Small
·
2023
·
IF 13.3
Wei Yang,Qi Liu,Lijuan Hou,Qiang Yang,Daobin Mu,Guoqiang Tan,Li Li,Renjie Chen,Feng Wu
Iron-based sulfate cathodes of alluaudite Na 2+2 δ Fe 2− δ (SO 4 ) 3 (NFS) in sodium-ion batteries with low cost, steady cycling performance, and high voltage are promising for grid-scale energy storage systems. However, the poor electronic conductivity and the limited understanding of the phase-evolution of precursors hinder obtaining high-rate capacity and the pure phase. Distinctive NFS@C@ n %CNTs ( n = 1, 2, 5, 10) sphere-shell conductive networks composite cathode materials are constructed creatively, which exhibit superior reversible capacity and rate performance. In detail, the designed NFS@C@2%CNTs cathode delivers an initial discharge capacity of 95.9 mAh g −1 at 0.05 C and up to 60 mAh g −1 at a high rate of 10 C. The full NFS@C@2%CNTs//HC cell delivers a practical operating voltage of 3.5 V and mass-energy density of 140 Wh kg −1 at 0.1 C, and it can also retain 67.37 mAh g −1 with a capacity retention rate of 96.4% after 200 cycles at 2 C. On the other hand, a novel combination reaction mechanism is first revealed for forming NFS from the mixtures of Na 2 Fe(SO 4 ) 2 · n H 2 O ( n = 2, 4) and FeSO 4 ·H 2 O during the sintering process. The inspiring results would provide a novel perspective to synthesize high-performance alluaudite sulfate and analogs by aqueous methods.
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Small
·
2025
·Vol. 21
·期 19
·2500271
·
IF 12.1
Weiyi Li,Bijiao He,Fang Zhang,Yan Xin,Shen Cai,Huajun Tian
Na 2+2x Fe 2–x (SO 4 ) 3 (NFSO) is a promising cathode material for sodium-ion batteries (SIBs) due to its low cost and high operating potential (≈3.8 V). However, poor intrinsic electronic conductivity and sluggish kinetics are major drawbacks to its practical application. Herein, magnesium doped Na 2+2x Fe 2–x (SO 4 ) 3 microspheres (Na 2.54 (Fe 0.97 Mg 0.03 ) 1.73 (SO 4 ) 3 ) are synthesized via a designed spray-drying process. The optimized cathode material (NFSO@C-Mg0.02) possesses excellent rate performance up to 50C (50.8 mAh g −1 at 50C) and long-cycle stability (capacity retention of 78.3% even after 9000 cycles at 10C). Despite an increase in the mass loading to 10 mg cm −2 , the electrode continues to represent a reversible capacity of 72.1 mAh g −1 at 3C. Furthermore, NFSO@C-Mg0.02║HC full cell demonstrates superior cycling stability (80% capacity retention over 8000 cycles at 5C) and high energy density (≈310 Wh kg −1 , based on the cathode). In situ X-ray diffraction (XRD) results reveal that the Mg doping strategy successfully mitigates the variation in lattice volume. The density functional theory (DFT) calculations verify that the prominent rate performance is attributed to the enhanced Na + diffusion kinetics and low ionic-migration energy barrier. This work provides an effective strategy and a fundamental understanding to enhance the electrochemical performance of cathode materials for SIBs.
