Catalysts
·
2022
·Vol. 12
·期 11
·1435
·
IF 4.501
Fujian Yang,Cheng Yin,Mengqiao Zhang,Jiangwei Zhu,Xiuyuan Ai,Wenchao Shi,Guilong Peng
The activation of persulfate (PS) by Fe(III) for the removal of environmental organic pollutants was severely limited by the low reduction rate from Fe(III) to Fe(II). In present study, we reported that reducing sulfur species (i.e., SO32−, HSO3−, S2−, and HS−) under low concentration could significantly accelerate the Fe(III)/Fe(II) cycle in the Fe(III)/PS system. Under the condition of 1.0 mM Fe(III) and 4.0 mM PS, the removal performance of Fe(III)/PS system was poor, and only 21.6% of BPA was removed within 40 min. However, the degradation efficiency of BPA increased to 66.0%, 65.5%, 72.9% and 82.7% with the addition of 1.0 mM SO32−, HSO3−, S2−, and HS−, respectively. The degradation efficiency of BPA was highly dependent on solution pH and the concentration of reducing sulfur species. When the reductant was excessive, the removal efficiency would be significantly inhibited due to the elimination of reactive species. This study provided some valuable insights for the treatment of organic wastewater containing these inorganic reducing ions.Keywords:persulfate;reducing sulfur species;cycle;degradation
研究领域:
环境科学
·
化学
✓ 已验证
DOI
高影响因子
Journal of Sulfur Chemistry
·
2025
·
IF 1.6
Yongpeng Ma,Jianghui Du,Haobing Yan,Chaobin Shi
Molybdenum disulfide (MoS2) is considered a favorable absorbent for removing heavy metals. However, due to its various morphologies, MoS2 exhibits significant differences in its performance for removing mercury from flue gas. In the present study, the flower-like, spherical MoS2 and W-MoS2 were prepared by regulating the interlayer spacing and doping tungsten (W) in MoS2 for removing gaseous mercury (Hg0). The results show that the number of active sulfur sites (S2- and S22-) was critical to the adsorption performance of MoS2 for Hg0. The flower-like MoS2 demonstrated optimum properties below 125°C which attributed to the presence of dominated S2- sites, while spherical MoS2 and W-MoS2 showed a wider application temperature range (up to 175°C) during Hg0 removal which attributed to the unsaturated sulfur S22- and active oxygen. In terms of the mechanism, Hg0 is directly inserted into the Mo-S bond of MoS2 to form a transition state [Hg·Mo]-S, and then the original Mo-S is interrupted to form a new β-Hg-S bond, or combine with surface oxidation to form HgO. The oxygen in the flue gas can supplement the surface active oxygen on the MoS2, which enables the circulation of Mo5+. Hg0 also reacted with S22- to form α-HgS.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
ChemElectroChem
·
2020
·Vol. 8
·期 1
·90-95
·
IF 4.154
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
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Yahui Wang,Qihuang Huo,Huijun Chen,Yu Feng,Jiancheng Wang,Sheng Wang,Liping Chang,Weiren Bao
To develop the high value utilization of high organic sulfur coal instead of combustion as well as save the cost of mercury pollution control, we attempted to transmute the inherent sulfur of high organic sulfur coal, in the case of LF coal (which is from Linfen city, China), to active sulfur species for mercury capture by doping metal oxides, and CuO performed best among various metal oxides. The sorbent (or activated sample) prepared from LF coal with doping CuO is labelled LF+Cu-A, around which a series of experiments were conducted. Firstly, the effects of operational conditions, including GHSV (gas hourly space velocity), temperature and flue components, on the mercury capture performance of LF+Cu-A were thoroughly investigated, and results showed that LF+Cu-A had an excellent mercury capture performance. The average mercury capture efficiency is 97.8 % during a two-hour test under N 2 +O 2 +H 2 O+SO 2 +NO atmosphere with GHSV of 240000 h −1 and temperature of 120 °C. Secondly, the experimental data were fitted by four kinetic models, and it is found that the mercury adsorption process under low temperatures (60, 90, 120 °C) and high temperature (150 °C) are in the best agreement with the pseudo-first-order model and the intra-particle diffusion model respectively. Last, the mercury capture mechanisms of LF+Cu-A were revealed by Hg-TPD (Hg-temperature programed desorption) experiment, Raman analysis and XPS (X-ray photoelectron spectrometer) spectra, and it is indicated that the multiple sulfur species and Cu 2+ play roles in the mercury capture process, during which elemental mercury are oxidized to HgS and fixed on the surface of LF+Cu-A.
