CHEMICAL ENGINEERING SCIENCE
·
2019
·
IF 3.372
Yuning Tang,Sa Wang,Xin Zhou,Ying Wu,Shikai Xian,Zhong Li
A facile and efficient room-temperature synthesis approach was proposed to prepare MOF material Cu(Qc) 2 (henceforth called RT-Cu(Qc) 2 ) with ultramicropores. RT-Cu(Qc) 2 was successfully synthesized at room-temperature by means of (Zn, Cu) hydroxyl double salt as intermediate within 1–12 h. The resulting RT-Cu(Qc) 2 exhibited excellent water vapor stability and its C 2 H 6 uptake reached 2.19 mmol/g at 288 K and 1 bar. Its C 2 H 6 /C 2 H 4 and C 2 H 6 /CH 4 uptake ratio at 298 K and 1 bar were up to 3.70 and 22.67, superior to benchmark MAF-49, Cu(Qc) 2 and ZIF-7. Its IAST-predicted C 2 H 6 /C 2 H 4 and C 2 H 6 /CH 4 selectivity reached 4.1 (1:1 v:v) and 35.9 (1:9 v:v) at 288 K and 1 bar, higher than most of ethane-capturing MOFs. Molecular simulation revealed well-defined host–guest match between Cu(Qc) 2 and ethane. Fixed bed experiments confirmed that ethane/ethylene or ethane/methane mixtures can be completely separated using RT-Cu(Qc) 2 . RT-Cu(Qc) 2 has great potential for separation of ethane/ethylene and the recovery of ethane from natural gas.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Haozhen Dou,Bin Jiang,Xiaoming Xiao,Mi Xu,Xiaowei Tantai,Baoyu Wang,Yongli Sun,Luhong Zhang
Protic ionic liquids (PILs) were utilized for the fabrication of composite membranes containing silver salt as the C2H4 transport carrier to perform C2H4/C2H6 separation for the first time. The intrinsic nanostructures of PILs were adopted to construct fast and selective C2H4 transport nanochannels. The investigation of structure–performance relationships of composite membranes suggested that transport nanochannels (polar domains of PILs) could be tuned by the sizes of cations, which greatly manipulated activity of the carrier and determined the separation performances of membranes. The role of different carriers in the facilitated transport was studied, which revealed that the PILs were good solvents for dissolution and activation of the carrier due to their hydrogen bond networks and waterlike properties. The operating conditions of separation process were investigated systemically and optimized, confirming C2H4/C2H6 selectivity was enhanced with the increase of silver salt concentration, the flow rate of sweep gas, and the feed ratio of C2H4 to C2H6, as well as the decrease of the transmembrane pressure and operating temperature. Furthermore, the composite membranes exhibited long-term stability and obtained very competitive separation performances compared with other results. In summary, PIL composite membranes, which possess good long-term stability, high C2H4/C2H6 selectivity, and excellent C2H4 permeability, may have a good perspective in industrial C2H4/C2H6 separation.
研究领域:
化学工程
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2018
·
IF 3.956
Tian-qi Lei,Yan-hu Cheng,Chang-xi Miao,Wei-ming Hua,Ying-hong Yue,Zi Gao
Dehydrogenation of ethane to ethylene in the presence or absence of CO 2 over silica-doped TiO 2 supported Ga 2 O 3 catalysts was investigated. The silica doping of TiO 2 support greatly improved the dehydrogenation activity in the absence of CO 2 , which can be ascribed to the increased acid sites. The initial activity in the presence of CO 2 decreased after the silica doping, due to the reduction in reverse water-gas shift ability. However, the selectivity as well as the stability increased, resulting in higher steady ethylene yield. A dynamic process consisting of alternative oxidative dehydrogenation/regeneration cycles by gasifying the carbon deposit with air for 10 min after each cycle of 6 h reaction was also performed and relatively stable ethane conversion ~30% and ethylene yield ~25% can be achieved. The different catalytic behaviors are probably associated with the different state of gallium species, caused by the different interaction between the Ga 2 O 3 and support.
