WATER RESEARCH
·
2022
·
IF 13.4
Zhen Wang,Yangyi Yu,Qin Guo,Chaoting Guan,Jin Jiang
Multiple reactive intermediates have been proposed to be involved in peroxydisulfate (PDS) activation by zerovalent iron (ZVI), including sulfate radical (SO 4 ·− ) produced via iron-oxide shell mediated electron transfer, ferryl ion species (Fe(IV)) formed from Fe(II)-PDS interaction, and hydroxyl radical ( · OH) generated by ZVI aerobic oxygenation. In this study, evolution of the relative role of these intermediates in microscale and nanoscale ZVI (mZVI vs. nZVI) activated PDS processes is comparatively investigated by using a methyl phenyl sulfoxide (PMSO) probe that selectively reacts with Fe(IV) to produce methyl phenyl sulfone (PMSO 2 ). Interestingly, during PMSO transformation by mZVI/PDS process, yields of PMSO 2 (η(PMSO 2 )) exhibit three-stage behavior that they first increase to a maximum (∼80% but lower than 100%) (Stage I) and then plateau for a period (Stage II) followed by a decrease phase (Stage III). Accordingly, the relative role of Fe(IV) in PMSO transformation is unceasingly improved in Stage I and subsequently reaches equilibrium with that of free radicals in Stage II, while it finally decreases in Stage III. Similar η(PMSO 2 ) evolution trends are obtained in nZVI/PDS process, except that the η(PMSO 2 ) increase in Stage I is negligible, possibly due to the exceptional fast nZVI dissolution. It was further clarified by tert -butyl alcohol scavenging assay that, in addition to Fe(IV), the free radical involved in Stages I and II is SO 4 ·− , while · OH was dominant in Stage III. Moreover, studies on O 2 effect reveal that ZVI aerobic oxygenation participates in mZVI corrosion during the entire process, while it is only involved in nZVI corrosion when PDS content is reduced to a low concentration, indicating that the reactivities of PDS and O 2 are similar in mZVI corrosion, but differ greatly in nZVI corrosion. Additionally, effects of reactant dose and pH on η(PMSO 2 ) evolution are also explored. Dynamics of the relative role of different reactive oxidants should be taken into account in further applications of ZVI/PDS in situ chemical remediation technology considering their different chemistries.
研究领域:
环境科学
·
化学工程
·
水处理
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DOI
高影响因子
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.
研究领域:
材料科学
·
光学
·
晶体学
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DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Xiaohua Jing,Jianying Huang,Jiani Shi,Zihan Zhao,Jingbo Hao,Xiaoning Tang
In this study, five novel ionic liquids (ILs), namely [N888][Cyanex 272], [N888][P507], [N888][Cl], [N888][NO3], and [N888]2[SO4], were synthesized through an organic acid–base reaction, followed by separation using rotary evaporation. Their structures were confirmed by 1H and 13C NMR spectroscopy, showing full consistency with theoretical predictions and no impurity peaks. Under identical extraction conditions, the ILs exhibited the following separation efficiency order for Co2+ from Ni2+: [N888]2[SO4]>[N888][Cl] > [N888][P507] > [N888][Cyanex 272]>[N888] [NO3]. Density functional theory (DFT) calculations revealed that these differences in separation performance arose from variations in the ionic radii of the IL anions. With a simple single-stage extraction under optimized conditions, [N888]2[SO4] enabled near-complete separation of Co2+ from Ni2+, achieving an extraction efficiency of 99.5 ± 2.14% and a separation factor approaching + ∞. Thermodynamic analysis confirmed that the extraction process was endothermic and nonspontaneous. The Co2+ -loaded IL-based extraction phase was efficiently stripped using diluted sulfuric acid, with a stripping efficiency of 99.3 ± 0.57%. Using sodium hydroxide as a precipitant, the solid powder of Co(OH)2 was obtained from the Co2+-containing aqueous phase. Co(OH)2 was characterized qualitatively and quantitatively by XRD and ICP-OES, and its morphology was also analyzed using SEM. The recycled IL-based extraction phase, after activation with dilute sulfuric acid, was analyzed via FT-IR spectroscopy. This regenerated IL-based extraction phase was reused for the separation of Co2+ from Ni2+, showing no degradation in performance after three cycles. Based on these findings, a process flowchart was designed for the efficient preparation of Co(OH)2 from minerals or secondary resources using the [N888]2[SO4]-based extraction phase.
