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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2023 · IF 9.9

Anion receptor and heavy metal-free redox mediator decorated separator for lithium-sulfur batteries

Xin Guan,Huijie Pei,Xiaoyu Chen,Chen Chang,Siyuan Shao,Yu-Mo Zhang,Xingping Zhou,Hui Nie,Xiaolin Xie

The adsorption-catalysis synergy for accelerated conversion of polysulfides is critical toward the electrochemical stability of lithium-sulfur battery (LSB). Herein, a non-metallic polymer network with anion receptor units, trifluoromethanesulfonyl (CF 3 SO 2 -) substituted aza-ether, was in-situ integrated on PE separator, working as an efficient host for anchoring lithium thiophosphates (LPS) as redox mediators and polysulfides through Lewis acid-base interaction. The anchored LPS on the modified PE separator displayed a robust chemical adsorption ability towards polysulfides through the formation of S S bond. Meanwhile, LPS decreased the energy barrier of Li 2 S nucleation and promoted redox reaction kinetics. The battery with LPS decorated separator revealed a long cycling lifespan with a per cycle decay of 0.056 % after 600 cycles, and a competitive initial capacity of 889.1 mAh/g when the of sulfur cathode increased to 3 mg cm −2 . This work developed a new design strategy to promote the utilization of lithium phosphorus sulfide compounds in LSB.

研究领域: 电化学 · 能源材料 · 纳米材料 · 界面化学 · 储能技术
✓ 已验证 DOI 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Organic-inorganic multi-scale enhanced interfacial engineering of sulfide solid electrolyte in Li-S battery

Yang Bai,Yanbiao Zhao,Weidong Li,Linghui Meng,Yongping Bai,Guorong Chen

The developing sulfide solid electrolyte is a promising way to overcome shuttle effect of polysulfide in the traditional liquid Li-S battery. However, an air stable sulfide solid electrolyte and competitive solid–solid interface structure must be constructed firstly. Herein, we have designed an organic–inorganic multi-scale composite electrolytes to overcome the interfacial issues of solid state Li-S batteries (SSLSBs). The organic–inorganic composite electrolyte consists of a gel polymer electrolyte (GPE) and an oxygen doped inorganic sulfide solid electrolyte. The O doped sulfide solid electrolyte improves its chemical stability and suppresses the lithium dendrites. A thin GPE film protects the crystal structural stability during cycles and greatly enhances the performance of O doped sulfide solid electrolyte due to the GPE not only constructs soft interface contact between S cathode and solid electrolyte, but also builds lithium ion transport paths by ionic liquid between them. Those SSLSBs display a very good cycling performance with the specific capacity of 1023 mAh/g after 50 cycles at 60 °C and 541 mAh/g after 150 cycles at 30 °C under same rate of 0.1 C. This study demonstrates that the development of advanced solid-state Li-S battery needs to fully integrate a number of technical advantages.

研究领域: 电化学 · 材料科学 · 固态电池 · 能源存储 · 界面化学 · 纳米材料 · 电极材料
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Frontiers in Chemistry · 2022 · IF 5.545

The effect of different poly fibers separator-modified materials on blocking polysulfides for high performance Li-S batteries

Ling Meng,Zhaoxia Sun,Guanghang Sun,Xiting Zhang,Meng Dan,Jin Long,Jian Hu

Herein, we reported that KOH impregnation can generate a large number of porous structures with fruitful nitrogen self-doped groups during the carbonized process for poly (p-phenylene terephthalamide) fiber and poly (p-phenylene benzobisoxazole) fiber (denoted as PPTA and PBO, respectively). The intrinsical insulation, volume change, and shuttle effect of polysulfides then can be more significantly improved for the PBO-coated separator than the PPTA case. The discharge capacity primary achieves 1,322 mA h/g, which retains 827 mA h/g even after 200 cycles at 0.2 C for the cell with PBO-coated separator. The reversible specific discharge capacity maintains 841 mA h/g with a Coulomb efficiency of 99.7% at 5 C. The nitrogen self-doped nanocarbon particles are etched by KOH with the simple one-step preparation, which has promising application as Li-S battery cathode.

