JOURNAL OF POWER SOURCES
·
2015
·
IF 6.217
Sheng Liang,Chu Liang,Yang Xia,Haohui Xu,Hui Huang,Xinyong Tao,Yongping Gan,Wenkui Zhang
Lithium sulfide (Li 2 S) is regarded as a promising cathode material for lithium–sulfur (Li–S) batteries in terms of its high theoretical specific capacity of 1166 mAh g −1 and good compatibility with lithium metal-free anodes. However, Li 2 S suffers from poor cycling stability and rate capability resulted from the serious shuttle effect of lithium polysulfides and its low electronic and ionic conductivity . Here, we present a facile ball milling combined with carbon coating method to synthesize porous carbon-coated Li 2 S (Li 2 S@C) composites with a high Li 2 S content by using polystyrene (PS) as a carbon precursor. The Li 2 S@C composites show a high reversible specific capacity of 676 mAh g −1 (equal to 971 mAh g −1 sulfur) after 3 cycles at the current density of 0.1 A g −1 , superior cycling stability with an average decay rate of 0.18% per cycle over 200 cycles, and improved rate capability of 416 mAh g −1 at the current density of 1.0 A g −1 . The enhanced electrochemical properties of Li 2 S can be attributed to the porosity and core–shell structure of the Li 2 S@C composites, which increased the electronic and ionic conductivity of Li 2 S and alleviated the shuttle effect of intermediate lithium polysulfides in the discharge/charge process.
研究领域:
材料科学
·
电化学
·
能源存储
·
纳米材料
·
功能材料
✓ 已验证
DOI
高影响因子
JOURNAL OF ORGANIC CHEMISTRY
·
2020
·
IF 4.335
Shimin Xie,Lebin Su,Min Mo,Wang Zhou,Yongbo Zhou,Jianyu Dong
An alternative thioesterification reaction via copper-catalyzed oxidative coupling of readily available aroylhydrazides with disulfides is developed, in which oxidative expulsion of N2 overcomes the activation barrier between the carboxylic acid derivatives and the products. The reaction produces various thioesters in good to excellent yields with good functional group tolerance. In the reaction, stable and easily available aroylhydrazides are used as acyl sources and the relatively odorless disulfides are used as S sources. Mechanistic investigations demonstrate that the reaction of copper salt and oxidant (NH4)2S2O8 allows for achievement of tandem processes, including deprotonation, free-radical-mediated denitrogenation, and C–S bond formation.
研究领域:
有机化学
·
催化反应
✓ 已验证
DOI
高影响因子
ENERGY & FUELS
·
2020
·
IF 3.421
Jiatao Xiang,Zhen Zhang,Luning Tian,Qinghua Zhao,Haiping Yang,Xiong Zhang,Jingai Shao,Shihong Zhang,Hanping Chen
In order to enhance wet flue gas desulfurization efficiency and reduce cost, the effects of different series of additives (typical organic acids, organic salts, inorganic salts, organic amines, and their mixture) on the desulfurization properties, including pH buffering characteristics of slurry, dissolution characteristics of CaCO3, oxidation characteristics of CaSO3, desulfurization efficiency, and economic cost were investigated in this work. The results show that the pH buffering capacity is sodium benzoate ≈ Na2SO4 > adipic acid > double oxazine. The dissolution promoting effect of CaCO3 is acetic acid > double oxazine ≈ sodium acetate > MgSO4. The additives that can significantly promote the oxidation of CaSO3 are adipic acid, citric acid, acetic acid, MgSO4, and Na2SO4. Without an additive, the desulfurization efficiency of CaCO3 slurry decreased to 85.87% after 4 h. After the addition of the composite additive (CA-3), the desulfurization efficiency of CaCO3 slurry remained 96.53% for 4 h, increasing by 10.66%. The main reasons for the enhancement in the desulfurization process may be a collection of three factors: the reversible hydrolysis reactions of acetic acid and sodium acetate, the formation of an acid–base conjugate system by sodium benzoate, and the formation of a neutral ion pair MgSO3 by MgSO4 in the slurry. In addition, the composite additive has been used in the Dabie mountain power plant of China. The economic benefit analysis shows that the desulfurization unit of 4 × 640 MW coal-fired power plant can save 1.26 million dollars per year by composite additive.
