super P and Al 2 O 3 on the two sides, respectively. As a result, this strategy solves the problems of polysulfide shuttle effect and poor sulfur conduction at the same time. The initial discharge specific capacity of lithium-sulfur batteries, which assembled with the super P + PP + Al 2 O 3 separator, could reach 1247 mAh g -1 at the current density of 0.1 C. After 60 discharge / charge cycles, the discharge capacity was still 987 mAh g -1 , with a capacity retention of 79%. This method of simultaneous modification on both sides of the separator provides a new idea for the modification of lithium-sulfur batteries.

研究领域: 储能技术 · 材料科学 · 电化学
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JOURNAL OF POLYMER SCIENCE PART A-POLYMER CHEMISTRY · 2019 ·Vol. 57 ·期 13 ·1460-1466 · IF 2.591

Aromatic amine-terminated polysulfide oligomer: Synthesis and application in self-healable polyurea

Wentong Gao,Jianwei Xu,Pengfei Zuo,Hao Dong,Yiwu Quan,Pengshan Chang

The dynamic chemistry of disulfide bonds has emerged as one of the most powerful tools used for the fabrication of organic compounds and self-healing materials. In this article, a novel aromatic amine-terminated polysulfide oligomer is first synthesized from thiol-terminated polysulfide oligomer and bis(4-aminophenyl) disulfide via disulfide metathesis mechanism. The resulting oligomer is confirmed by FTIR and 1 H NMR spectra and then successfully applied in constructing self-healable polyurea material (A-LP23-I), which combines the advantages of higher strength of polyureas and excellent self-healing ability of polysulfide-based materials. After subjecting to a temperature of 75 °C for 48 h, both the tensile strength and ultimate elongation of A-LP23-I restore to more than 90% of the original values (3.32 MPa and 396%). This study demonstrates a novel strategy for synthesizing aromatic amine-terminated oligomer. © 2019 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2019, 57, 1460–1466

CAS / MDL: 68-12-2 109-99-9
研究领域: 材料科学 · 有机化学
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RSC Advances · 2016 ·Vol. 6 ·期 62 ·57346-57356 · IF 3.289

Effects of LAGP electrolyte on suppressing polysulfide shuttling in Li–S cells

Xue-ling Wu,Jun Zong,Han Xu,Wei Wang,Xing-jiang Liu

In this work, the solid electrolyte of Li1.5Al0.5Ge1.5(PO4)3 (LAGP) is used to suppress polysulfides shuttling in Li–S cells. Firstly, the H-type visible cell is assembled by using a LAGP glass ceramic plate and normal poly-propylene (PP) separator. It is demonstrated that the LAGP glass ceramic plate is quite effective in shutting-down the migration of polysulfide ions and improving the utilization ratio of the sulfur cathode. However, in the commercial production of Li–S batteries it is not possible to use the LAGP glass ceramic plate as a membrane due to its brittle characteristics. Herein, the LAGP modified separator has been prepared by a simple casting procedure and applied in Li–S cells. The Li-ion conductivity of the LAGP modified separator is 6.280 × 10−4 S cm−1 at room temperature. The Li-ion transference number and the Gurley value of the modified separator show that the diffusion of the polysulfide anions can be suppressed effectively. The discharge capacity of the Li–S cell with the modified separator at the 50th cycle can reach 770.1 mA h g−1, while that of the Li–S cell with the routine PP separator is only 658.4 mA h g−1 at the 50th cycle. The superior utilization of sulfur in the Li–S cells indicates that using the LAGP modified separator is a viable way to overcome the shuttling problem for practical Li–S batteries.

研究领域: 材料科学 · 电化学
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Nanoscale Advances · 2022 ·Vol. 5 ·期 2 ·435-442 · IF 5.598

High-capacity polysulfide–polyiodide nonaqueous redox flow batteries with a ceramic membrane

Mao Chen,Hongning Chen

Nonaqueous redox flow batteries (NRFBs) have been regarded as promising large-scale electrochemical energy storage technology due to the wider solvent stable potential windows and greater selection of materials. However, the application of NRFBs is greatly limited considering the low capacity and high cost of active materials. In this work, we design and demonstrate a high-capacity polysulfide (PS)–polyiodide (PI) NRFB in Li-ion based 1,3-dioxolane (DOL) and 1,2-dimethoxyethane (DME) (v/v ∼ 1 : 1) organic electrolyte. The high solubility and low cost of PS (5 M) and PI (4 M) can achieve the high capacity and high applicability of NRFBs, which is attractive for realizing large-scale stationary energy storage. The highest volumetric capacity of 28 Ah L−1 based on a full cell is achieved with 1.5 M PS-4 M PI. The high coulombic efficiency (∼100%) and capacity retention (>99%) for 100 cycles in the PS–PI system is demonstrated by using a Li-ion conducting ceramic membrane. Voltage control is applied for both PS and PI to avoid the formation of irreversible solid Li2S and I2, which ensures the high stability of battery reaction. In situ UV-vis spectroscopy reveals the high reversibility of PS and PI in DOL/DME. A continuous flow mode test of the PS–PI system is also demonstrated to realize >300 hours stable cycling performance which implies good applicability for a long-term process. The successful demonstration of this high-capacity PS–PI nonaqueous system provides a new direction to promote the application of NRFBs in more fields.

