APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Liming Yang,Guangzhen Liu,Zhenglin Chen,Zhiyan Guo,Tian Liu,Hui Shi,Penghui Shao,Xianchuan Xie,Wenwei Li,Xubiao Luo
Transition metal sulfides have demonstrated excellent heavy metal detoxification in previous studies. However, the activity of their S-functional sites is usually not maximized because they are not precisely regulated. Herein, we report a new short-term cathodic tuned CuS crystals (C-tuned CuS) distortion strategy, ultrafast detoxicating over 95% Cr(VI) in 1 min，its detoxification rate was elevated by five orders of magnitude times compared to the untuned one. The high Cr(VI) detoxification performance is mainly attributed to the layered sulfur atoms tuning within series of cathodic potential shown by In-situ Raman. Besides, the four-tuning stages of C-tuned CuS lattice distortion based on the variation of Raman peak height and redshift changes was investigated by density functional theory (DFT) calculations, showing that the S-S bonds was stretched under cathodic tuning, extending from 2.106 to 2.345 Å. The stretched S-S bonds with enhanced polarity and electron activity prevailed the formation of transient Cr-S bonds with Cr(VI), favoring the direct electron transfer without O mediation, thus reducing the Cr(VI) reduction energy barrier. Cathodic tuning CuS crystal distortion, a “Plug and Play” strategy, show a new electron-level microscopic insights into wastewater reduction techniques development.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-17
·
IF 14.7
Zheng Botuo,Zhong Liling,Wang Xiaoxiao,Lin Peiyao,Yang Zezhou,Bai Tianwen,Shen Hang,Zhang Huagui
Inverse vulcanization exploits S 8 to synthesize polysulfides. However, evolution of products and its mechanism during inverse vulcanization remains elusive. Herein, inverse vulcanization curves are obtained to describe the inverse vulcanization process in terms of three stages: induction, curing and over-cure. The typical curves exhibit a moduli increment before declining or plateauing, reflecting the process of polysulfide network formation and loosing depending on monomers. For aromatic alkenes, in the over-cure, the crosslinked polysulfide evolves significantly into a sparse network with accelerated relaxation, due to the degradation of alkenyl moieties into thiocarbonyls. The inverse vulcanization product of olefins degrades slowly with fluctuated relaxation time and modulus because of the generation of thiophene moieties, while the inverse vulcanization curve of dicyclopentadiene has a plateau following curing stage. Confirmed by calculations, the mechanisms reveal the alkenyl groups react spontaneously into thiocarbonyls or thiophenes via similar sulfur-substituted alkenyl intermediates but with different energy barriers.
研究领域:
材料科学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2020
·
IF 7.489
Yuwei Ma,Guangtong Hai,Dimberu G. Atinafu,Wenjun Dong,Rongjie Li,Changmin Hou,Ge Wang
Carbon -MoS 2−x @CdS (C-MoS 2−x @CdS) core-shell nanostructures with controlled surface sulfur (S) vacancies were prepared via a glucose assisted hydrothermal growth method. The glucose acted as a reducing agent of C-MoS 2−X to partially reduce Mo 4+ ions to Mo 3+ and served as a carbon source to insert the amorphous carbon into the layered MoS 2−X simultaneously. The presence of Mo 3+ result in the surface S-vacancies, which can provide more additional active sites and enhance the photocatalytic performance. Moreover, the inserted carbon in layered MoS 2−X enhanced the electron mobility and decreased the resistance electron transfer. Density functional theory (DFT) calculation confirmed that the surface S-vacancies and the amorphous carbon increase the projected density of states at the conduct band edge, which could enhance the photo-absorption and photo-responsibility. The result is consistent with the photocatalytic H 2 production experiment . C2-10%MoS 2−x @CdS presented a high H 2 evolution rate of 61,494 μmol h −1 g −1 under visible light irrigation (λ ≥ 420 nm), which is 1.98 times and 158 times higher than that of sample without S-vacancies (10%MoS 2 @CdS) and pure CdS, respectively.
