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FUEL · 2020 · IF 5.578

Catalytic hydroconversion of extraction residues from two Chinese lignites to arenes

Mei-Xia Zhao,Ning Yang,Heng-Shen Xie,Zheng Zhao,Zhi-Min Zong,Xian-Yong Wei

A solid superacid TFMSA/MPZCA was prepared by impregnating trifluoromethanesulfonic acid (TFMSA) into mesoporous zirconia-coated attapulgite (MPZCA). Using TFMSA/MPZCA, the catalytic hydrocracking of coal-related model compounds (CRMCs) oxybis(methylene)dibenzene (OBMDB), benzyloxybenzene (BOB), and di(1-naphthyl)methane (DNM) and the catalytic hydroconversion (CHC) of extraction residues (ERs, isometric carbon disulfide/acetone-insoluble portion) from Huozhou lignite (HL) and Shaerhu lignite (SL) in cyclohexane without H 2 were investigated. According to the model reactions, H + released from TFMSA in TFMSA/MPZCA plays a crucial role in cleaving the > C alk -O- and > C ar -C < bridged linkages (BLs) in the CRMCs, and the BLs of > C alk -O- in OBMDB and BOB can be completely cleaved at 170 °C and 190 °C for 3 h, respectively, while the BL of > C ar -C < in DNM was not completely cleaved even at 320 °C. At 300 °C, the yields of soluble portions (SPs) from the CHC of HL- and SL-derived ERs significantly increase compared with the non-catalytic hydroconversion of both ERs. Arenes are predominantly abundant in the SPs from the CHC of both ERs and the most abundant compound in the SPs is mesitylene.

研究领域: 化学工程 · 能源科学
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FUEL · 2018 · IF 4.908

Catalytic hydroconversion of Yiwu lignite over solid superacid and solid superbase

Zhong-Qiu Liu,Xian-Yong Wei,Fang-Jing Liu,Guang-Hui Liu,Zhi-Min Zong

Trifluoromethanesulfonic acid supported on attapulgite powder (TFMSA/AP) and Mg 2 Si/γ-Al 2 O 3 were facilely prepared by impregnating TFMSA onto AP and Mg 2 Si onto γ-Al 2 O 3 . The extraction residue from Yiwu lignite (YL ER ) was subjected to non-catalytic hydroconversion (NCHC) and catalytic hydroconversion (CHC) over TFMSA/AP and Mg 2 Si/γ-Al 2 O 3 , respectively. Detailed molecular compositions of the soluble portions from the NCHC (SP NCHC ) and CHC over TFMSA/AP (SP CHC-A ) and Mg 2 Si/γ-Al 2 O 3 (SP CHC-B ) were characterized with a gas chromatograph/mass spectrometer. As a result, the yields of SP CHC-A and SP CHC-B are 19.6% and 17.5%, respectively, which are much higher than that of SP NCHC (1.04%), suggesting that both TFMSA/AP and Mg 2 Si/γ-Al 2 O 3 show excellent activity for the CHC of YL ER . Arenes and arenols are predominant in SP CHC-A and SP CHC-B , respectively, while large amounts of alkanoates were detected in SP NCHC . The results indicate that TFMSA/AP effectively catalyzes the cleavage of C ar –C alk and C alk –O bridged bonds (BBs) in YL ER , while Mg 2 Si/γ-Al 2 O 3 significantly promotes the cleavage of C–O BBs in YL ER . Di(1-naphthyl)methane, 1-methylnaphthalene, oxydibenzene, and benzyloxybenzene were used as coal-related model compounds (CRMCs) for the CHC to further explore the catalysis of TFMSA/AP and Mg 2 Si/γ-Al 2 O 3 . The results show that TFMSA/AP not only releases mobile H + but also heterolytically splits H 2 to form an immobile H − and a mobile H + , leading to the cleavage of C alk –C ar and C alk –O BBs in the CRMCs. In contrast, Mg 2 Si/γ-Al 2 O 3 facilitates heterolytically splitting H 2 to an immobile H + and a mobile H − , resulting in the cleavage of C–O BBs in the CRMCs.