研究领域: 电化学 · 能源材料 · 纳米材料科学 · 电池技术 · 功能高分子材料
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Journal of Materials Chemistry A · 2016 ·Vol. 4 ·期 40 ·15343-15352 · IF 8.262

A lightweight multifunctional interlayer of sulfur–nitrogen dual-doped graphene for ultrafast, long-life lithium–sulfur batteries

Lu Wang,Zhi Yang,Huagui Nie,Cancan Gu,Wuxing Hua,Xiangju Xu,Xi'an Chen,Ying Chen,Shaoming Huang

Lithium–sulfur batteries are a promising candidate for next-generation battery systems owing to their low cost and high theoretical capacity and energy density. However, the notorious shuttle effect of the intermediate polysulfides as well as low conductivity of sulfur greatly limits their practical applications. Here, we introduce a new design that uses a porous-CNT/S cathode (PCNT–S) coupled with a lightweight multifunctional porous sulfur–nitrogen dual-doped graphene (SNGE) interlayer. It is confirmed that the introduced SNGE has outstanding conductivity, high ability to trap polysulfides, ability to modulate Li2S2/Li2S growth, and the functionality to protect separator integrity. With such rich functionalities, the SNGE interlayer enables the PCNT–S cathode to deliver a reversible specific capacity of ∼1460 mA h g−1 at 0.25C and a much higher rate performance, up to 40C, with a capacity retention of 130 mA h g−1. Critically, these cathodes exhibited ultrahigh cyclability when cycled at 8C for 1000 cycles, exhibiting a capacity degradation rate of 0.01% per cycle. To the best of our knowledge, such a low capacity degradation rate beyond 5C in the cathodes of advanced Li–S batteries has been reported only rarely. These results impressively revealed the outstanding high-power output performance of the Li–S batteries.

研究领域: 电化学 · 能源材料 · 纳米材料 · 储能技术 · 电池化学 · 材料科学 · 应用物理
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Nanoscale · 2018 ·Vol. 10 ·期 23 ·10999-11005 · IF 7.233

Three-dimensional sp2 carbon networks prepared by ultrahigh temperature treatment for ultrafast lithium–sulfur batteries

Chunping Ruan,Zhi Yang,Huagui Nie,Xuemei Zhou,Zeqing Guo,Lu Wang,Xingwei Ding,Xi'an Chen,Shaoming Huang

The current challenge in the development of high-performance lithium–sulfur (Li–S) batteries is to facilitate the redox kinetics of sulfur species as well as to suppress the shuttle effect of polysulfides, especially at high current rates. Herein, aiming the application of Li–S at high current rates, we coupled a sp2 carbon configuration consisting of 3D carbon nanotubes/graphene prepared by ultrahigh temperature treatment (2850 °C) with S (2850CNTs–Gra–S) for application in Li–S batteries. The 2850CNTs–Gra as the host material exhibits a nearly perfect sp2 hybridized structure because ultrahigh temperature treatment not only repairs the raw defects in CNTs and graphene, but it also forms new sp2 C–C bonds between them. The 3D sp2 carbon network ensures ultrafast ion/electron transfer and efficient heat dissipation to protect the integrity of the separator when the Li–S battery is running at an ultrahigh rate. Based on these unique advantages, the 2850CNTs–Gra–S cathode shows a high current rate performance. Critically, it still delivers a considerable specific capacity after 1500 cycles even at a current rate of 15C and exhibits an extremely low capacity degradation rate of 0.0087% per cycle.

研究领域: 电化学储能 · 材料科学 · 纳米碳材料 · 能源化学 · 电池技术
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Functional Materials Letters · 2024 · IF 1.2

Lignocellulose-based gel polymer electrolyte composited by a special additive of elemental sulfur with outstanding performances in lithium–sulfur batteries

Chao Zou,Yun Huang,Xingquan Wei,Amin Song,Wenhao Ren,Saisai Li,Junyuan Gan,Xing Li,Mingshan Wang,Yuanhua Lin

Gel polymer electrolyte (GPE) based on polymer matrix of lignocellulose and gelatinized potato starch is prepared, and elemental sulfur is introduced as an additive for the first time. The polymer matrix has shown excellent performances including liquid electrolyte uptake, tensile strength and thermal stability. The ionic conductivity and electrochemical stability window of the corresponding GPE are improved with the introduction of the elemental sulfur. Furthermore, the addition of elemental sulfur can be reduced into short-chain Li 2 S and Li 2 S 2 on the surface of lithium anode to further elevate the capacity of battery. Meanwhile, the short-chain Li 2 S and Li 2 S 2 in the solid electrolyte interphase (SEI) film on the surface of lithium metal can improve SEI’s mechanical properties and the interface compatibility between GPE and lithium metal. The multi-component synergistic effect of GPE provides the battery with superior cycle stability and excellent electrochemical performances. Bio-based GPE will exhibit a promising and alternative way for the practical application of lithium–sulfur batteries.

