CELLULOSE
·
2019
·Vol. 27
·期 3
·1451-1463
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IF 3.917
Zhou Lipeng,Gao Dongting,Yang Jingru,Yang Xiaomei,Su Yunlai,Lu Tianliang
Abstract Conversion of cellulose to chemicals is an economic and environmental route for biomass utilization. In this work, efficient conversion of cellulose to alkyl levulinates and levulinic acid was realized by oxidation pretreatment combined with alcoholysis over Al 2 (SO 4 ) 3 catalyst. Proper pre-oxidation conditions including oxidation temperature and time are important. By pre-oxidation, part of hydroxymethyl groups on cellulose was converted to carboxyl groups which provide the Brønsted acid sites near the glycosidic bonds to improve the depolymerization of cellulose to monosaccharide. Al 2 (SO 4 ) 3 ·18H 2 O can play both Brønsted and Lewis acid roles in methanol and catalyze the conversion of monosaccharide to alkyl levulinates and levulinic acid. After pre-oxidation at optimized conditions, cellulose can be converted into methyl levulinate and levulinic acid over Al 2 (SO 4 ) 3 in methanol efficiently, and total yield of methyl levulinate and levulinic acid can reach 66.8% at 180 °C for 3 h. Furthermore, the simple and cheap Al 2 (SO 4 ) 3 catalyst is recyclable which is important for the practical application. Graphic abstract
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Nano Energy
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2024
·
IF 16.8
Changyu Liu,Kean Chen,Fumin Li,Along Zhao,Zhongxue Chen,Yongjin Fang,Yuliang Cao
Polyanion-type Fe-based sulfates are one of the most promising cathode candidates for sodium-ion batteries (SIBs) due to the low cost and high voltage. However, their practical application is still hindered by the poor air stability. Herein, we report a novel anion-doped Na 2.9 Fe 1.7 (SO 4 ) 2.7 (PO 4 ) 0.3 cathode material with higher air stability and faster ion/electron transport kinetics compared to pristine Na 2.6 Fe 1.7 (SO 4 ) 3 cathode as evidenced by first-principles calculations. The obtained Na 2.9 Fe 1.7 (SO 4 ) 2.7 (PO 4 ) 0.3 not only manifests a high discharge capacity of 100.4 mAh g −1 with an operating voltage of ∼3.57 V (Na + /Na), but also exhibits excellent rate performance (∼86.7 mAh g −1 at 30 C) and cycle stability over 6000 cycles (capacity retention of 76.3%). Particularly, Na 2.9 Fe 1.7 (SO 4 ) 2.7 (PO 4 ) 0.3 cathode still maintain its original crystal structural and sodium-storage property after exposure to air for one week. The high-voltage, long-life, and air-stable Na 2.9 Fe 1.7 (SO 4 ) 2.7 (PO 4 ) 0.3 could be a competitive cathode candidate for low-cost sodium-ion batteries.
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CHEMICAL ENGINEERING JOURNAL
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2014
·
IF 4.058
Liang Xiao,Ya Xiong,Shuanghong Tian,Chun He,Qingxian Su,Zhanhao Wen
A coordination supramolecular polymer, [Cu(bipy)(SO 4 )] n , was prepared as an adsorbent. It has a molecular structure of one-dimensional chain with dense adsorption sites. Three divalent dyes including Congo red, Orange G and Reactive Brilliant red X-3B were tested as pollutants in the adsorption study. The adsorbent showed extraordinary adsorption capacity for all three dyes, reaching 2429 mg/g, 915 mg/g and 1333 mg/g for Congo red, Reactive Brilliant red X-3B and Orange G, respectively. The Langmuir isotherm model can well describe the adsorption isotherm. In kinetic study, all of the three dyes presented a model of pseudo second-order. According to the kinetic rate constants, the adsorption processes are very fast and different for three dyes. The difference can be attributed to the divalent character and the different structure of the dye’s molecule. Based on their discrepancy of adsorption velocity, separation of dyes was attempted through kinetic separation between Congo red and X-3B. A separation coefficient was developed, which can well describe the separation performance results. The results show that the two dyes can be separated quickly and efficiently by [Cu(bipy)(SO 4 )] n .