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL POLLUTION
·
2021
·
IF 8.071
Na Liu,Qing Hu,Chao Wang,Lizhi Tong,Chih-Huang Weng,Longzhen Ding
This study demonstrated that nitrogen-doped carbon materials (NCMs) could effectively catalyze the chlorine elimination process in hexachloroethane (HCA) declorination in sulfide-containing environments for the first time. The k obs values of HCA dechlorination by sulfide in the presence of 10 mg/L NCMs were higher than that of no mediator at pH 7.3 by one or two orders of magnitude. The catalytic capabilities of NCMs on HCA dechlorination were evident in common ranges of natural pH (5.3–8.9) and it could be accelerated by the increase of pH but be suppressed by the presence of dissolved humic acid . Moreover, NCMs exhibited much better catalytic capability on HCA dechlorination compared to the carbon materials, mainly owing to the combined contributions of pyridine N, including enhanced nucleophilic attack to HCA molecule by generating newborn C–S–S and activation of HCA molecule by elongating C–Cl bonds. The functions of pyridine N in micron-sized NCMs with mesopores were better than in nano-sized NCMs on HCA dechlorination. These findings displayed the potential of NCMs, when released into sulfide-containing environments, may significantly increase the dechlorination of chlorinated aliphatic hydrocarbons.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2012
·Vol. 26
·期 11
·600-603
·
IF 2.061
Dongsheng Bai,Huanwang Jing,Guangjian Wang
The synthesis of cyclic carbonates from epoxides and carbon dioxide catalyzed by cyanocobalamin and n -Bu 4 NI system was achieved under 0.8 MPa CO 2 pressure at 140°C without organic solvents. Propylene carbonate was obtained in 99% yield within 6 h under the optimized reaction conditions. The cyanocobalamin catalyst could be recycled with water and retained moderate catalytic activity. Copyright © 2012 John Wiley & Sons, Ltd.
研究领域:
化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
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2015
·
IF 3.942
Cen Tang,Yanxia Jin,Jiqing Lu,Xiaonian Li,Guanqun Xie,Mengfei Luo
A series of Mg catalysts supported on SiO 2 were prepared by an incipient wetness impregnation method and tested for gas phase dehydrochlorination of 1,1,2-trichloroethane. It was found that these catalysts were very active and selective for the reaction. The catalytic performance depended on the Mg loading rather than the Mg precursors as the catalysts using Mg(NO 3 ) 2 ·6H 2 O and MgCl 2 ·6H 2 O as the precursors showed the similar performance. A catalyst containing 10 wt.% of Mg showed the best performance with a steady state TCE conversion of 92% and cis -dichloroethene selectivity of 91%. Moreover, characterizations of the catalysts revealed the formation of Cl-containing Mg species on the surface during the reaction. The analyses of the compositions of the stable catalysts under working conditions indicated a Cl/Mg ratio of 1, suggesting that Mg(OH)Cl could be the active sites for the reaction.