研究领域:
化学工程
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材料科学
·
环境科学
·
无机化学
·
分离技术
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产品关联
DOI
高影响因子
Small
·
2024
·
IF 13
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
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MATERIALS CHEMISTRY AND PHYSICS
·
2016
·
IF 2.101
Xiaoniu Yu,Chunxiang Qian
Nano-sized CePO 4 @NaCe(SO 4 ) 2 (H 2 O) and CePO 4 with hexagonal phase have been prepared by simply varying the reactant P/Ce molar ratio in bacterial liquid. The phase composition of two samples was checked via Fourier transform infrared spectroscopy (FTIR), energy dispersive analysis of X-rays (EDS) and X-ray diffraction (XRD) analyses, displaying the presence of CePO 4 @NaCe(SO 4 ) 2 (H 2 O) and CePO 4 with average crystallite size are 32.34 and 15.61 nm, respectively. The scanning electron microscopy (SEM) images show that nano-clusters and sphere-like in shape with a narrow diameter distribution were observed in two samples. The transmission electron microscopy (TEM) photographs further indicate obtained CePO 4 @NaCe(SO 4 ) 2 (H 2 O) and CePO 4 nanoparticles correspond to nanosheets and nanorods , respectively. The emission spectra of CePO 4 @NaCe(SO 4 ) 2 (H 2 O) and CePO 4 display a broad band of 300–380 nm range with the strongest emission at 342 nm in the violet region.
研究领域:
材料科学
·
纳米技术
·
化学
·
生物学
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产品关联
DOI
高影响因子
Energy Storage Materials
·
2025
·
IF 20.2
Yong Li,Qiming Xiao,Yun Zhao,Shu Zhao,Bin Liu
Alluaudite-type Na 2+2x Fe 2-2x (SO 4 ) 3 (NFS) compounds, as a promising polyanionic cathode material for sodium-ion batteries (SIBs), have attracted considerable attention owing to their cost-effectiveness and elevated operating voltage. Nevertheless, practical implementation of NFS has been hindered by inherent limitations including insufficient crystallinity and compromised electronic/ionic conductivity. Herein, we propose a pioneering dual-strategy integrating cation substitution with crystal engineering to synthesize Mg 2+ -doped single-crystalline NFS enveloped by flash graphene (denoted as [email protected] ). Through synchrotron radiation characterization complemented by density functional theory (DFT) simulations, we verified the preferential occupation of magnesium at the target iron site. Notably, while preserving the fundamental alluaudite framework, this strategic doping induced a band structure modulation with reduced bandgap and diminished Na⁺ diffusion barriers, synergistically enhancing charge transfer kinetics. The optimized [email protected] cathode delivers remarkable rate performance (63 mAh g -1 at 100C vs 21 mAh g -1 for the undoped counterpart) and unprecedented cyclability, retaining 92.8 % capacity after 7,000 cycles at 50C. In addition, the pillar effect of Mg 2+ in the crystal, as evidenced by in-situ XRD results, greatly inhibited the migration of Fe 3+ during cycling, maintaining the stable structure and resulting in outstanding cycling stability under drastic conditions. These findings establish a universal crystal engineering paradigm for developing high-performance polyanionic cathodes in energy storage systems.
研究领域:
材料科学
·
电化学
·
储能技术
·
纳米技术
·
固态化学
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产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2019
·
IF 4.85
Ya-Ping Gong,Yun-Xiang Ma,Shao-Ming Ying,Jiang-Gao Mao,Fang Kong
Two new indium sulfate tellurites, namely, In2(SO4)(TeO3)(OH)2(H2O) and In3(SO4)(TeO3)2F3(H2O), were synthesized by hydrothermal method in a one-pot reaction. Their pure phase yields have been successfully optimized to 76% and 21%, respectively. In2(SO4)(TeO3)(OH)2(H2O) crystallized in centrosymmetric (CS) space group P21/n, while In3(SO4)(TeO3)2F3(H2O) formed a non-centrosymmetric (NCS) and chiral space group P212121. The CS compound features a 2D layered structure composed of 2D indium oxide layers decorated by sulfate tetrahedra and tellurite groups. The NCS compound displays a 3D network consisting of indium tellurite layers bridged by sulfate tetrahedra. Powder second harmonic generation measurements disclosed that In3(SO4)(TeO3)2F3(H2O) exhibits a weak frequency-doubling efficiency about 11% of the commercial KDP. Its powder laser damage threshold quantity was estimated to be 79.6 MW/cm2, which is about 36 times that of AGS. The two samples present wide optical band gaps of 4.86 and 4.10 eV, respectively, which were determined by Te, In, and O atoms based on density functional theory calculations.
