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APPLIED SURFACE SCIENCE · 2018 · IF 4.439

Flower-like molybdenum disulfide/carbon nanotubes composites for high sulfur utilization and high-performance lithium–sulfur battery cathodes

Maru Dessie Walle,Ke Zeng,Mengyuan Zhang,Yajuan Li,You-Nian Liu

Lithium–sulfur (Li–S) batteries have attracted an increasing attention for advanced energy storage devices, because of their high energy density, low cost and lower environmental impacts. However, their commercial applications are still hampered with the low conductivity and sulfur utilization, the low sulfur loading and the serious capacity fading at a high current rate. Herein, we prepared flower-like molybdenum disulfide and carbon nanotubes (MoS 2 /CNTs) composites with mesoporous structures for high sulfur utilization cathodes. The flower-like MoS 2 can immobilize sulfur and obstruct the solubility of polysulfide within the structures. The MoS 2 /CNTs-S cathode with 2.6 mg cm −2 sulfur loading and capacity per area of 3.83 mA h cm −2 delivers an initial specific discharge capacity of 1473 mA h g −1 with 88.0% sulfur utilization and maintains a reversible capacity of 855.5 mA h g −1 with coulombic efficiency up to 96.6% after 50 cycles at the current rate of 0.2 C (335.0 mA g −1 ). Impressively, the MoS 2 /CNTs-S cathode at 5 C shows the high specific capacity of 1254 mA h g −1 with 76.0% sulfur utilization and maintains 384.0 mA h g −1 with an average coulombic efficiency of 91% after 200 cycles. The MoS 2 /CNTs-S cathode could be a good candidate for high-performance Li–S battery.

CAS / MDL: 308068-56-6
研究领域: 材料科学 · 能源存储技术
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ACS Applied Materials & Interfaces · 2020 · IF 8.758

Toward Commercially Viable Li-S Batteries: Overall Performance Improvements Enabled by a Multipurpose Interlayer of Hyperbranched Polymer-Grafted Carbon Nanotubes

Shizhen Li,Honglei Zhang,Wanru Chen,Yulong Zou,Hangqi Yang,Jingbo Yang,Chuang Peng

Shuttle effect and the low utilization of dissolved lithium polysulfides (LiPSs) are two prevailing concerns in Li-S battery (LSB) research. Energy efficiency on the other hand is often overlooked but vital to the commercial deployment of battery technology. In this work, a composite of hyperbranched poly(amidoamine)-modified multiwalled carbon nanotubes (PAMAM-CNTs) is successfully prepared by chemical grafting and employed as an interlayer material in LSBs. The high content and highly dispersed polar functional groups of PAMAM can efficiently adsorb and enhance the redox reaction of LiPSs. The CNTs function as a scaffold and current collector that reduces the internal polarization. The assembled LSB displays a high energy efficiency of 86% and a low capacity fading rate of 0.037% per cycle over 1200 cycles at 2 C. The cell also shows excellent cycle performance, high sulfur utilization, and improved stability at a high areal capacity of 9 mAh cm–2 (achieved at a sulfur loading of 8.7 mg cm–2) and low electrolyte/sulfur ratio of 6.1 mL g–1. This thin (12 μm) and lightweight (0.34 mg cm–2) interlayer has a negligible impact on the overall cell energy density.

研究领域: 材料科学 · 电化学
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Joule · 2024 · IF 38.6

An energetic K+-S aqueous battery with 96% sulfur redox utilization

Boya Wang,Wanhai Zhou,Yanyan Zhang,Tengsheng Zhang,Xinran Li,Yutong Feng,Ruizheng Zhao,Wei Li,Ahmed Elzatahry,Yasser Hassan,Dongyuan Zhao,Dongliang Chao

Potassium-sulfur electrochemistry represents a compelling energy storage technology due to its cost-efficient chemicals and unparalleled capacity. However, achieving high sulfur redox utilization (SRU) remains a great challenge during K + storage due to K 2 S n kinetics inertia. Here, for the first time, we unveil an aqueous K + -S electrochemistry, leveraging boosted K 2 S n conversion kinetics in water. A stable two-electron charge transfer process is achieved via tuning K 2 S solubility. Spectroscopic evaluation and molecular dynamics simulations reveal a unique solid-liquid-solid conversion pathway (S ↔ K 2 S 4 ↔ K 2 S), which effectively avoids soluble K 2 S shuttling. Consequently, an unprecedented K + storage capacity of 1,619 mAh g −1 ( ca. 96% SRU) can be achieved with 95% initial Coulombic efficiency, appealing cyclability over 500 times, and a high-energy density of 392 Wh kg S+Zn −1 . These findings signify a paradigm shift and introduce transformative opportunities for the design of safe and high-energy aqueous batteries.

