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
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电化学
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能源存储技术
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DOI
PubMed
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
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电化学
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储能技术
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纳米技术
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固态化学
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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
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材料科学
·
光学
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DOI
PubMed
高影响因子
ZEITSCHRIFT FUR ANORGANISCHE UND ALLGEMEINE CHEMIE
·
2021
·Vol. 647
·期 12
·1269-1276
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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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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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JOURNAL OF SOLID STATE CHEMISTRY
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2018
·
IF 2.179
Ting-Ting Ruan,Wen-Wen Wang,Chun-Li Hu,Xiang Xu,Jiang-Gao Mao
Two new lead(II) borate-sulfate mixed-anion compounds, namely, Pb 4 (BO 3 ) 2 (SO 4 ) and Pb 2 [(BO 2 )(OH)](SO 4 ), have been prepared by using high-temperature melt method or hydrothermal reaction . These compounds exhibit two different types of 3D structures composed of the same anionic units of BO 3 triangles and SO 4 tetrahedra which are interconnected by lead(II) cations. In Pb 4 (BO 3 ) 2 (SO 4 ), the lead(II) ions are bridged by borate anions into 3D [Pb 4 (BO 3 ) 2 ] 2+ architectures with 1D tunnels of 8-member rings along the a -axis, which are filled by the sulfate anions. In Pb 2 [(BO 2 )(OH)](SO 4 ), the lead(II) ions are interconnected by borate and sulfate anions into 2D Pb-B-O and Pb-S-O layers parallel to the ab plane, respectively, and these layers are further condensed into the 3D lead(II) borate-sulfate framework. TGA and DSC studies indicate that Pb 4 (BO 3 ) 2 (SO 4 ) is congruently melting with a melting point of 689 °C whereas Pb 2 [(BO 2 )(OH)](SO 4 ) decomposes at approximately 335 °C. UV/Vis/NIR optical diffuse reflectance spectrum measurements reveal the optical band gaps of 4.03 and 4.08 eV for Pb 4 (BO 3 ) 2 (SO 4 ) and Pb 2 [(BO 2 )(OH)](SO 4 ), respectively. Furthermore, the electronic structures of Pb 4 (BO 3 ) 2 (SO 4 ) have also been calculated.
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高影响因子
ZEITSCHRIFT FUR ANORGANISCHE UND ALLGEMEINE CHEMIE
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2020
·Vol. 646
·期 20
·1688-1695
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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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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 .
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Tiezheng Niu,Junzhuo Cai,Penghui Shi,Guohua Zhao
Sulfate-based electrochemical advanced oxidation is of rising importance for pollutant removal , however, adscititious sulfate has adverse effects on water salinity . A novel electrochemical system which could exploit the existed SO 4 2− for in situ generation of SO 4 − was successfully constructed with boron doped diamond (BDD) anode and hierarchical 1D Co 3 O 4 nanowire array cathode. The in situ electrochemical electron paramagnetic spectroscopy and titration were used to study the positive correlation between the increase of sulfate radicals (SRs) and the efficient activation of peroxydisulfate (PDS) by hierarchical 1D Co 3 O 4 nanowire array cathode. Electrochemical impedance and X-ray photoelectron spectroscopy revealed that the efficient activation of PDS by the Co 3 O 4 cathode was derived from the excellent electron transport capability of the 1D nanostructure , and the electric field accelerates the reduction of Co(III). The novel hierarchical 1D Co 3 O 4 nanowire array cathode can completely degrade dibutyl phthalate in 45% less time with 38% less energy compared to a traditional graphite cathode without the requirement of extra chemicals. The possible mechanism of anodic PDS accumulation and cathodic SRs generation was firstly revealed, and this advanced electrochemical oxidation system provides a good reference for the in situ sustainable remediation in sulfate-containing water.
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高影响因子
ZEITSCHRIFT FUR ANORGANISCHE UND ALLGEMEINE CHEMIE
·
2014
·
IF 1.251
Fengting Chen,Jiachang Zhao,Jingli Xu,Yuandong Wu
The hetero-bimetallic polyanionic compound BiCu 2 (TeO 3 )(SO 4 )(OH) 3 was synthesized using hydrothermal techniques. Single-crystal X-ray diffraction analysis revealed that title compound crystallizes in the monoclinic space group P 2 1 / n (No. 14) with lattice parameters a = 9.5513(15), b = 6.3022(10), c = 13.955(2) Å, β = 102.845(3)°, and Z = 4. The structure of title compound is a three-dimensional tunnel framework consisting of edge-sharing two-dimensional [Cu 3 O 10 ] 14– layers linked by BiO 8 bicapped trigonal prisms, TeO 3 2– trigonal pyramids and SO 4 2– tetrahedra. Along [010], each Cu(1)O 6 octahedron shares two edges with adjacent Cu(1)O 6 units to form infinite one-dimensional zigzag chains, which are connected by double inverted Cu(2)O 6 octahedral units via edge sharing (O9 ··· O8). The suitability of crystal for optical applications was investigated by UV/Vis/NIR spectroscopy. Raman and FTIR spectra were used to confirm the presence of various functional groups such as TeO 3 2– , SO 4 2– , OH – in the crystals.
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高影响因子
CRYSTAL GROWTH & DESIGN
·
2018
·
IF 3.972
Fangfang He,Qian Wang,Cuifang Hu,Wen He,Xueying Luo,Ling Huang,Daojiang Gao,Jian Bi,Xin Wang,Guohong Zou
Two new antimony sulfate chlorides named (NH4)2SbCl(SO4)2 and (NH4)SbCl2(SO4) were successfully synthesized through solvent-free synthesis method. (NH4)2SbCl(SO4)2 exhibits a three-dimensional framework constructed of [SbCl(SO4)2]2– chains and NH4+ ions. And the NH4+ cations play the role of charge balance and provide the hydrogen bond constructed with oxygen atoms. (NH4)SbCl2(SO4) shows a two-dimensional layer structure that is composed of the regularly stacked [SbCl2(SO4)]− chains via hydrogen-bonding interactions. Both of the titled compounds possess the same chemical composition and the similar Sb–Cl–SO4 chains, while hydrogen-bonding interactions and lone-pair cations play the synergistic effect on the framework structures and macroscopic centricities resulting in that the (NH4)2SbCl(SO4)2 is centrosymmetric and the (NH4)SbCl2(SO4) is non-centrosymmetric (NCS). Powder second harmonic generation (SHG) measurements indicated that the NCS compound (NH4)SbCl2(SO4) is type I phase-matchable and exhibits SHG responses of ∼1.7 times that of KH2PO4.
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