研究领域:
化学工程
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催化科学
✓ 已验证
DOI
高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
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2015
·Vol. 133
·期 9
·
IF 1.768
Fang Qiu,Minle Peng,Zhimei Wei,Xiaojun Wang,Jie Yang
A novel kind of sulfonated polyethersulfonephenylethane (SPESPE) was successfully synthesized firstly in this work. Then the SPESPE was introduced in polyethersulfone (PES) microspheres prepared by the electrospraying technique. The microspheres were applied to adsorbing bisphenol A (BPA) from its aqueous solution. Compared with the PES microspheres, the adsorption capacity of PES/SPESPE microspheres for BPA was increased significantly. Furthermore, the adsorption capacity of PES/SPESPE microspheres was enhanced by increasing the amounts of SPESPE in the microspheres. The pH of solution had influence on the adsorption capacity of PES/SPESPE microspheres. The kinetic data of adsorption were found to follow pseudo-second-order model. The Freundlich isotherm model was suitable to describe the equilibrium adsorption data. The microspheres also showed excellent regeneration and reuse ability. These results indicated that the PES/SPESPE microspheres have the potential to be used in environmental application. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016 , 133 , 43066.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
WATER AIR AND SOIL POLLUTION
·
2016
·Vol. 227
·期 9
·1-14
·
IF 1.551
Danish Muhammad,Gu Xiaogang,Lu Shuguang,Zhang Xiang,Fu Xiaori,Xue Yunfei,Miao Zhouwei,Ahmad Ayyaz,Naqvi Muhammad,Qureshi Abdul Sattar
This study primarily focused on the performance of 1,1,1-trichloroethane (1,1,1-TCA) and trichloroethylene (TCE) degradation involving redox reactions in zeolite-supported nanozerovalent iron composite (Z-nZVI)-catalyzed sodium percarbonate (SPC) system in aqueous solution with five different chelating agents (CAs) including oxalic acid (OA), citric acid monohydrate (CAM), glutamic acid (GA), ethylenediaminetetraacetic acid (EDTA), and L-ascorbic acid (ASC). The experimental results showed that the addition of OA achieved almost 100 % degradation of 1,1,1-TCA and TCE. The addition of CAM and GA also significantly increased the contaminant degradation, while excessive addition of them inhibited the degradation. In contrast, EDTA and ASC showed negative impacts on 1,1,1-TCA and TCE degradation, which might be due to the strong reactivity with iron and OH ● scavenging characteristics. The efficiency with CA addition on 1,1,1-TCA and TCE degradation decreased in the order of OA > CAM > GA > no CAs > EDTA > ASC. The extensive investigations using probe compound tests and scavenger tests revealed that both contaminants degraded primarily by OH ● and O 2
–● in chelated Z-nZVI-catalyzed SPC system. The significant improvement in 1,1,1-TCA and TCE degradation efficiency was accredited due to the (i) increase in concentration of Fe 2+ and (ii) continuous generation of OH ● radicals and maintenance of its quantity, ensuring more stability in the aqueous solution. Finally, the complete mineralization of 1,1,1-TCA and TCE in the OA-chelated, Z-nZVI-catalyzed SPC system was confirmed without any chlorinated intermediate by-products detected, demonstrating a great potential of this technique in the application of groundwater remediation.
Schematic representation of the reactive oxygen species in the chelated Z-nZVI-catalyzed percarbonate system for the degradation of 1,1,1-TCA and TCE
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CHEMISTRY
·
2021
·Vol. 40
·期 8
·918-924
·
IF 6
Jisheng Xu,Chengxiang Shi,Shuguang Zhang,Qiancheng Zheng,Lun Pan,Xiangwen Zhang,Ji-Jun Zou
Comprehensive Summary Non-oxidative ethane dehydrogenation is a promising route to produce ethene. Herein, PtSn supported catalysts were investigated to achieve better ethane dehydrogenation performance by introduction of different Zr promoters, i.e. , framework Zr and ZrO 2 , to mesoporous MCM-41. In-situ XRD, TEM and CO chemisorption show that aggregation of metal particles and phase segregation of Pt 3 Sn to Pt and PtSn 3 at high temperature occur for PtSn/M, leading to bad ethane dehydrogenation activity. Strong interaction between ZrO 2 and PtSn species, as proved by XPS, results in restrained metal particles, which promotes the initial reactivity. However, Pt phase generated on surface is disadvantageous for the desorption of produced ethene as indicated by CO-IR and C 3 H 6 -TPD, and pyridine-IR and NH 3 -TPD indicate strong acidity generated. Both deactivate the catalyst rapidly by deep dehydrogenation and coking. Moderate interaction between PtSn species and Si-O-Zr with much weaker acidity is formed when framework Zr is incorporated into MCM-41, which benefits the dispersion of metal particles, formation of Pt 3 Sn/Pt species and stabilization of metal species from phase segregation. Outstanding initial ethane conversion and ethene selectivity of ca. 99% were achieved for the optimal PtSn/ZrM, which is more coking-tolerant and stable by generating graphitic carbon mainly on support instead of active metals.