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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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A review on catalytic & non-catalytic bio-oil upgrading in supercritical fluids

Sainab Omar, Yang Yang, Jiawei Wang

《化学科学与工程前沿（英文）》 2021年 第15卷 第1期   页码 4-17 doi: 10.1007/s11705-020-1933-x

摘要： This review article summarizes the key published research on the topic of bio-oil upgrading using catalytic and non-catalytic supercritical fluid (SCF) conditions. The precious metal catalysts Pd, Ru and Pt on various supports are frequently chosen for catalytic bio-oil upgrading in SCFs. This is reportedly due to their favourable catalytic activity during the process including hydrotreating, hydrocracking, and esterification, which leads to improvements in liquid yield, heating value, and pH of the upgraded bio-oil. Due to the costs associated with precious metal catalysts, some researchers have opted for non-precious metal catalysts such as acidic HZSM-5 which can promote esterification in supercritical ethanol. On the other hand, SCFs have been effectively used to upgrade crude bio-oil without a catalyst. Supercritical methanol, ethanol, and water are most commonly used and demonstrate catalyst like activities such as facilitating esterification reactions and reducing solid yield by alcoholysis and hydrolysis, respectively.

关键词： bio-oil     upgrading     supercritical     review    

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Probing the catalytic activity of M-N

Fan Ge, Qingan Qiao, Xin Chen, You Wu

《化学科学与工程前沿（英文）》 2021年 第15卷 第5期   页码 1206-1216 doi: 10.1007/s11705-020-2017-7

摘要： In this work, the detailed oxygen reduction reaction (ORR) catalytic performance of M-N O (M= Fe, Co, and Ni; = 1–4) has been explored via the detailed density functional theory method. The results suggest that the formation energy of M-N O shows a good linear relationship with the number of doped O atoms. The adsorption manner of O on M-N O changed from end-on ( = 1 and 2) to side-on ( = 3 and 4), and the adsorption strength gradually increased. Based on the results for binding strength of ORR intermediates and the Gibbs free energy of ORR steps on the studied catalysts, we screened out two highly active ORR catalysts, namely Co-N O and Ni-N O , which possess very small overpotentials of 0.27 and 0.32 V, respectively. Such activities are higher than the precious Pt catalyst. Electronic structure analysis reveals one of the reasons for the higher activity of Co-N O and Ni-N O is that they have small energy gaps and moderate highest occupied molecular orbital energy levels. Furthermore, the results of the density of states reveal that the O doping can improve the electronic structure of the original catalyst to tune the adsorption of the ORR intermediates.

关键词： M-N-C catalyst     oxygen doping     oxygen reduction reaction     catalytic activity     density functional theory    

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Effects of support acidity on the reaction mechanisms of selective catalytic reduction of NO by CH

Shicheng XU, Junhua LI, Dong YANG, Jiming HAO

《环境科学与工程前沿（英文）》 2009年 第3卷 第2期   页码 186-193 doi: 10.1007/s11783-009-0016-5

摘要： The reaction mechanisms of selective catalytic reduction (SCR) of nitric oxide (NO) by methane (CH ) over solid superacid-based catalysts were proposed and testified by DRIFTS studies on transient reaction as well as by kinetic models. Catalysts derived from different supports would lead to different reaction pathways, and the acidity of solid superacid played an important role in determining the reaction mechanisms and the catalytic activities. Higher ratios of Br?nsted acid sites to Lewis acid sites would lead to stronger oxidation of methane and then could facilitate the step of methane activation. Strong Br?nsted acid sites would not necessarily lead to better catalytic performance, however, since the active surface NO species and the corresponding reaction routes were determined by the overall acidity strength of the support. The reaction routes where NO moiety was engaged as an important intermediate involved moderate oxidation of methane, the rate of which could determine the overall activity. The reaction involving NO moiety was likely to be determined by the step of reduction of NO. Therefore, to enhance the SCR activity of solid superacid catalysts, reactions between appropriate couples of active NO species and activated hydrocarbon intermediates should be realized by modification of the support acidity.

