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Sulfonic acid-functionalized mesoporous silica catalyst with different morphology for biodiesel production

《化学科学与工程前沿（英文）》 2022年 第16卷 第8期   页码 1198-1210 doi: 10.1007/s11705-021-2133-z

摘要： Sulfonic acid functionalized mesoporous silica based solid acid catalysts with different morphology were designed and fabricated. The synthesized materials were characterized by various physicochemical and spectroscopic techniques like scanning electron microscope-energy dispersive X-ray spectroscopy, Fourier transform infrared spectroscopy, Brunauer–Emmett–Teller surface area, thermogravimetric analysis and n-butylamine acidity. The shape of catalysts particles plays an important role in its activity. The sulfonic acid functionalized mesoporous silica catalysts of spherical shape and the cube shape were assessed for catalytic activity in biodiesel production. The catalytic biodiesel production reaction over the catalysts were studied by esterification of free fatty acid, oleic acid with methanol. The effect of various reaction parameters such as catalyst concentration, acid/alcohol molar ratio, catalyst amount, reaction temperature and reaction time on catalytic activity were investigated to optimize the conditions for maximum conversion. It was sulfonated cubic shape mesoporous silica which exhibited better activity as compared to the spherical shape silica catalysts. Additionally, the catalyst was regenerated and reused up to three cycles without any significant loss in activity. The present catalysts exhibit superior performance in biodiesel production and it can be used for the several biodiesel feedstock’s that are rich in free fatty acids.

关键词： solid acid catalyst     mesoporous silica     sulfonic acid     biodiesel     esterification     oleic acid    

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Precise regulation of acid pretreatment for red mud SCR catalyst: Targeting on optimizing the acidity

《环境科学与工程前沿（英文）》 2022年 第16卷 第7期 doi: 10.1007/s11783-021-1447-x

摘要：

• The optimum SCR activity was realized by tuning the acid pretreatment.

关键词： Air pollution control     Nitrogen oxides     Selective catalytic reduction     Red mud     Solid waste utilization    

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Review of SO42-/MxOy solid superacid catalysts

Yanni WU, Shijun LIAO

《化学科学与工程前沿（英文）》 2009年 第3卷 第3期   页码 330-343 doi: 10.1007/s11705-009-0208-3

摘要： Some metal oxides modified with sulfate ions form highly acidic or superacidic catalysts. solid superacid catalysts, play a vital role in more and more fields such as organic synthesis, fine chemicals, pharmaceuticals, and means for strengthening environmental safeguards. This review highlights the recent development of solid superacid catalysts based on , including synthesis method, characterization of acid sites and acid strength, and applications.

关键词： solid superacid catalyst     synthesis method     characterization     applications    

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Biodiesel production by the transesterification of cottonseed oil by solid acid catalysts

CHEN He, PENG Baoxiang, WANG Dezheng, WANG Jinfu

《化学科学与工程前沿（英文）》 2007年 第1卷 第1期   页码 11-15 doi: 10.1007/s11705-007-0003-y

摘要： Methyl esters (biodiesel) were produced by the transesterification of cottonseed oil with methanol in the presence of solid acids as heterogeneous catalysts. The solid acids were prepared by mounting HSO on TiO · nHO and Zr(OH), respectively, followed by calcining at 823K. TiO-SO and ZrOSO showed high activity for the transesterification. The yield of methyl esters was over 90% under the conditions of 230°C, methanol/oil mole ratio of 12:1, reaction time 8 h and catalyst amount (catalyst/oil) of 2% (w). The solid acid catalysts showed more better adaptability than solid base catalysts when the oil has high acidity. IR spectral analysis of absorbed pyridine on the samples showed that there were Lewis and BrØnsted acid sites on the catalysts.