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高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
·
2018
·
IF 2.179
Huili Liu,Zhuxiu Zhang,Jihai Tang,Zhaoyang Fei,Qing Liu,Xian Chen,Mifen Cui,Xu Qiao
In this article, we use defect engineering approach to fine-tune the pore size of MOF-808-SO 4 . A series of defective MOF-808-SO 4 with different pore size were prepared by varying the amount of isophthalic acid as the defective ligand during the synthesis. We obtained a linear correlation between the concentration of the defective ligand and the pore size via regression analysis. The pore size exerts a significant effect on the catalytic activity in the addition reaction of isobutylene with ethylene glycol. The highest conversion of ethylene glycol was found over MOF-808-20%-SO 4 (2.25 nm) with the largest pore size, whereas MOF-808-5%-SO 4 (1.46 nm) and MOF-808-10%-SO 4 (1.53 nm) exhibited higher selectivity toward ethylene glycol mono-tert-butyl ether. There is a linear correlation between the pore size and catalytic activity only when the pore size ranges from 1.4 to 2.0 nm. MOF-808-15%-SO 4 with the pore size of 1.99 nm exhibits the highest yield of ethylene glycol mono-tert-butyl ether.
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JOURNAL OF CATALYSIS
·
2021
·
IF 7.92
Jiawei Ji,Meizan Jing,Xiuwen Wang,Wei Tan,Kai Guo,Lulu Li,Xin Wang,Wang Song,Lijun Cheng,Jingfang Sun,Weiyu Song,Changjin Tang,Jian Liu,Lin Dong
The occurrence of NH 3 -SCR (selective catalytic reduction of NO with NH 3 ) reaction on catalyst surface typically requires acid and redox sites. However, the role of acid-redox interaction on NH 3 -SCR performance is still obscure due to complex acidities and entangled acid-redox sites. Herein, three types of model Ce 2 (SO 4 ) 3 -CeO 2 catalysts with distinct interfaces are constructed to reveal the effect of acid-redox interaction on NH 3 -SCR performance. That is, SO 4 2- /CeO 2 -VS (vapor sulfation of ceria) with strong acid-redox interfacial contact, SO 4 2- /CeO 2 -WI (wet impregnation), and SO 4 2- /CeO 2 -SG (solid grinding) with limited interfaces. It is found the redox property is significantly disturbed as a result of the electron-withdrawing effect from the sulfate. Theoretical result unravels that the introduction of Ce 2 (SO 4 ) 3 retards the oxygen vacancy formation over CeO 2 . Due to restricted interfaces in SO 4 2- /CeO 2 -SG, the negative influence from acid sites is greatly alleviated. Further mechanism study discloses the weakened acid-redox interaction actually changes the nature of surface NO x species, resulting in the generation of reactive species (*O-N-O* and cis -N 2 O 2 2- ) and the promotion of surface reaction via Langmuir-Hinshelwood (L-H) mechanism.
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Xiaojie Qiu,Shengjiong Yang,Mawuli Dzakpasu,Xiaoping Li,Dahu Ding,Pengkang Jin,Rongzhi Chen,Qionghua Zhang,Xiaochang C. Wang
Mn 0.8 Fe 2.2 O 4 magnetic nanocrystals (Mn 0.8 Fe 2.2 O 4 MNCs) are synthesized by thermal treatment of a metal-organic framework (MOF) template, and their physicochemical properties are characterized in detail. The Mn 0.8 Fe 2.2 O 4 MNCs exhibited highly efficient performance for the catalytic degradation of Bisphenol A (BPA) by peroxymonosulfate (PMS) activation at various initial pH, catalyst dosage, and PMS concentration. A leaching solution experiment evidenced that PMS activation by the Mn 0.8 Fe 2.2 O 4 MNCs is a heterogeneous process. Interestingly, scavenging experiments and electron paramagnetic resonance (EPR) analysis demonstrated that HO is the dominant radical for BPA degradation, rather than SO 4 − . The scavenger experiment indicated that the surface-bound radicals may play the crucial role for BPA degradation. Increasing Cl − or decreasing bicarbonate concentrations in solution enhanced the catalytic degradation process significantly through non-radical pathways. The Mn 0.8 Fe 2.2 O 4 MNCs exhibited desirable stability and reusability, that the spent Mn 0.8 Fe 2.2 O 4 MNCs could be significantly regenerated by thermal treatment at 450 °C in open air. Findings from this study would expand the applications of MOFs and also provide new insights into the enhancement of degradation efficiency during PMS activation processes.
