CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2020
·
IF 2.627
Jiyuan Li,Mifen Cui,Zhuxiu Zhang,Xian Chen,Qing Liu,Zhaoyang Fei,Jihai Tang,Xu Qiao
Isooctane attracts great interest in recent years because of its promising potential as friendly-environmental gasoline, which is obtained by dimerization of isobutene with a hydrogenation step. Herein, a solid acid catalyst sulfated zirconia modified by ZnO was prepared. The oligomerization of isobutene had been investigated over ZrO 2 -SO 4 and ZnO( X )/ZrO 2 -SO 4 catalyst in order to find efficient catalysts for the production of isobutene oligomers . The presence of ZnO obviously enhanced the dimerization of isobutene and ZnO( X )/ZrO 2 -SO 4 exhibited the highest di-isobutene yield of 60%. Kinetic studies showed the higher trimerization-to-dimerization activation energy ratios of ZnO( X )/ZrO 2 -SO 4 than those of ZrO 2 -SO 4 from 353 to 393 K. In addition, reaction rate of dimerization was higher than trimerization over ZnO( X )/ZrO 2 -SO 4 . The high L/B ratio manifested the capability to enhance the selectivity of C 8 in isobutene dimerization. Furthermore, ZnO( X )/ZrO 2 -SO 4 exhibited stable conversion for the dimerization of isobutene.
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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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TURKISH JOURNAL OF CHEMISTRY
·
2022
·Vol. 45
·期 4
·1133-1145
·
IF 1.151
WANG DING-KAI,ZHAO WEI,CUI MING-YU,GUO TIAN-TIAN,FU SHUI-YUAN,LI WEI-GANG
A series of Zr(SO4)2/SiO2 solid acid catalysts with different Zr(SO4)2 loadings were prepared by water-soluble-impregnation method at room temperature. Then, the prepared catalysts were characterized by Fourier transform infrared spectroscopy, transmission electron microscopy and energy-dispersive X-ray spectrum, X-ray diffraction, adsorption/desorption of N2, and temperature-programmed desorption of NH3. The results showed that the active component Zr(SO4)2 was successfully adhered to the mesoporous SiO2, and the acid amount of Zr(SO4)2/SiO2 increased with the increasing of the Zr(SO4)2 loadings. Finally, the wheat stalk was used as raw material and depolymerized over Zr(SO4)2/SiO2 to produce ethyl levulinate (EL). The reaction mixture was separated and purified by filtration and vacuum distillation. The kinetic characteristics and the reaction pathway were also studied. A comparative study showed that 20 wt.% Zr(SO4)2/SiO2 exhibited higher catalytic activity. When reaction temperature, time, catalyst dosage and Zr(SO4)2 loadings were 190 °C, 50 min, 20 wt.% and 30 wt.%, the EL yield reached a maximum of 17.14%. The relative content of EL exceeded 90% after three steps of distillation.
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EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2020
·Vol. 2020
·期 10
·854-858
·
IF 2.529
Yaoguo Shen,Xiaoling Xue,Wenyuan Tu,Zhiqun Liu,Renwen Yan,Hong Zhang,Junrong Jia
Graphical An ultraviolet-transparent sulfate Cs 2 Ca 2 (SO 4 ) 3 has been synthesized. It exhibits a moderate second harmonic generation efficiency and has good thermal stability higher than those of most nonlinear optical sulfates reported recently. The noncentrosymmetric structure is one prerequisite of a nonlinear optical (NLO) material. Here, a sulfate Cs 2 Ca 2 (SO 4 ) 3 with a noncentrosymmetric structure was synthesized by high-temperature solid-state reaction, and its crystals were grown by spontaneous crystallization. Single-crystal X-ray diffraction indicates that Cs 2 Ca 2 (SO 4 ) 3 features a three-dimensional framework constituted by corner-sharing CaO 6 octahedra and SO 4 tetrahedra. Optical characterizations suggest that Cs 2 Ca 2 (SO 4 ) 3 is transparent down to 200 nm and exhibits a moderate second-order NLO response of about 0.6 × KH 2 PO 4 . Electronic band structure calculations were performed to elucidate the optical origin. Furthermore, the title compound has good thermal stability of up to about 1000 K, which is greatly higher than those of NLO sulfates reported recently. This work may shed useful light on the development of new NLO sulfates with high thermal stability.