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Journal of Materials Chemistry A
·
2025
·Vol. 13
·期 35
·29450-29460
·
IF 9.5
Yushen Qian,Mengxue Wu,Anyu Hu,Honghao Deng,Nawal K. Almaymoni,Abdullah N. Alodhayb,Jie Li,Jiahong Pan,Ping Chen,Zhicong Shi
Sodium iron sulfate (Na2+2xFe2−x(SO4)3, NFS) is a promising cathode material for sodium-ion batteries (SIBs) for large-scale energy storage systems due to its low cost and long life. However, NFS is an insulator and cannot reversibly store sodium ions to a large extent. To address this problem, an NFS material integrated with carbon nanotubes (CNTs) is developed in this work. The incorporation of CNTs effectively converts NFS from an insulator to a semiconductor, thereby significantly enhancing the electrochemical performance. The NFS@CNTs material incorporates an alluaudite-type framework that improves electronic conductivity, thereby enhancing rate capability and cycling life. By introducing 10 wt% CNTs, the NFS@CNTs composite achieves a high working voltage of 3.8 V (vs. Na/Na+) and an impressive high-rate specific capacity of 80 mA h g−1 at a rate of 20C. Furthermore, it can retain 81.4% of the initial specific capacity after 20 000 cycles at a rate of 50C, demonstrating an outstanding cycling stability. This work not only provides an in-depth understanding of the potential of NES to be used as a high-rate, long-lasting cathode material for SIBs but also lays the foundation for SIBs in large-scale energy storage applications.
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JOURNAL OF HAZARDOUS MATERIALS
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2020
·
IF 9.038
Tiantian Chen,Zhenyang Yu,Ting Xu,Rong Xiao,Wenhai Chu,Daqiang Yin
Sulfate radical (SO 4 ·- )-based advanced oxidation processes (AOPs) attract increasing attention in the control of micropollutants. However, SO 4 ·- can react with other chemicals present in water and result in undesired oxidation by-products (OBPs) generation. The formation and degradation mechanisms of CX 3 R-type OBPs during cobalt catalyzed peroxymonosulfate (Co 2+ /PMS) oxidation were investigated. In the formation of CX 3 R-type OBPs, both Co 3+ and SO 4 ·- could convert chloride to free chlorine that then reacted with natural organic matter, leading to the formation of CX 3 R-type OBPs. The concentrations of trichloromethane, chloral hydrate, dichloroacetonitrile, dichloroacetamide and trichloroacetamide after 15 min reaction were 9.8, 3.9, 1.2, 5.9 and 22.3 nM, respectively. Compared to SO 4 ·- , Co 3+ played a more significant role in the CX 3 R-type OBP formation and calculated toxicity values of CX 3 R-type OBPs. CX 3 R-type OBPs could not only be formed but also be degraded at the same time during Co 2+ /PMS oxidation. As for the degradation of CX 3 R-type OBPs, both Co 3+ and SO 4 ·- could transform CX 3 R-type OBPs to chloride. Compared to Co 3+ , SO 4 ·- played a more important role in the degradation of CX 3 R-type OBPs and the conversion from chloride to final by-product chlorate. The adverse effects that results from Co 3+ need more attention in SO 4 ·- -based AOPs application.
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ELECTROCHIMICA ACTA
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2016
·
IF 4.803
Zhen Liu,Huajun Zhou,Simon S. Ang,Jian-Jun Zhang
Here we report the evaluation of natrochalcite (Na[Cu 2 (OH)(H 2 O)(SO 4 ) 2 ]), an anionic layered structure [Cu 2 (OH)(H 2 O)(SO 4 ) 2 ] − charge-balanced by Na + , as an anode material for both Li- and Na-ion batteries. It delivers 224 mAh/g and 175 mAh/g in the first discharge in the Li + - and Na + -cells respectively, and decomposes to form amorphous matrixes during this step. In the subsequent charge, the original layered structure is unusually partially recrystallized back from the matrixes, resulting in 53 mAh/g and 35 mAh/g discharge capacities in the second discharge respectively. In subsequent cycling, Li + in the electrolyte is found to replace the original Na + during cycling in the Li + -cell and the electrode in the Li + -cell demonstrates better capacity retention rates than that in the Na + -cell, possibly due to Li + being smaller than Na + and thus decomposition-recrystallization cycles being more reversible during cycling in the Li + -cell.