研究领域:
材料科学
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能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ADVANCED MATERIALS
·
2021
·Vol. 33
·期 16
·2100229
·
IF 30.849
Yanxia Wang,Yangyang Lai,Jun Chu,Zichao Yan,Yun-Xiao Wang,Shu-Lei Chou,Hua-Kun Liu,Shi Xue Dou,Xinping Ai,Hanxi Yang,Yuliang Cao
Room-temperature (RT) sodium–sulfur (Na–S) batteries hold great promise for large-scale energy storage due to the advantages of high energy density, low cost, and resource abundance. The research progress on RT Na–S batteries, however, has been greatly hindered by the sluggish kinetics of the sulfur redox reactions. Herein, an elaborate multifunctional architecture, consisting of N-doped carbon skeletons and tunable MoS 2 sulfiphilic sites, is fabricated via a simple one-pot reaction followed by in situ sulfurization. Beyond the physical confinement and chemical binding of polarized N-doped carbonaceous microflowers, the MoS 2 active sites play a key role in catalyzing polysulfide redox reactions, especially the conversion from long-chain Na 2 S n (4 ≤ n ≤ 8) to short-chain Na 2 S 2 and Na 2 S. Significantly, the electrocatalytic activity of MoS 2 can be tunable via adjusting the discharge depth. It is remarkable that the sodiated MoS 2 exhibits much stronger binding energy and electrocatalytic behavior compared to MoS 2 sites, effectively enhancing the formation of the final Na 2 S product. Consequently, the S cathode achieves superior electrochemical performance in RT Na–S batteries, delivering a high capacity of 774.2 mAh g −1 after 800 cycles at 0.2 A g −1 , and an ultrahigh capacity retention with a capacity decay rate of only 0.0055% per cycle over 2800 cycles.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ORGANIC CHEMISTRY
·
2017
·
IF 4.849
Qiujie Tang,Zhaogang Bian,Wei Wu,Jin Wang,Ping Xie,Charles U. Pittman,Jr.,Aihua Zhou
The method for constructing C–S bonds is very important in organic synthesis. Here a new sulfenylation method to generate flavone thioether derivatives was developed by employing aromatic or alkyl halides, S powder and Na2S2O3 as reactants. Good yields of regioselective Calkyl–S and Caryl–S-substituted flavones were generated under relatively environmentally friendly and simple conditions. This method might be potentially applicable to large scale production, and it enriches current sulfenylation methods.
研究领域:
有机化学
·
药物合成
✓ 已验证
DOI
PubMed
高影响因子
Energy Storage Materials
·
2017
·
IF 0
Chunlong Dai,Linyu Hu,Min-Qiang Wang,Yuming Chen,Jin Han,Jian Jiang,Yan Zhang,Bolei Shen,Yubin Niu,Shu-Juan Bao,Maowen Xu
Lithium-sulfur (Li-S) batteries are of great importance as promising electrochemical-energy storage systems in view of their overwhelming advantage of energy density . However, their commercial applications are still far away mainly due to fast capacity decay in a high sulfur content caused by low utilization of active material and severe polysulfide dissolution during electrochemical cycling. Here we have designed and prepared uniform α-Ni(OH) 2 hollow spheres constructed from ultrathin nanosheets with the thickness of ~3.5 nm as a hollow sulfur nanosphere host for Li-S batteries. Specifically, the synthesized hierarchical hollow spheres not only manifest the advantages of hollow structure and robust protective shell to encapsulate a very high content of sulfur up to 81 wt%, but also offer sufficient functionalized surfaces to directly bond and entrap polysulfides in hollow sphere. When used as cathode materials for Li-S batteries, the S@Ni(OH) 2 double-shell hollow hybrids exhibit a highly stable cycle life over 1000 cycles at 1 C with a very small capacity decay rate of only ~0.04% per cycle.
