CHINESE JOURNAL OF CATALYSIS
·
2022
·
IF 12.92
Zhaopeng Liu,Youming Ni,Zhongpan Hu,Yi Fu,Xudong Fang,Qike Jiang,Zhiyang Chen,Wenliang Zhu,Zhongmin Liu
The utilization of metal oxide-zeolite catalysts in the syngas-to-olefin reaction is a promising strategy for producing C 2 –C 4 olefins from non-petroleum resources. However, the effect of the crystal phase of metal oxides on the catalytic activity of these oxides is still ambiguous. Herein, typical metal oxides (ZnO/ZrO 2 ) with different crystal phases (monoclinic ( m -ZrO 2 ) and tetragonal ( t -ZrO 2 )) were employed for syngas conversion. The (ZnO/ m -ZrO 2 +SAPO-34) composite catalyst exhibited 80.5% selectivity for C 2 –C 4 olefins at a CO conversion of 27.9%, where the results are superior to those (CO conversion of 16.4% and C 2 –C 4 olefin selectivity of 76.1%) obtained over (ZnO/ t -ZrO 2 +SAPO-34). The distinct differences are ascribed to the larger number of hydroxyl groups, Lewis acid sites, and oxygen defects in ZnO/ m -ZrO 2 compared to ZnO/ t -ZrO 2 . These features result in the formation of more formate and methoxy intermediate species on the ZnO/ m -ZrO 2 oxides during syngas conversion, followed by the formation of more light olefins over SAPO-34. The present findings provide useful information for the design of highly efficient ZrO 2 -based catalysts for syngas conversion.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
INORGANICA CHIMICA ACTA
·
2019
·
IF 2.433
Dang Yang,Qiao Gan,Huafeng Chen,Weilun Ying,Junyi Zhao,Xiaoyu Jia,Dirong Gong
Four cobalt complexes supported by phosphine oxide (P=O) donors (9,9-dimethyl-9H-xanthene-4,5-diyl)bis(diphenylphosphine oxide) cobalt dichloride (Co1) , (9,9-dimethyl-9H-xanthene-4,5-diyl)bis(diphenylphosphine oxide) cobalt bromide (Co2) , N, N'-(pyridine-2,6-diyl)bis(P,P-di- tert -butylphosphinic amide) cobalt dichloride (Co3) and N, N'-(pyridine-2,6-diyl)bis(P,P-di- tert -butylphosphinic amide) cobalt dichloride (Co4) were prepared and characterized. Their catalyses performances in polymerization of isoprene, butadiene, myrcene as well as MMA and styrene were examined. In combination with AlEt 2 Cl, Co1 and Co2 are able to convert isoprene to polyisoprene, whereas the activities of Co3 and Co4 are much low. The resultant polyisoprene are mixture of cis -1,4 and 3,4 isomers, whose ratio are not significantly affected by the type of catalysts and polymerization conditions. Isoprene was found to be more active than myrcene, and butadiene in the case of Co1 /AlEt 2 Cl, suggestive of compromised sterical and electronic effect from the alkyl group at 2-positon of monomers. The Co1 /AlEt 2 Cl system is also moderately active in polymerizations of methyl methacrylate and styrene. Therefore, the current catalysts provided dual polymerization reactivities towards conjugated dienes and olefins that are rare in transition metals catalyzed coordinative polymerization.