关键词： selective catalytic reduction (SCR)     nitric oxide (NO)     methane     support acidity     Br?nsted acid sites     NOy species    

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Preparation of rare-earth metal complex oxide catalysts for catalytic wet air oxidation

LI Ning, LI Guangming, YAO Zhenya, ZHAO Jianfu

《环境科学与工程前沿（英文）》 2007年 第1卷 第2期   页码 190-195 doi: 10.1007/s11783-007-0033-1

摘要： Catalytic wet air oxidation (CWAO) is one of the most promising technologies for pollution abatement. Developing catalysts with high activity and stability is crucial for the application of the CWAO process. The Mn/Ce complex oxide catalysts for CWAO of high concentration phenolcontaining wastewater were prepared by coprecipitation. The catalyst preparation conditions were optimized by using an orthogonal layout method and single-factor experimental analysis. The Mn/Ce serial catalysts were characterized by Brunauer Emmett Teller (BET) analysis and the metal cation leaching was measured by inductively coupled plasma torch-atomic emission spectrometry (ICP-AES). The results show that the catalysts have high catalytic activities even at a low temperature (80?C) and low oxygen partial pressure (0.5 MPa) in a batch reactor. The metallic ion leaching is comparatively low (Mn<6.577 mg/L and Ce<0.6910 mg/L, respectively) in the CWAO process. The phenol, COD, and TOC removal efficiencies in the solution exceed 98.5% using the optimal catalyst (named CSP). The new catalyst would have a promising application in CWAO treatment of high concentration organic wastewater.

关键词： torch-atomic emission     Brunauer     Catalytic     process     stability    

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Properties and catalytic mechanism of -glutamyltranspeptidase from NX-2

WANG Qian, YAO Zhong, XUN Zhijing, XU Xiaoying, XU Hong, WEI Ping

《化学科学与工程前沿（英文）》 2008年 第2卷 第4期   页码 456-461 doi: 10.1007/s11705-008-0075-3

摘要： Since -glutamyltranspeptidase (GGT) especially catalyses the transfer of the -glutamyl moiety to a variety of amino acids and short peptides, GGT has important practical value for enzymatic synthesis of -glutamyl compounds. In this paper, the GGT produced from NX-2 was purified by a combination of ammonium sulfate fractionation and ion exchange chromatography, and the properties of purified GGT were investigated. At the conditions of pH 10.0, D-glutamine (D-Gln)/L-tryptophan (L-Trp) with a molar ratio of 5 : 7, a temperature 40°C and a reaction time of 4 h, a higher conversion rate of 42% was obtained. According to the time course, the catalytic mechanism of enzymatic synthesis of -D-glutamyl-L-tryptophan (-D-Gln-L-Trp) was discussed. It was demonstrated that the GGT can catalyze not only the reaction of transpeptidation, but also the irreversible hydrolysis of the products which results in the decrease of the yield of the products. The affinity parameter of GGT to D-Gln (Km) was 5.08 mmol·L and the maximum reaction rate of transpeptidation () was determined as 0.034 mmol·min·L, while the affinity parameter of GGT to -D-Gln-L-Trp (’) was 2.267 mmol·L, and the maximum reaction rate of hydrolysis (’) was 0.012 mmol·min·L.

关键词： catalytic mechanism     mmol·min·L     D-glutamine     affinity parameter     important practical    

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Multi-stage ammonia production for sorption selective catalytic reduction of NO

Chen ZHANG, Guoliang AN, Liwei WANG, Shaofei WU

《能源前沿（英文）》 2022年 第16卷 第5期   页码 840-851 doi: 10.1007/s11708-021-0797-1

摘要： Sorption selective catalytic reduction of nitrogen oxides (NOx) (sorption-SCR) has ever been proposed for replacing commercial urea selective catalytic reduction of NOx (urea-SCR), while only the single-stage sorption cycle is hitherto adopted for sorption-SCR. Herein, various multi-stage ammonia production cycles is built to solve the problem of relative high starting temperature with ammonia transfer (AT) unit and help detect the remaining ammonia in ammonia storage and delivery system (ASDS) with ammonia warning (AW) unit. Except for the single-stage ammonia production cycle with MnCl2, other sorption-SCR strategies all present overwhelming advantages over urea-SCR considering the much higher NOx conversion driven by the heat source lower than 100°C and better matching characteristics with low-temperature catalysts. Furthermore, the required mass of sorbent for each type of sorption-SCR is less than half of the mass of AdBlue for urea-SCR. Therefore, the multifunctional multi-stage sorption-SCR can realize compact and renewable ammonia storage and delivery with low thermal energy consumption and high NOx conversion, which brings a bright potential for efficient commercial de-NOx technology.