CAS / MDL: 127-08-2 7704-34-9
研究领域: 材料科学 · 电化学
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JOURNAL OF POWER SOURCES · 2020 · IF 8.247

Promoting the conversion of Li2S by functional additives phenyl diselenide in Lithium–Sulfur batteries

Xueya Zhang,Jie Li,Chunhui Gao,Chenyang Shi,Liang He,Qian Xiang,Bo Hong,Yanqing Lai,Zhian Zhang,Kai Zhang

Lithium–Sulfur (Li–S) battery is a promising device in the field of electrochemical energy storage since its high specific capacity and low cost. However, the low insoluble Li 2 S conversion efficiency and uncontrollable deposition on the electrodes lead to low sulfur utilization, poor reversibility and rapid capacity decay. Consequently, the practical application of Li–S battery is limited. Herein, phenyl diselenide (PDSe) is added into the conventional electrolyte try to improve the batteries performance. The results show that the Se–Se bond in PDSe is broken and the Li–S bond in Li 2 S is elongated induced by PDSe. Moreover, PDSe promotes Li 2 S conversion and reduces Li 2 S deposition on the electrodes. As a result, the batteries using the electrolyte with PDSe exhibit enhanced discharge capacity and improved rate performance. Particularly, the batteries with 5.0 wt% PDSe additive exhibit a high initial discharge capacity of 1585.6 mAh g −1 , even after 300 cycles at 0.5 C, the batteries still maintain 916.5 mAh g −1 , which is much higher than conventional batteries of 618.7 mA h g −1 .

研究领域: 材料科学 · 电化学
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Energy & Environmental Science · 2025 · IF 30.8

Integrating solid interfaces for catalysis in all-solid-state lithium–sulfur batteries

Yun Cao,Chuannan Geng,Chen Bai,Linkai Peng,Jiaqi Lan,Jiarong Liu,Junwei Han,Bilu Liu,Yanbing He,Feiyu Kang,Quan-Hong Yang,Wei Lv

All-solid-state lithium–sulfur batteries (ASSLSBs) hold great promise for achieving high energy densities. However, their practical applications are hindered by low sulfur utilization and limited cycle life attributed to the sluggish sulfur reaction kinetics. Although catalysis is an effective way to address kinetic limitations, it often becomes ineffective because solid contact between the catalyst and the sulfur species cannot form the molecular-level interfaces necessary for catalytic reactions. Here, we propose a micropore confining and fusing strategy to integrate the catalysis reaction interfaces on a molecule-level. The prepared microporous carbon sheet confines the small molecule sulfur and catalyst clusters in its sub-2 nm micropores, enabling the formation of integrated sulfur-catalyst-carbon interfaces, which fundamentally achieves a molecular-scale contact for solid catalysis and eliminate the interfacial mismatches in the solid cathodes. Such interfaces significantly enhance the sulfur reaction kinetics and utilization even at high rates. Moreover, the large micropore volume (2.0 cm3 g−1) accommodates the substantial volume changes of sulfur, stabilizing interparticle interfaces both within the cathode and at the cathode/electrolyte interface and finally enabling exceptional cycling stability. The assembled battery shows a remarkable specific capacity of over 1000 mA h g−1 at 1.0C and retains over 85% capacity after 1400 cycles, both among the highest ever reported. The interface engineering proposed in this study offers a practical route for ASSLSB applications.

CAS / MDL: 7791-13-1
研究领域: 材料科学 · 电化学 · 能源存储技术
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JOURNAL OF ALLOYS AND COMPOUNDS · 2024 · IF 5.8

Dual-functional SnO2-CNT-PANI||PP=|SnO2 separator for enhanced lithium-sulfur battery stability and capacity

Haihong Yin,Zhirun Qian,Yunfeng Wu,Zhipeng Chen,Fuzhi Wang,Tingting Chen,Bocheng Su,Kangwei Wen,Haijian Chen,Zhenguo Wang,Lin Qin