研究领域:
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Fuming Lai,Renjing Duan,Xiaoshi Lang,Tan Wang,Tingting Qu,Lan Li,Qinzhi Lai,Kedi Cai
Lithium-sulfur batteries are considered a favourable contender for next-generation energy storage systems owing to their high energy density (2600 Wh·kg −1 ). However, the severe "shuttle effect" of polysulfides and the slow redox kinetics involving phase transitions have seriously limited the commercialization of lithium-sulfur batteries. On this basis, in this paper, a type of nanoflower structure rare-earth lanthanum ion (La 3+ ) doping Sn 3 O 4 with a large number of catalytic active interfaces is designed via a facile one-step hydrothermal method. When serves as a capture centre to immobilize polysulfides, it exhibits a strong chemical adsorption capacity. Moreover, due to the unique 4 f electron configuration of the rare-earth elements, nanoflower structure La 3+ doping Sn 3 O 4 (La@Sn 3 O 4 ) as sulfur-wrapped matrix has a strong catalytic activity, which can effectively accelerate the conversion process of polysulfides. At the same time, the catalytic mechanism of La@Sn 3 O 4 /S composite cathode material targeting the solid to liquid phase transformation of polysulfides is effectively revealed via in-situ Raman spectroscopy test and the initial discharge capacity can reach 1429.6 mAh·g −1 at a current density of 0.1 C, and the capacity retention rate is 76.5 % after 130 cycles.
研究领域:
材料科学
·
能源存储技术
✓ 已验证
DOI
高影响因子
WATER RESEARCH
·
2015
·
IF 5.528
Kuo Liu,Junhe Lu,Yuefei Ji
Formation of halogenated disinfection by-products (DBPs) in sulfate radical ( SO 4 − ) based oxidation processes attracted considerable attention recently. However, the underlying reaction pathways have not been well explored. This study focused on the transformation of Br − in cobalt activated peroxymonosulfate (Co 2+ /PMS) oxidation process. Phenol was added as a model compound to mimic the reactivity of natural organic matter (NOM). It was revealed that Br − was efficiently transformed to reactive bromine species (RBS) including free bromine and bromine radicals (Br , Br 2 − , etc.) in Co 2+ /PMS system. SO 4 − played a principal role during this process. RBS thus generated resulted in the bromination of phenol and formation brominated DBPs (Br-DBPs) including bromoform and bromoacetic acids, during which brominated phenols were detected as the intermediates. Br-DBPs were further degraded by excessive SO 4 − and transformed to bromate ultimately. Free bromine was also formed in the absence of Co 2+ , suggesting Br − could be oxidized by PMS per se . Free bromine was incorporated to phenol sequentially leading to Br-DBPs as well. However, Br-DBPs could not be further transformed in the absence of SO 4 − . This is the first study that elucidated the comprehensive transformation map of Br − in PMS oxidation systems, which should be taken into consideration when PMS was applied to eliminate contamination in real practice.
研究领域:
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Jingru Li,Sufu Liu,Yongliang Cui,Shengzhao Zhang,Xianzhang Wu,Jiayuan Xiang,Min Li,Xiuli Wang,Xinhui Xia,Changdong Gu,Jiangping Tu
Uncontrollable dendrite growth and low Coulombic efficiency are the two main obstacles that hinder the application of rechargeable Li metal batteries. Here, an optimized amount of potassium hexafluorophosphate (KPF6, 0.01 M) has been added into the 2 M LiTFSI/ether-based electrolyte to improve the cycling stability of lithium–sulfur (Li–S) batteries. Due to the synergistic effect of self-healing electrostatic shield effect from K+ cations and the LiF-rich solid electrolyte interphases derived from PF6– anions, the KPF6 additive enables a high Li Coulombic efficiency of 98.8% (1 mA cm–2 of 1 mAh cm–2). The symmetrical Li cell can achieve a stable cycling performance for over 200 cycles under a high Li utilization up to 33.3%. Meanwhile, the polysulfide shuttle has been restrained due to the higher concentration of the LiTFSI in the electrolyte. As a result, the assembled Li–S full cell displays excellent capacity retention with only 0.25% decay per cycle in the final electrolyte. Our work offers a smart approach to improve both the anode and cathode performance by the electrolyte modification of rechargeable Li–S batteries.