研究领域:
无机化学
·
材料科学
·
光学
✓ 已验证
DOI
PubMed
高影响因子
ZEITSCHRIFT FUR ANORGANISCHE UND ALLGEMEINE CHEMIE
·
2021
·Vol. 647
·期 12
·1269-1276
·
IF 1.492
Jiayuan Zhang,Xiao Zhao,Yuandong Wu,Dajiang Mei,Shaoguo Wen,Thomas Doert
Two new antimony (III) tellurite sulfates [Sb 2 (TeO 4 )](SO 4 ) ( 1 ) and [Sb 2 (TeO 3 ) 2 ](SO 4 ) ( 2 ) were successfully synthesized through a conventional hydrothermal method and their crystal structures were determined by X-ray single crystal analysis. [Sb 2 (TeO 4 )](SO 4 ) crystallizes in the triclinic space group P ī (No. 2) with lattice parameters a=5.572(2), b=7.247(2), c=9.540(3) Å, V=358.5(2) Å 3 , and Z=2, while [Sb 2 (TeO 3 ) 2 ](SO 4 ) crystallizes in the orthorhombic space group Pbca (No. 61) with lattice parameters a=7.368(2), b=14.571(3), c=16.521(3) Å, V=1773.7(6) Å 3 , and Z=8. The structure of [Sb 2 (TeO 4 )](SO 4 ) features a three-dimensional framework, composed of [SbO 4 ] trigonal bipyramids and [TeO 4 ] polyhedra to form a cationic 2 ∞[Sb 2 (TeO 4 )] 2+ corrugated cationic layers along [100], linked by SO 4 2− anions. [Sb 2 (TeO 3 ) 2 ](SO 4 ) forms a three-dimensional framework consisting of two dimensional wrinkled layers of 2 ∞[Sb 2 (TeO 3 ) 2 ] 2+ that are linked by SO 4 2− anions. The band gaps of 4.16 eV and 3.72 eV for [Sb 2 (TeO 4 )](SO 4 ) and [Sb 2 (TeO 3 ) 2 ](SO 4 ) respectively are estimated from the solid state UV-vis-NIR diffuse reflectance spectra. Thermal analysis indicated that both compounds are thermally stable up to about 500 °C. The electrochemical specific capacity of [Sb 2 (TeO 4 )](SO 4 ) was determined to 245 mA h g −1 on the first cycle in a Li-ion half-cell, the capacity remains at about 106 mA h g −1 after 500 cycles.
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产品关联
DOI
高影响因子
ZEITSCHRIFT FUR ANORGANISCHE UND ALLGEMEINE CHEMIE
·
2019
·Vol. 645
·期 10
·745-751
·
IF 1.337
Xiaofang Li,Yuandong Wu,Dajiang Mei,Thomas Doert
Three new alkali metal transition metal sulfate-oxalates, RbFe(SO 4 )(C 2 O 4 ) 0.5 · H 2 O and Cs M (SO 4 )(C 2 O 4 ) 0.5 · H 2 O ( M = Mn, Fe) were prepared through hydrothermal reactions and characterized by single-crystal X-ray diffraction, solid state UV/Vis/NIR diffuse reflectance spectroscopy, infrared spectra, thermogravimetric analysis, and powder X-ray diffraction. The title compounds all crystallize in the monoclinic space group P 2 1 / c (no. 14) with lattice parameters: a = 7.9193(5), b = 9.4907(6), c = 8.8090(6) Å, β = 95.180(2)°, Z = 4 for RbFe(SO 4 )(C 2 O 4 ) 0.5 · H 2 O; a = 8.0654(11), b = 9.6103(13), c = 9.2189(13) Å, β = 94.564(4)°, Z = 4 for CsMn(SO 4 )(C 2 O 4 ) 0.5 · H 2 O; and a = 7.9377(3), b = 9.5757(4), c = 9.1474(4) Å, β = 96.1040(10)°, Z = 4 for CsFe(SO 4 )(C 2 O 4 ) 0.5 · H 2 O. All compounds exhibit three-dimensional frameworks composed of [ M O 6 ] octahedra, [SO 4 ] 2– tetrahedra, and [C 2 O 4 ] 2– anions. The alkali cations are located in one-dimensional tunnels.
