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Na2SO4
Small · 2024 · IF 13

Uncovering the Nonequilibrium Evolution Mechanism between Na2+2δFe2−δ(SO4)3 Cathode and Impurities in the Na2SO4-FeSO4·7H2O Binary System for High-Voltage Sodium-Ion Batteries

Wei Yang,Qi Liu,Qiang Yang,Xinyu Zhang,Zhuolin Yang,Daobin Mu,Li Li,Renjie Chen,Feng Wu

Sodium-ion batteries are increasingly recognized as ideal for large-scale energy storage applications. Alluaudite Na 2+2 δ Fe 2− δ (SO 4 ) 3 has become one of the focused cathode materials in this field. However, previous studies employing aqueous-solution synthesis often overlooked the formation mechanism of the impurity phase. In this study, the nonequilibrium evolution mechanism between Na 2+2 δ Fe 2− δ (SO 4 ) 3 and impurities by adjusting ratios of the Na 2 SO 4 /FeSO 4 ·7H 2 O in the binary system is investigated. Then an optimal ratio of 0.765 with reduced impurity content is confirmed. Compared to the poor electrochemical performance of the Na 2.6 Fe 1.7 (SO 4 ) 3 (0.765) cathode, the optimized Na 2.6 Fe 1.7 (SO 4 ) 3 @CNTs (0.765@CNTs) cathode, with improved electronic and ionic conductivity, demonstrates an impressive discharge specific capacity of 93.8 mAh g −1 at 0.1 C and a high-rate capacity of 67.84 mAh g −1 at 20 C, maintaining capacity retention of 71.1% after 3000 cycles at 10 C. The Na 2.6 Fe 1.7 (SO 4 ) 3 @CNTs//HC full cell reaches an unprecedented working potential of 3.71 V at 0.1 C, and a remarkable mass-energy density exceeding 320 Wh kg −1 . This work not only provides comprehensive guidance for synthesizing high-voltage Na 2+2 δ Fe 2− δ (SO 4 ) 3 cathode materials with controllable impurity content but also lays the groundwork of sodium-ion batteries for large-scale energy storage applications.

研究领域: 材料科学 · 电化学 · 能源存储技术
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ORE GEOLOGY REVIEWS · 2024 · IF 3.2

Raman spectral quantification of Li2SO4, Na2SO4, K2SO4 and Cs2SO4 at 25 to 250 °C and its potential implications for the determination of sulfate contents in natural fluid inclusions

Chen Chen,Linbo Shang,Yunhe Zhou,Ziqi Jiang,Xinsong Wang,I-Ming Chou,Jianguo Li,Zhenglong Wang

The quantitative study of the sulfate content in natural fluid inclusions (FIs) will help our understanding of the processes of metal transport and related mineralization. The sulfate-rich FIs typically contain several types of sulfates with diverse cations such as Na + , K + , and so on. In order to get the sulfates contents in natural FIs, in situ Raman spectral quantitative calibration method is used to calibrate the Li 2 SO 4 , Na 2 SO 4 , K 2 SO 4 and Cs 2 SO 4 solutions at temperatures ranging from 25 °C to 250 °C in our study. The results show that the A (SO 4 2− )/ A (H 2 O) ratio increases linearly with increasing m SO 4 2− in sulfate solutions containing single cation of Li, Na, K or Cs at the set temperatures, where A is Raman peak area and m is molality (mol/kg H 2 O), and a negative linear relationship exists between k (quantitative calibration coefficient) and temperature for sulfate solutions with specific cations up to 250 °C. Meanwhile, the slopes and the intercepts of the k-T correlation curves are obviously different among sulfate solutions with different cations, and the coefficients k of these sulfate solutions at certain temperature decrease with the increase of atomic number of the cation, in accordance with the following order: Li +  > Na +  > K +  > Cs + . As Na + and K + are the main cations in the natural sulfate-bearing FIs, the quantification of the multi-cation (Na ± K ± Li) sulfate solutions was evaluated by using the Raman quantitative calibration curves of Li 2 SO 4 , Na 2 SO 4 , K 2 SO 4 and Cs 2 SO 4 separately, the errors exist due to the use of calibration curves with different cations; the average concentration errors derived from the use of Na 2 SO 4 or K 2 SO 4 Raman quantitative calibration curves are within about 5 %, while those from the use of Li 2 SO 4 or Cs 2 SO 4 Raman quantitative calibration curves are within about 15 %. Therefore, the acceptable errors suggest that the calibration curves of individual sulfates can be applied to the determination of sulfate content of natural sulfate-bearing FIs.