关键词： BrØnsted     reaction     presence     cottonseed     biodiesel    

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Reconstruction of Cu–ZnO catalyst by organic acid and deactivation mechanism in liquid-phase hydrogenation

《化学科学与工程前沿（英文）》 2023年 第17卷 第9期   页码 1311-1319 doi: 10.1007/s11705-022-2281-9

摘要： A reconstructed Cu–ZnO catalyst with improved stability was fabricated by organic acid treatment method for the liquid-phase hydrogenation of dimethyl succinate to 1,4-butanediol. According to the characterization results of the fresh Cu–ZnO and reconstructed Cu–ZnO, three different forms of ZnO were suggested to be presented on the catalysts: ZnO having strong interaction with Cu species, ZnO that weakly interacted with Cu species and isolated ZnO. The first form of ZnO was believed to be beneficial to the formation of efficient active site Cu+, while the latter two forms of ZnO took the main responsibility for the deactivation of Cu–ZnO catalysts in the liquid-phase hydrogenation of diesters. The reconstruction of the Cu–ZnO catalyst by the organic acid treatment method resulted in a new Cu–ZnO catalyst with more Cu+ and less ZnO species that leads to deactivation. Furthermore, the deactivation mechanism of Cu–ZnO catalysts in liquid-phase diester hydrogenation in continuous flow system was proposed: the deposition of the polyesters on the catalysts via transesterification catalyzed by weakly interacted ZnO and isolated ZnO leads to the deactivation. These results provided meaningful instructions for designing highly efficient Cu–Zn catalysts for similar ester hydrogenation systems.

关键词： liquid phase     hydrogenation     Cu–ZnO     deactivation mechanism     1     4-butanediol     diester    

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Nitrogen-doped carbon black supported Pd nanoparticles as an effective catalyst for formic acid electro-oxidation

Na SUN, Minglei WANG, Jinfa CHANG, Junjie GE, Wei XING, Guangjie SHAO

《能源前沿（英文）》 2017年 第11卷 第3期   页码 310-317 doi: 10.1007/s11708-017-0491-5

摘要： Pd nanoparticles supported on nitrogen doped carbon black (Vulcan XC-72R) with two different levels of doping were prepared by the microwave-assisted ethylene glycol reduction process and used as catalyst for the formic acid electro-oxidation (FAEO). The results indicate that the different nitrogen doping contents in Pd/N-C catalysts have a significant effect on the performance of FAEO. A higher N content facilitates the uniform dispersion of Pd nanoparticles on carbon black with narrow particle size distribution. Furthermore, the electrochemical results show that the catalyst with a higher N-doping content possesses a higher catalytic activity and a long-term stability for FAEO. The peak current density of the Pd/N-C (high) catalyst is 1.27 and 2.31 times that of the Pd/N-C (low) and homemade Pd/C-H catalyst. The present paper may provide a simple method for preparation of high-performance anode catalyst for direct formic acid fuel cells (DFAFCs).

关键词： formic acid electro-oxidation     nitrogen doped     oxidized carbon     nitrogen content    

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Benzenesulfonic acid-grafted UIO-66 with improved hydrophobicity as a stable Brønsted acid catalyst

《化学科学与工程前沿（英文）》 2023年 第17卷 第10期   页码 1389-1398 doi: 10.1007/s11705-022-2285-5

摘要： Hydrothermal and catalytic stability of UIO-66 MOFs with defective structures are critical aspects to be considered in their catalytic applications, especially under the conditions involving water, moisture and/or heat. Here, we report a facile strategy to introduce the macromolecular acid group to UIO-66 to improve the stability of the resulting UIO-66−PhSO3H MOF in aqueous phase catalysis. In detail, UIO-66−PhSO3H was obtained by grafting benzenesulfonic acid on the surface of the pristine UIO-66 to introduce the hydrophobicity, as well as the Brønsted acidity, then assessed using catalytic hydrolysis of cyclohexyl acetate (to cyclohexanol) in water. The introduction of hydrophobic molecules to UIO-66 could prevent the material from being attacked by hydroxyl polar molecules effectively, explaining its good structural stability during catalysis. UIO-66−PhSO3H promoted the conversion of cyclohexyl acetate at ca. 87%, and its activity and textural properties were basically intact after the cyclic stability tests. The facile modification strategy can improve the hydrothermal stability of UIO-66 significantly, which can expand its catalytic applications in aqueous systems.

