JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Haoxiang Zhong,Lingzhi Zhang
The low sulfur utilization and the serious shuttle effect of polysulfides severely hamper practical application of Li-S batteries. Herein, sulfur cathodes with the multi-functional structures, featured with double-layered hollow carbon sphere with up to 50 nm interlayer space (DLHC-50) in situ grown Co-SnS catalytic layer is designed and synthesized for lithium sulfur batteries. Co-SnS/DLHC-50 can encapsulate 72% sulfur, higher than 63% for Co-SnS/DLHC-20 due to the large interlayer spaces of DLHC-50. Meanwhile, polysulfides are also effectively restricted via physical entrapment from DLHC-50 as well as chemical binding between Co-SnS and polysulfides. Benefiting from the well-constructed host framework, Co-SnS/DLHC-50 @S shows higher specific capacity/capacity retention of 760.4 mA h g −1 /72.9% after 500 cycles at 0.5 C, than that of 546.5 mA h g −1 /62.2% and 668.9 mA h g −1 /62.2%, for DLHC-50 @S, and Co-SnS/DLHC-20 @S, respectively. In addition, the strategy can be also extended to prepare other metal oxides (sulfides)/DLHC-50 for wide applications. Therefore, this work demonstrates a promising route to combat some bottlenecks such as low sulfur utilization, and the shuttle effect of polysulfides for Li-S batteries.
研究领域:
材料科学
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能源存储
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Hailong Li,Wei Zheng,Jianping Yang,Wenqi Qu,Lijian Leng,Yong Feng,Qingjie Guo,Zequn Yang
Fundamental barriers remaining yet impeding the rational design of metal sulfide (MS)-based sorbents for efficient elemental mercury (Hg 0 ) capture are the lack of a quantitative understanding between the amount of the most active ligands (i.e., under-coordinated sulfur) and the Hg 0 removal performance of MS. The intrinsic diversity and complexity of the sulfur species, which make it difficult to exclusively control the abundance of under-coordinated sulfur in MS while keeping its valence generally unchanged, is the primary challenge to be overcome. A dedicated tin sulfide (SnS x ) nanosheet was thus adopted to this end by adjusting its size and the exposure ratio of edge mono-sulfide. Unlike other methods used for the construction of under-coordinated sulfur, e.g., doping heteroatoms, introducing defects, straining lattice, etc., this novel method achieved the independent adjustment of the abundance of under-coordinated sulfur in MS. A linear relationship was hence established, indicating that, with the molar ratio of under-coordinated sulfur in SnS x increased by 1 %, its Hg 0 capture capacity was enhanced by ∼ 0.9 mg g −1 . This quantitative relationship was further taken as valuable guidance serving the Hg 0 capture performance improvement of SnS x with the co-consideration of its textural properties. The applicability of this quantitative relationship may be further extended across the MS community, saving the time spending in experiments and stepping towards the rational design of MS-based Hg 0 sorbents.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Yiqun Chen,Baitian Zeng,Liying Long,Qing Shao,Zizheng Liu,Feng Wu,Pengchao Xie
The ultraviolet/persulfate (UV/PS) process has attracted more and more attention for water treatment. However, it runs the risk of producing bromate in the presence of bromide ions. In this work, we propose a new strategy using sulfite to inhibit bromate formation. The results show that the addition of sulfite significantly reduced the formed bromate in the UV/PS system by 61.2% and 24.5% in 30 min and 120 min, respectively. Increasing sulfite dosage or pH could enhance bromate control. From the standpoint of reaction kinetics, sulfite is likely to inhibit bromate formation by reducing bromine radicals (Br ) back to bromide ions, the energy profile of which was quantified by density functional theory (DFT) calculations. In the UV/PS/sulfite system, the conversion of SO 3 − to HO was observed, indicating that sulfite also served as a source of reactive radicals. Moreover, sulfite apparently promoted the degradation of benzoic acid and phenol in a UV/PS system, showing advantages over other inorganic reductants. As a result, we discovered that sulfite could not only help control bromate formation in UV/PS but also improve the system’s oxidation capacity.