CAS / MDL: 1344-28-1 1493-13-6
研究领域: 化学工程 · 煤炭化学
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FUEL · 2022 · IF 8.035

Sulfate-enhanced low-temperature activity of Pt/γ-Al2O3 for landfill gas deoxygen

Xinyu Yang,Zezhi Chen,Huijuan Gong,Feng Lin,Tingting Zhu,Ziyi Yang

Deoxygen is a crucial step for landfill gas (LFG) recycling and purification. Pt/γ-Al 2 O 3 is the most active catalyst for LFG deoxygen via catalytic methane oxidation . It is challenging but significant to further improve the performance of this type of catalyst. In regard of homogeneous and heterogeneous activation of methane by superacids , here we demonstrate LFG deoxygen via catalytic methane oxidation using a solid superacid catalyst, Pt/SO 4 2- /Al 2 O 3 , synthesized using pre-sulfated γ-Al 2 O 3 support by impregnated with sulfuric acid . In comparison to Pt/γ-Al 2 O 3 , Pt/SO 4 2- /Al 2 O 3 catalysts exhibit exceptionally improved activity and minimum complete O 2 conversion at a temperature of 264 ℃, a decrease of about 51 ℃. This value is superior to the state-of-the-art Pt-based deoxygen catalysts. Characterizations and theoretical calculations indicate that sulfation enhances the amount of acid sites on γ-Al 2 O 3 support and induces electron deficiency of the supported Pt species (+0.28|e|), thus boosting the low-temperature activity. Furthermore, the Pt/SO 4 2- /Al 2 O 3 catalyst maintained its initial activity after six runs without any detectable coke deposition. This discovery offers simple and effective strategies to precisely design higher performance application-oriented Pt based deoxygen catalysts.

CAS / MDL: 18497-13-7
研究领域: 催化 · 环境工程 · 材料科学
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Materials Today Communications · 2020 · IF 2.678

Comparative study on flame retardancy of multiple solid super acids-containing epoxy resin composites

Xuexi Chen,Jiahui Shen,Mei Wan,Ming Gao,Lina Yue

Five different solid superacids (SO 4 2− /TiO 2 -M X O Y ), including SO 4 2- /TiO 2 -CuO, SO 4 2- /TiO 2 -ZrO 2 , SO 4 2- /TiO 2 -Fe 2 O 3 , SO 4 2- /TiO 2 -MnO, and SO 4 2- /TiO 2 -MoO 3 , were successfully synthesized and characterized. Then, the fire retarded performance, smoke suppression and thermal stability of the epoxy resin (EP)/melamine coated ammonium polyphosphate (MAPP)/SO 4 2− /TiO 2 -M X O Y composites were investigated in details. The results showed that these SO 4 2− /TiO 2 -M X O Y can effectively enhance the limiting oxygen index (LOI) values of the EP/MAPP composites. Compared with that of the EP/MAPP composites, the total heat release (THR) values of the EP/MAPP/SO 4 2− /TiO 2 -Fe 2 O 3 , EP/MAPP/SO 4 2− /TiO 2 -ZrO 2 , EP/MAPP/SO 4 2− /TiO 2 -MnO and EP/MAPP/SO 4 2− /TiO 2 -MoO 3 composites were remarkably reduced by 6%, 27 %, 32 % and 25 %, respectively, and the peak of heat release rate (PHRR) values of the EP/MAPP/SO 4 2− /TiO 2 -Fe 2 O 3 , EP/MAPP/SO 4 2− /TiO 2 -ZrO 2 , EP/MAPP/SO 4 2− /TiO 2 -CuO, EP/MAPP/SO 4 2− /TiO 2 -MnO and EP/MAPP/SO 4 2− /TiO 2 -MoO 3 composites were reduced by 0.3 %, 56.8 %, 23.6 %, 26.9 % and 36.9 %, respectively. Moreover, for the solid superacids-containing EP composites, the initial decomposition temperatures ( T i ) and the temperatures at the maximum mass loss rate ( T Max ) were advanced, and the char yields at 800 °C were much increased, which was indicated the considerable effect on the thermal degradation and char formation. Hence, the MAPP and SO 4 2− /TiO 2 -M X O Y had good synergistic flame retardancy and smoke suppression, and the best for SO 4 2− /TiO 2 -MnO.