关键词： selective catalytic reduction (SCR)     nitrogen oxides (NOx)     ammonia     composite sorbent     chemisorption    

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Selective catalytic reduction of NO

Pavlo I. Kyriienko

《化学科学与工程前沿（英文）》 2020年 第14卷 第4期   页码 471-491 doi: 10.1007/s11705-019-1847-7

摘要： Research results regarding selective catalytic reduction (SCR) of NO with ethanol and other C oxygenates as reductants over silver-alumina catalysts are summarized. The aspects of the process mechanism, nature of active sites, role of alumina and silver (especially in the formation of bifunctional active sites), effects of reductants and reaction conditions are discussed. It has been determined that key stages of the process include formation of reactive enolic species, their interaction with NO and formation of nitroorganic compounds which transform to NCO species and further to N . The results obtained over various silver-alumina catalysts demonstrate the perspectives of their application for reducing the level of nitrogen oxides in engine emissions, including in the presence of water vapor and sulfur oxides. Ways to improve the catalysts for the SCR of NO with C oxygenates are outlined.

关键词： SCR     nitrogen oxides     silver-alumina catalyst     silver species     ethanol     oxygenates    

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Effect of different acid anions on highly efficient Ce-based catalysts for selective catalytic reduction

《化学科学与工程前沿（英文）》 2023年 第17卷 第10期   页码 1399-1411 doi: 10.1007/s11705-023-2345-5

摘要： Three kinds of Ce-based catalysts (CePO4, CeVO4, Ce2(SO4)3) were synthesized and used for the selective catalytic reduction (SCR) of NO by NH3. NH3-SCR performances were conducted in the temperature range of 80 to 400 °C. The catalytic efficiencies of the three catalysts are as follow: CePO4 > CeVO4 > Ce2(SO4)3, which is in agreement with their abilities of NH3 adsorption capacities. The highest NO conversion rate of CePO4 could reach about 95%, and the catalyst had more than 90% NO conversion rate between 260 and 320 °C. The effect of PO43–, VO43– and SO42– on NH3-SCR performances of Ce-based catalysts was systematically investigated by the X-ray photoelectron spectroscopy analysis, NH3 temperature programmed desorption, H2 temperature programmed reduction and field emission scanning electron microscopy tests. The key factors that can enhance the SCR are the existence of Ce4+, large NH3 adsorption capacity, high and early H2 consumptions, and suitable microstructures for gas adsorption. Finally, CePO4 and CeVO4 catalysts also exhibited relatively strong tolerance of SO2, and the upward trend about 8% was detected due to the sulfation enhancement by SO2 for Ce2(SO4)3.

关键词： CePO4     CeVO4     Ce2(SO4)3     selective catalytic reduction     NO removal    

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synthesis of functional MFI zeolite materials: Method development, crystallization mechanisms, and catalytic

Zhaoqi Ye, Hongbin Zhang, Yahong Zhang, Yi Tang

《化学科学与工程前沿（英文）》 2020年 第14卷 第2期   页码 143-158 doi: 10.1007/s11705-019-1852-x

摘要： As an important zeolite material, MFI zeolites, as well as their controllable synthesis, are of great interest in both basic and applied science. Among the developed synthetic approaches, the seed-induced method has gradually evolved into a facile, low-cost, and even green alternative to give zeolites the desirable physicochemical properties. In this review, we briefly summarize the development of seed-induced syntheses of diverse functional MFI zeolites, where the “living” seed crystals not only direct the formation of zeolitic framework but also function as special “templates” or “units” to fine-tune the zeolite materials with diverse sizes, shapes, compositions, morphologies and pore structures. Moreover, on the basis of their structural features and crystallization behaviors in seed-induced synthesis, we reveal the roles of seeds and discuss the related crystallization mechanisms including both classical and non-classical pathways. We also want to guide readers to investigate the structure-performance relationships between these functional MFI zeolite catalysts and suitable catalytic reactions.