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Small Methods · 2021 ·Vol. 5 ·期 10 ·2100839 · IF 14.188

Suppressing Polysulfide Shuttling in Lithium–Sulfur Batteries via a Multifunctional Conductive Binder

Shiming Chen,Zhibo Song,Yuchen Ji,Kai Yang,Jianjun Fang,Lu Wang,Zijian Wang,Yan Zhao,Yunlong Zhao,Luyi Yang,Feng Pan

Exhibiting high specific energy and low cost, lithium–sulfur batteries are considered promising candidates for the next-generation battery. However, its wide applications are limited by the insulating nature of the sulfur, dissolution of polysulfide species, and large volume change of the sulfur cathode. In this work, a conductive binder, crosslinked polyfluorene (C-PF) is synthesized and employed in Li–S batteries to enhance the overall electrochemical performance from the following three aspects: 1) possessing high electronic conductivity, C-PF facilitates lowered areal resistance for the sulfur electrode and leads to an improved rate capability; 2) owing to the cross-linked polymer structure, favorable mechanical properties of the electrode can be achieved, hence the well-preserved electrode integrity; 3) forming strong binding with various polysulfide species, C-PF manages to trap them from diffusing to the Li anode, which greatly improves the cycling stability of Li–S cells. Through designing a multifunctional binder to comprehensively enhance the Li–S cathode, this proposed approach could be broadly applied to fully harness the energy from S redox in addition to cathode material modifications.

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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Imidazole-modified separator for uniform polysulfide anchoring and accelerated redox in LiS batteries

Xiangwei Zhao,Qin Dong,Wei Hong,Rong Li,Xinglong Gou,Ruiyi Gan,Tao Wang,Cunpu Li

Despite their ultrahigh theoretical energy density, the practical application of lithium‑sulfur (Li S) batteries is hindered by severe lithium polysulfides (LiPSs) shuttling and sluggish redox kinetics. To address these challenges, an imidazole polymer layer is grafted onto the polypropylene (PP) separator, enabling equivalent interactions with various LiPSs. Density functional theory (DFT) calculations reveal that this uniform anchoring originates from electrostatic interactions, which promote the redox conversion of LiPSs. Meanwhile, the imidazole-modified separator improves electrolyte affinity, facilitating efficient lithium-ion transport. The low self-discharge, excellent cycling stability, and preserved electrode morphology confirm the successful suppression of LiPSs shuttling. Moreover, pouch cells assembled with the imidazole-modified separator exhibit a capacity of 0.45 Ah, demonstrating the practical feasibility of this separator design. This “equivalent anchoring and accelerated conversion” mechanism offers a new pathway toward high-performance Li S batteries with mitigated shuttle effect.

研究领域: 储能 · 材料科学 · 电化学 · 电池技术
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JOURNAL OF POWER SOURCES · 2025 · IF 7.9

Boosting the electrochemical properties of polysulfide by iron(Ⅱ) phthalocyanine and its mechanism

Tianyi Zhou,Hao Yuan,Bo Hu,Xiaolong Wang,Lin Hu,Wei Xie,Linlin Wu,Suqin Liu

The sulfur/iron (S/Fe) redox flow battery (RFB) offers attractive attributes such as high safety, environmental compatibility, and low cost, making it a promising candidate for large-scale energy storage. However, its development is hindered by the sluggish kinetics of polysulfide reduction during charging. Herein, we report iron phthalocyanine (FePc) supported on graphite felt as a highly effective electrocatalyst for the S 4 2− /S 2 2− redox couple. The FePc-based S/Fe RFB achieves an energy efficiency of 67.9 % at 120 mA/cm 2 and exceptional stability over 1000 cycles. Electrochemical analysis shows enhanced kinetics, with a higher exchange current density and a lower Tafel slope (76.5 mV dec −1 ) compared to the blank electrode (388.6 mV dec −1 ). The full cell delivers a peak power density of 206.4 mW/cm 2 and maintains over 75 % energy efficiency at 80 mA/cm 2 . Combined experimental and theoretical results reveal that FePc preferentially stabilizes polysulfide via middle-sulfur adsorption, facilitates S–S bond elongation, and promotes electron transfer. The insights gained into the catalytic role of FePc in polysulfide conversion provide a foundation for designing high-performance, durable, and cost-effective RFBs.

CAS / MDL: 6674-22-2
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APPLIED SURFACE SCIENCE · 2024 · IF 6.3

Boron doped MXenes as redox catalyst for highly efficient and reversible polysulfide conversion

Dongqing Xu,Luting Shi,Xianqiang Li,Yapeng Tian,Zhuosen Wang,Xinwei Cui

Due to the accumulation of soluble polysulfides during the process reaction process, the shuttle effect emerges and significantly impacts the electrochemical performance. The development of novel efficient catalysts and adsorbents is a very popular way to fabricate the sulfur host materials. MXene as one of the most novel and popular materials have been wildly used in electrochemical energy storage. While the limited catalytic activity and adsorption capacity hindering its application in lithium sulfur batteries. Here, we introduced boron atoms as dopants in a creative modification of MXene (B-MXene). The introduced B atoms can effectively mitigate the “shuttle effect” through chemical adsorption, owing to their electron-deficient nature. Furthermore, the introduction of boron atoms and vacancy can modify the electronic structure, enhancing the catalytic activity of MXene by providing empty perpendicular-orientation orbitals. As a result, B-MXene exhibited excellent electrochemical performance, maintaining at 943 mA h g −1 at a current density of 1.0C, after 500cycles, with a corresponding decay rate as low as 0.046 %. This work proposes an efficient strategy to fabricate highly efficient electrocatalysts for advanced lithium-sulfur batteries (Li-S batteries).

研究领域: 材料科学 · 电化学 · 能源存储 · 纳米材料 · 催化化学
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