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Nanomaterials
·
2025
·Vol. 15
·期 4
·283
·
IF 4.3
Zhiyuan Song,Sidra Chaudhary,Zainab Bibi,Yong Wu,Qinxiang Jia,Xiaoyong Li,Yang Sun
Two hydrophilic copolymers containing functional groups such as carboxyl, amido, and sulfonic acid are synthesized using ammonium persulfate-catalyzed free radical polymerization in water. Aluminum sulfate is then introduced, resulting in two polymer complexes that exhibit reduced cement setting times (initial, 1.16–2.44 min; final, 2.02–3.14 min) and improved compressive (24 h, 5.81–7.25 MPa) and flexural (24 h, 2.80–2.99 MPa) strengths compared to pure aluminum sulfate-facilitated cementing (initial, 19.11 min; final, 37.05 min; compressive, 24 h, 5.51 MPa; flexural, 24 h, 2.56 MPa). Following this, ball-milled illite powder is added, and the resulting admixtures further display slightly prolonged setting times (initial, 2.35–2.99 vs. 1.16–2.44 min; final, 3.98–4.35 vs. 2.02–3.14 min), along with comparable compressive strengths (5.85–7.11 vs. 5.81–7.25 MPa) and enhanced flexural strengths (3.92–5.83 vs. 2.80–2.99 MPa). Notably, a unique adhesive pozzolanic clinker, Ca54MgAl2Si16O90(54CaO·MgO·Al2O3·16SiO2), emerges in the presence of illite-based admixtures, contributing to the mechanical strength development of the hydrated mortars. Although illite itself is hydrophobic, the coating of ball-milled illite powder with aluminum sulfate and copolymers facilitates its dispersion into the gaps and pores of the cement matrix during setting, thereby increasing the flexural strength. This work presents an interesting approach to utilizing illite materials in cement applications, which is significant for reducing CO2emissions during cement production and use.
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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.
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Journal of Chemistry
·
2021
·Vol. 2021
·期 1
·5556295
·
IF 2.506
Zongqiang Zhu,Hongqu Yang,Jie Liu,Yinian Zhu,Shen Tang,Lihao Zhang,Xingxing Wang
Basic ferric sulfate-arsenates [FeSAsOH, Fe(SO 4 ) x (AsO 4 ) y (OH) z ·nH 2 O] were prepared and characterized to study their potential fixation of arsenic in the oxidizing and acidic environment through a dissolution for 330d. The synthetic solids were well-shaped monoclinic prismatic crystals. For the dissolution of the sample FeSAsOH–1 [Fe(SO 4 ) 0.27 (AsO 4 ) 0.73 (OH) 0.27 ·0.26H 2 O] at 25–45°C and initial pH 2, all constituents preferred to be dissolved in the order of AsO 4 3− > SO 4 2− > Fe 3+ in 1–3 h, in the order of SO 4 2− > AsO 4 3− > Fe 3+ from 1–3 h to 12–24 h, and finally in the order of SO 4 2− > Fe 3+ > AsO 4 3− . The released iron, sulfate, and arsenate existed dominantly as Fe 3+ /Fe(OH) 2+ /FeSO 4 + , HSO 4 − /SO 4 2− /FeSO 4 + , and H 3 AsO 4 0 /H 2 AsO 4 − , respectively. The higher initial pHs (6 and 10) could obviously inhibit the release of Fe 3+ from solid into solution, and the solid components were released in the order of SO 4 2− > AsO 4 3− > Fe 3+ . The crystal tops were first dissolved, and the crystal surfaces were gradually smoothed/rounded until all edges and corners disappeared. The dissociations were restricted by the Fe-O(H) breakdown in the FeO 6 octahedra and obstructed by the OH − and AsO 4 tetrahedra outliers; the lowest concentration of the dissolved arsenic was 0.045 mg/L. Based on the dissolution experiment at 25°C and pH 2, the solubility products ( K sp ) for the basic ferric sulfate-arsenate [Fe(SO 4 ) 0.27 (AsO 4 ) 0.73 (OH) 0.27 ·0.26H 2 O], which are equal to the ion activity products (logˍIAP) at equilibrium, were calculated to be -23.04 ± 0.01 with the resulting Gibbs free energies of formation (Δ G f o ) of −914.06 ± 0.03 kJ/mol.