研究领域:
环境科学
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化学工程
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DOI
高影响因子
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
2023
·Vol. 120
·期 42
·e2312091120
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IF 11.1
Xia Lin,Junwei Zhang,Huihui Yan,Jiaxi Xu,Zhonghao Miao,Guangchang Shu,Shuyuan Zhao,Tianyuan Zhang,Haoxiang Yu,Lei Yan,Liyuan Zhang,Jie Shu
Metal-sulfur batteries have received great attention for electrochemical energy storage due to high theoretical capacity and low cost, but their further development is impeded by low sulfur utilization, poor electrochemical kinetics, and serious shuttle effect of the sulfur cathode. To avoid these problems, herein, a triple-synergistic small-molecule sulfur cathode is designed by employing N, S co-doped hierarchical porous bamboo charcoal as a sulfur host in an aqueous Cu-S battery. Expect the enhanced conductivity and chemisorption induced by N, S synergistic co-doping, the intrinsic synergy of macro-/meso-/microporous triple structure also ensures space-confined small-molecule sulfur as high utilization reactant and effectively alleviates the volume expansion during conversion reaction. Under a further joint synergy between hierarchical structure and heteroatom doping, the resulting sulfur cathode endows the Cu-S battery with outstanding electrochemical performance. Cycled at 5 A g−1, it can deliver a high reversible capacity of 2,509.8 mAh g−1 with a good capacity retention of 97.9% after 800 cycles. In addition, a flexible hybrid pouch cell built by a small-molecule sulfur cathode, Zn anode, and gel electrolytes can firmly deliver high average operating voltage of about 1.3 V with a reversible capacity of over 2,500 mAh g−1 under various destructive conditions, suggesting that the triple-synergistic small-molecule sulfur cathode promises energetic metal-sulfur batteries.
研究领域:
材料科学
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电化学
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能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Small
·
2023
·Vol. 19
·期 37
·2301085
·
IF 13.3
Guo Liu,Qi Zeng,Xinyi Sui,Shuhao Tian,Xiao Sun,Qingfeng Wu,Xijuan Li,Yuhao Zhang,Kun Tao,Erqing Xie,Zhenxing Zhang
Polysulfide shuttle effect and sluggish sulfur reaction kinetics severely impede the cycling stability and sulfur utilization of lithium-sulfur (Li-S) batteries. Modulating d-band electronic structures of molybdenum disulfide electrocatalysts via p/n doping is promising to boost polysulfide conversion and suppress polysulfide migration in lithium-sulfur batteries. Herein, p-type V-doped MoS 2 (V-MoS 2 ) and n-type Mn-doped MoS 2 (Mn-MoS 2 ) catalysts are well-designed. Experimental results and theoretical analyses reveal that both of them significantly increase the binding energy of polysulfides on the catalysts’ surface and accelerate the sluggish conversion kinetics of sulfur species. Particularly, the p-type V-MoS 2 catalyst exhibits a more obvious bidirectional catalytic effect. Electronic structure analysis further demonstrates that the superior anchoring and electrocatalytic activities are originated from the upward shift of the d-band center and the optimized electronic structure induced by duplex metal coupling. As a result, the Li-S batteries with V-MoS 2 modified separator exhibit a high initial capacity of 1607.2 mAh g −1 at 0.2 C and excellent rate and cycling performance. Moreover, even at a high sulfur loading of 6.84 mg cm −2 , a favorable initial areal capacity of 8.98 mAh cm −2 is achieved at 0.1 C. This work may bring widespread attention to atomic engineering in catalyst design for high-performance Li-S batteries.
研究领域:
材料科学
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电化学
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催化科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Catalysis
·
2023
·Vol. 6
·期 2
·174-184
·
IF 37.8
Hua Wuxing,Shang Tongxin,Li Huan,Sun Yafei,Guo Yong,Xia Jingyi,Geng Chuannan,Hu Zhonghao,Peng Linkai,Han Zhiyuan,Zhang Chen,Lv Wei,Wan Ying
Understanding sulfur conversion chemistry is key to the development of sulfur-based high-energy-density batteries. However, unclear relationships between the electronic structure of the catalyst and its activity are the major problem. Here, we provide a direct correlation between the p electron gain of S in p -block metal sulfides and the apparent activation energies ( E a ) for the sulfur reduction reaction (SRR), in particular, Li 2 S n to Li 2 S conversion, which is the rate-determining step of the SRR. The maximum p charge occurs in bismuth sulfide and results in the lowest E a and a high SRR rate in the cathode. Li–S batteries with the Bi 2 S 3 catalyst work steadily at a high rate of 5.0C with a high-capacity retention of ~85% after 500 cycles. A high areal capacity of ~21.9 mAh cm −2 was obtained under a high sulfur loading of 17.6 mg cm −2 but a low electrolyte/sulfur ratio of 7.5 μl mg −1 .