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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

High-efficiency NO electroreduction to NH3 over honeycomb carbon nanofiber at ambient conditions

Ling Ouyang,Qiang Zhou,Jie Liang,Longcheng Zhang,Luchao Yue,Zerong Li,Jun Li,Yongsong Luo,Qian Liu,Na Li,Bo Tang,Abdulmohsen Ali Alshehri,Feng Gong,Xuping Sun

Electrocatalytic NO reduction is a promising technology for ambient NO removal with simultaneous production of highly value-added NH 3 . Herein, we report that honeycomb carbon nanofiber coated on carbon paper acts as an efficient metal-free catalyst for ambient electroreduction of NO to NH 3 . In 0.2 M Na 2 SO 4 solution, such catalyst achieves an NH 3 yield of 22.35 μmol h −1  cm −2 with a high Faradaic efficiency of up to 88.33%. Impressively, it also shows excellent stability for 10-h continuous electrolysis. Theoretical calculations reveal that the most active center of functional groups is –OH group for NO reduction with a low energy barrier (ΔG of 0.29 eV) for the potential-determining step (*NO + H → *HNO).

研究领域: 环境科学 · 材料科学 · 电化学 · 催化
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Polyamide nanofiltration membrane modified with defective covalent organic framework interlayer for selective ion sieving

Yin-Xin Fang,Zhen-Liang Xu,Sun-Jie Xu

Generally, thin-film composite (TFC) membranes prepared using piperazine (PIP) and trimesoyl chloride (TMC) exhibit good Na 2 SO 4 rejection, but their MgCl 2 rejection is not satisfactory. In this study, a defective covalent organic framework (COF) interlayer with residual unreacted amine groups was fabricated via interfacial polymerization (IP) by changing the catalyst concentration. Introduction of the COF layer into a polyamide (PA) separation membrane modified the pore size of the PA layer, thereby improving the rejection of divalent cations. The pore size of the PA layer decreased and the surface morphology of the membrane was converted from nodular to a hybrid morphology of “ridge-and-valleys’’ and nodules, indicating that the residual unreacted amine groups on the COF interlayer successfully reacted with the acyl chloride groups. The optimal membrane (PIP/COF-A/PES) exhibited high rejection of divalent ions (Na 2 SO 4 of 98.3% and MgCl 2 of 94.3%), and the membrane showed excellent capability for separating mono/divalent ions. Overall, a method of preparing nanofiltration membranes by modifying the PA layer to enhance the rejection of divalent cations was demonstrated.

CAS / MDL: 4422-95-1 108-45-2
研究领域: 材料科学 · 化学工程 · 纳米技术 · 膜技术
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JOURNAL OF MEMBRANE SCIENCE · 2023 · IF 9.5

Catalyst-anchored secondary polymerization for highly permeable acid-resistant nanofiltration membrane preparation

Yang Cao,Yinhua Wan,Chulong Chen,Jianquan Luo

Nanofiltration (NF) is considered a competitive technique for acidic stream treatments. However, poorly reactive acid-resistant monomers normally cause thick and uneven separation layers with ultra-low permeability. Herein, catalyst-anchored secondary polymerization is employed after the interfacial polymerization (IP) reaction between trimesoyl chloride (TMC) and 3-aminobenzenesulfonamide (ABSA) to fabricate an extremely acid-resistant NF membrane. Acylation catalysts in ethanol are grafted on the nascent layer by reacting with residual acyl chloride groups to enhance the monomer reactivity, while the ethanol-induced nascent layer structure regulation greatly improves the surface uniformity. Benefiting from the improved self-inhibition effect and optimized phase integrity of the modified IP process, the resulting acid-resistant membrane has unprecedented water permeance (up to 31.4 Lm −2 h −1 bar −1 ), desirable Na 2 SO 4 rejection (92.8%), high dye/H + selectivity and impressive acid stability (20 wt% of H 2 SO 4 for 50 days), outperforming almost all advanced acid-resistant NF membranes. Our work provides a versatile approach for the synthesis of high-performance specialty membranes.

研究领域: 材料科学 · 化学工程 · 膜技术 · 环境科学
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Advanced Energy Materials · 2024 · IF 24.4