关键词： seed-induced synthesis     MFI zeolite     synthesis mechanism     catalytic property    

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Tuning the catalytic selectivity in electrochemical CO

Jiafang XIE,Yuxi HUANG,Hanqing YU

《环境科学与工程前沿（英文）》 2015年 第9卷 第5期   页码 861-866 doi: 10.1007/s11783-014-0742-1

摘要： Electrochemical conversion of CO to hydrocarbons can relieve both environmental and energy stresses. However, electrocatalysts for this reaction usually suffer from a poor product selectivity and a large overpotential. Here we report that tunable catalytic selectivity for hydrocarbon formation could be achieved on Cu nanomaterials with different morphologies. By tuning the electrochemical parameters, either Cu oxide nanowires or nanoneedles were fabricated and then electrochemically reduced to the corresponding Cu nanomaterials. The Cu nanowires preferred the formation of C H , while the Cu nanoneedles favored the production of more CH , rather than C H . Our work provides a facile synthetic strategy for preparing Cu-based nanomaterials to achieve selective CO reduction.

关键词： electrochemical CO2 reduction     Cu oxide     nanostructure     selectivity     hydrocarbon formation    

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Thermodynamic analysis of reaction pathways and equilibrium yields for catalytic pyrolysis of naphtha

《化学科学与工程前沿（英文）》 2022年 第16卷 第12期   页码 1700-1712 doi: 10.1007/s11705-022-2207-6

摘要： The chain length and hydrocarbon type significantly affect the production of light olefins during the catalytic pyrolysis of naphtha. Herein, for a better catalyst design and operation parameters optimization, the reaction pathways and equilibrium yields for the catalytic pyrolysis of C5–8 n/iso/cyclo-paraffins were analyzed thermodynamically. The results revealed that the thermodynamically favorable reaction pathways for n/iso-paraffins and cyclo-paraffins were the protolytic and hydrogen transfer cracking pathways, respectively. However, the formation of light paraffin severely limits the maximum selectivity toward light olefins. The dehydrogenation cracking pathway of n/iso-paraffins and the protolytic cracking pathway of cyclo-paraffins demonstrated significantly improved selectivity for light olefins. The results are thus useful as a direction for future catalyst improvements, facilitating superior reaction pathways to enhance light olefins. In addition, the equilibrium yield of light olefins increased with increasing the chain length, and the introduction of cyclo-paraffin inhibits the formation of light olefins. High temperatures and low pressures favor the formation of ethylene, and moderate temperatures and low pressures favor the formation of propylene. n-Hexane and cyclohexane mixtures gave maximum ethylene and propylene yield of approximately 49.90% and 55.77%, respectively. This work provides theoretical guidance for the development of superior catalysts and the selection of proper operation parameters for the catalytic pyrolysis of C5–8 n/iso/cyclo-paraffins from a thermodynamic point of view.

关键词： naphtha     catalytic pyrolysis     reaction pathway     equilibrium yield    

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Preparation and catalytic performance of La0.8Sr0.2CoO3 supported on the mullite fiber ceramic

ZENG Lingke, LIU Yanchun, LIU Ping′an, WANG Hui, SHUI Anze, DUAN Bilin

《化学科学与工程前沿（英文）》 2007年 第1卷 第4期   页码 372-376 doi: 10.1007/s11705-007-0067-8

摘要： The perovskite-type LaSrCoO supported on the mullite fiber porous ceramics was prepared by means of the impregnating method, and was then characterized by scanning electron microscopy (SEM) and X-ray diffraction (XRD); thus we can come to the conclusion that the perovskite-type composite oxidant can disperse on the surface of mullite fiber ceramics. The catalytic activity of the LaSrCoO for NO and CO was evaluated. The effect of the doped 0.1 wt-% PdCl on the catalytic activity of the perovskite-type LaSrCoO was also discussed. The results show that the conversion rates of NO and CO respectively reaches 74.5% and 99% at 601°C without doped Pd, and both reach 100% at 350°C with a little doped Pd.

关键词： porous     conversion     catalytic activity     electron microscopy     perovskite-type LaSrCoO    

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Recent advances and challenges of nitrogen/nitrate electro catalytic reduction to ammonia synthesis

《能源前沿（英文）》 doi: 10.1007/s11708-023-0908-2

摘要： The Haber-Bosch process is the most widely used synthetic ammonia technology at present. Since its invention, it has provided an important guarantee for global food security. However, the traditional Haber-Bosch ammonia synthesis process consumes a lot of energy and causes serious environmental pollution. Under the serious pressure of energy and environment, a green, clean, and sustainable ammonia synthesis route is urgently needed. Electrochemical synthesis of ammonia is a green and mild new method for preparing ammonia, which can directly convert nitrogen or nitrate into ammonia using electricity driven by solar, wind, or water energy, without greenhouse gas and toxic gas emissions. Herein, the basic mechanism of the nitrogen reduction reaction (NRR) to ammonia and nitrate reduction reaction (NO3− RR) to ammonia were discussed. The representative approaches and major technologies, such as lithium mediated electrolysis and solid oxide electrolysis cell (SOEC) electrolysis for NRR, high activity catalyst and advanced electrochemical device fabrication for NO3 − RR and electrochemical ammonia synthesis were summarized. Based on the above discussion and analysis, the main challenges and development directions for electrochemical ammonia synthesis were further proposed.