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2026
·
IF 1.7
Li Shiyu,Fu Chengyun,Zhou Duo,Tian Qiang,Henderson Mark Julian,Zhu Shan,Yan Minhao
The adsorption of Sr 2+ and Cs + onto Gaomiaozi bentonite colloids (GMZC) was investigated to evaluate their role in radionuclide migration. The results show that within a concentration range of 20–100 mg·L⁻ 1 for Sr 2+ and Cs + , the distribution coefficient decreases with increasing ion concentration. The mechanistic study indicates that the adsorption of Sr 2+ is predominantly governed by surface complexation, whereas that of Cs + is mainly driven by ion exchange. Furthermore, Sr 2+ induces structural ordering of GMZC layers and promotes particle aggregation. However, in Na-Cl-SO 4 groundwater, the bentonite suspension showed poor stability and a significantly weakened adsorption capacity for both 90 Sr and 137 Cs, demonstrating the decisive impact of water chemistry on its barrier function.
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ACS Catalysis
·
2021
·
IF 13.084
Jinqiu Guo,Zongjing Feng,Jun Xu,Jie Zhu,Guanghui Zhang,Yaping Du,Hongbo Zhang,Chunhua Yan
Ethanol transformation with high product selectivity is a great challenge, especially for high weight molecules. Here, we show a combination study of kinetic, thermodynamic, and in situ spectroscopy measurements to probe the selective upgrading of ethanol over lamellar Ce(OH)SO4·xH2O catalysts, with 60–70% Ce3+ preserved during the catalysis. High methyl phenols (MPs) selectivity at ∼80% within condensation products was achieved at ∼50% condensation yield (3.0 kPa C2H5OH, 15 kPa H2, Ar balanced, 693 K, 1 atm, gas hourly space velocity (GHSV) ∼5.4 min–1), with acetaldehyde, acetone, 4-heptanone, and 2-pentanone as the key reaction intermediates. Kinetic measurements with the assistance of isotope labeling proved that MPs generated from the kinetically relevant step (KRS) of C–C bond coupling of enolate nucleophilically attacks surface C2H4O following a Langmuir–Hinshelwood model. Low ethanol and water pressures and high acetaldehyde and hydrogen pressures were proved to be favored for MPs generation rather than dehydration, in which hydrogen could reduce the amount of lattice oxygen and facilitate the preparation of MPs while water and ethanol both compete with acetaldehyde for active sites during catalysis. On the basis of in situ X-ray diffraction (XRD), quasi-in situ X-ray photoelectron spectroscopy (XPS), and Raman characterizations, the Ce(OH)SO4 crystal structure was proved to be maintained along with ethanol activation, and the Ce3+–OH Lewis acid–base pair was proved to be the active species for the selective C–C bond coupling. The KRS assumption was also supported by the apparent activation energy assessment within the reaction network on dehydration, dehydrogenation, aldol condensation, and cyclization and a series of negligible kinetic isotope effects (KIEs). This system can be easily extended to some other systems related to C–C bond coupling and is attracting attention on converting oxygenate platform molecules over lanthanide species.
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Journal of Materials Chemistry C
·
2018
·Vol. 6
·期 45
·12240-12244
·
IF 5.976
Yanqiang Li,Sangen Zhao,Pai Shan,Xianfeng Li,Qingran Ding,Shuai Liu,Zhenyue Wu,Sasa Wang,Lina Li,Junhua Luo
Sulfates have long been ignored as nonlinear optical materials over the past decades. Here we report a new sulfate deep-ultraviolet nonlinear optical material Li8NaRb3(SO4)6·2H2O synthesized by the facile water solution method. It crystallizes in the asymmetric monoclinic space group C2 (No. 5). Its single-crystal structure features a three-dimensional framework made up of SO4 and LiO4 tetrahedra. Powder second-harmonic generation tests demonstrate that Li8NaRb3(SO4)6·2H2O is phase-matchable with a second-harmonic generation response of about 0.5 × KH2PO4. Ultraviolet-visible-near-infrared diffuse reflectance spectra illustrate that the ultraviolet cutoff edge of Li8NaRb3(SO4)6·2H2O may be as low as λ < 190 nm. Theoretical calculations reveal that the optical properties of Li8NaRb3(SO4)6·2H2O are mainly attributed to S–O groups. All these results reveal that Li8NaRb3(SO4)6·2H2O may possess potential use in the deep-ultraviolet nonlinear optics field. We believe that the discoveries in our work will attract scientists’ attention to sulfate systems for their potential as deep-ultraviolet nonlinear optical materials.
