SCIENCE OF THE TOTAL ENVIRONMENT
·
2020
·
IF 6.551
Chenhui Wei,Shujun Yin,Heyun Fu,Xiaolei Qu,William A. Mitch,Dongqiang Zhu
Here we investigated the mediation efficiency of different size fractions of rice straw-derived black carbon (BC) using sulfide-induced nitrobenzene reduction as a model system. The bulk BC was divided into three size fractions: dissolved BC (size <0.45 μm), colloidal BC (0.45 μm < size < 1 μm), and particulate BC (size > 1 μm). With the presence of BC fractions (250 mg/L) nitrobenzene reduction by Na 2 S was significantly facilitated, wherein the mediation efficiency was positively correlated with the BC fraction's oxygen group content in an order of particulate BC < colloidal BC ≪ dissolved BC. Consistently, the oxidation treatment of particulate BC with O 3 or HNO 3 improved the mediation efficiency, whereas the reduction treatment with NaBH 4 reduced the mediation efficiency. The supernatant collected with dialysis or filtration of suspension of BC materials pre-reacted with Na 2 S could effectively reduce nitrobenzene, suggesting that reactive reducing sulfur species were produced in aqueous solutions by reacting sulfide only with BC materials. This was evidenced by the fact that polysulfides and polysulfide radicals were both detected in the supernatant. As demonstrated by electron paramagnetic resonance analysis, the quinone moieties at the surface of BC materials accepted electrons from sulfide and turned into semiquinone free radicals, consequently leading to formation of reactive reducing sulfur species and thus enhanced nitrobenzene reduction. The strong mediation efficiency on redox reactions observed for colloidal BC and dissolved BC combined with their significant mobility in subsurface environments indicate that these carbonaceous materials may play an important role in the fate process of organic contaminants as both carriers and catalysts. Capsule The surface quinone moieties of BC induce the formation of reactive reducing sulfur species by acting as one-electron acceptors and facilitate nitrobenzene reduction by sulfide.
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PubMed
高影响因子
Surfaces and Interfaces
·
2025
·
IF 6.3
Senyang Wang,Yingdi Zhou,Bo Huang,Jingyi Qi,Mengting Hua,Xiaoshi Jin,Ling Li
The practical progression of quantum-dot sensitized solar cells (QDSSCs) due to the poor stability, which directly related to the leakage and volatileness of liquid electrolyte. Herein, the sodium alginate (SA) polysulfide gel electrolyte prepared by grinding method was first applied in the quasi-solid state QDSSCs. It has a pore structure which can elevate the rapid diffusion of ions. And the cross-linked interface with photoanode is smooth and non-adherent. The SA polysulfide gel electrolyte was used in Zn-Cu-In-Se (ZCISe) QDSSCs for standard experiments. The QDSSCs are able to materialize the photoelectric conversion efficiency (PCE) of 8.85 % (V oc is 0.63 V, J sc is 26.16 mA·cm −2 , FF is 51.80), which is 6 % higher than the liquid polysulfide QDSSCs (8.34 %). Above all, the stability is 3.2 times higher than that of liquid polysulfide electrolyte. The research fulfilled the goal of both efficiency and stability, also environmentally friendly.
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高影响因子
JOURNAL OF POWER SOURCES
·
2024
·
IF 8.1
Jiuqing Liu,Chen Duan,Zikun Hong,Junying He,Fanli Zeng,Chen Cheng,Ya Chen,Qihou Li,Zehao Chen,Liandong Tang,Zhirong Chen
The application of lithium-sulfur battery is seriously hindered by the shuttle of dissolved polysulfide between sulfur cathode and lithium anode, by which is not selectively inhibited by the conventional separator. Developing functional separator is considered as a preferred solution for this issue, but it is always challenged by the tedious preparation process. Herein, interfacial polymerization (IP) is employed to modify the surface property of ZrO 2 nanoparticles embedded polyetherimide (PZ) based separator, and the integration of pore size adjustment, electrostatic repulsion and physical adsorption into one is facilely achieved to effectively inhibit the polysulfide shuttle. Consequently, the optimized PZ separator presents a high lithium-ion transference number (0.55) and diffusion coefficient (2.16 × 10 −8 cm s −1 ). Compared with the pristine one, the electrochemical performance of the assembled lithium-sulfur battery is obviously enhanced, and an initial discharge specific capacity of 1242 mAh g −1 and a capacity retention of 68 % after 200 cycles are obtained.