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
Catalysts
·
2022
·Vol. 12
·期 5
·493
·
IF 4.501
Gengzhe Song,Qi Wang,Liang Yang,Duohua Liao,Shuang Li
A series of the layered double oxides supported molybdenum oxide catalysts were synthesized and evaluated in the oxidative dehydrogenation of ethane with CO2(CO2-ODHE). The 22.3 wt% Mo/LDO catalyst delivered a 92.3%selectivity to ethylene and a 7.9% ethane conversion at relatively low temperatures. The molybdenum oxide catalysts were fully characterized by XRD, BET, SEM, TEM, UV–vis, Raman TG, and XPS. Isolated [MoO4]2−dominated on the surface of the fresh 12.5 wt% Mo/LDO catalyst. With the increase of the Mo content, the Mo species transformed from [MoO4]2−to [Mo7O24]6−and [Mo8O26]4−on the 22.3 wt% and 30.1 wt% Mo/LDO catalysts, respectively. The redox mechanism was proposed and three Mo species including [MoO4]2−, [Mo7O24]6−, and [Mo8O26]4−showed quite different functions in the CO2-ODHE reaction: [MoO4]2−, with tetrahedral structure, preferred the non-selective pathway; [Mo7O24]6−, with an octahedral construction, promoted the selective pathway; and the existence of [Mo8O26]4−reduced the ability to activate ethane. This work provides detailed insights to further understand the relationship between structure–activity and the role of surface Mo species as well as their aggregation state in CO2-ODHE.Keywords:ethane;oxidative dehydrogenation;molybdenum oxide;CO2;Mo/LDO catalyst
研究领域:
化学工程
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2023
·
IF 2.8
Zhang Yakun,Xu Lin,Wang Wen,Wu Qing,Zhang Yi
The efficient conversion of ethane has attracted more and more attention because of the shale gas revolution. The coupling of ethane dehydrogenation (EDH) and benzene alkylation over the 1.5Pt/HZSM-5 realize high activity close to the thermodynamic equilibrium of EDH at 500 ℃ and 0.9 bar ethane partial pressure. Meanwhile, the coupled reaction shows long-term stability during 22 h with a slightly decreased ethane conversion of 0.03% per hour and as high as 42% selectivity of ethylbenzene. Based on various characterization, including XRD, HR-TEM, NH 3 -TPD, Py-IR, TGA, it is confirmed that the coupling reaction could convert ethylene, formed by EDH over Pt sites, to ethylbenzene via benzene alkylation over Brönsted acidic sites (BAS) subsequently, and suppressing the sintering of Pt species and coke deposition induced by aromatization and deep dehydrogenation, resulting in high activity and long-time steady state. Graphical Abstract
研究领域:
化学工程
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2019
·Vol. 10
·期 3
·835-843
·
IF 5.726
Yan Zhang,Shide Wu,Xia Xu,Heqing Jiang
Rapid deactivation by coke deposition is the main obstacle of ethane aromatization over Zn/ZSM-5. In this work, using the prepared nanosized Zn/HZSM-5, an almost threefold product yield and significantly improved stability were achieved in comparison with those of the microsized catalyst. XRD and XPS analyses indicated that a higher percentage of reactive [ZnOZn]2+ species was maintained during ethane aromatization over nano-Zn/HZSM-5 than micro-Zn/HZSM-5. In addition, the evolution of carbon deposits over nanosized and microsized Zn/ZSM-5 was investigated during prolonged ethane aromatization reaction using Raman spectroscopy and thermogravimetry measurements. Compared to the microsized catalyst, the nanosized zeolite facilitated the faster escape of light aromatics and the precursors of carbon deposits from the zeolite pores, thus suppressing the accumulation of coke deposits and improving the catalyst stability. Based on the nanosized Zn/HZSM-5, a protocol of isothermal reaction followed by regeneration was developed by periodically removing carbonaceous deposits, and an ∼25–35% product yield was achieved after 10 reaction–regeneration cycles.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）