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Materials Chemistry Frontiers
·
2025
·
IF 6.4
Xiyue Zhang,Yingjie Zhou,Minjie Hou,Xiecheng Yang,Kun Ren,Peng Dong,Jiaqian Qin,Da Zhang,Feng Liang
To meet the urgent requirement for sustainable energy storage technologies, incorporating effective waste management into the design of energy storage materials can achieve a closed-loop supply chain from waste to energy. Herein, extrinsic pseudocapacitive (PDC) cathode materials with different carbon contents were synthesized using FeSO4·7H2O waste through a simple ball milling and annealing process, which enhances sodium storage kinetics and achieves waste recycling. The results indicate that NFSO particles and graphite flakes create a disordered porous structure, which enhances the PDC effect, thus overcoming the slow migration rate of sodium-ions. Specifically, the diffusion coefficient of NFSO/C-10 increased by around an order of magnitude compared to that of NFSO, increasing from 10−12 to 10−11. The discharge capacity reached 84 mA h g−1 at 0.2C (1C = 91 mA g−1). The present work realizes the high-value reuse of waste and highlights the crucial role of the PDC effect in enhancing diffusion dynamics, which opens up a new direction for the design and synthesis of high-rate iron-based sulfate cathode materials.
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RESEARCH ON CHEMICAL INTERMEDIATES
·
2017
·Vol. 43
·期 8
·4353-4368
·
IF 1.369
Yuan Hong,He Jie,Li Ruilan,Ma Xiaoqin
The solid acid catalysts SO 4
2− /TiO 2 were prepared by the impregnation technique under two preparation conditions which were different in calcination temperature and concentration of impregnation solution of H 2 SO 4 . The characterization was carried out by using Fourier transform infrared spectrometer (FTIR), X-ray diffraction (XRD), temperature programmed desorption of NH 3 (NH 3 -TPD), N 2 -BET, X-ray fluorescence and thermal gravity (TG)–differential scanning calorimetry (DSC). The characteristic peaks in the FTIR spectrum were essentially the same within the calcination temperature range of 400–600 °C. The XRD results indicated that the sample could show partial specific peaks of the anatase phase as the calcination temperature was higher than 400 °C. The obvious strong acid and superacid sites of the prepared SO 4
2− /TiO 2 were conformed by the NH 3 -TPD results. The BET surface areas of 102–206 m 2 /g were measured by the N 2 -BET method, and the pore size distributions were essentially mesoporous. The TG–DSC results showed that SO 4
2− /TiO 2 would decompose at about 500 °C in the air. The solid acid SO 4
2− /TiO 2 were used for the epoxidation of castor oil. The lowest iodine value of the product was 52.65/100 g when the reaction temperature was 65 °C, reaction time was 10 h and catalyst loading was 15 wt.%.