关键词： metal−organic frameworks (MOFs)     UIO-66     hydrolysis of cyclohexyl acetate     hydrophobicity     Brønsted acidity    

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ZnZr/HZSM-5 as efficient catalysts for alkylation of benzene with carbon dioxide

《化学科学与工程前沿（英文）》 2023年 第17卷 第4期   页码 404-414 doi: 10.1007/s11705-022-2215-6

摘要： Alkylation of benzene with carbon dioxide and hydrogen to produce toluene and xylene could increase the added-value of surplus benzene as well as relieve environmental problems like green-house effect. In this work, the alkylation benzene with carbon dioxide and hydrogen reaction was proceeded by using the mixture of zinc-zirconium oxide and HZSM-5 as bifunctional catalyst. The equivalent of Zn/Zr = 1 displays the best catalytic performance at 425 °C and 3.0 MPa, and benzene conversion reaches 42.9% with a selectivity of 90% towards toluene and xylene. Moreover, the carbon dioxide conversion achieves 23.3% and the carbon monoxide selectivity is lower than 35%, indicating that more than 50% carbon dioxide has been effectively incorporated into the target product, which is the best result as far as we know. Combined with characterizations, it indicated that the Zn and Zr formed a solid solution under specific conditions (Zn/Zr = 1). The as-formed solid solution not only possesses a high surface area but also provides a large amount of oxygen vacancies. Additionally, the bifunctional catalyst has excellent stabilities that could keep operating without deactivation for at least 80 h. This work provides promising industrial applications for the upgrading of aromatics.

关键词： carbon dioxide     alkylation of benzene     solid solution catalyst     bifunctional catalyst    

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A Pt-Bi bimetallic nanoparticle catalyst for direct electro-oxidation of formic acid in fuel cells

Shu-Hong LI, Yue ZHAO, Jian CHU, Wen-Wei LI, Han-Qing YU, Gang LIU, Yang-Chao TIAN

《环境科学与工程前沿（英文）》 2013年 第7卷 第3期   页码 388-394 doi: 10.1007/s11783-012-0475-y

摘要： Direct formic acid fuel cells are a promising portable power-generating device, and the development of efficient anodic catalysts is essential for such a fuel cell. In this work Pt-Bi nanoparticles supported on micro-fabricated gold wire array substrate were synthesized using an electrochemical deposition method for formic acid oxidation in fuel cells. The surface morphology and element components of the Pt-Bi/Au nanoparticles were characterized, and the catalytic activities of the three Pt-Bi/Au nanoparticle electrodes with different Pt/Bi ratios for formic acid oxidation were evaluated. It was found that Pt Bi /Au had a much higher catalytic activity than Pt Bi /Au and Pt Bi /Au, and Pt Bi /Au exhibited a current density of 2.7 mA·cm , which was 27-times greater than that of Pt/Au. The electro-catalytic activity of the Pt-Bi/Au electrode for formic acid oxidation increased with the increasing Bi content, suggesting that it would be possible to achieve an efficient formic acid oxidation on the low Pt-loading. Therefore, the Pt-Bi/Au electrode offers a promising catalyst with a high activity for direct oxidation of formic acid in fuel cells.