研究领域:
材料科学
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电化学
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电池技术
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催化
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2016
·
IF 3.15
Yanling An,Pan Wei,Meiqiang Fan,Da Chen,Haichao Chen,QiangJian Ju,Guanglei Tian,Kangying Shu
In this study, a dual-shell hollow polyaniline/sulfur-core/polyaniline (hPANI/S/PANI) composite was prepared by successively depositing PANI, S, and PANI on the surface of a template silicon sphere. The electrochemical properties of this composite were evaluated using a lithium plate as an anode in lithium/sulfur cells. The hPANI/S/PANI composite showed a discharge capacity of 572.2 mAh g −1 after 214 cycles at 0.1 C, and the Coulombic efficiency was above 87% in the whole charge/discharge cycle. The improved cycle property of the hPANI/S/PANI composite can be ascribed to the fine sulfur particles homogeneously deposited on the PANI surface and sprawled inside the two PANI layers during the charge/discharge cycle. This behavior stabilized the nanostructure of sulfur and enhanced its conductivity.
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
Inorganic Chemistry Frontiers
·
2018
·Vol. 5
·期 4
·785-792
·
IF 5.106
Jianmei Han,Baojuan Xi,Zhenyu Feng,Xiaojian Ma,Junhao Zhang,Shenglin Xiong,Yitai Qian
Although the melt-diffusion method was applied to fabricate sulfur-based cathode for lithium–sulfur batteries, more efforts should be devoted to the development of synthetic methodology of sulfur-based hybrids. Herein, we report a sulfur–hydrazine hydrate chemistry-based method to prepare the composite of sulfur and N-doped reduced graphene oxide (S@N-rGO) with 76% sulfur content. Relying on the reaction of sulfur and hydrazine hydrate, cyclo-sulfur was broken to form soluble polysulfides. The subsequent refluxing with GO suspension rendered the transformation of soluble polysulfides to sulfur crystal homogeneously deposited on N-rGO due to direct nucleation from solution. Simultaneously, the nitrogen doping of GO was realized with hydrazine hydrate as doping agent in the one-pot route. The as-obtained S@N-rGO composite displayed a good rate capability and excellent capacity stability up to 300 cycles. This study may provide a new and facile method to construct the composite of sulfur and N-doped carbonaceous matrix, which makes the hybrid a competitive cathode material for lithium–sulfur batteries (LSBs).
研究领域:
材料科学
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电化学
✓ 已验证
DOI
高影响因子
Journal of Energy Chemistry
·
2019
·
IF 5.162
Ziyang Jia,Hongzhang Zhang,Ying Yu,Yuqing Chen,Jingwang Yan,Xianfeng Li,Huamin Zhang
Lithium–sulfur (Li–S) batteries have great potential as an electrochemical energy storage system because of the high theoretical energy density and acceptable cost of financial and environment. However, the shuttle effect leads to severe capacity fading and low coulombic efficiency. Here, graphitic carbon nitride (g–C 3 N 4 ) is designed and prepared via a feasible and simple method from trithiocyanuric acid (TTCA) to anchor the polysulfides and suppress the shuttle effect. The obtained g–C 3 N 4 exhibits strong chemical interaction with polysulfides due to its high N–doping of 56.87 at%, which is beneficial to improve the cycling stability of Li–S batteries. Moreover, the novel porous framework and high specific surface area of g–C 3 N 4 also provide fast ion transport and broad reaction interface of sulfur cathode, facilitating high capacity output and superior rate performance of Li–S batteries. As a result, Li–S batteries assembled with g–C 3 N 4 can achieve high discharge capacity of 1200 mAh/g at 0.2 C and over 800 mAh/g is remained after 100 cycles with a coulombic efficiency more than 99.5%. When the C–rate rises to 5 C, the reversible capacity of Li–S batteries can still maintain at 607 mAh/g.