An Aqueous All-Quinone-Based Redox Flow Battery Employing Neutral Electrolyte

Gaojing Yang,Yaxun Zhu,Zhimeng Hao,Qiu Zhang,Yong Lu,Zhenhua Yan,Jun Chen

Redox flow batteries (RFBs) are considered as promising candidates for large-scale energy storage. However, traditional RFBs based on toxic metal ions have deficiencies in resource utilization and environmental protection. Considering the corrosiveness of acidic and alkaline electrolytes and sustainability of energy storage devices, neutral aqueous organic redox flow batteries (AORFBs) have more development prospects. Herein, an AORFB is reported, using 9,10-anthraquinone-2,7-disulfonic salt (2,7-AQDS) and 1,4-dihydroxyphenylsulfonate potassium (HQS) as negative and positive electroactive materials, respectively. It is found that the anions in the neutral solution further affected the solubility and kinetics of the electroactive materials by affecting the hydrogen bond in the solution, and the Na 2 SO 4 solution showed the optimal comprehensive performance. Therefore, an all-quinone AORFB employing neutral Na 2 SO 4 electrolytes with a cell voltage of 0.9 V is constructed, which presented a capacity utilization of 70.1% and delivered stable cycling performance at 60 mA cm −2 . This work designs an innovative neutral all-quinone AORFB and points out how anions affect the properties of the electrolyte by affecting hydrogen bonds within the solution. These findings open a new avenue for the design and application of neutral all-organic aqueous RFBs.

研究领域: 能源存储 · 电化学 · 材料科学
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JOURNAL OF MEMBRANE SCIENCE · 2021 · IF 8.742

MXene nanocomposite nanofiltration membrane for low carbon and long-lasting desalination

Qiang Xue,Kaisong Zhang

Current membranes have limitations in permeability and selectivity, and require long-time stability, which drive the development of high-performance nanofiltration (NF) membranes. MXene is a new type of highly hydrophilic and negatively charged two-dimensional (2D) nanosheets material, especially its supernatant has good dispersibility and stability. The MXene supernatant containing several layers was treated as aqueous solvent for interfacial polymerization, consequently the prepared MXene nanocomposite membrane could maintain high permeselectivity even under low pressures required for low carbon. The characterization results showed that the MXene nanocomposite membrane had better hydrophilicity and higher negative charge. At the same time, the Na 2 SO 4 rejection was increased to 97.6% and the pure water flux was improved by about 1.7 times compared with the pristine membrane. In the BSA antifouling test and 58-day persistent desalination test, the MXene nanocomposite membrane showed the better antifouling property, high rejection and good stability. As an excellent 2D modifier, MXene provided fresh ideas and guidance for low-carbon and persistent NF membranes with excellent separation performance.

研究领域: 材料科学 · 环境工程 · 纳米技术 · 水处理
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DESALINATION · 2023 · IF 9.9

Nano-wrinkled polyamide membrane preparation via heterogeneous surface-regulated interfacial polymerization for enhanced desalination performance

Zhiwen Li,Yanchao Xu,Liguo Shen,Renjie Li,Yang Jiao,Hongjun Lin,Chuyang Y. Tang

Nano-wrinkled morphology and ultrathin thickness are desirable membrane structures in polyamide membranes, particularly for high-performance applications in desalination and wastewater treatment . In this study, we present the fabrication of a nano-wrinkled polyamide membrane with ultrathin thickness on a heterogeneous surface that features hydrophilic UiO-66-NH 2 nanoparticles embedded on a hydrophobic polyethersulfone surface using a heterogeneous surface regulated interfacial polymerization approach. The presence of the heterogeneous surface induces the formation of aqueous phase microphases under the organic phase due to the unbalanced interfacial tension, which serves as a template for the formation of the polyamide film. This results in the creation of a nano-wrinkled polyamide layer upon drying. Furthermore, the hydrogen bonding interaction between the UiO-66-NH 2 and piperazine (PIP) slows down the PIP release, which contributes to the ultrathin thickness of the polyamide layer. The polyamide membrane obtained in this study exhibits a pure water permeance (PWP) of 26.1 L bar −1 ·h −1 ·m −2 and a Na 2 SO 4 rejection of 97.5 %. The PWP is 6.15 times higher than that of a control membrane fabricated through conventional interfacial polymerization. Our work offers a novel approach to tailor the structure of polyamide membranes via heterogeneous surface regulated interfacial polymerization, which has potential applications in environmental desalination.

研究领域: 材料科学 · 环境工程 · 膜技术 · 水处理
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DESALINATION · 2022 · IF 11.211

Engineering novel high-flux thin-film composite (TFC) hollow fiber nanofiltration membranes via a facile and scalable coating procedure

