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
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环境科学
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DOI
高影响因子
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.
研究领域:
催化化学
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环境科学
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材料科学
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产品关联
DOI
高影响因子
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.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2021
·Vol. 45
·期 45
·21278-21284
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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
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材料科学
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化学工程
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DOI
高影响因子
Water
·
2024
·Vol. 16
·期 9
·1281
·
IF 3
Xiuneng Zhu,Jie Qiu,Yexing Wang,Yulin Tang,Yongji Zhang
There is more and more research focusing on the removal of dioxane by advanced oxidation technology at this stage, and this study investigated the efficacy of an advanced oxidation system with UV-activated persulfate (UV/PDS). This method had the advantages of fast reaction rate, simple equipment and convenient operation. Free radical quenching test and electron paramagnetic resonance (EPR) analysis showed that the main active radicals in the reaction system wereSO4−and ·OH. This study also investigated that the optimal parameters were the initial PDS dosage of 3 mM, the UV intensity of 0.190 mM/cm2, the pH between 5 and 7 and the initial dioxane concentration of 50 mg/L. Additionally, after a reaction time of 150 min, the total organic carbon (TOC) content still remained at 83.53%, which revealed that the mineralization degree of organic matter was not fully achieved through UV/PDS treatment. The concentration ofSO42−in the reaction system was 74.69 mg·L−1, which complied with the standard concentration specified. Furthermore, the cytotoxicity of the system exhibited an initial increase followed by a subsequent decrease, under the influence of the intermediates. It showed that the technology could efficiently degrade organic pollutants.
研究领域:
环境科学
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化学工程
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水处理
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DOI
高影响因子
ACS Applied Materials & Interfaces
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2022
·
IF 10.383
Jie Wu,Yuanyuan Zhang,Bin Zhang,Siwei Li,Ping Xu
Development of low-cost, efficient, and durable electrocatalysts for the oxygen evolution reaction (OER) is crucial for multiple energy conversions and storage devices. Herein, Zn-doped CoS2 nanoarrays supported on carbon cloth, Co(Zn)S2/CC, are fabricated through a facile sulfidization of CoZn metal–organic frameworks. This precatalyst, Co(Zn)S2/CC, with a well-defined nanoarray structure affords excellent OER catalytic activity (η = 248 mV at 10 mA/cm2) and long-term durability in 1 M KOH. X-ray photoelectron and in situ Raman spectroscopic studies indicate that Co(Zn)S2 undergoes surface reconstruction with the generation of Co(Zn)OOH adsorbed with SO42– at the surface during the OER process. The Zn dopant is calculated to impact on the electronic structure of Co species and further the adsorption of intermediates. This work not only provides a novel method for the synthesis of bimetallic sulfides but also gives insights into the doping effect on the OER performance of transition metal sulfides.
研究领域:
电化学
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材料科学
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能量转换与存储
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产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Shi-Wen Lv,Xiaoran Wang,Xing Wei,Yi Zhang,Yanqing Cong,Lin Che
Nowadays photocatalysis assisted advanced oxidation processes exhibited a great application prospects in pollution control. Herein, for the first time, a series of transition metal modified UiO-66-NH 2 (namely Fe-UiO-66-NH 2 , Co-UiO-66-NH 2 and Ni-UiO-66-NH 2 ) were synthesized via a simple method. After that, these functional materials were employed as photocatalyst to activate PMS for degrading BPA under visible light irradiation. Significantly, prepared Fe-UiO-66-NH 2 exhibited the highest photocatalytic activity among these samples. More importantly, proposed Fe-UiO-66-NH 2 /PMS/light oxidation system showed excellent degradation ability for various organic pollutants, including BPA, TC, OFX, IBP as well as SMX. Owing to the occurrence of d-d transitions after the coordination of transition metal ions, UiO-66-NH 2 displayed the enhanced utilization efficiency of visible light. Furthermore, introduced Fe ion as a mediator could boost the charge transfer by the cluster-to-metal way, thereby effectively inhibiting the recombination of photogenerated electrons and holes. In addition, embedding cluster-to-metal charge transfer in UiO-66-NH 2 modified the band structure, and both SO 4 −• and OH were major active species in the photocatalytic reaction system. Developed Fe-UiO-66-NH 2 /PMS/light oxidation system with good stability also presented great antibacterial performance. To sum up, current work could provide some novel inspirations for designing the high-efficiency photocatalyst.
研究领域:
环境科学
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材料科学
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化学
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DOI
高影响因子
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
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土木工程
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建筑材料
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水泥化学
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聚合物复合材料
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Peng Chen,Yejing Gou,Jiaming Ni,Yumeng Liang,Bingqiao Yang,Feifei Jia,Shaoxian Song
Base on the strong activation activity and affinity of transition metal ions and MoS 2 for peroxymonosulfate (PMS), respectively, Co(Ⅱ)-doped MoS 2 nano-flowers (Co-MoS 2 NFs) with a great photo-response property was facilely synthesized to achieve a more efficient PMS activation for ofloxacian (OFX) degradation. It was found that Co-MoS 2 NFs exhibits superior catalytic activity for OFX degradation under visible-light irradiation, which was attributed to the synergetic effect of doped Co(Ⅱ) and photo-generated carriers to PMS activation. Besides, Co-MoS 2 NFs was able to efficiently degrade OFX within 4 cycles in the presence of PMS while leaked minute amount of Mo and Co ions, implying the excellent cycle stability of Co-MoS 2 NFs. Furthermore, SO 4 •− and 1 O 2 were detected as the primary reactive radicals for OFX degradation in the Co-MoS 2 NFs-PMS system through EPR and quenching tests. This new strategy of coupling doped Co(Ⅱ) and photo-generated carriers for more efficient PMS activation, which will greatly benefit the development of SO 4 •− -based AOPs as well as cater to the demand for environmental remediation in the future.
研究领域:
环境科学
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材料科学
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化学工程
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Peishan Li,Hui Ma,Sijia Qian,Yi Chen,Bo Lai,Shengyan Pu
Ferric sulfide is an appealing activator in persulfate (PS) activation process for degrading pollutants from aqueous environment, but the drawback of easy-agglomeration lead to a low utilization efficiency. In this study, we modified nFeS with sodium carboxymethyl cellulose (CMC) to improve its stability, and the performance for PS activation and p -nitrophenol (PNP) degradation is tested. After modification, the size further decreased from 23.8 to 18.4 nm, but with higher stability and catalytic reactivity. The CMC and nFeS is bonded by bidentate bridging of Fe-O bond. The degradation performance increased ∼7 times. The PS activation with CMC-nFeS activator shows higher reaction rate constant (0.093 min -1 ) with ∼90% of PNP removed compared to the pure nFeS with ∼80% of PNP removal at a low rate (0.014 min -1 ) with the same condition of 0.6 g/L activator, 8 mM PS, room temperature and initial pH in 90 min. Acidic condition and high temperature were more favorable for releasing Fe(II) to activate PS and produce active radicals. SO 4 - ·and HO·radicals played critical roles to attack on PNP. Detailed XPS analysis of the activator before and after reaction described the removal pathway as heterogeneous and homogeneous systems. Density Functional Theory (DFT) simulation results confirmed that CMC addition effectively decreased the interaction energy and improved adsorption ability of PS onto the activator surface.
研究领域:
环境科学
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化学工程
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材料科学
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产品关联
DOI
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.
研究领域:
有机化学
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催化化学
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药物化学
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合成方法学
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杂环化学
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DOI
高影响因子
Green Energy & Environment
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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
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催化
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水处理
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DOI
高影响因子
危险品化学品经营许可证（带存储）