研究领域:
材料科学
·
电化学能源存储
✓ 已验证
DOI
高影响因子
ACS ES&T Engineering
·
2025
·
IF 6.7
Zulv Huang,Xipeng Wei,Lijuan Zhang,Tao Chen,Yi Huang,Zhangwei Yang,Wanqing Zeng,Hongxing Chen,Lingtian Xie,Bo Yan
Microbial reduction of pentavalent vanadium [V(V)] to less toxic tetravalent vanadium [V(IV)] is associated with the biogeochemical cycling of sulfur. However, the capability of elemental sulfur-reducing bacteria (S0RB) to reduce V(V) in the presence of elemental sulfur (S0) remains largely unexplored. Herein, we systematically investigated the V(V) reduction capabilities and underlying mechanisms of Bacillus megaterium R01, a S0RB strain isolated from the stone coal mining region. Under sulfur-depleted conditions, B. megaterium R01 demonstrated limited reduction capacity (<54.3% removal efficiency for 200 mg/L V(V)). In contrast, S0 supplementation enabled near-complete V(V) reduction (97.6 ± 2.1%) even at elevated concentrations (400 mg/L), achieving a relatively low carbon consumption rate (TOC/V(V) of ∼0.6). Sulfhydryl (SH) compounds, reaching 424.2 ± 9.9 μmol/L within 5 days, were likely crucial for reducing V(V) to V(IV). This mechanism differs from that of other V-reducing bacteria. The transcriptome analysis revealed that the up-regulation of genes associated with sulfur metabolism, cysteine, and methionine metabolism in B. megaterium R01 is likely to contribute to its enhanced resistance toward V(V). Additionally, the biosynthesis of intracellular BSH in B. megaterium R01, and the extracellular SH groups (e.g., Trx and TrxR encode enzymes) play an irreplaceable role in reducing V(V) by B. megaterium R01. This study enhances our understanding of V(V) reduction in sulfur-rich environments and suggests a promising approach for remediating V(V)-contaminated groundwater, sediments, and soils.
研究领域:
环境微生物学
·
污染修复
·
生物地球化学
✓ 已验证
产品关联
DOI
高影响因子
Advanced Energy Materials
·
2019
·Vol. 9
·期 36
·1901896
·
IF 24.884
Wenzhi Tian,Baojuan Xi,Zhenyu Feng,Haibo Li,Jinkui Feng,Shenglin Xiong
Lithium-sulfur batteries (LSBs) have been regarded as a competitive candidate for next-generation electrochemical energy-storage technologies due to their merits in energy density. The sluggish redox kinetics of the electrochemistry and the high solubility of polysulfides during cycling result in insufficient sulfur utilization, severe polarization, and poor cyclic stability. Herein, sulfiphilic few-layered MoSe 2 nanoflakes decorated rGO (MoSe 2 @rGO) hybrid has been synthesized through a facile hydrothermal method and for the first time, is used as a conceptually new-style sulfur host for LSBs. Specifically, MoSe 2 @rGO not only strongly interacts with polysulfides but also dynamically strengthens polysulfide redox reactions. The polarization problem is effectively alleviated by relying on the sulfiphilic MoSe 2 . Moreover, MoSe 2 @rGO is demonstrated to be beneficial for the fast nucleation and uniform deposition of Li 2 S, contributing to the high discharge capacity and good cyclic stability. A high initial capacity of 1608 mAh g −1 at 0.1 C, a slow decay rate of 0.042% per loop at 0.25 C, and a high reversible capacity of 870 mAh g −1 with areal sulfur loading of 4.2 mg cm −2 at 0.3 C are obtained. The concept of introducing sulfiphilic transition-metal selenides into the LSBs system can stimulate engineering of novel architectures with enhanced properties for various energy-storage devices.
研究领域:
材料科学
·
能源存储技术
✓ 已验证
DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2024
·
IF 5.9
Teng Shi,Miao-Yu Zhang,Qiang Sun
Lithium-sulfur battery has ultra-higher theoretical specific capacity (1675 mA h g −1 ) and theoretical energy density (2600 W h kg −1 ) compared with other commercially applied rechargeable battery system. However, some drawbacks, such as shuttle effect, poor conductivity and so on, disrupt the process of its industrialization and commercializes. In this study, spherical sulfur-containing polymer with short sulfur chain (sulfur chain length controlled at -S 2 -) was synthesized as cathode material for lithium storage. Two sulfur-containing polymer samples with particle size of 300 nm and 1000 nm were designed and synthesized to investigate the electrochemical properties of lithium storage. The obtained two sulfur-containing polymer cathode materials both exhibit higher lithium electroactivity with only one single discharge plateau at 2.1 V. Moreover, the cathode material with larger particle size displays faster reaction kinetics, showing stable long cyclic performance, i.e. and high specific capacity of 618 mA h g −1 after 150 cycles at a current density of 100 mA g −1 .
研究领域:
材料科学
·
能源存储
✓ 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）