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.
研究领域:
化学
·
环境科学
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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 COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Zhiming Sun,Rui Zhu,Tianle Ding,Xiangwei Zhang,Chunquan Li
Persulfate activation technology based on sulfate radicals is currently a hot spot in the field of environmental governance. In our work, α-FeOOH was successful in situ loaded on kaolinite surface through a simple one-step hydrothermal process. The prepared composites were systematically characterized, and the relationship between the structural properties and peroxymonosulfate activation properties was explored. Interestingly, compared to bare α-FeOOH, the introduction of kaolinite in composite induced the transformation of α-FeOOH crystal and affected the morphology, where uniformly dispersed nanoparticles rather than rod-like agglomerated crystals appeared. The received FeOOH/kaolinite composite exhibited admirable adsorption and degradation of ciprofloxacin performance with the removal efficiency of 86.1%, and the degradation rate constant was up to 5.2 times higher than that of bare α-FeOOH. In addition, the main active species in the catalytic oxidation system are surface-bound SO 4 •− , • OH and free 1 O 2 . This work would give a deep insight into the role of natural minerals in composite catalytic materials and the construction of high-efficient mineral-based composite materials.
研究领域:
环境科学
·
催化
·
材料科学
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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.
研究领域:
材料科学
·
土木工程
·
建筑材料
·
水泥化学
·
聚合物复合材料
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 45
·期 45
·21278-21284
·
IF 3.591
Yanqing Cong,Xiang Chen,Wanxing Wang,Shi-Wen Lv
The photocatalytic technique is an attractive strategy to activate persulfate for generating free radicals in the wastewater purification process. Herein, CdS nanoparticles with unique optical properties were employed to decorate the COF-based photocatalyst (denoted as TpMA) containing C3N4 active units via a feasible method. Interestingly, TpMA decorated with CdS nanoparticles exhibited enhanced optical absorbability and a small charge transfer resistance. Benefitting from the close interfacial connections between CdS nanoparticles and TpMA, the recombination of photogenerated electrons and holes could be effectively inhibited. As expected, the obtained CdS@TpMA composites displayed excellent photocatalytic activity, which could activate persulfate to produce SO4−˙ and ˙OH under visible light irradiation. In comparison with pristine CdS nanoparticles and TpMA, the 25% CdS@TpMA composite presented the best photocatalytic degradation ability, and 97.6% of diclofenac sodium, 95.2% of tetracycline and 93.8% of ibuprofen could be effectively removed within 70 min. The corresponding TOC removal efficiencies were more than 60%. More significantly, the 25% CdS@TpMA composite displayed great performance and structural stabilities. Furthermore, a possible photocatalytic mechanism was also proposed. In short, the current work not only provides a promising candidate for degrading drug residues, but also offers some novel viewpoints for further research.
研究领域:
环境科学
·
材料科学
·
化学工程
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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.
研究领域:
有机化学
·
催化化学
·
药物化学
·
合成方法学
·
杂环化学
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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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高影响因子
Materials
·
2024
·Vol. 17
·期 19
·4762
·
IF 3.1
Zhiyuan Song,Zainab Bibi,Sidra Chaudhary,Qinxiang Jia,Xiaoyong Li,Yang Sun
A water-soluble ternary copolymer bearing carboxyl, sulfonic, and amide functional groups was synthesized using ammonium persulfate-catalyzed free radical polymerization in water, resulting in high monomer conversion. This copolymer was then complexed with aluminum sulfate, forming an admixture containing Al(SO 4 )(OH)·5H 2 O, which was subsequently combined with silica gel. Characterization revealed that the synthesized copolymer formed a large, thin membrane that covered both the aluminum compounds and the silica gel blocks. The introduction of this complex admixture, combining the copolymer and aluminum sulfate, not only reduced the setting times of the cement paste but also enhanced the mechanical strengths of the mortar compared to using aluminum sulfate alone. The complex admixture led to the formation of katoite, metajennite, and C 3 A (tricalcium aluminate) in the mortar, demonstrating significant linking effects, whereas pure aluminum sulfate could not completely transform C 3 S within 24 h. Further addition of silica gel to the complex admixture further shortened the setting times of the paste, slightly reduced compressive strength, but improved flexural strength compared to the initial complex admixture. The silicon components appeared to fill the micropores and mesopores of the mortar, accelerating cement setting and enhancing flexural strength, while slightly decreasing compressive strength. This study contributed to the development of new cementing accelerators with improved hardening properties.
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Green Energy & Environment
·
2020
·
IF 6.395
Hongmin Zhang,Qingzhu Jia,Fangyou Yan,Qiang Wang
In this study, a series of CuMgAl layered double oxides (CuMgAl-LDOs) were obtained via calcination of CuMgAl layered double hydroxides (CuMgAl-LDHs) synthesised via a co-precipitation method. The results show that CuMgAl-LDO can be prepared using an optimal Cu : Mg : Al molar ratio of 3 : 3 : 2, NaOH : Na 2 CO 3 molar ratio of 2 : 1, and calcination temperature of 600 °C. CuMgAl-LDO is a characteristic of mesoporous material with a lamellar structure and large specific surface area. The removal efficiency of sulfameter (SMD) based on CuMgAl-LDO/persulfate (PS) can reach > 98% over a wide range of initial SMD concentrations (5–20 mg L −1 ). The best removal efficiency of 99.49% was achieved within 120 min using 10 mg L −1 SMD, 0.3 g L −1 CuMgAl-LDO, and 0.7 mmol L −1 PS. Kinetic analysis showed that the degradation of SMD was in accordance with a quasi-first-order kinetic model. The stability of the CuMgAl-LDO catalyst was verified by the high SMD removal efficiency (> 97% within 120 min) observed after five recycling tests and low copper ion leaching concentration (0.89 mg L −1 ), which is below drinking water quality standard of 1.3 mg L −1 permittable in the U.S. Radical scavenging experiments suggest that SO 4 · − is the primary active species participating in the CuMgAl-LDO/PS system. Moreover, our mechanistic investigations based on the radical scavenging tests and X-ray photoelectron spectroscopy (XPS) results indicate that Cu (II) –Cu (III) –Cu (II) circulation is responsible for activating PS in the degradation of SMD and the degradation pathway for SMD was deduced. Accordingly, the results presented in this work demonstrate that CuMgAl-LDO may be an efficient and stable catalyst for the activation of PS during the degradation of organic pollutants.
研究领域:
环境科学
·
催化
·
水处理
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危险品化学品经营许可证（带存储）