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International Journal of Electrochemical Science · 2023 · IF 1.5

NiFe2O4-Coated Activated Carbon Composite as a Cathode Material for Lithium–Sulfur Batteries

Riguang Cheng,Lixian Sun,Fen Xu,Yumei Luo,Chenchen Zhang,Yongpeng Xia,Sheng Wei,Yanxun Guan,Mengmeng Zhao,Qi Lin,Hao Li

Lithium–sulfur batteries are promising as next-generation rechargeable energy-storage devices because of their high energy density, low cost, and environmental friendliness. However, sulfur cathodes suffer from low specific capacity caused by the poor electrical conductivities of the active materials and fast capacity decay resulting from polysulfide dissolution/shuttling. Herein, we report a facile and low-cost method to solve these problems using an activated carbon (AC)–NiFe 2 O 4 /S hybrid material in which NiFe 2 O 4 is uniformly distributed on AC through a simple wet impregnation method. The AC–NiFe 2 O 4 /S material not only has a strong catalytic effect on sulfur reduction, but also provides strong binding sites to trap polysulfide intermediates. An AC–NiFe 2 O 4 /S electrode shows favorable electrochemical properties including stable reversible capacity (0.24% capacity decay per cycle at 0.1 C, retaining a capacity of 602.7 mAh g −1 after 170 cycles; stable cycling at 0.5 C, retaining a capacity of 501.9 mAh g −1 after 100 cycles), excellent rate performance, and fast electrochemical reaction kinetics compared with those of a reference AC/S electrode, which are attributed to the synergistic effects between NiFe2O4 and AC.

研究领域: 材料科学 · 电化学
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Mechanistic insights into rapid sulfite activation with cobalt sulfide towards iohexol abatement: Contribution of sulfur conversion

Ying Wu,Yiyuan Xing,Xiaodan Zhao,Zuoming Zhou,Guohua Jing

Recently, activation of sulfite for production of sulfate radical (SO 4 •− ) has emerged for abatement of organic contaminants. Herein, with regard to the excellent activation efficacy of Co(II) and the enhanced electron donating capacity by sulfur species, cobalt sulfide (CoS) was proposed for efficient sulfite activation towards iohexol abatement via SO 4 •− –based advanced oxidation processes. CoS exhibited better activation performance than typical CoO and Co 3 O 4 with a sharp decline of iohexol within 0.5 min, for which superior electron transfer efficiency of CoS was confirmed by Electrochemical impedance spectroscopy (EIS). The contribution of SO 4 •− and HO • to iohexol abatement was demonstrated by radical quenching experiment and Electron paramagnetic resonance (EPR). The influences of various parameters (solution pH, CoS and sulfite dosage, iohexol concentration), co-existing anions (HCO 3 − , HPO 4 2− , Cl − and NO 3 − ) and humic acid on iohexol abatement were investigated, as well as, the effect of different water matrixes on iohexol abatement was also evaluated. A possible mechanism was proposed based on ionic strength experiment, Transmission electron microscope-Energy dispersive spectrometer (TEM-EDS), X-ray photoelectron spectroscopy (XPS) and Raman. The superior activation performance of CoS could be attributed to the inner-sphere complexation between CoS and sulfite and enhanced > Co(III)/>Co(II) recycling induced by reductive sulfur species via rapid electron transfer. In addition, the iohexol degradation pathways were analyzed. This study highlights the contribution of sulfur conversion in the sulfite activation process and is expected to provide a facile CoS enhanced sulfite activation method for efficient abatement of organic contaminants.