研究领域:
材料科学
·
能源存储
✓ 已验证
DOI
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Yingjie Cheng,Li He,Dong Mao,Xuejian Shi,Chunzhong Wang,Fengxue Duan,Pengyan Xue,Yizhan Wang,Yingjin Wei
The active electronic states in 1T-MoS 2 are highly desirable for catalyzing polysulfides conversion. However, stable 1T-MoS 2 is difficult to produce using common approaches. Herein, V uniformly doped in-plane 1T-2H heterostructured MoS 2 nanosheets (V-MoS 2 ) are prepared by a facile hydrothermal method with a polyoxometalate precursor containing periodic Mo and V atomic arrangement. The doping of V induces the phase transition from semiconducting 2H-MoS 2 to metallic 1T-MoS 2 and stabilizes the resulted 1T phase. Importantly, the incorporation of V not only modifies the surface electronic property of MoS 2 , enhancing the active site density, but also improves the adsorption of polysulfides and the catalytic efficiency for sulfur redox reactions. With these advantages, the Li-S batteries using V-MoS 2 electrocatalyst achieve accelerated reaction kinetics and superior electrochemical performance. When the S loading of the cathode is 5.41 mg cm −2 , a favorable discharge capacity of 4.98 mAh cm −2 is obtained with satisfying cycle stability. This work provides an efficient atomic engineering approach for the design of high performance electrocatalyst for Li-S batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 39
·20604-20611
·
IF 11.301
Liang-Liang Gu,Jian Gao,Chuang Wang,Sheng-You Qiu,Ke-Xin Wang,Xiao-Tian Gao,Ke-Ning Sun,Peng-Jian Zuo,Xiao-Dong Zhu
Lithium–sulfur (Li–S) batteries are regarded as one of the most promising candidates for next-generation energy storage systems due to their advantages of its high specific capacity and low material cost. Regrettably, the electrical insulation nature of sulfur, the volume expansion during lithiation, and the internal shuttle effect aroused by the polysulfides dissolution are the central issues for sulfur cathodes. Here, CoFe2O4@C nanocages derived from Prussian blue analogues and polydopamine were utilized as a sulfur host to address these problems. The polar Co–Fe oxide afforded chemical adsorption sites for anchoring polysulfides to reduce the shuttling effect. The hollow core structure of the nanocages could withstand the large volume change during lithiation and delithiation processes. The conductive carbon layer on the nanocages could ameliorate the extremely low electrical conductivity of S and Li2S. The S/CoFe2O4@C cathode demonstrated high capacity and excellent cyclability (821 mA h g−1 after 100 cycles at 0.5C). More importantly, the combinational strategies of good conductivity, physical space encapsulation, and chemical adsorption provide a means of resolving the current cathode issues in Li–S batteries.
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
CERAMICS INTERNATIONAL
·
2021
·
IF 4.527
Jiawei Long,Tianli Han,Mengfei Zhu,Xiaoyong Xu,Jinjin Li,Junjie Niu,Jinyun Liu
Lithium-sulfur battery cathodes still remain a challenge on capacity decay due to the shuttle effect even though a series of strategies have been tried. Here we report a novel matryoshka-like CuS@void@Co 3 O 4 architecture of double micro-cubes ( μ -cubes) that locks sulfur between the CuS core and the Co 3 O 4 shell. Plenty of existing spaces between the μ -cubes suffice a high loading of sulfur and volumetric accommodation. The robust, double closed cubes configuration greatly enhances the confinement of polysulfides . In parallel, the CuS core increases the electronic conductivity and contributes to additional capacity, while the Co 3 O 4 shell ensures a better interface activity. A high Li + ion diffusion coefficient is obtained during the sulfur and lithium sulfide transformation. The constructed battery displays an initial capacity up to 1480 mAh g −1 , and a Coulombic efficiency (CE) exceeding 99%. A capacity retention higher than 500 mAh g −1 with a CE larger than 99.8% after cycling 400 times at 0.2 C are achieved. In addition, under a temperature of −5 °C, a high capacity of 700 mAh g −1 at 0.2 C after 200 cycles is achieved, indicating a good low-temperature tolerance.