CAS / MDL: 89-63-4 99-99-0 99-08-1
研究领域: 材料科学 · 化学工程
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RSC Advances · 2014 ·Vol. 4 ·期 64 ·34161-34167 · IF 3.708

Char strengthened by carbon microspheres formed in situ during combustion of IFR/EVA composites catalyzed by solid super acid

Wenpeng Ding,Juan Li,Kang Tao

Solid super acid (SSA) as a kind of green catalyst was introduced into conventional intumescent flame retardant (IFR)/ethylene-vinyl acetate (EVA) composites to increase their flame retardant efficiency. The IFR used was a combination of ammonium polyphosphate coated by melamine resin (MAPP) and pentaerythritol (PER) with weight ratio at 3 : 1. TGA results showed that the SSA promoted the reaction between MAPP and PER. The thermal degradation temperature of the IFR/EVA composites with 1.5 wt% SSA was significantly increased by 95 °C compared to that of IFR/EVA. The UL 94 V-0 rating can be achieved for EVA composites with 13 wt% total amount of IFR and SSA, while the EVA composites with individual 13 wt% IFR only passed the UL-94 V-2 rating. The char residues at 800 °C of SSA/IFR/EVA composites were 5.8 wt%, which was higher than 2.4 wt% of IFR/EVA composites. Many carbon microspheres were observed by SEM which were deposited in the char matrix after the cone calorimeter test. These carbon microspheres had better graphite structure, thus the char was strengthened and could resist more heat and gas flow erosion. The synergistic effect between the gas phase and condensed phase was considered the main factor for the increase of flame retardant properties.

CAS / MDL: 127-18-4
研究领域: 材料科学 · 化学工程
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CHEMICAL ENGINEERING SCIENCE · 2016 · IF 2.75

Fabrication and characterization of novel hollow fiber catalytic packing of PFSA–PES–ZrO2 (shell)–TiO2 (core) solid superacid via wet-spinning method

Chen-Hao Ji,Shuang-Mei Xue,Zhen-Liang Xu,Xiao-Hua Ma

In this work, a novel hollow fiber catalytic packing (HFCP) was fabricated of ZrO 2 (shell)/TiO 2 (core) (TZ) solid superacid nanoparticles , perfluorinated sulfonic acid resin (PFSA) and polyethersulfone (PES) via wet-spinning method. TZ was a homemade binary solid superacid nanoparticles with core–shell structure using superfine titania (5   nm) as the core and mesoporous tetragonal phase zirconia as the shell. It was synthesized through the hydrolysis of zirconium oxychloride in the presence of titania nanoparticles and cetyltrimethylammonium bromide (CTAB) hexagonal crystals covered on the titania core and followed by calcination and acidification. HFCPs demonstrated well catalytic performance in the esterification test of ethanol and acetic acid due to the superacid sites on the surface of TZ and PFSA polymer chain. And the superacid sites on the PFSA polymer chain could be sufficiently exposed by the embedding of the nanoparticles. At the same time, HFCPs also showed ultrahigh recovery which was more than 99.5% in 6 runs because of the well integrality benefited from the wet-spinning method. The specific surface area (SSA) and pore size distribution were analyzed by N 2 adsorption–desorption, the result showed that the SSA of HFCPs decreased with the increasing of the PFSA additive amount. The SSA of the HFCP with the best catalytic performance could be up to 90.60   m 2 /g, in which the PFSA weight proportion was 13%. The XRD pattern and HRTEM image showed the HFCPs i.e. the zirconia shell of TZ formed uniform tetragonal phase. Other characterizations such as FT-IR, XPS, SEM and TEM were utilized to determine the chemical composition and morphology of the HFCPs and TZ, the results showed the novel catalytic packing was a suitable catalyst for the acid catalyzed reactions.

CAS / MDL: 7699-43-6
研究领域: 材料科学 · 催化化学
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ACS Sustainable Chemistry & Engineering · 2020 · IF 7.632

Nanoscale Solid Superacid-Coupled Polybenzimidazole Membrane with High Ion Selectivity for Flow Batteries

Lei Hu,Yue Du,Li Gao,Mengting Di,Ning Zhang,Yu Pan,Xiaoming Yan,Baigang An,Gaohong He

Nanoscale solid superacid SO42–/ZrO2/WO3 is coupled into imidazole-hydroxyl-quaternary ammonium co-functionalized polybenzimidazole (PG112) to address the trade-off effect of membrane for large-scale flow battery application. Nanoscale SO42–/ZrO2/WO3 particles with high sulfonic groups are dispersed in membrane as redox-active ion barriers and proton carriers, which mitigate the electrolyte crossover and maintain high ion conductivity. The VO2+ permeability of the prepared membrane (7.86 × 10–10 cm2 s–1) is significantly lower than those of PG112 (3.93 × 10–9 cm2 s–1) and Nafion 212 (7.76 × 10–8 cm2 s–1) membranes. The vanadium flow battery with this membrane exhibits a longer self-discharge duration time of 231 h compared with Nafion 212 (35 h) and PG112 (88 h) membranes. High coulombic efficiencies of 97.5–99.2% at 40–120 mA cm–2 are obtained for the prepared membrane, which are higher than those for Nafion 212 (78.0–92.8%) and PG112 membranes (96.2–98.6%). Stable cycle performance and low retention capacity are also observed, suggesting the excellent chemical stability of the prepared membrane in vanadium flow battery operation. This work provides a prospective and applicable membrane to enhance the performance of flow battery.