关键词： electrochemical ammonia synthesis     nitrogen     nitrate     nitrogen reduction reaction (NRR) to ammonia     nitrate reduction reaction (NO–3 RR)    

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Process analysis of syngas production by non-catalytic POX of oven gas

Fuchen WANG , Xinwen ZHOU , Wenyuan GUO , Zhenghua DAI , Xin GONG , Haifeng LIU , Zunhong YU ,

《能源前沿（英文）》 2009年 第3卷 第1期   页码 117-122 doi: 10.1007/s11708-008-0078-2

摘要： A non-catalytic POX of oven gas is proposed to solve the problem of secondary pollution due to solid wastes produced from the great amount of organic sulfur contained in oven gas in the traditional catalytic partial oxidation (POX) process. A study of the measurement of flow field and a thermodynamic analysis of the process characteristics were conducted. Results show that there exist a jet-flow region, a recirculation-flow region, a tube-flow region, and three corresponding reaction zones in the non-catalytic POX reformer. The combustion of oven gas occurs mainly in the jet-flow region, while the reformation of oven gas occurs mainly in the other two regions. Soot would not be formed by CH cracking at above 1200°C. Since there are very little C hydrocarbons in oven gas, the soot produced would be very tiny, even if they underwent cracking reaction. The integrated model for entrained bed gasification process was applied to simulate a non-catalytic POX reformer. It indicated that the proper oxygen-to-oven gas ratio is 0.22–0.28 at different pressures in the oven gas reformation process.

关键词： oven gas     non-catalytic POX process     syngas    

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标题 作者 时间 类型 操作

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

A review on catalytic & non-catalytic bio-oil upgrading in supercritical fluids

Sainab Omar, Yang Yang, Jiawei Wang

期刊论文

Probing the catalytic activity of M-N

Fan Ge, Qingan Qiao, Xin Chen, You Wu

期刊论文

Effects of support acidity on the reaction mechanisms of selective catalytic reduction of NO by CH

Shicheng XU, Junhua LI, Dong YANG, Jiming HAO

期刊论文

Preparation of rare-earth metal complex oxide catalysts for catalytic wet air oxidation

LI Ning, LI Guangming, YAO Zhenya, ZHAO Jianfu

期刊论文

Properties and catalytic mechanism of -glutamyltranspeptidase from NX-2

WANG Qian, YAO Zhong, XUN Zhijing, XU Xiaoying, XU Hong, WEI Ping

期刊论文

Multi-stage ammonia production for sorption selective catalytic reduction of NO

Chen ZHANG, Guoliang AN, Liwei WANG, Shaofei WU

期刊论文

Selective catalytic reduction of NO

Pavlo I. Kyriienko

期刊论文

Effect of different acid anions on highly efficient Ce-based catalysts for selective catalytic reduction

期刊论文

synthesis of functional MFI zeolite materials: Method development, crystallization mechanisms, and catalytic

Zhaoqi Ye, Hongbin Zhang, Yahong Zhang, Yi Tang

期刊论文

Tuning the catalytic selectivity in electrochemical CO

Jiafang XIE,Yuxi HUANG,Hanqing YU

期刊论文

Thermodynamic analysis of reaction pathways and equilibrium yields for catalytic pyrolysis of naphtha

期刊论文

Preparation and catalytic performance of La0.8Sr0.2CoO3 supported on the mullite fiber ceramic

ZENG Lingke, LIU Yanchun, LIU Ping′an, WANG Hui, SHUI Anze, DUAN Bilin

期刊论文

Recent advances and challenges of nitrogen/nitrate electro catalytic reduction to ammonia synthesis

期刊论文

Process analysis of syngas production by non-catalytic POX of oven gas

Fuchen WANG , Xinwen ZHOU , Wenyuan GUO , Zhenghua DAI , Xin GONG , Haifeng LIU , Zunhong YU ,

期刊论文