研究领域:
电化学
·
材料科学
✓ 已验证
DOI
高影响因子
WATER SCIENCE AND TECHNOLOGY
·
2022
·Vol. 86
·期 8
·1876-1886
·
IF 2.43
Qin Yingzhi,Zhang Xin,Yuan Guang-En
In this study, low concentration of ferrous ions (Fe 2+ ) was added into natural molybdenite (MDN) activated peroxymonosulfate (PMS) process to degrade a typical azo dye, orange G (OG). It was found that the addition of Fe 2+ promoted OG degradation and simultaneously reduced the leaching of toxic Mo ions significantly. Further, the utilization efficiency of MDN was improved immensely, which was estimated from reuse experiment. MDN mainly acted as the reductant to promote cycling of Fe 3+ /Fe 2+ redox couple through reducible sulfur and Mo(IV) on its surface. Sulfate radicals (SO 4 •- ), hydroxyl radical (•OH) and singlet oxygen ( 1 O 2 ) were verified as the main reactive oxygen species responsible for OG degradation by scavenging tests and electron paramagnetic resonance. Some experiment parameters, such as MDN dosage, Fe 2+ concentration, PMS concentration, initial solution pH and coexisting anion, all affected OG degradation efficiency. In a word, this work provides a new method of enhancing PMS activation by MDN using low concentration of Fe 2+ for degradation of organic pollutants in water. MDN was applied as an efficient co-catalyst for permonosulfate activation. The sulfur element on MDN surface was able to reduce generated Fe 3+ . , , and were responsible for the removal of OG in MDN/Fe 2+ /PMS system. The Fe 2+ was demonstrated to promote the reusability of MDN.
研究领域:
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
Materials Today Energy
·
2024
·
IF 9
Yawei Guo,Weijing Zuo,Xiangkun Wu,Lan Zhang
Sulfurized polyacrylonitrile (SPAN) is a promising cathode material for long-life lithium-sulfur batteries (LSBs) due to its enhanced electronic conductivity as well as the eliminated shuttle effect. However, the uncontrollable lithium dendrite issue as well as slow kinetics of thick electrodes still hinders its practical application. Herein, an in situ polymerized electrolyte (PGE) based on vinyl carbonate and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) is designed and prepared to enhance the plating/stripping stability of the metal lithium while ensuring the cathode/electrolyte interfacial ion transportation. The optimized electrolyte, PGE-D, shows a satisfying ionic conductivity of 0.46 mS/cm at 25 °C; in the meantime, the polymer matrix hinders the diffusion of TFSI − anion and results in a high Li + transference number ( t L i + ) of 0.73. Benefiting from the high affinity of the flowable PGE precursor to the thick SPAN cathode as well as enhanced lithium compatibility, the Li||SPAN battery with high areal loading of 14.1 mg/cm 2 exhibits a high reversible specific capacity of 556.5 mAh/g and retains 76.3% of its capacity after 90 cycles.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Liang-Liang Zhang,Kai-Xuan Yang,Cai-Long Xue,Wan-Xi Li,Bo-Qiong Li,Yi-En Du,Yong-Qiang Chen,Ya-Jie Liu
The design of an active and sulfur-resistant catalyst for dibenzothiophene (DBT) hydrodesulfurization (HDS) in crude oil purification is highly desirable but remains a grand challenge. Here, two carbon-supported cobalt phosphide catalysts Co 2 P/C and CoP/C, and a reference sample Co/C are successfully synthesized using a metal–organic-frameworks (MOFs) precursor. A P/Co ratio dependence on crystal phases is found, leading to the formation of two pure-phase cobalt phosphide catalysts CoP/C and Co 2 P/C. Catalyst evaluation in HDS of DBT shows that the CoP/C catalyst exhibits a higher activity and stability than Co 2 P/C and Co/C, giving a 93.7 % DBT conversion with 100 h stability under 3 MPa and 380 ◦C. Moreover, a 67.4 % biphenyl yield characterizes the dominance of the direct desulfurization (DDS) pathway. The obtained catalytic performance over the CoP/C catalyst is also superior to the published cobalt phosphide catalysts. Multiple characterization techniques co-evidence that the copious specific surface area, efficient electron transport from Co to P, high thermal stability of Co nanoparticles (NPs), and strong sulfur resistance account for the enhanced catalytic performance of CoP/C. The findings of this report suggest that phosphorus-modified cobalt over the carbon support can act as a promising catalyst for the HDS of DBT.