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高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2022
·Vol. 28
·期 31
·e202200363
·
IF 5.02
Ting-Ting Zhang,Cheng-Ye Yang,Jin Qu,Wei Chang,Yu-Hao Liu,Xian-Zhi Zhai,Hong-Jun Liu,Zhi-Guo Jiang,Zhong-Zhen Yu
Graphical A polymer encapsulation strategy is designed to synthesize atomic Fe and N co-doped hollow carbon nanospheres (Fe−NHC) with Fe−N x sites for modifying commercial PP separator of LSBs to suppress the shuttle effect and promote the sluggish kinetics of intermediate polysulfides. Therefore, the battery with the Fe−NHC/PP separator delivers outstanding cycling and rate performances. Even at a harsh current density of 4 C, a high capacity of 824 mA h g −1 is achieved, indicating the superiority of the Fe-NHC/PP separator in LSBs. As competitive next-generation rechargeable batteries, lithium-sulfur batteries (LSBs) suffer from the shuttle effect and the sluggish kinetics of intermediate polysulfides during charge and discharge processes, adversely affecting their electrochemical performances and actual applications. Herein, we demonstrate a polymer encapsulation strategy to synthesize atomic Fe and N co-doped hollow carbon nanospheres (Fe−NHC) with Fe−N x sites for modifying commercial PP separator of LSBs to suppress the shuttle effect and promote the kinetics of intermediate polysulfides. Benefiting from the excellent structural design, the doped-N with positive charges could effectively adsorb negatively charged soluble polysulfides, help attract the soluble polysulfides to the Fe atoms and boost the catalytic transformation of the soluble polysulfides. Additionally, such a thin carbon shell could provide a short mass diffusion pathway and hence promote the adsorption and the catalytic conversion. Therefore, the battery with the Fe−NHC/PP separator delivers outstanding cycling and rate performances. At the large current density of 1 C, the specific capacity is 1079 mA h g −1 and maintains a low loss of 0.076 % per cycle within 500 cycles. Even at a harsh current density of 4 C, a high capacity of 824 mA h g −1 is still achieved, indicating the advantage of the Fe−NHC/PP separator in LSBs.
研究领域:
材料科学
·
电化学
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高影响因子
Energy Storage Materials
·
2021
·
IF 17.789
Chao Yue Zhang,Guo Wen Sun,Zu De Shi,Qian Yu Liu,Jiang Long Pan,Yan Chun Wang,Hao Zhao,Geng Zhi Sun,Xiu Ping Gao,Xiao Jun Pan,Jin Yuan Zhou
Atom-intercalated transition metal disulfides (TMDs) have attached much attention mainly due to their highly improved conductivity. But it is few reported that the atom intercalation can enable the TMDs have unexpected catalytic properties, caused by the unit-cell deformation in them. In this work, a type of V 0.25 -intercalated VS 2 (V 5 S 8 ) nanoflakes was designed via a direct vulcanization method combining Kirkendall heat diffusion effect, and used as the promotor for lithium-sulfur batteries (LSBs). The V 5 S 8 possesses a NiAs crystal structure, in which V atoms occupy the interlayer spacing between VS 2 monolayers, which will unavoidably cause the unit-cell deformation. As expected, the CNF@V 5 S 8 /S cathodes show a specific capacity of 1260 mAh g −1 at 0.2 C, and can keep 73.65% of the capacity with charge/discharge rate increasing 10 times; while the CNF@VS 2 /S ones can only retain 54.0% of the initial capacity. Moreover, the CNF@V 5 S 8 /S cathodes show an ultralow decay rate of only 0.0312% per cycle for 1500 cycles at 5 C. Furthermore, the catalysis effect of V 5 S 8 on the conversion of lithium polysulfide (Li 2 S n , n = 1, 2, 4, 6 and 8) and S 8 clusters were systematically discusses. Besides, the V 5 S 8 can further enable LSBs achieve a high areal capacity (8.2 mAh cm −2 with sulfur loading of 7.8 mg cm −2 ) and a high dynamic flexible stability at bending angle between 0 and 180 °.