研究领域: 环境科学 · 化学工程
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PLoS One · 2019 ·Vol. 14 ·期 1 ·e0208125 · IF 2.776

Study on dielectric properties of high organic sulfur coking coal and modeling sulfur compounds

Chuanchuan Cai,Tao Ge,Mingxu Zhang

Coking coal is geologically scarce resource and most of them cannot be directly used in steel making due to their higher sulfur content. One desulfurization method that has great potential for massive application is microwave desulfurization, which removes the relatively stubborn organic sulfur under mild conditions. The dielectric properties of coals determine the efficiency of the microwave energy absorption. The key to describing the mechanism of microwave desulfurization and further improvement of the desulfurization efficiency is the dielectric response of organic sulfur compounds in coal to microwave. This study focuses on existing formand microwave response of organic sulfur components of three typical coking coal in China. Resultsshowed that the major organic sulfur in selected coals is thiophene which has a stable structure and is the most difficult to be removed. Several dielectric peaks (dielectric loss)andsignificant differencesofeach selected coal samples are observed. The microwave absorption peaks of the model sulfur compounds are identified to be within 9-11GHz. The real parts of the relative dielectric constants (hereinafter referred to as ε ′) shows a decreasing trend as: diphenyl sulfoxide > diphenyl sulfone > diphenyl sulfide > dibenzothiophene > Octadecane thiol. Response to microwaveare observed to be distinctively different between sulfur-containing and sulfur-free model compounds. The dielectric polarization of mixture (coal mixed with model sulfur compounds) is greater than pure coal. Meanwhile the higher the sulfur content of the coal, the greater the ε ′ is. Sulfur componentsin coal can significantly influence its polarization.

研究领域: 能源科学 · 材料科学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2021 · IF 5.316

Dual-function LiFePO4 modified separator for low-overpotential and stable Li-S battery

Ming Jin,Rui Gao,Guiru Sun,Haibo Li,Xiangxin Xue,Chaoqun Qu,Nan Li,Yuting Zhang,Zhao Wang,Ming Feng

Lithium sulfide (Li 2 S) compounds as cathode materials for Lithium-sulfur (Li-S) battery have attracted more and more attention recently because of its high specific capacity, lower volume expansion and higher thermal stability of Li 2 S. However, high electrochemical barrier of the Li 2 S cathode and “shuttle effect” from S species on anode still block the development of Li-S batteries. Herein, LiFePO 4 (LFP) is employed as dual-function separator modifier to establish hybrid cathode. The modified separator will reduce overpotential for effective and durable sulfur redox reactions at the same time, it can also efficiently immobilize the lithium polysulfides (LiPSs) through the Lewis acid-base interaction of LiPSs and LFP. The battery systems based on the as-developed LFP modified separator exhibit an excellent rate capability, high sulfur utilization and outstanding cycling performance. The capacity retention can reach 83.9% after 400 cycles at 0.2 C, and the capacity can reach 594 mAh g −1 at up to 2 C. Current facile and low-cost strategy to modified Li-S battery systems on one hand offers an effective pathway to enhance electrochemical performance, on the other hand inspire new strategies on reducing the activation barrier of Li 2 S for improved sulfur electrochemistry as well.

CAS / MDL: 10377-48-7 872-50-4
研究领域: 材料科学 · 电化学 · 能源存储
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ELECTROCHIMICA ACTA · 2017 · IF 4.798

In situ synthesized Li2S@porous carbon cathode for graphite/Li2S full cells using ether-based electrolyte

Ning Wang,Naiqin Zhao,Chunsheng Shi,Enzuo Liu,Chunnian He,Fang He,Liying Ma

Lithium-sulfur (Li-S) batteries have been recognized as one of the promising next-generation energy storage devices owing to their high energy density, low cost and eco-friendliness. As for cathode’s performance, the main challenges for developing highly-efficient and long-life Li-S batteries are to retard the polysulfides diffusion into electrolyte and the reaction with metallic lithium (Li). Especially, the safety issues, derived from metallic Li in anode, must be overcome. Herein, we fabricated lithium sulfide@porous carbon composites (Li 2 S@PC) by an in-situ reaction between the lithium sulfate (Li 2 SO 4 ) and the pyrolytic carbon from glucose. The nanosized Li 2 S particles were uniformly distributed in the carbon matrix, which not only significantly improve electronic conductivity of the electrode but also effectively trap the dissolved polysulfides. Furthermore, on the basis of the graphite’s electrochemical features in ether-based electrolyte, we assembled graphite-Li 2 S@PC full cells using the obtained Li 2 S@PC composites as the cathode, graphite as the anode and the DOL/DME with LiNO 3 additive as the electrolyte. A unique strategy was proposed to activate the full-cells in descending order using constant voltage and current to charge the cut-off voltage. This Li-S full cell exhibits stable cycling performance at 0.5 C over 100 cycles. Because graphite-Li 2 S batteries are suitable to the lithium-ion batteries industry, our preliminary results here will shed a new light on the cell design and industrial production.