研究领域:
催化化学
·
能源材料科学
✓ 已验证
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2014
·
IF 4.086
Yaohui Qu,Zhian Zhang,Xiahui Zhang,Guodong Ren,Xiwen Wang,Yanqing Lai,Yexiang Liu,Jie Li
Sulfur has a high specific capacity of 1675 mAh g −1 as lithium battery cathode, but its rapid capacity fading due to polysulfides dissolution presents a significant challenge for practical applications. Here we report a novel hierarchical porous honeycomb carbon (HPHC) for lithium-sulfur battery cathode with effective trapping of polysulfides. The HPHC was prepared by a simple template process, and a sulfur-carbon composite based on HPHC was synthesized for lithium-sulfur batteries by a melt-diffusion method. It is found that the elemental sulfur was dispersed inside the three-dimensionally hierarchical pores of HPHC based on the analyses. Electrochemical tests reveal that the sulfur-HPHC composite shows high rate capability and long cycling stability as cathode materials. The sulfur-HPHC composite with sulfur content of 66.3 wt% displays an initial discharge capacity of 923 mAh g −1 and a reversible discharge capacity of 564 mAh g −1 after 100 cycles at 2 C charge-discharge rate. In particular, the sulfur-HPHC composite presents a long term cycling stability up to 300 cycles at 1.5 C. The results illustrate that the electrochemical reaction constrained inside the interconnected macro/meso/micropores of HPHC would be the dominant factor for the excellent high rate capability and long cycling stability of the sulfur cathode, and the three-dimensionally honeycomb carbon network would be a promising carbon matrix structure for lithium-sulfur battery cathode.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES
·
2024
·Vol. 129
·期 3
·e2023JD040017
·
IF 3.8
Yangyang Liu,Tao Wang,Qiuyue Ge,Wenbo You,Kejian Li,Wei Wang,Lifang Xie,Longqian Wang,Xiaozhong Fang,Xuejun Ruan,Le Yang,Runbo Wang,Liwu Zhang
Carbonate radical anion ( C O 3 . − ${\mathrm{C}{\mathrm{O}}_{3}}^{.-}$ ) is generally overlooked in atmospheric chemistry. Our recent work emphasizes the important role of carbonate radicals produced on mineral dust surfaces in fast sulfate production under solar irradiation in the presence of CO 2 at specifically low RH and light intensity. Yet so far how C O 3 . − ${\mathrm{C}{\mathrm{O}}_{3}}^{.-}$ involves and affects secondary sulfate production under diverse RH, light intensity, and complex constituent matrix remains unknown, which essentially limits our comprehensive knowledge of C O 3 . − ${\mathrm{C}{\mathrm{O}}_{3}}^{.-}$ initiated SO 2 oxidation scheme in the atmosphere. Herein, we explored the heterogeneous SO 2 oxidation over both model and authentic dust and clays in the presence of CO 2 at atmospheric relevant RHs and light intensities. Interestingly, we observe that CO 2 promotes sulfate yield over authentic dust and clays at atmospheric-relevant RH and light intensity. This observation relates to the favorable kinetic between SO 2 oxidation and C O 3 . − ${\mathrm{C}{\mathrm{O}}_{3}}^{.