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APPLIED ENERGY
·
2019
·
IF 8.426
Zain Ali Saleh Bairq,Hongxia Gao,Yufei Huang,Haiyan Zhang,Zhiwu Liang
A significant impediment to the widespread adoption of amine-based post-combustion technique for CO 2 capture from flue gas is the huge energy demand for amine solvent regeneration. In this study, five novel bifunctional heterogeneous catalysts e.g., SO 4 2− /ZrO 2 /SiO 2 with different molar ratios of zirconia and SO 4 2− /ZrO 2 as a parent catalyst were synthesized and applied to evaluate their effectiveness in enhancing the CO 2 desorption and solvent regeneration of 5M monoethanolamine solution with CO 2 loading of 0.5 ± 0.01 mol CO 2 /mol monoethanolamine at 97 °C. The catalysts were characterized by Fourier transform-infrared spectrometry, pyridine-infrared spectroscopy, X-ray diffraction, N 2 -adsorption-desorption, and ammonia-temperature programmed desorption. The results demonstrated that these catalysts can significantly reduce the heat duty for CO 2 desorption by 36.48% compared to without catalyst and enhance desorption rate by 35.1%. The results also showed that SO 4 2− /ZrO 2 /SiO 2 15% presented the highest efficiency compared to the other SO 4 2− /ZrO 2 /SiO 2 ratios and the super solid acid catalyst SO 4 2− /ZrO 2 . Additionally, to investigate if the catalysts induce any unfavorable effects on the amine, the absorption of CO 2 by regenerated amine solvent was studied. Finally, a reaction mechanism for the amine solvent regeneration with the synthesized catalyst e.g., SO 4 2− /ZrO 2 /SiO 2 was suggested.
研究领域:
化学工程
·
环境科学
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FUEL
·
2022
·
IF 8.035
Chengrui Wang,Yanhong Fang,Zhenghao Wang,Mujun Long,Dengfu Chen,Huamei Duan,Yandong Li,Guoquan Zhang
Partially oxidizing methane into syngas via a two-step chemical looping scheme was a promising option for methane transformation. Ce 2 (SO 4 ) 3 was selected to explore the performance and mechanism of methane chemical looping partial oxidation (CLPOM) to syngas. Thermodynamic and kinetic analysis forecast the Ce 2 (SO 4 ) 3 as a promising candidate for CLPOM. Compared with literature, Ce 2 (SO 4 ) 3 not only had an outstanding syngas selectivity, but also an appropriate CH 4 conversion and molar ratio, and CH 4 conversion could reach 90.5 % of thermodynamic result. As revealed via characterization, Ce 2 (SO 4 ) 3 (1 0 2) surface had the highest peak intensity and the migration of lattice oxygen played an important role in CLPOM. Some of them were tend to agglomeration and these small particles were less than 5 μm. Density functional theory calculations demonstrated that CH 4 series dehydrogenation products tended to adsorb at O site and CH 3 → CH 2 + H was the rate-determining step. The reaction of surface lattice oxygen atoms and migration of the internal lattice oxygen atoms could inhibit carbon deposition, promote CH 4 conversion and syngas generation in experiment. Compared with NiO, Ce 2 (SO 4 ) 3 had a lower energy barrier of lattice oxygen migration, which could increase the reaction rate.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Ting Li,Xiaomeng Wang,Yanmei Chen,Jianru Liang,Lixiang Zhou
Heterogeneous Fenton has become a promising economical and environmentally-friendly method for water treatment, however, the production of abundant radical resources (e.g., O 2 − , OH) are oftentimes limited by finite Fe 2+ species to activate H 2 O 2 . Therefore, development of a new iron-bearing solid modified with diverse functional groups for generating a large of radicals in heterogeneous Fenton is significance. Here, we constructed a Fe 3 O 4 -modified schwertmannite (Fe 3 O 4 /Sch) catalyst to activate H 2 O 2 , SO 4 2− and O 2 to produce three kinds of radicals in heterogeneous Fenton reaction. Specifically, Fe 3 O 4 /Sch catalyst was synthesized to improve its surface properties such as the contents of surface Fe 2+ species as H 2 O 2 or O 2 activators to produce OH or O 2 − , the SO 4 2− of Sch surface as SO 4 − precursor, and electron transfer between Fe 3+ and Fe 2+ . Degradation rate of ciprofloxacin (CIP) for 6 min was up to 97% in Fe 3 O 4 /Sch-H 2 O 2 system, which was higher than that in Sch-H 2 O 2 or Fe 3 O 4 -H 2 O 2 . After four successive cyclic experiments, degradation rate of CIP was still achieved 97% within 10 min in Fe 3 O 4 /Sch-H 2 O 2 system. The formation pathways of the relevant active radicals and the degradation pathways of CIP were also proposed by theoretically calculated and LC-MS data. This finding has not only developed an efficient heterogeneous Fenton catalyst, but also given a new idea of SO 4 − generation by modified iron oxyhydroxysulfate mineral for application of heterogeneous Fenton technology.
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