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CONSTRUCTION AND BUILDING MATERIALS
·
2025
·
IF 8
Zhiyuan Song,Sidra Chaudhary,Yan Ding,Yujiao Yan,Kewei Peng,Yong Wu,Qinxiang Jia,Xiaoyong Li,Yang Sun
This study develops a series of functional admixtures for ordinary Portland cement based on a synthesized water-soluble terpolymer and its ball-milled composites with aluminum sulfate. The foundational admixture significantly accelerates cement setting, achieving an initial setting time of 4.33 min and a final setting time of 7.98 min, performance that exceeds the Chinese National Standard GB/T 35159–2017 requirements for flash-setting admixtures (which specify ≤5 min for initial setting and ≤12 min for final setting), while delivering a 24-hour compressive strength of 5.0 MPa and flexural strength of 1.6 MPa. The acceleration mechanism is attributed to the in-situ formation of the active intermediate (H 3 O)Al 3 (SO 4 ) 2 (OH) 6 . Incorporating potassium titanate whiskers—A3 derived from anatase (TiO 2 ) and A4 from metatitanic acid (TiO 2 ·H 2 O)—forms microcapsule-structured composites that further enhance performance. The A3-based composite reduces initial setting time to 3.83 min and final setting time to 7.10 min, while significantly improving mechanical strength, achieving a 24-hour compressive strength of 6.8 MPa that nearly meets the GB/T 35159–2017 standard requirement of ≥ 7.0 MPa at 24 h. A4-based whiskers provide comparable acceleration and demonstrate superior long-term flexural strength, reaching 5.1 MPa at 28 days. Mechanistic analysis reveals aluminum species drive rapid setting while whiskers enhance strength through distinctive phase transformations during hydration. Furthermore, 3-aminopropyltriethoxysilane-modified whiskers (both A3 and A4) produce admixtures that function as potent set retarders while simultaneously increasing 24-hour compressive and flexural strengths by 113 % and 91 % respectively compared to plain cement mortar, demonstrating exceptional superplasticizer characteristics. A key finding is the whisker-specific optimization strategy: silane pretreatment benefits A3 for achieving both accelerated setting and high strength, whereas unmodified A4 performs better in the same application. This work elucidates the design principles and mechanisms of tunable multifunctional cement admixtures, establishing strategic pathways for developing advanced construction materials suitable for applications ranging from shotcrete to oil well cementing.
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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.
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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.
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高影响因子
SYNTHESIS-STUTTGART
·
2019
·Vol. 51
·期 17
·3221-3230
·
IF 2.867
Wei Sun,Mingjuan Zhang,Peilang Li,Yiqun Li
A novel and highly efficient one-pot synthesis of polysubstituted imidazoles from α-hydroxyphenylacetic acids, diphenylacetylene, and amines has been achieved by Pd(OAc)2/Ce(SO4)2/Bi(NO3)3 trimetallic catalytic system. A series of control experiments showed that this overall reaction occurs through a one-pot cascade process combining the steps of decarboxylation of α-hydroxyphenylacetic acids, Wacker-type oxidation of diphenylacetylene, and Debus–Radziszewski annulation of aryl aldehydes and benzil generated in situ, as well as amines. This reaction represents a novel multicomponent reaction using α-hydroxyphenylacetic acids and diphenylacetylene as sources of aryl aldehydes and a β-diketone. This process exhibits a broad substrate scope and a good functional group tolerance to assemble the corresponding polysubstituted imidazoles in excellent yields (72–88%) under mild conditions.
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