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高影响因子
IONICS
·
2025
·
IF 2.6
Han Jingjing,Ju Xiaocheng,Xiao Yi,Liang Xinyu,Zhang Guoli,Jia Xiaoxia,Yang Zhewei,Pan Yuede
Nickel disulfide (NiS 2 ) is a promising electrochemical storage material for varied charge carrier ions. However, previous preparation approaches for NiS 2 -based materials have been haunted by the low utilization efficiency of the sulfur atoms in the precursor and the detrimental byproduct of SO 2 . Inspired by the unique crystal structure of NiS 2 , composed of Ni 2+ cations and S 2 2− anions, herein, we develop an environmentally friendly synthesis method for crystalline NiS 2 with 100% utilization efficiency of precursor sulfur atoms through the precipitation reaction between Ni 2+ and S 2 2− , which can happen at varied temperatures and in different solvents. Furthermore, a NiS 2 /S composite is in situ formed by the co-precipitation reaction between Ni 2+ and S 8 2− , which can also occur at varied temperatures and in different solvents. As demonstration, both the NiS 2 and NiS 2 /S have been applied for the electrochemical storage of nonaqueous Na + ions and aqueous Cu 2+ ions. Owing to the in situ formed elemental sulfur with higher theoretical capacity and the considerable conductivity provided by the framework of NiS 2 in the NiS 2 /S composite, it exhibits superior electrochemical performance compared to NiS 2 in terms of capacity, rate, and cycling stability. The polysulfide anions produced in the process of nonaqueous sodium ion storage enhance the electrochemical kinetics, and the sulfur can be converted into Cu 2 S through the intermediate of CuS in the process of aqueous copper ion storage. The sodium ion storage capacity of NiS 2 /S is retained at 578.5 mAh g −1 after 375 cycles at 2.0 A g −1 , and its reversible copper ion storage can sustain a long life of 1500 cycles at 1.0 A g −1 . Our work paves the way towards liquid-state inorganic synthesis of metal sulfides composed of metal cations and disulfide anions.
研究领域:
材料科学
·
环境科学
·
电化学
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高影响因子
RARE METALS
·
2023
·Vol. 42
·期 8
·2562-2576
·
IF 8.8
Liu Si-Ming,Chen Meng-Xun,Xie Ying,Liu Deng-Hua,Zheng Jin-Fei,Xiong Xiang,Jiang Heng,Wang Li-Chang,Luo Heng,Han Kai
All-solid-state lithium-sulfur (Li-S) battery is regarded as next-generation high energy density and safety battery system. The key challenge is to develop a compatible high-performance solid-state electrolyte. Herein, a two birds with one stone strategy is proposed to simultaneously enhance Li + conductivity and polysulfide adsorptivity of poly(ethylene oxide) (PEO)-based polymer electrolyte via the integration of Nb 2 CT x MXene. Moreover, the sheet size of Nb 2 CT x MXene is crucial for the enhancement of Li + conductivity and polysulfide adsorptivity, attributing to the difference in a specific surface area related to the percolation effect. By tuning the sheet size of Nb 2 CT x MXene from 500–300 nm to below 100 nm, the ionic conductivity of the PEO electrolyte is increased to 2.62 × 10 −4 S·cm −1 with improved Li + transference number of 0.37 at 60 °C. Furthermore, theoretical calculation and X-ray photoelectron spectroscopy (XPS) conjointly prove that polysulfides could be effectively adsorbed by Nb 2 CT x nanosheets via forming Nb−S bonding to inhibit their shuttle in the PEO framework. As a result, the all-solid-state Li-S cell exhibits an initial capacity of 1149 mAh·g −1 at 0.5C and good cycling stability with 491 mAh·g −1 after 200 cycles. The results demonstrate the necessity of polysulfide inhibition and the application of Nb 2 CT x MXene in PEO-based electrolytes for all-solid-state Li-S batteries. Graphic
研究领域:
材料科学
·
储能技术
·
电化学
·
纳米材料
·
固态电池
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高影响因子
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