研究领域: 材料科学 · 电化学 · 储能技术 · 高分子科学 · 纳米技术
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Asia-Pacific Journal of Chemical Engineering · 2022 ·Vol. 17 ·期 5 ·e2790 · IF 1.777

Effect of chemical desulfurization on coal properties and sulfur structure based on microwave technology

Bingyi Zhou,Tao Ge,Xiaoman Luo,Zhaohui Wang,Yueyue Qiao,Chuanchuan Cai,Jingyao Xu

Under the two frequency microwave conditions of 915 and 2450 MHz, orthogonal tests were designed to investigate the effects of organic acid reagent, microwave irradiation time, and mixing time of additives and coal samples on the desulfurization effect of coal. Results show that the effect of irradiation time on the experimental desulfurization efficiency under frequency microwave conditions is large and is the main factor. The desulfurization effect under 915 MHz microwave condition is better than 2450 MHz microwave condition. Two sets of experimental optimal coal samples were used for characterization and analysis. Thermogravimetric analysis revealed that the combustion temperature range of the coal samples is shortened and the integrated combustion index is considerably higher after the microwave irradiation experiment. Fourier-transform infrared spectroscopy analysis showed that the overall chemical structure of the coal samples does not change significantly after the experimental treatment. X-ray photoelectron spectroscopy analysis showed that the intensity of organic sulfur in coal samples is weakened after microwave irradiation, the characteristic peaks of thiols and thioethers are reduced to a great extent, and an increase in the intensity of sulfoxide organic sulfur is observed. On the basis of the results of experimental analysis and quantum chemical simulation calculations, the mechanism of organosulfur structure removal under the action of microwave is revealed.

研究领域: 能源化学 · 煤化学 · 环境工程 · 材料科学 · 物理化学 · 分析化学 · 清洁燃料技术
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e-Journal of Surface Science and Nanotechnology · 2012 · IF 0

Controlled Synthesis of Calcium Sulfate and Calcium Vanadate Nanostructures

L. Z. Pei,Y. Q. Pei,Y. K. Xie,Z. Y. Cai

Calcium sulfate and calcium vanadate nanostructures have been synthesized by a hydrothermal route using calcium sulfate and sodium vanadate as the raw materials. The products were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and photoluminescence (PL) spectrum. XRD and SEM observation show that the products are composed of calcium sulfate nanosheets with orhorhombic CaSO4 phase and calcium vanadate nanorods with tetragonal CaV4O9 phase. The size and morphology of the products can be adjusted by controlling the hydrothermal conditions and raw materials. The size of calcium sulfate nanosheets and calcium vanadate nanorods increases obviously with increasing the hydrothermal temperature and reaction time. The formation process of the calcium sulfate and calcium vanadate nanostructures is also discussed. [DOI: 10.1380/ejssnt.2012.585]

研究领域: 无机化学 · 材料科学 · 纳米技术 · 固体化学 · 功能材料
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CRYSTENGCOMM · 2023 ·Vol. 25 ·期 19 ·2939-2945 · IF 3.1

Enhancing birefringence of non-π-conjugated sulfate systems through rare-earth metal-centered polyhedra

Jingdong Yan,Dongdong Chu,Fangfang Zhang,Zhihua Yang,Shilie Pan,Xueling Hou

By the introduction of trivalent rare-earth metal-centered polyhedra [LnO6F4] (Ln = La, Gd) into alkali metal sulfates, two novel sulfate fluorides, NaLn2(SO4)2F3 (Ln = La, Gd), were successfully synthesized via a high-temperature solution method in sealed quartz tubes. The two compounds are isomorphic and feature a structure composed of [LnO6F4] (Ln = La, Gd) polyhedra, [NaO4F3] polyhedra, and [SO4] groups. The UV-vis-NIR diffuse reflection spectra, infrared spectra, and thermal stability are also presented. Meanwhile, theoretical calculations reveal that NaLa2(SO4)2F3 has a moderate birefringence (0.041 at 1064 nm) which is significantly improved compared with Na2SO4. And the enhancement of birefringence can be ascribed to the introduction of rare-earth metal-centered polyhedra by a real space atom-cutting method. This work shows that the introduction of trivalent rare-earth metal-centered polyhedra is one of the effective strategies for bolstering the birefringence performance of non-π-conjugated sulfate systems.