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Metals
·
2024
·Vol. 14
·期 10
·1142
·
IF 2.6
Jiabao Li,Yang Cai,Jianling Huang,Shiqian Zhao,Deliang Cheng
Mg-based alloy anodes suffer from severe corrosion in alkaline electrolytes, which substantially impedes their cycle life and thereby limits their suitability as anode materials for nickel–metal hydride (Ni-MH) batteries. This work modifies the conventional 6 M KOH electrolyte by adding 0.1 M Al2(SO4)3·18H2O. The electrochemical hydrogen storage properties of Mg0.45Ti0.05Ni0.50alloy in this electrolyte and its microstructural evolution during cycling are studied. In the 6 M KOH + 0.1 M Al2(SO4)3·18H2O electrolyte, a protective layer consisting of Mg2Al(OH)7is formed on the surface of the Mg0.45Ti0.05Ni0.50alloy anode during charge/discharge cycling instead of Mg(OH)2, effectively preventing further corrosion and improving its cycle life. The Mg0.45Ti0.05Ni0.50alloy anode delivers a maximum discharge capacity of 479.0 mAh g−1and maintains 318.4 mAh g−1after 30 cycles in the 6 M KOH + 0.1 M Al2(SO4)3·18H2O electrolyte, which is significantly superior to that achieved in the 6 M KOH electrolyte (471.1 mAh g−1and 201.8 mAh g−1, respectively). This work provides a new strategy for improving the cycle stability of Mg-based alloy anodes.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Yujiao An,Xiaowan Li,Zihao Liu,Zhilan Wang,Xiaoquan Lu
Quinones, widely considered as environmental pollutants in wastewater, have been identified as redox-active substances capable of activating persulfate for decontamination purpose. However, the mechanism of peroxydisulfate (PDS) activation by quinones under alkaline conditions remains elusive. In this study, methyl- p -benzoquinone (MBQ) was chosen as a model quinone to elucidate the intrinsic mechanism of activating PDS. The results showed that MBQ/PDS system can effectively degrade atrazine (ATZ) under alkaline conditions (especially at pH 10.5) and achieve simultaneous removal of MBQ. Derivatization analysis, quenching experiments and electron spin resonance tests revealed that the self-transformation product of MBQ, methyl-semiquinone radical (MSQ − ), played a major role in activating PDS while alkali served as an auxiliary activator. Specifically, MSQ − functioned as a mediator in PDS activation, regulating the generation of sulfate radical (SO 4 − ) and hydroxyl radical ( OH), thereby inducing the degradation of ATZ through free radical pathways. Two degradation pathways of ATZ were proposed based on UPLC-Q-TOF-MS analysis and DFT calculation. ECOSAR evaluation indicated MBQ/PDS system can detoxify ATZ, yet it remains imperative to concern the formation of more toxic by-products. Furthermore, MBQ/PDS system exhibited strong resistance to water matrixes (excluding Cl − ) and favorable degradation capabilities towards diverse contaminants. This work broadened the possibility of applying the persulfate system in actual water bodies with alkaline environments, achieving the dual benefit of degrading target contaminants and simultaneously removing the activator quinones themselves, providing a novel “treating pollution with waste” water treatment strategy.
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Energy Technology
·
2024
·
IF 3.6
Dongyin Niu,Tiantian Zhang,Xuedan Zhang,Yufei Tan,Lukai Zhai
Under the background of vigorously promoting clean heating, the introduction of phase-change energy storage technology into heating systems has become a new hot issue. In this study, a novel KAl(SO 4 ) 2 ·12H 2 O/expanded graphite (EG) shape-stabilized composite phase-change material (PCM), with a melting temperature of 91.6 °C, latent heat of 245.7 kJ kg −1 , and high heat conductivity of 2.07 W m −1 K −1 , is prepared to manufacture a PCM-based module for space heating. This phase-change electric heating module is developed, and its heat storage and release characteristics are investigated through experimental and numerical studies. The numerical model is validated by experimental results. In view of the numerical simulation, the structure of the module is optimized and its thermal performance is studied. Based on the optimized module, a peak-valley time-of-use (TOU) electric heating module is finally proposed. It is revealed that the module exhibits good thermal performance and is capable of satisfying the indoor heating demand. The effective heat storage and release duration is 8.12 and 15.34 h, which can perfectly realize the operating mode under the “peak-valley TOU electricity” mechanism. In this study, it is demonstrated that peak–valley electric energy storage heating devices have broad prospects in building space heating and provides reference for future application.