关键词： catalyst     electrochemical deposition     formic acid oxidation     fuel cell     gold wire array     microfabrication    

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Mesoporous silicon sulfonic acid as a highly efficient and stable catalyst for the selective hydroamination

Jingbin Wen, Kuiyi You, Minjuan Chen, Jian Jian, Fangfang Zhao, Pingle Liu, Qiuhong Ai, He’an Luo

《化学科学与工程前沿（英文）》 2021年 第15卷 第3期   页码 654-665 doi: 10.1007/s11705-020-1973-2

摘要： In this work, a new mesoporous silicon sulfonic acid catalyst derived from silicic acid has been successfully prepared by the chemical bonding method. The physicochemical properties of mesoporous silicon sulfonic acid catalysts have been systematically characterized using various techniques. The results demonstrate that sulfonic acid groups have been grafted on silicic acid by forming a new chemical bond (Si–O–S). The mesoporous silicon sulfonic acid exhibits excellent catalytic performance and stability in the vapor phase hydroamination reaction of cyclohexene with cyclohexylamine. Cyclohexene conversion of 61% and 97% selectivity to dicyclohexylamine was maintained after running the reaction for over 350 h at 280 °C. The developed mesoporous silicon sulfonic acid catalyst shows advantages of low cost, superior acid site accessibility, and long term reactivity stability. Moreover, a possible catalytic hydroamination reaction mechanism over silicon sulfonic acid was suggested. It has been demonstrated that the sulfonic acid groups of the catalyst play an important role in the hydroamination. The present work provides a simple, efficient, and environmentally friendly method for the hydroamination of cyclohexene to valuable dicyclohexylamine, which also shows important industrial application prospects.

关键词： mesoporous silicon sulfonic acid     catalytic hydroamination     cyclohexene     dicyclohexylamine     vapor phase    

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Visbreaking of heavy petroleum oil catalyzed by SO/ZrO solid super-acid doped with Ni or Sn

JING Ping, LI Qingbiao, HAN Mei, SUN Daohua, JIA Lishan, FANG Weiping

《化学科学与工程前沿（英文）》 2008年 第2卷 第2期   页码 186-190 doi: 10.1007/s11705-008-0035-y

摘要： SO/ZrO solid super-acid catalysts (SZ) doped with Ni or Sn (Ni/SZ, Sn/SZ) were prepared for catalytic visbreaking of heavy petroleum oil from Shengli oil field. The visbreaking reactions were carried out at 240°C and 3–4 MPa for 24 h using a heavy petroleum oil to catalyst mass ratio of 100 : 0.05. The effect of water content on viscosity of heavy petroleum oil was also investigated. Both catalysts can promote thermolysis of heavy petroleum oil and the viscosity was reduced from 0.319 Pa·s to 0.135 Pa·s for Ni/SZ and 0.163 Pa·s for (Sn/SZ) with visbreaking rates of 57.7% and 48.9%, respectively. After visbreaking, the saturated hydrocarbon content increased while aromatics, resin, asphaltene, sulfur and nitrogen content decreased. The presence of water was disadvantageous to visbreaking of heavy petroleum oil.

关键词： thermolysis     Shengli     asphaltene     SO/ZrO     presence    

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Development of solid base catalyst X/Y/MgO/-AlO for optimization of preparation of biodiesel from L.seed

WANG Rui, YANG Song, YIN Shitao, SONG Baoan, BHADURY Pinaki S., XUE Wei, TAO Shuwei, JIA Zhaohui, LIU Da, GAO Liang

《化学科学与工程前沿（英文）》 2008年 第2卷 第4期   页码 468-472 doi: 10.1007/s11705-008-0074-4

摘要： The preparation and regeneration conditions of the identified catalyst X/Y/MgO/-AlO with high catalytic activity were studied and optimized. The biodiesel was prepared by transesterification of seed oil produced in Guizhou with methanol at its reflux temoerature in the presence of X/Y/MgO/-AlO The pilot plant tests were carried out in a 100 L reaction vessel. Both average yield and fatty acid methyl esters (FAME) content reached more than 96.50% under the optimum reaction conditions of the pilot plant tests designed with an oil/methanol molar ratio of 1 : 10, catalyst concentration of 1.00%, and reaction time of 3 h at reflux temperature. In addition, analysis shows that the quality of biodiesel meets the standard EN 14214.