研究领域:
高分子化学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2022
·Vol. 29
·期 14
·e202203095
·
IF 5.02
Zihan Zhou,Xingwen Wang,Junjie Li,Yu Gao,Rui Yu,Rongli Jiang
Graphical A green and efficient strategy for synthesizing phosphorus modified ZSM-5 zeolite is proposed by grinding phosphorus source, silicon source and aluminum source with the solvent-free conditions. Phosphorus-modified ZSM-5 zeolites exhibited higher light olefin selectivity and longer catalytic lifetime (33 h) in methanol to olefin reaction when the weight hourly space velocity was 4 h −1 . The traditional hydrothermal synthesis strategy of ZSM-5 zeolite is energy-consumption accompanying by pollution issues. Herein, phosphorus-modified layered ZSM-5 zeolites (PZ) were obtained by one-pot synthesis under solvent-free conditions. The synthesized samples were fully characterized by XRD, SEM, BET, NH 3 -TPD and FTIR. The effect of phosphorus addition on the morphology and catalytic activity of ZSM-5 was investigated. The results showed that phosphorus-modified ZSM-5 zeolites exhibited higher light olefin (ethylene and propylene) selectivity (above 50 %) and longer catalytic lifetime (33 h) in methanol to olefin (MTO) reaction when the weight hourly space velocity was 4 h −1 . Phosphorus-modified ZSM-5 zeolite synthesized by in situ solvent-free method, which not only reduced the discharge of sewage but also showed a simple method to realize the introduction of phosphorous species, which provided a new idea for phosphorus modification of ZSM-5 zeolite.
研究领域:
材料科学
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催化化学
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF SURFACTANTS AND DETERGENTS
·
2016
·Vol. 20
·期 1
·183-191
·
IF 1.853
Wang Yong,Liu Xiaochen,Jiao Tiliu,Niu Jinping
Comparison of surface and interfacial properties of internal olefin sulfonates (IOS) and alpha olefin sulfonates (AOS) shows that hydrocarbon chain branching has a significant influence on interfacial properties at the air–water, pentadecane–water and parafilm–water interfaces. The isomeric branched IOS shows a higher critical micelle concentration and are more effective in reducing the surface tension at the air–water interface by occupying a larger area per molecule. IOS exhibits better dynamic air–water interfacial properties due to a lower meso-equilibrium surface tension. The equilibrium interfacial tensions for AOS and IOS have no remarkable difference at the pentadecane–water interface. The water wettability and electrolyte tolerance are enhanced with branched hydrocarbon chain olefin sulfonates.
研究领域:
化学工程
·
表面化学
✓ 已验证
DOI
高影响因子
JOURNAL OF MOLECULAR CATALYSIS B-ENZYMATIC
·
2014
·
IF 2.745
Long-Hua Zhou,Na Wang,Guan-Nan Chen,Qi Yang,Sheng-Yong Yang,Wei Zhang,Yang Zhang,Xiao-Qi Yu
Lipase-catalyzed direct vinylogous Michael addition reactions of electron-deficient vinyl malononitriles to nitroalkenes are reported for the first time. A series of nitroalkenes reacting with vinyl malononitriles generate the corresponding products with moderate to high yields in the presence of Lipozyme ® (immobilized lipase from Mucor miehei ) with excellent diastereoselectivities in all reactions under optimized conditions. Docking studies were performed to further elucidate the differences between the various enzymes and substrates. Furthermore, we demonstrated the synthetic potential of the multi-functional products by performing reactions that employed the electron-deficient alkylidene double bond.
研究领域:
有机化学
·
生物催化
·
合成化学
✓ 已验证
产品关联
DOI
高影响因子
CRYSTENGCOMM
·
2020
·Vol. 22
·期 37
·6182-6188
·
IF 3.117
Xueshuai Chen,Rongli Jiang,Huilin Hou,Zihan Zhou,Xingwen Wang
ZSM-5/SAPO-34 zeolite composites were successfully synthesized by adding ZSM-5 into SAPO-34 synthetic gel under hydrothermal synthesis conditions, and SAPO-34 as a part of the composite zeolite was synthesized from LAPONITE® as the Si source. The presence of ZSM-5 in the synthetic gel affects the nucleation and crystal growth rate, and core–shell structured zeolite composites can be formed by adding an appropriate amount of ZSM-5. LAPONITE® itself contains Li and Mg atoms which were subsequently introduced into the framework of the SAPO-34 part in the composites via depolymerization–reorganization during the process of crystallization. Furthermore, the depolymerized LAPONITE® can be converted in situ into zeolitic precursors and act as crystalline seeds under hydrothermal conditions. Compared with the ZSM-5/SAPO-34 zeolite composites synthesized from tetraethylorthosilicate (TEOS) instead of LAPONITE® as the Si source, the ZSM-5/SAPO-34 composites synthesized from LAPONITE® exhibited higher selectivity to light olefins and longer lifetime in the MTO reaction. This work provides a convenient route to the synthesis of ZSM-5/SAPO-34 zeolite composites with excellent MTO performance.