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Science Bulletin
·
2023
·
IF 18.9
Along Zhao,Fangjie Ji,Changyu Liu,Shihao Zhang,Kean Chen,Weihua Chen,Xiangming Feng,Faping Zhong,Xinping Ai,Hanxi Yang,Yongjin Fang,Yuliang Cao
Fe-based polyanionic sulfate materials are one of the most promising candidates for large-scale applications in sodium-ion batteries due to their low cost and excellent electrochemical performance. Although great achievements have been gained on a series of Na 6−2 x Fe x (SO 4 ) 3 (NFSO- x , 1.5 ≤ x ≤ 2.0) materials such as Na 2 Fe 2 (SO 4 ) 3 , Na 2 Fe 1.5 (SO 4 ) 3 , and Na 2.4 Fe 1.8 (SO 4 ) 3 for sodium storage, the phase and structure characteristics on these NFSO- x are still controversial, making it difficult to achieve phase-pure materials with optimal electrochemical properties. Herein, six NFSO- x samples with varied x are investigated via both experimental methods and density functional theory calculations to analyze the phase and structure properties. It reveals that a pure phase exists in the 1.6 ≤ x ≤ 1.7 region of the NFSO- x , and part of Na ions tend to occupy Fe sites to form more stable frameworks. The NFSO-1.7 exhibits the best electrochemical performance among the NFSO- x samples, delivering a high discharge capacity (104.5 mAh g −1 at 0.1 C, close to its theoretical capacity of 105 mAh g −1 ), excellent rate performance (81.5 mAh g −1 at 30 C), and remarkable cycle stability over 10,000 cycles with high-capacity retention of 72.4%. We believe that the results are useful to clarify the phase and structure characteristics of polyanionic materials to promote their application for large-scale energy storage.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2022
·
IF 11.357
Yixin Huang,Jing Zou,Jinbin Lin,Haoyu Yang,Mengyun Wang,Jiawen Li,Wei Cao,Baoling Yuan,Jun Ma
The activation of peroxydisulfate (PDS) by organic compounds has attracted increasing attention. However, some inherent drawbacks including quick activator decomposition and poor anti-interference capacity limited the application of organic compound-activated PDS. It was interestingly found that 2,2′-azino-bis (3-ethylbenzothiazoline-6-sulfonate) (ABTS) could act as both activator and electron shuttle for PDS activation to enhance diclofenac (DCF) degradation over a pH range of 2.0–11.0. Multiple reactive species of ABTS•+, •OH, and SO4•– were generated in the PDS/ABTS system, while only ABTS•+ and •OH directly contributed to DCF degradation. ABTS•+, generated via the reactions of ABTS with PDS, SO4•–, and •OH, was the dominant reactive species of DCF degradation. No significant decomposition of ABTS was observed in the PDS/ABTS system, and ABTS acted as both activator and electron shuttle. Four possible degradation pathways of DCF were proposed, and the toxicity of DCF decreased after treatment with the PDS/ABTS system. The PDS/ABTS system had good anti-interference capacity to common natural water constituents. Additionally, ABTS was encapsulated into cellulose to obtain ABTS@Ce beads, and the PDS/ABTS@Ce system possessed excellent performance on DCF degradation. This study proposes a new perspective to reconsider the mechanism of activating PDS with organic compounds and highlights the considerable contribution of organic radicals on contaminant removal.
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CRYSTAL RESEARCH AND TECHNOLOGY
·
2024
·
IF 1.5
Luyong Zhang,Shibin Wang,Zhencheng Wu,Xueling Hou,Zhihua Yang,Fangfang Zhang,Shilie Pan
Tetrahedral oxygenated groups with large highest occupied molecular orbital-lowest unoccupied molecular orbital (H gaps such as [SO 4 ] are beneficial for deep ultraviolet (DUV) transmission but usually make against generating sufficient birefringence due to the small polarizability anisotropy. Thus, it is extremely difficult to obtain DUV transmission and large birefringence simultaneously in the search for DUV birefringent materials in sulfates. Herein, two new ammonium-rare earth metal sulfates, NH 4 Y(SO 4 ) 2 ·H 2 O and NH 4 YSO 4 F 2 , with DUV transmission are presented. Meanwhile, both exhibit greatly elevated birefringence through the involvement of NH 4 + units, compared to Y 2 (SO 4 ) 3 ·8H 2 O. Their optical properties are further investigated by theoretical calculations, and the effect of the introduction of NH 4 + into yttrium sulfate on optimizing the structures and properties is discussed. This work may provide a new perspective for further exploration of DUV birefringent materials in tetrahedral oxygenated group sulfates.
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