Lithium-sulfur batteries (LSBs) provide high capacity and energy density for advanced energy storage but encounter performance and safety issues due to lithium polysulfides (LiPSs) dissolution and dendrite formation. This study introduces a dual-functional SnO 2 -CNT-PANI||PP=|SnO 2 separator (DF-SNCPS) aimed at improving the stability and safety of LSBs. The separator includes a SnO 2 -CNT-PANI layer on the sulfur cathode side for enhanced electrical conductivity and polysulfide adsorption and a SnO 2 nanoparticle (nano-SnO 2 ) layer on the lithium anode side to regulate lithium-ion concentration and inhibit dendrite growth. Density functional theory (DFT) and the phase field method have verified the relevant material's catalytic performance and dendrite suppression ability. These methods have provided a comprehensive understanding of the underlying mechanisms, providing auxiliary explanations for their role in catalyzing polysulfide conversion and suppressing lithium dendrite growth. This innovative design mitigates the shuttle effect and enhances cyclic stability and sulfur utilization, achieving a notable cyclic performance with a capacity retention of 0.05 % per cycle over 800 cycles at 1 C. The synergistic effects of the modified separator present a viable pathway for LSB commercialization.

研究领域: 材料科学 · 能源存储 · 电池技术 · 纳米技术 · 电化学
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ACS Applied Materials & Interfaces · 2023 · IF 9.5

CO2-Activation Nanofiber Carbon Paper as a High-Performance Interlayer for Trapping Polysulfides in Li–S Batteries

Ling Meng,Chenying Song,Qixuan Lin,Guanghang Sun,Jin Long,Xiting Zhang,Hailong Li,Jian Hu,Siyu Ye

Lithium–sulfur (Li–S) batteries have high theoretical energy density but low sulfur utilization due to the inherent insulating nature of sulfur and the shuttle effect of polysulfides. Herein, the CO2-activation carbon paper was prepared by poly(p-phenylenebenzobisoxazole) (PBO) nanofiber and was first applied as an interlayer for efficiently alleviating the shuttle effect of polysulfides in Li–S batteries. This interlayer exhibits good flexibility and strength with rich −C═O and −COOH functional groups on the three-dimensional porous structure, which improves chemical adsorption on Li2Sx species and ion rapid diffusion via interconnected diffusion channels and thus enhances the electrochemical kinetics. The initial specific capacity is 1367.4 mAh g–1 and remains 999.8 mAh g–1 after 200 cycles at 0.2C and 780.1 mAh g–1 at 5C, and the Coulombic efficiency is high, up to 99.8%, which is much better than that for the carbon paper without CO2 activation. The highly conductive flexible PBO carbon paper may bring breakthroughs in performance and thus lead to more practical applications of Li–S batteries.

CAS / MDL: 68-12-2 7704-34-9
研究领域: 材料科学 · 电化学 · 能源存储
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Rationally designing composite gel polymer electrolyte enables high sulfur utilization and stable lithium anode

Pengfei Xie,Ruyi Yang,Yingke Zhou,Bingyin Zhang,Xiaohui Tian

The lithium-sulfur battery is an attractive energy-storage device with low cost and high energy density. However, its development is still restricted by “shuttle effect”, lithium dendrite growth and safety problem. Herein, a novel PEO-PAN-LLZO composite gel polymer electrolyte (CGPE) was designed to overcome these issues. A porous composite membrane with excellent mechanical and interfacial properties was formed after casting dispersion of PAN, PEO, LLZO sheets, which can effectively absorb electrolyte, inhibit “shuttle effect” and protect lithium anode. A conductive acetylene black layer was coated on the membrane to further hinder the migration and enhance the redox kinetics of polysulfides. The CGPE based lithium-sulfur battery displays remarkably high specific capacities (1459 and 942 mAh/g at 0.1 and 1C respectively) and outstanding cycling performance (555 mAh/g at 1C after 500 cycles, average decay/cycle of 0.082%). The unique CGPE is promising for the practical application of high-performance lithium-sulfur battery.

研究领域: 电化学储能 · 材料科学 · 纳米复合材料 · 能源化学 · 固态离子学 · 电池技术
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ADVANCED FUNCTIONAL MATERIALS · 2021 ·Vol. 31 ·期 28 ·2102314 · IF 18.808

Interfacial Engineering of Bifunctional Niobium (V)-Based Heterostructure Nanosheet Toward High Efficiency Lean-Electrolyte Lithium–Sulfur Full Batteries

Haodong Shi,Jieqiong Qin,Pengfei Lu,Cong Dong,Jian He,Xiujian Chou,Pratteek Das,Jiemin Wang,Liangzhu Zhang,Zhong-Shuai Wu