研究领域: 材料科学 · 光学材料 · 无机化学
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CHINESE JOURNAL OF CHEMICAL ENGINEERING · 2016 · IF 1.207

Simultaneous desulfurization and denitrification of sintering flue gas via composite absorbent

Jie Wang,Wenqi Zhong

Experiments on simultaneous absorption of SO 2 and NO X from sintering flue gas via a composite absorbent NaClO 2 /NaClO were carried out. The effects of various operating parameters such as NaClO 2 concentration ( m s ), NaClO concentration ( m p ), molar ratio of NaClO 2 /NaClO ( M ), solution temperature ( T R ), initial solution pH, gas flow ( V g ) and inlet concentration of SO 2 ( C S ) and NO ( C N ) on the removal efficiencies of SO 2 and NO were discussed. The optimal experimental conditions were determined to be initial solution pH   =   6, T R   =   55   °C and M   =   1.3 under which the average efficiencies of desulfurization and denitrification could reach 99.7% and 90.8%, respectively. Moreover, according to the analysis of reaction products, it was found that adding NaClO to NaClO 2 aqueous solution is favorable for the generation of ClO 2 and Cl 2 which have significant effect on desulfurization and denitrification. Finally, engineering experiments were performed and obtained good results demonstrating that this method is practicable and promising.

研究领域: 环境工程 · 化学工程 · 能源技术 · 污染控制 · 工业生态学
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WATER SCIENCE AND TECHNOLOGY · 2022 ·Vol. 85 ·期 6 ·1813-1823 · IF 2.43

Heterogeneous activation of H2O2/Na2S2O8 with iron ore from water distribution networks for pollutant removal

Zhong Dan,He Fu,Ma Wencheng,Wu Yichuan,Dong Jiaju

In this study, we investigated using the main composition of pipe deposits from water distribution networks as catalyst to activate dual-oxidant H 2 O 2 /Na 2 S 2 O 8 system to produce radicals for perchloroethylene and chloramphenicol removal. According to the results, the degradation efficiency of perchloroethylene by H 2 O 2 /Na 2 S 2 O 8 system was 92.05% within 8 h. Due to the slow conversion between ≡Fe 3+ and ≡Fe 2+ , the hydroxylamine was introduced to reduce reaction time. As for the results, the degradation efficiency of chloramphenicol in the H 2 O 2 /Na 2 S 2 O 8 system with hydroxylamine assistance was 73.31% within 100 min. Meanwhile, several key affecting factors and the kinetic models were investigated. The primary radicals were identified by electron paramagnetic resonance and radical scavenging tests. Eleven degradation products were confirmed by high-resolution liquid chromatography-mass spectrometry. The result of this study provided the theoretical basis for resource utilization of pipe deposits in water treatment in case of emerging contamination events.

研究领域: 环境科学 · 水处理 · 材料化学
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Desalination and Water Treatment · 2024 · IF 1

Enhanced molybdenum (VI) adsorption by zirconia sol-modified nanoscale iron sulfide: performance, mechanism and influencing factors

Jian-jun Lian,Meng Wu,Hong-yan Wu,Yan-ting Liu,Qing Xu,Man-jun Miao,Jian-hua Yang,Ke-ke Mao,Bo Chen,Feng Xue,Qiao-ping Kong,Ming-hao Shang,Xiu-ling Li

The significant increase in demand for molybdenum (Mo) resources has led to excessive molybdate (Mo(VI)) content in water, posing a challenge to the innovation of Mo(VI) removal technology in water bodies. Nanoscale iron sulfide (FeS) has an important effect on the environmental behavior of Mo(VI) in aquatic solutions. To address the issue of easy agglomeration and poor stability of FeS, zirconia sol-modified nanoscale iron sulfide (Zr-FeS) was synthesized, and the adsorption behavior of Zr-FeS on Mo(VI) from diverse aquatic solutions was also investigated in this study. The results showed that the removal rate of Mo(VI) was increased from 28.60% to 78.32% within pH value of 7.0 when Zr/Fe molar ratio was elevated from 0 to 0.5. Moreover, the Mo(VI) adsorption efficiency by Zr-FeS was closely related to pH values, and acid conditions were beneficial for Mo(VI) adsorption. The pseudo-second-order model demonstrated a better fit to the data compared to other models. The maximum adsorption capacity of Zr-FeS towards Mo(VI) value calculated by Langmuir isotherm model was 118.48 mg/g at 298 K. The thermodynamic analysis revealed that the adsorption process of Mo(VI) was endothermic, entropically favorable, and spontaneous in nature. Competing anions (e.g., PO 4 3– , HCO 3 – , and SO 4 2– ) partially inhibited the adsorption process of Mo(VI) by Zr-FeS. While the process was less affected by dissolved oxygen and aging. The results of Fourier-transform infrared spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy, and density functional theory (DFT) calculations revealed that the main mechanisms for Mo(VI) removal were hydrogen bonding, electrostatic interaction and surface complexation. The high stability and fast adsorption rate indicated that Zr-FeS was a promising material to remove Mo(VI) from the aquatic solutions.

研究领域: 环境科学 · 材料科学 · 化学工程
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