CAS / MDL: 25249-54-1 9003-39-8
研究领域: 材料科学 · 电化学 · 能源存储
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Metals · 2023 ·Vol. 13 ·期 3 ·603 · IF 2.9

Enhanced Separation of Sulfur and Metals from Polymetallic Sulfur Slag through Recrystallizing Regulation of Sulfur Crystals

Fanyun Chen,Qingshan Gao,Jing Zhang,Hao Deng,Chen Tian,Zhang Lin

Elemental sulfur is an important non-metallic material that is widely used in various fields including chemical, metallurgical and sulfuric acid industries. Polymetallic sulfur slag (PSS) is an important secondary resource for the recovery of sulfur. However, separation of sulfur from PSS is difficult due to the tight binding of some thiophilic metals to sulfur. Herein, we proposed a recrystallization method for the effective separation of sulfur and metals by using organic solvents to control the particle size of sulfur crystals. It was suggested that the particle size of sulfur recovered in the close to saturation state of toluene is about 2000 μm, while the purity is as high as 99.6%. Moreover, the recovery rate is over 95%, which is more than the current commonly used flotation method. The growth mechanism of sulfur crystals under different saturation conditions lays a foundation for the deepening of the growth theory of large-size sulfur crystals. This method realized the effective separation of sulfur from metal sulfides such as FeS2and ZnS, which provided an important guidance for the recovery of sulfur resources through a novel method of recrystallizing regulation.

CAS / MDL: 7704-34-9
研究领域: 冶金学 · 材料科学
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mBio · 2024 ·Vol. 15 ·期 3 · IF 5.1

Rhodobacteraceae methanethiol oxidases catalyze methanethiol degradation to produce sulfane sulfur other than hydrogen sulfide

Qun Cao,Xuanyu Liu,Qingda Wang,Zongzheng Liu,Yongzhen Xia,Luying Xun,Huaiwei Liu

Methanethiol (MT) is a sulfur-containing compound produced during dimethylsulfoniopropionate (DMSP) degradation by marine bacteria. The C–S bond of MT can be cleaved by methanethiol oxidases (MTOs) to release a sulfur atom. However, the cleaving process remains unclear, and the species of sulfur product is uncertain. It has long been assumed that MTOs produce hydrogen sulfide (H2S) from MT. Herein, we studied the MTOs in the Rhodobacteraceae family—whose members are important DMSP degraders ubiquitous in marine environments. We identified 57 MTOs from 1,904 Rhodobacteraceae genomes. These MTOs were grouped into two major clusters. Cluster 1 members share three conserved cysteine residues, while cluster 2 members contain one conserved cysteine residue. We examined the products of three representative MTOs both in vitro and in vivo. All of them produced sulfane sulfur other than H2S from MT. Their conserved cysteines are substrate-binding sites in which the MTO–S–S–CH3 complex is formed. This finding clarified the sulfur product of MTOs and enlightened the MTO-catalyzing process. Moreover, this study connected DMSP degradation with sulfane sulfur metabolism, filling a critical gap in the DMSP degradation pathway and representing new knowledge in the marine sulfur cycle field.