研究领域:
环境科学
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能源技术
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Qun Wang,Han Zeng,Youheng Liang,Ye Cao,Yang Xiao,Jun Ma
The heterogeneous catalyst Mackinawite (FeS) was applied to activate periodate (IO 4 − ) to degrade endocrine disruptors bisphenol AF (BPAF). This study investigated the influence of FeS dosage, periodate dosage, BPAF concentration, initial pH value and inorganic ions on BPAF degradation by FeS/IO 4 − system. The results showed that the BPAF was effectively degraded by FeS/IO 4 − system. The acidic pH exhibited higher efficiency in BPAF degradation compared with alkaline and neutral conditions. Furthermore, the BPAF degradation was dramatically promoted in the presence of Cl − and SO 4 2− , whereas CO 3 2− inhibited BPAF degradation. The radical scavenging tests and EPR indicated that singlet oxygen ( 1 O 2 ), superoxide radicals (O 2 − ) and SO 4 − were committed to the degradation of BPAF, among which O 2 − , 1 O 2 were predominant radicals. The separate experiments showed that Fe(Ⅱ) participated in the activation of periodate. Furthermore, the effects of sulfur species (including the S 2− , SO 3 2− ) on BPAF degradation by FeS/IO 4 − system were studied. The radical quenching tests suggested that S 2− and SO 3 2− were responsible for producing SO 4 − . The findings of this study elucidated an approach for the removal of micro-pollutants in the water environment through heterogeneous activation of periodate by FeS.
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Storage
·
2024
·
IF 8.9
Shuiping Cai,Hanyan Wu,Xuejie Gao,Xinyang Chen,Chen Cheng,Xiaofei Yang,Runcang Sun
Lithium‑sulfur batteries (LSBs) with high energy density (2600 Wh kg −1 ) have emerged as prominent candidates among current energy storage systems. However, their progress is hindered by serious shuttle effects, sluggish redox reaction kinetics, and volume expansion. Recently, flexible cellulose materials have shown promising results in inhibiting shuttles and mitigating volume expansion. Nevertheless, a significant gap exists between the practical delivered capacity and the theoretical capacity due to slow sulfur species conversion kinetics. Herein, H 3 PW 12 O 40 (PW 12 ) serves as a bidirectional electrocatalyst anchored on the flexible cellulose substrate, to enhance the conversion behavior of sulfur species and prevent the accumulation and deactivation of active sulfur. Additionally, cellulose acts as a self-supporting host, mitigating shuttling effects and slowing volume expansion, which improving the utilization rate of active substances. As a result, the LSBs assembled with synthetic cathodes (S/PW 12 &PDA@CL) delivered a high initial capacity of 1491 mAh g −1 at 0.1C, and a low-capacity attenuation of only 0.16 % per cycle after 300 cycles at 1.0C. Moreover, even at a high sulfur loading of 2.5 mg cm −2 , S/PW 12 &PDA@CL could still possess a high initial-discharge specific capacity of 1080.6 mAh g −1 at 1.0C and achieved >200 stable cycles.