Chuanfeng Wang,Yingbo Chen,Xiaoyu Hu,Pengfei Guo

A novel defect-free polyamide/(polyether sulfone/poly(vinylidene fluoride)) PA/(PES/PVDF) thin-film composite (TFC) hollow fiber membrane (HFM) with desirable separation characteristics were developed through a facile and scalable coating procedure. By the introduction of piperazine (PIP) monomers into the PES coating solutions, the functional monomer-enriched PES coating layer was formed on the shell side of porous matrix-reinforced hollow fiber (HF) support through phase inversion process. Subsequently, PIP and TMC was interfacial polymerized during the fiber coating line to form a thin and defect-free polyamide (PA) functional layer for TFC HFM with high water permeability. Furthermore, the introduction of aqueous monomers only into the PES layer allowed economizing the cost of membrane manufacturing compared with bulk modification of the membrane substrate. Interestingly, the formation of bowl-like structures endowed the separation layer with higher permeation surface area and thus favored high water permeability. On combining these separation features, the optimized TFC membranes presented a high pure water permeability (PWP) of 13.8 L·m −2 ·h −1 ·bar −1 , approximately twice than that of conventional TFC membrane, with a satisfying Na 2 SO 4 rejection of 98.2%. Moreover, the PA/(PES/PVDF) TFC HFM exhibited excellent stability, backwash ability and anti-fouling ability, suggesting its huge potential for the water purification . Compared with the conventional two-step IP process on flat sheet membrane , the in-situ IP procedure performed on HF greatly simplifies the manufacturing process , shortens the production period and reduces monomer usage while the high packing density and great surface area per unit volume are obtained. This work may provide a simple and economical strategy for engineering high-performance TFC HFM.

研究领域: 材料科学 · 化学工程 · 环境工程 · 膜技术
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JOURNAL OF NANOPARTICLE RESEARCH · 2022 ·Vol. 24 ·期 11 ·1-10 · IF 2.533

Synthesis of 1D WO3 nanostructures using different capping agents for pseudocapacitor applications

Di Jing,Gai Xikun,Jamakanga Ropafadzo,Lou Jie,Zhu Minzhi,Li Yin,Yang Ruiqin,Ma Qingxiang

To investigate the correlation between electrochemical performance and physicochemical properties, three types of 1D WO 3 nanostructures were fabricated by hydrothermal method using K 2 SO 4 , Na 2 SO 4 , and (NH 4 ) 2 SO 4 as capping agents. Hexagonal phase was obtained with the assistant of Na 2 SO 4 and (NH 4 ) 2 SO 4 , while monoclinic phase was developed using K 2 SO 4 as agent. WO 3 nanostructures prepared by (NH 4 ) 2 SO 4 and Na 2 SO 4 exhibited superior specific capacitance (400 F/g and 388 F/g) relative to WO 3 prepared by K 2 SO 4 (259 F/g), suggesting hexagonal phase is more suitable for energy storage. The nanostructures prepared using Na 2 SO 4 exhibited inferior rate performance compared with those obtained by (NH 4 ) 2 SO 4 due to low specific surface area and high crystallinity. The electrochemical performance demonstrated nanostructures prepared by (NH 4 ) 2 SO 4 was surface-controlled whereas those using Na 2 SO 4 and K 2 SO 4 were battery-type material. These findings raise the prospects of developing tungsten oxide for energy storage. Graphical abstract

研究领域: 材料科学 · 电化学 · 纳米技术 · 能源存储
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JOURNAL OF MEMBRANE SCIENCE · 2023 · IF 9.5

Gradient crosslinking optimization for the selective layer to prepare polyvinyl alcohol (PVA) nanofiltration (NF) membrane: The enhanced filtration performance and potential rejection for EDCs

Haojie Zeng,Feiyun Sun,Jianjun Zhang,Ying Wang,Songwen Yang,Dingyu Xing

Polyvinyl alcohol (PVA) has been employed and crosslinked as the selective layer of NF membranes with enhanced hydrophilicity. However, the influences of different crosslinking methods and agents on the reaction mechanism and membrane performance still need to be comprehensively studied. In this study, NF membranes were prepared by coating crosslinking (CC-membrane) and gradient crosslinking (GC-membrane) methods. Compared with CC-membrane, the GC-membrane possessed a 65% higher flux with Na 2 SO 4 rejection around 90%, under the optimal preparation conditions with PVA content of 0.10%, curing at 80 °C for 10 min. Crosslinking agents including 1,3,5-benzenetricarboxylic acid (TMA), 4,4′-(hexafluoroisopropylidene) diphthalic anhydride (6FDA) and pyromellitic dianhydride (PMDA) with different spatial structure were used to optimize the GC-membrane. As confirmed by SEM, XPS, FTIR and contact angle tests, the 6FDA-GC membrane showed a thinner, smoother and more hydrophilic selective layer, and kept an excellent balance between the water flux (88.6 L/m 2 h) and Na 2 SO 4 rejection (88.7%). This is because the 6FDA with a large molecule and flexible spatial structure could form a more integrated crosslinking structure compared to PMDA. Meanwhile, the 6FDA-GC membrane showed rejections of over 80% towards the endocrine-disrupting compound 17α-Ethinylestradiol and exhibited stable antifouling ability and durability. Overall, this work studied systematically the influences of various crosslinking agents on the GC-membrane, and verified the potential of hydrophilic PVA membranes for nanofiltration.

研究领域: 材料科学 · 化学工程 · 环境科学 · 膜技术
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