High-efficiency lithium–sulfur (Li–S) batteries depend on an advanced electrode structure that can attain high sulfur utilization at lean-electrolyte conditions and minimum amount of lithium. Herein, a twinborn holey Nb 4 N 5 –Nb 2 O 5 heterostructure is designed as a dual-functional host for both redox–kinetics–accelerated sulfur cathode and dendrite-inhibited lithium anode simultaneously for long-cycling and lean-electrolyte Li–S full batteries. Benefiting from the accelerative polysulfides anchoring–diffusion–converting efficiency of Nb 4 N 5 –Nb 2 O 5 , polysulfide-shutting is significantly alleviated. Meanwhile, the lithiophilic nature of holey Nb 4 N 5 –Nb 2 O 5 is applied as an ion-redistributor for homogeneous Li-ion deposition. Taking advantage of these merits, the Li–S full batteries present excellent electrochemical properties, including a minimum capacity decay rate of 0.025% per cycle, and a high areal capacity of 5.0 mAh cm −2 at sulfur loading of 6.9 mg cm −2 , corresponding to negative to positive capacity ratio of 2.4:1 and electrolyte to sulfur ratio of 5.1 µL mg −1 . Therefore, this work paves a new avenue for boosting high-performances Li–S batteries toward practical applications.

研究领域: 材料科学 · 电化学 · 能源存储
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Nanoscale · 2018 ·Vol. 10 ·期 38 ·18407-18414 · IF 7.233

Ternary confined-functional sulfur composite with a host–sulfur–container architecture for lithium/sulfur batteries

Yong Wang,Xin Liang,Jufeng Yun,Pengcheng Shi,Peng Lu,Yi Sun,Hongfa Xiang

In this work, a ternary confined-functional sulfur composite with a Host–Sulfur–Container structure is designed and synthesized for high performance lithium sulfur batteries. The host in this unique architecture is porous carbon, which contains interconnected macropore tunnels and meso/micropores on the macropore tunnel walls. These hierarchical pores exhibit a synergistic effect to adsorb sulfur in their spaces and provide more nucleation sites to direct the uniform coating of sulfur. Moreover, the interconnected porous structure can facilitate electron transfer and also ensure high sulfur utilization. Furthermore, the poly(3,4-ethylenedioxythiophene) layer container improves the conductivity of the electrode, prevents the diffusion of dissolved polysulfide, and prevents volume expansion during the charge–discharge processes. As a result, the electrode with the poly(3,4-ethylenedioxythiophene)/sulfur/porous carbon composite and Host–Sulfur–Container architecture maintains a reversible capacity of 831.9 mA h g−1 after 200 cycles at a current density of 0.5 C and presents long-term cycling stability with 0.088% capacity decay per cycle over 500 cycles at 1 C. This indicates that the prepared Host–Sulfur–Container composite is a promising cathode material for lithium–sulfur batteries, and its hierarchical tunnel pore carbon host with meso/micropores inside shows great potential in the energy storage field.

CAS / MDL: 126213-50-1 9002-93-1
研究领域: 材料科学 · 能源存储 · 电池技术
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APPLIED SURFACE SCIENCE · 2023 · IF 6.7

MoP nanoparticles dispersed on P, N co-doped graphite nanosheets as separator-modified material in high-loading lithium-sulfur batteries

Jinwei Tian,Yu Cui,Lele Zhang,Chao Peng,Xiangfei He,Liang Chen,Yulin Bai,Chunli Guo,Yuede Pan,Gang Li,Yanzhen Liu,Han Chen

The cruising range of lithium batteries in new energy vehicles became main issue, so lithium-sulfur batteries (LSBs) with high theoretical energy density are becoming great expectations. However, the polysulfide-shuttle behavior and slow redox kinetics of the electrochemical processes result in a fast capacity and cycle life fade in LSBs, especially at high sulfur loads. In this paper, MoP nanoparticles were dispersed on P, N co-doped graphitic nanosheets (MoP/PNC) by one-step high-temperature phosphating method, which as a separator-modified material achieved an excellent electrochemical performance. The initial discharge specific capacity can reach 1470 mAh g −1 at a current density of 0.2C and the capacity attenuation per cycle in 600 cycles is only 0.074% (1C). Surprisingly, LSBs with MoP/PNC -modified separator can deliver a high area capacity of 9.30 mAh cm −2 with a sulfur loading up to 7.43 mg cm −2 on the positive electrode. The above-mentioned excellent electrochemical performances benefited from the synergistic effects of strong catalytic conversion ability of MoP and the physical/chemical adsorption and catalytic capability of PNC, which resulted in low polysulfide permeability and high sulfur utilization.

研究领域: 材料科学 · 电化学 · 能源存储 · 纳米技术
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