CAS / MDL: 13520-92-8 7783-03-1
研究领域: 材料科学 · 电化学 · 能源技术
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JOURNAL OF POROUS MATERIALS · 2019 ·Vol. 27 ·期 2 ·429-440 · IF 1.947

Preparation, characterization, and application of ordered mesoporous S2O82−/ZrO2–SiO2 with high specific surface area

Wang Yunjie,Yuan Hong,Zhang Zhi,Ke Yihu

A series of ordered mesoporous S 2 O 8 2−/ ZrO 2 –SiO 2 (OMSZS) solid superacids with different calcination temperatures (400–650 °C) was synthesized using zirconium n-propoxide and tetraethyl orthosilicate as the raw materials and P123 as a structure-directing agent by solvent evaporation-post-dipping method. Transmission electron microscopy and small-angle X-ray diffraction results showed that the OMSZS were all ordered. The nitrogen adsorption results indicated that the specific surface area of OMSZS could reach up to 331–385 m 2 /g, whereas the average pore diameters were in the range of 3.1–3.2 nm. The pyridine infrared results mainly displayed Lewis acids, and the ammonia (NH 3 )-temperature programmed desorption characterization showed that the NH 3 desorption of the OMSZS calcined at 550 °C was 61 cm 3 /g STP. The catalytic performance of the OMSZS was investigated by the transesterification reaction of waste frying oil and methanol. The yield of fatty acid methyl ester could reach up to 94% at 200 °C reaction temperature for 6 h. After repeated use for four times, the catalyst still featured good activity and the yield was 78%.

研究领域: 材料科学 · 催化化学
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Catalysts · 2025 ·Vol. 15 ·期 3 ·255 · IF 4

A Radio Frequency Plasma-Modified SO42−-S2O82−/SnO2-Al2O3 Solid Superacid Catalyst Applied for the Esterification of Tyrosine

Changhui Zhu,Xudong Zhang,Wenling Xu,Yanni Zheng,Baohe Tian,Xi Chen,Wenchao Zhu

To overcome the limitations of conventional catalysts in sterically hindered esterification reactions, a radio frequency (RF) plasma-modifiedSO42−/S2O82−/SnO2-Al2O₃ solid superacid catalyst was synthesized via sol-gel and impregnation, followed by RF plasma treatment and calcination. Comprehensive characterization revealed that the RF plasma modification endowed the catalyst with a uniform particle distribution (4.32 nm average size), larger specific surface area (104.44 m2·g−1), elevated total acid content (142.86 μmol·g−1), and increased oxygen vacancy concentration (16.4%), compared to the conventional sol-gel–impregnation–calcination-prepared catalyst. The RF plasma-modifiedSO42−-S2O82−/SnO2-Al2O3was subsequently applied to perform the esterification reaction of Tyr, with a higher steric hindrance. Mechanistic studies indicated that the plasma-induced surface etching and electronic redistribution/intensified electron-withdrawing capability ofSO42−/S2O82−groups synergistically strengthened Brønsted/Lewis acidity. For the esterification of tyrosine—a sterically demanding substrate—the modified catalyst achieved a 92.1% methyl tyrosine yield under the optimized conditions (180 °C, 0.8 MPa N2, 6 h), where the catalyst exhibited a better mechanical strength and better lifetime with five cycles. This work not only provides a scalable plasma-assisted strategy for tuning solid superacids but also establishes an eco-friendly alternative to traditional catalysts, and was applied to the esterification reactions of some high-steric-hindrance substrates.