关键词： temperature     presence     addition     catalytic activity     catalyst X/Y/MgO/-AlO    

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Catalytic ozonation of organic compounds in water over the catalyst of RuO

Jianbing WANG,Guoqing WANG,Chunli YANG,Shaoxia YANG,Qing HUANG

《环境科学与工程前沿（英文）》 2015年 第9卷 第4期   页码 615-624 doi: 10.1007/s11783-014-0706-5

摘要： This research investigates the performances of RuO /ZrO -CeO in catalytic ozonation for water treatment. The results show that RuO /ZrO -CeO was active for the catalytic ozonation of oxalic acid and possessed higher stability than RuO /Al O and Ru/AC. In the catalytic ozonation of dimethyl phthalate (DMP), RuO /ZrO -CeO did not enhance the DMP degradation rate but significantly improved the total organic carbon (TOC) removal rate. The TOC removal in catalytic ozonation was 56% more than that in noncatalytic ozonation. However this does not mean the catalyst was very active because the contribution of catalysis to the overall TOC removal was only 30%. The adsorption of the intermediates on RuO /ZrO -CeO played an important role on the overall TOC removal while the adsorption of DMP on it was negligible. This adsorption difference was due to their different ozonation rates. In the catalytic ozonation of disinfection byproduct precursors with RuO /ZrO -CeO , the reductions of the haloacetic acid and trihalomethane formation potentials (HAAFPs and THMFPs) for the natural water samples were 38%–57% and 50%–64%, respectively. The catalyst significantly promoted the reduction of HAAFPs but insignificantly improved the reduction of THMFPs as ozone reacts fast with the THMs precursors. These results illustrate the good promise of RuO /ZrO -CeO in catalytic ozonation for water treatment.

关键词： ozonation     ruthenium     oxalic acid     dimethyl phthalate     disinfection byproduct    

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Biodiesel production from waste frying oil in sub- and supercritical methanol on a zeolite Y solid acidcatalyst

Jorge MEDINA-VALTIERRA, Jorge RAMIREZ-ORTIZ

《化学科学与工程前沿（英文）》 2013年 第7卷 第4期   页码 401-407 doi: 10.1007/s11705-013-1354-1

摘要： Waste frying oil (WFO) is a very important feedstock for obtaining biodiesel at low cost and using WFO in transesterification reactions to produce biodiesel helps eliminate local environmental problems. In this study biodiesel was produced from WFO in sub- and super-critical methanol on a zeolite Y solid acid catalyst. The procedure was optimized using a design of experiments by varying the methanol to WFO molar ratio, the reaction temperature, and the amount of catalyst. Typical biodiesel yields varied from 83 to nearly 100% with methyl esters content ranging from 1.41–1.66 mol·L and typical dynamic viscosities of 22.1-8.2 cP. Gas chromatography was used to determine the molecular composition of the biodiesel. The reaction products contained over 82 wt-% methyl esters, 4.2 wt-% free acids, 13.5 wt-% monoglycerides, and 0.3 wt-% diglycerides. The transesterification of WFO with methanol around its critical temperature combined with a zeolite Y as an acid catalyst is an efficient approach for the production of biodiesel with acceptable yields.

关键词： biodiesel     methanol     critical temperature     waste frying oil     zeolite Y    

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Formic acid dehydrogenation reaction on high-performance PdAu alloy nanoparticles prepared by the eco-friendly