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DOI
高影响因子
ZEITSCHRIFT FUR ANORGANISCHE UND ALLGEMEINE CHEMIE
·
2020
·Vol. 646
·期 20
·1688-1695
·
IF 1.24
Shuangsheng Cheng,YuanDong Wu,Dajiang Mei,Shaoguo Wen,Thomas Doert
Four alkali metal bismuth sulfates, NaBi(SO 4 ) 2 · H 2 O ( 1 ) and ABi(SO 4 ) 2 [A = K ( 2 ), Rb ( 3 ), Cs ( 4 )], were successfully synthesized by hydrothermal methods. The crystal structure of 1 features a three-dimensional tunnel framework constructed by BiO 9 tri-capped trigonal prisms and SO 4 tetrahedra interconnected via common corners and edges. Compound 2 exhibits a two-dimensional 2 ∞ [Bi(SO 4 ) 2 ] – double-layered structure, assembled by one-dimensional 1 ∞ [BiS(1)O 4 ] + chains which are linked via S(2)O 4 2– tetrahedra. The isostructural compounds 3 and 4 possess a two-dimensional layered structure, and the layers being composed by BiO 8 square antiprism and SO 4 tetrahedra. The alkali metal cations are located between the layers or in the tunnels of the structures, respectively. The differences in the crystal structures of the title compounds can mainly be attributed to the different sizes of the alkali metal cations and their different coordination environments. Thermogravimetric analysis evidence that compound 1 losses one equivalent of water at 120 °C whereas the anhydrous compounds 2 – 4 are stable up to about 450, 575, and 578 °C, respectively. The solid-state UV/Vis/NIR diffuse reflectance spectra indicate bandgaps of approximately 4.48, 4.43, 3.98, and 3.96 eV for compounds 1 – 4 , respectively.
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高影响因子
Catalysts
·
2020
·Vol. 10
·期 4
·384
·
IF 3.52
Pei Yu,Can Chen,Guangci Li,Zhong Wang,Xuebing Li
The esterification of malic acid using traditional homogenous catalysts suffers from the difficulty in reuse of the catalyst and undesirable side reactions. In this work, Zr(SO4)2/SiO2and Zr(SO4)2/activated carbon (AC) as solid acid catalysts were prepared for malic acid esterification with methanol. The conversion of malic acid over these two catalysts is comparable to that over H2SO4and unsupported Zr(SO4)2∙4H2O catalysts; however; a 99% selectivity of dimethyl malate can be realized on these two supported catalysts, which is much higher than that of conventional H2SO4(75%) and unsupported Zr(SO4)2∙4H2O (80%) catalysts, highlighting the critical role of AC and SiO2supports in tuning the selectivity. We suggest that the surface hydroxyls of AC or lattice O2−ions from SiO2donate electrons to Zr4+in Zr(SO4)2/AC and Zr(SO4)2/SiO2catalysts, which results in the increase in electron density on Zr4+. The enhanced electron density on Zr4+reduces the degree of H delocalization from crystal water and then decreases the Brønsted acid strength. Consequently, the reduced Brønsted acid strength of Zr(SO4)2/AC and Zr(SO4)2/SiO2catalysts suppresses the intermolecular dehydration side reaction. In addition, these two supported catalysts can be easily separated from the reaction system by simple filtration with almost no loss of activity.Keywords:malic acid;catalytic esterification;solid acid catalyst;Zr(SO4)2;intermolecular dehydration
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高影响因子
SOLID STATE SCIENCES
·
2015
·
IF 1.839
Xiao Zhao,Dajiang Mei,Jingli Xu,Yuandong Wu
The reactions of A 2 SO 4 ( A = K, Cs) and Sb 2 O 3 with H 2 SO 4 (98%) yielded single crystals of A Sb(SO 4 ) 2 ( A = K, Cs). The crystal structures were investigated by single crystal X-ray diffraction. KSb(SO 4 ) 2 crystallizes in the monoclinic space group P 2 1 / c (No. 14) with lattice parameters a = 10.6745(18), b = 7.1579(12), c = 8.7597(15) Å, β = 91.466(3) ° , V = 669.1(2) Å 3 , Z = 4. CsSb(SO 4 ) 2 crystallizes in the orthorhombic space group P 2 1 2 1 2 1 (No.19) with lattice parameters of a = 5.2429(8), b = 9.5942(16), c = 14.850(2) Å, V = 746.98(20) Å 3 , Z = 4. Both compounds show the Sb 3+ cations in same seesaw-type coordination of oxygen atoms from different SO 4 2 − anions, but exhibit complex two-dimensionally and one-dimensionally linked anionic structures. The alkali cations are located between the layers or chains. The compounds were characterized with FT-IR spectra and solid state UV–vis–NIR diffuse reflectance spectroscopy . The band gaps were estimated at 4.64 eV for KSb(SO 4 ) 2 and 4.68 eV for CsSb(SO 4 ) 2 .
研究领域:
化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）