CAS / MDL: 25155-30-0 10026-06-9
研究领域: 催化化学 · 生物有机化学
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NEW JOURNAL OF CHEMISTRY · 2021 ·Vol. 45 ·期 24 ·10850-10856 · IF 3.591

A novel site-induced biomolecule anchoring strategy based on solid superacid ZrO2/SO42- for fabricating label-free IgG electrochemical immunosensors

Xiaoyan Chen,Lin Song,Guanyang Zhu,Jing Ma,Ajing Xu,Wenya Zhao,Yingying Gu,Yarui An,Yuqing Miao

In this work, a unique zirconium dioxide solid superacid (ZrO2/SO42−) was utilized for the fabrication of an IgG electrochemical immunosensor. The treated ZrO2 formed a SO bond on the surface, which has the electron-attracting induction effect and can further enhance the quantity and stability of immobilized biomolecules. In addition, using a platinum nanoparticle–chitosan–reduced graphene oxide (PtNP–CHIT–rGO) nanocomposite as a substrate modification material not only improves the conductivity of the electrode, but also increases the effective surface area of the immunosensing platform. The proposed label-free immunosensor has a lower detection limit of 11.0 pg mL−1 and a wide linear range of 0.01–10.0 ng mL−1 and 10.0–4000.0 ng mL−1. Importantly, the immunosensor exhibits good selectivity, excellent stability and reproducibility, and is expected to be applied to the detection of other biomolecules.

CAS / MDL: 7782-42-5 1401-55-4
研究领域: 生物化学 · 分析化学 · 材料科学
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INORGANICA CHIMICA ACTA · 2018 · IF 2.264

Effective transesterification of triglyceride with sulphonated modified SBA-15 (SBA-15-SO3H): Screening, process and mechanism

Ningmeng Hu,Zhaoni Kong,Liang He,Ping Ning,Junjie Gu,Rongrong Miao,Xiangqian Sun,Qingqing Guan,Peigao Duan

Different morphologies of ZrO 2 were produced by different templates: ZrO 2 (CaCO 3 ), ZrO 2 (C 12 H 25 SO 3 Na), ZrO 2 (C 12 H 25 SO 4 Na), ZrO 2 (CTAB), and solid superacids, such as ZrO 2 /SBA-15, SO 4 2- /ZrO 2 , SO 4 2- /ZrO 2 /SBA-15, and SBA-15-SO 3 H. The catalytic transesterification activities of these catalysts were tested. The more highly acidic catalysts and higher surface areas led to higher catalytic activity. In particular, the conversion yield of triglyceride reached 90.1% and was maintained for 90 min at 200 °C with 5.0 wt% SBA-15-SO 3 H, indicating this material to be one of most effective acid catalysts for the transesterification process. The mechanism indicated that the most important process was the abstraction of hydrogen from alcohols and α-substituted carboxylic glycerides. In the initial transesterification, the alcohol hydrogen atoms could be attracted onto the surface. Then, the nucleophilic attack of the alcohol led to the α-substituted carboxylic glyceride. Finally, monoglycerides, diglycerides or glycerine were released from the surface by proton (H + ) replacement.

CAS / MDL: 64-17-5 538-24-9
研究领域: 化学工程 · 催化 · 材料科学
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JOURNAL OF NANOSCIENCE AND NANOTECHNOLOGY · 2015 ·Vol. 15 ·期 12 ·9887-9891 · IF 1.556

Crystal Structure and Antibacterial Activity of (E)-(5-ethyl-2-styryl-1,3-dioxan-5-yl) Methanol Synthesized with Nanosolid Superacid

Yuan Lin,Li Zhong Yan,Zhang Xing Yu,Li Wen Yi,Zhang Min,Yuan Xian You

A new chiral 1,3-dioxane compound was synthesized by aldol condensation reaction in this paper. The reaction of cinnamic aldehyde with 2.1 equiv. of 2,2-bis(hydroxymethyl) butanol in N, N-dimethylformamide and cyclohexane, nanosolid superacid SO2- 4/Fe2O3 was applied as catalyst, afforded the new chiral 1,3-dioxane compound (E)-(5-ethyl-2-styryl-1,3-dioxan-5-yl) methanol. The compound was fully characterized with infrared spectra, elemental analysis, melting points, 1H NMR and X-ray diffraction. Single crystal X-ray diffraction analysis revealed that the compound crystallized in the monoclinic system, space group P2(1) with a = 5·717(2) Å, b = 11·684(4) Å, c = 10·569(4) Å, α = 90·00°, β = 99·646(4)°, γ = 90·00°, V = 696·0(4) Å3, Z = 2, Dc = 1·185 g/cm−3, R = 0·0182, μ = 0·081 mm−1, F(000) = 268. In addition, the antibacterial activities of the compound against Bacillus subtilis, Escherichia coli and Staphylococcus aureus have been investigated.

研究领域: 有机化学 · 药物化学 · 微生物学
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