-}$ while auto-quenching of these radical ions is largely minimized due to the sufficient sites of crustal constituents. Furthermore, employing a suite of authentic dust and machine learning strategies, we evaluated the relative importance of each constituent within airborne minerals or clays as well as environmental conditions including relative humidity, light intensity, and CO 2 concentration in affecting SO 2 uptake capability. On this basis, sulfate formation mediated by dust-driven pathway, accounting for nearly ∼20.9% of overall contribution by the end of this century during some pollution episodes, even higher than gas-phase · OH $\cdot \text{OH}$ (∼16.9%), will be increased by 163% if CO 2 -initiated SO 2 oxidation scheme is incorporated. Key Points Carbonate radical-initiated SO 2 heterogeneous oxidation is sensitive to RH, CO 2 concentration, light intensity, and dust constituents Carbonate radicals promote atmospheric sulfate production on authentic dust and clay particles at haze-relevant conditions This previously unrecognized scheme will account for ∼20.9% of overall atmospheric sulfate formation by the end of this century Plain Language Summary How carbonate radical ions involve and affect sulfate formation under different RHs, light intensities, and complex component matrices remains an open question. Secondary sulfate production is facilitated by C O 3 . − ${\mathrm{C}{\mathrm{O}}_{3}}^{.-}$ over authentic dust particles in atmospheric relevant RH and light intensity. More importantly, this research emphasizes that CO 2 is not an inert greenhouse gas that rarely participates in atmospheric chemistry but a strong oxidant precursor that will produce C O 3 . − ${\mathrm{C}{\mathrm{O}}_{3}}^{.-}$ and subsequently trigger quick SO 2 oxidation via chain reactions. This dust-driven reaction channel mediated by C O 3 . − ${\mathrm{C}{\mathrm{O}}_{3}}^{.-}$ potentially contributes to nearly ∼1/5 of secondary sulfate production during some pollution hours if the growing intensive anthropogenic activities continue.
研究领域:
大气化学
·
环境科学
✓ 已验证
DOI
高影响因子
Journal of Energy Chemistry
·
2024
·
IF 14
Lei Ding,Dandan Li,Sihang Zhang,Zhaoyang Wang,Pengfang Zhang,Fanghui Du,Shuyue Zhao,Daoxin Zhang,Feng Yang,Shuo Zhang
Lithium-sulfur (Li-S) batteries with attractive capacity give remarkable potential for prospective high-capacity application scenarios but suffer a fatal flaw of short cyclability before large-scale commercialization especially owing to polysulfide (Li 2 S n ) transmembrane shuttling. To efficiently restrain chronic Li 2 S n shuttle and expedite Li + transfer, herein, a novel electriferous charge-mosaic S(TMC@Lys-Li) separator preparation approach is recommended. Interfacial polymerizations of lithiated lysine and trimesoyl chloride establish an electriferous charge-mosaic polyamide functional layer. Substituted Li within the charge-mosaic layer offers transition or replacement sites for smoothing Li + migrations, which constructs efficient Li + fast-transfer private channels and accelerates the Li + transfer rate to 9.4 times. Negatively charged polyamide skeleton synchronously heightens Li 2 S n rejections by combining Donnan and steric effects. S(TMC@Lys-Li) replenishes Li for homogenizing Li nucleation and growth, endowing stable plating/stripping behaviors over 250 cycles for Li-Cu batteries. Assembled Li-S cells thus exhibit excellent specific capacity and cyclability at multiple application scenarios such as long periods, high areal capacity, and fast charge, holding 78.1% retention after 500 cycles at 1 C. The superior thermal stability and self-discharge of S(TMC@Lys-Li) dramatically strengthen battery thermal runaway resistance even at 155 ℃, which ensures security for Li-S battery high-power and high-temperature operations. Above alluring features enable charge-mosaic separators to be potentially adopted in practical Li-S batteries demanding strict security, high-capacity density, and fast charge technology.
研究领域:
材料科学
·
能源存储技术
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）