研究领域:
材料科学
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能源存储技术
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL POLLUTION
·
2022
·
IF 9.988
Lulu Wang,Laihong Shen,Yuyang Long,Dongsheng Shen,Shouxi Jiang
Uncoupling chemical looping gasification (CLG), the organic sulfur evolution was simulated and explored qualitatively and quantitatively using typical sulfur compounds on TG-MS and temperature-programmed fixed bed. The HS radical in the reductive atmosphere easier converted to H 2 S and COS. H 2 O activated the evolution of S which was stably bonded to carbon, and H 2 generated from gasification and oxidation of reductive Fe by H 2 O contributed to the release of sulfur. The proportion of H 2 S released from sulfur compounds was greater than 87% in steam gasification, and more than 60% during CLG. Oxygen carriers promoted the conversion of sulfur to SO 2 in the mid-temperature region (500 °C–700 °C), and H 2 S in the high temperature region (700 °C–900 °C). Sulfur species played a pivotal role in sulfur evolution at low temperature of CLG. The organic sulfur in mercaptan and benzyl were more easily converted and escaped than in thiophene and phenyl . The thermal stability of sulfur species, the presence of steam and OC affected the initial temperature and peak concentration of gas sulfur release as well as sulfur distribution. Consequently, CLG strengthened the sulfur evolution, and made it possible to targeted restructure the distribution of sulfur by regulating process parameters, or blending fuel with different sulfur species for emission reduction, and selective conversion of sulfur.
研究领域:
能源科学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Wenjie Ma,Zhitao Shao,Jing Yao,Kaixin Zhao,Xinzhi Ma,Lili Wu,Xitian Zhang
The lithium sulfur (Li-S) battery is an active research area in the field of energy storage systems, but the shuttle effect is a serious obstacle hindering its application. Herein, a CoSe 2 /CoO Mott-Schottky catalyst is blended with carbon nanotubes (CNTs) and subsequently coated onto a commercial separator as a modifier, whereby the synergy between the high electrocatalytic activity of the CoSe 2 /CoO heterostructure and high conductivity of the CNTs selectively mediate the conversion of sulfur species. As a result, a cell with a CoSe 2 /CoO-CNTs modified separator displays a high initial discharge capacity of 1573 and 910 mAh/g at 0.1 and 2C, respectively. Furthermore, a low decay rate of 0.070% per cycle can be obtained over 500 cycles at 2C. The results of this study suggest that the as-prepared CoSe 2 /CoO-CNTs is an effective modifier that can improve the performance of Li-S batteries for use in next-generation energy storage systems. This study provides fundamental insights into the rational design of Mott-Schottky catalysts for practical high-performance Li-S batteries.
研究领域:
电化学
·
能源材料
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纳米材料
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催化化学
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储能技术
✓ 已验证
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2024
·
IF 4.1
Chuanxin Zong,Bo Hong,Furong Qin
Cell failure is easy occurring in Li-S cell. Electrolyte consumption caused by side-reactions between electrolyte and anode is one of the reasons for the cell failure, but the underlying mechanism for the cell failure is still not clear. To get insight into the electrolyte decomposition, in this work, online cell pressure tracking analysis (OCPTA) is applied to study the gassing effect caused by electrolyte decomposition reactions during charge–discharge processes and the study on depositing/stripping behavior of sulfur species performed. It is found that gassing effect is negligible in the cell with conventional ether-based electrolyte when electrolyte decomposing, but volume effect caused by sulfur species dissolution is notable. Together with the sulfur preferentially depositing on the top surface of cathode, it leads to electrolyte insufficiency on the top surface of electrodes, enhancing the risk of cell failure.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
JOURNAL OF PHYSICAL CHEMISTRY A
·
2020
·
IF 2.6
Tao Wang,Yangyang Liu,Yue Deng,Hanyun Cheng,Xiaozhong Fang,Liwu Zhang
The heterogeneous reaction of SO2 on manganese oxides is poorly understood. By means of in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), this study investigated the reaction kinetics and product fractions on four types of manganese oxides. Due to the positive and negative moisture impacts, 68% RH (relative humidity) becomes the most favorable condition for the uptake of SO2. Mn3O4 shows the greatest uptake capacity of SO2, followed by MnO2 and Mn2O3, with that of MnO being the weakest. Curve-fitting procedures were undertaken to further dissect the product spectra. Increased RH facilitates the physical adsorption of SO2 and generally weakens the oxidation capacity of manganese oxides. The oxidation ability is greatest for MnO, followed by MnO2 and Mn3O4, with that of Mn2O3 being the weakest. Additionally, the particle acidity (pH) was estimated by the ionization equilibrium of sulfurous acid and the relative contributions of S(IV) species. MnO and Mn3O4 become more acidic as RH increases while Mn2O3 and MnO2 are the most acidic at 50% RH, which can be attributed to the different uptake capacities of SO2 and H2O on each sample. Overall, for the heterogeneous reaction of SO2 on manganese oxides, both particle type and moisture condition influence the reaction kinetics and product fractions. This work improves the understanding of the heterogeneous process on atmospheric manganese-rich particles.