《能源前沿（英文）》   页码 751-762 doi: 10.1007/s11708-023-0895-3

摘要： Dehydrogenation of formic acid (FA) is considered to be an effective solution for efficient storage and transport of hydrogen. For decades, highly effective catalysts for this purpose have been widely investigated, but numerous challenges remain. Herein, the PdxAu1−x (x = 0, 0.2, 0.4, 0.5, 0.6, 0.8, 1) alloys over the whole composition range were successfully prepared and used to catalyze FA hydrogen production efficiently near room temperature. Small PdAu nanoparticles (5–10 nm) were well-dispersed and supported on the activated carbon to form PdAu solid solution alloys via the eco-friendly slow synthesis methodology. The physicochemical properties of the PdAu alloys were comprehensively studied by utilizing various measurement methods, such as X-ray diffraction (XRD), N2 adsorption–desorption, high angle annular dark field-scanning transmission electron microscope (HAADF-STEM), X-ray photoelectrons spectroscopy (XPS). Notably, owing to the strong metal-support interaction (SMSI) and electron transfer between active metal Au and Pd, the Pd0.5Au0.5 obtained exhibits a turnover frequency (TOF) value of up to 1648 h−1 (313 K, nPd+Au/nFA = 0.01, nHCOOH/nHCOONa = 1:3) with a high activity, selectivity, and reusability in the FA dehydrogenation.

关键词： FA dehydrogenation     face-centred cubic structures     PdAu solid solution alloy nanoparticles     slow synthesis methodology     SMSI effect    

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标题 作者 时间 类型 操作

Sulfonic acid-functionalized mesoporous silica catalyst with different morphology for biodiesel production

期刊论文

Precise regulation of acid pretreatment for red mud SCR catalyst: Targeting on optimizing the acidity

期刊论文

Review of SO42-/MxOy solid superacid catalysts

Yanni WU, Shijun LIAO

期刊论文

Biodiesel production by the transesterification of cottonseed oil by solid acid catalysts

CHEN He, PENG Baoxiang, WANG Dezheng, WANG Jinfu

期刊论文

Reconstruction of Cu–ZnO catalyst by organic acid and deactivation mechanism in liquid-phase hydrogenation

期刊论文

Nitrogen-doped carbon black supported Pd nanoparticles as an effective catalyst for formic acid electro-oxidation

Na SUN, Minglei WANG, Jinfa CHANG, Junjie GE, Wei XING, Guangjie SHAO

期刊论文

Benzenesulfonic acid-grafted UIO-66 with improved hydrophobicity as a stable Brønsted acid catalyst

期刊论文

ZnZr/HZSM-5 as efficient catalysts for alkylation of benzene with carbon dioxide

期刊论文

A Pt-Bi bimetallic nanoparticle catalyst for direct electro-oxidation of formic acid in fuel cells

Shu-Hong LI, Yue ZHAO, Jian CHU, Wen-Wei LI, Han-Qing YU, Gang LIU, Yang-Chao TIAN

期刊论文

Mesoporous silicon sulfonic acid as a highly efficient and stable catalyst for the selective hydroamination

Jingbin Wen, Kuiyi You, Minjuan Chen, Jian Jian, Fangfang Zhao, Pingle Liu, Qiuhong Ai, He’an Luo

期刊论文

Visbreaking of heavy petroleum oil catalyzed by SO/ZrO solid super-acid doped with Ni or Sn

JING Ping, LI Qingbiao, HAN Mei, SUN Daohua, JIA Lishan, FANG Weiping

期刊论文

Development of solid base catalyst X/Y/MgO/-AlO for optimization of preparation of biodiesel from L.seed

WANG Rui, YANG Song, YIN Shitao, SONG Baoan, BHADURY Pinaki S., XUE Wei, TAO Shuwei, JIA Zhaohui, LIU Da, GAO Liang

期刊论文

Catalytic ozonation of organic compounds in water over the catalyst of RuO

Jianbing WANG,Guoqing WANG,Chunli YANG,Shaoxia YANG,Qing HUANG

期刊论文

Biodiesel production from waste frying oil in sub- and supercritical methanol on a zeolite Y solid acidcatalyst

Jorge MEDINA-VALTIERRA, Jorge RAMIREZ-ORTIZ

期刊论文

Formic acid dehydrogenation reaction on high-performance PdAu alloy nanoparticles prepared by the eco-friendly

期刊论文