CAS / MDL: 119171-73-2 9003-99-0
研究领域: 微生物学 · 环境科学 · 海洋生物学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2017 · IF 3.359

Mechanism and kinetics of mercuric sulfide leaching with cuprous-thiosulfate solutions

Chao Han,Wei Wang,Feng Xie,Ting'an Zhang

Mercury is one of the most severe environmental pollutants due to its high toxicity, and the detoxification of mercury-containing solid wastes is a critical issue worldwide. In this work, thiosulfate solution has been used to leach mercury from mercuric sulfide. The influence of leaching conditions, including initial pH, molar ratio of copper to thiosulfate ([Cu]/[S 2 O 3 2− ]), and temperature on mercury leaching from mercuric sulfide, was investigated. The mercury leaching rate can reach as high as 92.37% after 7-h leaching under the optimized condition of initial pH 8.50, molar ratio of copper to thiosulfate 0.1 and leaching temperature 313   K. X-ray diffraction (XRD), scanning electron microscope-energy dispersive spectroscopy (SEM-EDS) and X-ray photoelectron spectroscopy (XPS) was used to analyze the leaching residue. The results show that copper in its thiosulfate complex can be substituted by mercury via Lewis substitution and cuprous sulfide was formed on the surface of leaching residue. The kinetics of mercuric sulfide leaching with cuprous-thiosulfate solutions was controlled by the product layer diffusion.

CAS / MDL: 1344-48-5
研究领域: 环境科学 · 化学工程
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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Construction of MoS2 nano-heterojunction via ZnS doping for enhancing in-situ photocatalytic reduction of gold thiosulfate complex

Weiquan Zhan,Yuan Yuan,Bingqiao Yang,Feifei Jia,Shaoxian Song

Recovery of gold thiosulfate complex ([Au(S 2 O 3 ) 2 ] 3− ) from leaching solutions has been recognized as a tough task, which limited the industrial promotion of eco-friendly thiosulfate leaching technique. In this work, MoS 2 /ZnS nano-heterojunction as a catalyst was proposed for the recovery of [Au(S 2 O 3 ) 2 ] 3− from leaching solution. The results indicated that [Au(S 2 O 3 ) 2 ] 3− could not only be efficiently recovered, but also in-situ reduced into Au 0 when MoS 2 /ZnS nano-heterojunction being used in the leaching solution. Mo 0.45 Zn 0.10 S exhibited an extremely high reduction capacity (1120.56 mg/g), which was 4.52 and 1.72 times of ZnS and MoS 2 , respectively. The great improvement was resulted from the ZnS doping on MoS 2 , which brought stronger light absorption, higher transferred efficiency and lower recombination of photogenerated electron-hole pairs of MoS 2 . In addition, the Au 0 could completely desorpt from MoS 2 /ZnS nano-heterojunctions in Na 2 S solution in less than 4 min, leading MoS 2 /ZnS nano-heterojunction to have remarkable cycling performances. This work provided a new insight for enhancing the recovery and in-situ reduction of gold thiosulfate complex from leaching solutions.

CAS / MDL: 7783-18-8
研究领域: 材料科学 · 环境科学
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ChemElectroChem · 2020 ·Vol. 8 ·期 1 ·90-95 · IF 4.154

Metal-Organic-Framework-Derived Porous Carbon Embedded with TiO2 Nanoparticles as a Cathode for Advanced Lithium–Sulfur Batteries

Chu Qi,Huilan Li,Jia Wang,Chengcheng Zhao,Cuimei Fu,Lina Wang,Tianxi Liu

Graphical MOF to a flame : This work demonstrates Ti-metal-organic-framework (Ti−MOF)-derived TiO 2 /C skeletons with in situ generated hierarchical pores and TiO 2 crystalline grains, which effectively encapsulate sulfur species and accelerate polysulfide conversion kinetics in lithium-sulfur batteries. The undesired internal shuttling of soluble polysulfide intermediates (Li 2 S n , 2

研究领域: 材料科学 · 能源存储
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2024 · IF 20.2

Short-term cathodic tuning atomic-level S-S interaction of CuS for heavy metal ultrafast detoxication

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
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Nature Communications · 2024 ·Vol. 15 ·期 1 ·1-17 · IF 14.7

Structural evolution during inverse vulcanization

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
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