研究领域:
环境化学
·
大气科学
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表面化学
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气溶胶化学
·
物理化学
✓ 已验证
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2024
·
IF 8
Qian Wang,Wenting Zhang,Mingzhe Cai,Yafei Ma,Ajuan Yu,Sheng Chen,Shusheng Zhang
The reactive sulfur species (RSS), in particular Cys, Hcy , GSH, and H 2 S, play an essential role in lots of critical physiological and pathological processes. To elucidate their complex interrelationships in signaling and metabolic pathways, suitable molecular tools to simultaneously distinguish Cys, Hcy , GSH, and H 2 S are urgently needed. Herein, we developed a novel cascade reaction-assisted trinal-site fluorescent probe BCS by connecting three functional fragments for simultaneously distinguishing Cys, Hcy , GSH, and H 2 S. The probe BCS exhibited red fluorescence in the absence of the four biological RSS. However, with the attendance of Cys, Hcy , GSH, and H 2 S, the probe showed different fluorescence patterns, including blue, blue/red, green/red, and no fluorescence, respectively. More importantly, based on the different RSS-induced fluorescence patterns and multi-color fluorescence imaging, probe BCS was used to discriminate and visualize all four biological RSS in both HepG2 cells and zebrafish. It is expected that probe BCS will have applications in the diagnosis and research of RSS-related diseases in the future.
研究领域:
生物化学
·
分子生物学
·
医学诊断
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Xiaohong Wang,Longfei Kang,Tianjian Li,Shanshan Wang,Haibo Ma,Yajun Tian,Jianqiang Sun,Jun Li
The redox dynamics of estuarine sediments critically influence the environmental fate of antibiotics, yet the mechanistic pathways under oxygen-fluctuating conditions have been insufficiently elucidated. This study elucidates the dual-function role of pyrite in mediating the oxidative and reductive degradation of three model antibiotics (sulfamethoxazole, SMX; norfloxacin, NOR; and chlortetracycline, CTC) under aerobic and anaerobic conditions. Systematic batch experiments coupled with reactive oxygen species analysis reveal a dual-function mechanism for pyrite involving oxidative degradation via •OH under aerobic conditions and reductive transformation under anaerobic conditions. Notably, sulfur species in pyrite serve as key electron donors, driving the defluorination and dechlorination reactions of NOR and CTC in the absence of molecular oxygen. X-ray absorption fine structure along with density functional theory simulations further demonstrate an S–Fe-antibiotic electron transfer pathway, wherein sulfide donates electrons via Fe(II) coordination sites. Field validation using natural estuary sediments corroborates the laboratory findings, highlighting the substantial contribution of pyrite-mediated reductive pathways to antibiotic attenuation. These findings advance the mechanistic insight into pyrite-driven redox processes in estuarine environments and underscore the overlooked role of sulfur species in mediating nonradical antibiotic degradation, with implications for natural attenuation and remediation strategies in sulfur-rich coastal systems.
研究领域:
环境科学
·
海洋化学
·
地球化学
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药理学
·
污染控制
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）