研究领域:
材料科学
·
电化学
·
能源存储技术
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2018
·
IF 5.116
Zhenqi Cui,Jia Yao,Tao Mei,Shiyuan Zhou,Baofei Hou,Jing Li,Jinhua Li,Jianying Wang,Jingwen Qian,Xianbao Wang
In our study, TiC-TiO 2 /S composite was successfully prepared with a simple and effective method. For this special micro-mesoporous structure, TiC-TiO 2 can be used as an efficient sulfur storing material, and also restrain the volume expansion of sulfur to a certain degree for its suitable specific surface area. TiO 2 and TiC can suppress the diffusion of polysulfides due to their strong interaction with polysulfides . At the same time, TiC also can remedy the nonconductive defect of sulfur for its good conductivity. With the help of above advantages, the TiC-TiO 2 /S cathode delivers an initial discharge specific capacity of 1218 mAh g −1 at 1 C (1 C = 1675 mA g −1 ) with the sulfur loading of 1.5 mg cm −2 . And when cycles at 0.5 C, a stable capacity of 714 mAh g −1 can be maintained after 500 cycles accompanied with the sulfur loading of 1.1 mg cm −2 .
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
APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Maru Dessie Walle,Mengyuan Zhang,Ke Zeng,Yajuan Li,You-Nian Liu
Despite their high energy density , low-cost, and low environmental impacts compared with the current state-of-the-art lithium-ion batteries, lithium–sulfur (Li S) batteries still suffer from the low sulfur content, dissolution of polysulfides and capacity loss, which hinder their commercial application. To address these issues, nitrogen-doped cubic carbon (NC) interwoven with carbon nanotubes (CNT) host is introduced to achieve high sulfur content for lithium–sulfur batteries. The NC/CNT composites are derived from metal–organic frameworks (MOFs), which can physically confine sulfur, thus providing efficient sulfur loading. The sulfur content in the as-obtained S@NC/CNT composite is as high as 89 wt%, while the cathode membrane has a sulfur loading of 3.6 mg cm − 2 . In addition, the NC/CNT composite can obstruct the dissolution and outward diffusion of polysulfides . Impressively, under the high sulfur content and high sulfur loading conditions, the S@NC/CNT cell exhibits initial specific capacity of 1141 mA h g − 1 at the current rate of 0.5C (837.5 mA g − 1 ) and the capacity retains 674.4 mA h g − 1 after 120 cycles. The S@NC/CNT cathode also shows high areal capacity (4.1 mA h cm − 2 ). The NC/CNT composite derived from MOFs has great potential applications for high‑sulfur loading cathodes.
研究领域:
材料科学
·
能源存储
✓ 已验证
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2019
·Vol. 43
·期 38
·15267-15274
·
IF 3.069
Dan Li,Jie Liu,Na Xu,Mengfan Wang,Xuejun Liu,Tingzhou Yang,Tao Qian,Chenglin Yan
The reduction of elemental sulfur to lithium sulfides is a complicated process and it involves a series of redox reactions; this leads to a variety of dominating obstructions for the commercial applications of lithium–sulfur (Li–S) batteries. Herein, we improved the performance of lithium–sulfur batteries by covalently immobilizing the discharge products on carbon nanofibers by using cysteamine as a medium, which enabled us to achieve unprecedented capacity retention of ∼87.6% after 500 cycles at a current rate of 1C (1C = 1675 mA g−1) with high sulfur loading of 4.5 mg cm−2. Significantly, in situ UV/vis spectroscopy and X-ray absorption spectroscopy (XAS) of the electrolyte offered direct evidence for the proposed mechanism. No detectable signals of dissoluble polysulfides in the electrolyte were observed at any intermediate states, indicating the effect of covalent bonds on the reduction of long-chain polysulfide Li2Sx (4 < x ≤ 8) production. Theoretically, DFT calculations indicated the presence of different S–S bond lengths in linear polysulfanes and verified the presence of short-chain polysulfide Li2Sx (1 ≤ x ≤ 4) intermediates during discharge. This strategy provides an important way to solve one of the essential issues limiting the commercial applications of Li–S batteries.
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
危险品化学品经营许可证（带存储）