研究领域:
化学工程
·
材料科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Dongyang Liu,Yuen Bai,Dongdong Chen,Nan Zhang,Liang Zhao,Jinsen Gao,Chunming Xu
This study investigates the co-cracking of n-hexane and 1-hexene, utilizing 1-hexene as an olefinic initiator to improve light olefin yields. Experimental investigations, kinetic analyses, and density functional theory calculations (DFT) were used to systematically explore cracking performance, interactions, and mechanisms for co-feeding. Comparied with single feeding of n-hexane, leading to higher light olefin yields (increased from 35.77 wt% to 58.61 wt%) when the olefin content is 20 wt%. Kinetic analysis revealed a shift from protolytic to hydrogen transfer cracking pathway when 1-hexene content exceeded 13.6 wt%, with the maximum cracking rate (13.12 h −1 ) constant at 20 wt% olefin content. DFT calculations showed a lower energy barrier for hydrogen transfer cracking between n-hexane and 1-hexene, compared to n-hexane cracking alone. Therefore, a co-cracking mechanism was proposed, involving paraffin activation through carbocation intermediates generated by olefin, followed by β-cracking to generated light olefins and carbenium ion regeneration, establishing a framework for paraffin-olefin co-conversion.
研究领域:
催化化学
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石油炼制
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反应动力学
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理论化学
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材料化学
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-10
·
IF 16.6
Yan Yong-Qing,Chen Ya,Wang Zhao,Chen Li-Hua,Tang Hao-Lin,Su Bao-Lian
Alkene feedstocks are used to produce polymers with a market expected to reach 128.4 million metric tons by 2027. Butadiene is one of the impurities poisoning alkene polymerization catalysts and is usually removed by thermocatalytic selective hydrogenation. Excessive use of H 2 , poor alkene selectivity and high operating temperature (e.g. up to 350 °C) remain the most significant drawbacks of the thermocatalytic process, calling for innovative alternatives. Here we report a room-temperature (25~30 °C) electrochemistry-assisted selective hydrogenation process in a gas-fed fixed bed reactor, using water as the hydrogen source. Using a palladium membrane as the catalyst, this process offers a robust catalytic performance for selective butadiene hydrogenation, with alkene selectivity staying around 92% at a butadiene conversion above 97% for over 360 h of time on stream. The overall energy consumption of this process is 0.003 Wh/mL butadiene , which is thousands of times lower than that of the thermocatalytic route. This study proposes an alternative electrochemical technology for industrial hydrogenation without the need for elevated temperature and hydrogen gas.
研究领域:
化学工程
·
电化学
·
催化
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL
·
2025
·
IF 7.5
Junjie Liu,Jianmin Wu,Qiwen Sun,Jiancheng Wang,Yan Sun,Hengxuan Zhang
The high-viscosity poly-alpha-olefin was prepared from Fischer-Tropsch mixed α-olefins (FTO) polymerization under [EBIZrCl 2 /Al( i Bu) 3 /[Ph 3 C] + [B(C 6 F 5 ) 4 ] - system (EBI = rac -C 2 H 4 (1-Ind) 2 ), and its mechanism was investigated by in situ UV–Vis, 1 H NMR and ESI-MS. The results show that the kinematic viscosity at 100°C (KV 100 ), viscosity index (VI) and yield of product reach to 306.3 cSt, 244 and 81.12 % under optimum reaction condition, respectively. Through adjusting temperature to 20°C, in situ UV–Vis, 1 H NMR and ESI-MS are conducted to monitor the formation of origin species (EBIZr( i Bu) 2 + ), active species (EBIZr-σ-y n + (y = nonenyl, decenyl and undecenyl, n ≥ 1)), reactivated species and dormant species (EBIZr-η 3 -(1-R-C m H m+1 ) + (R = n-propyl and m = 6 or 7 or 8)). The simultaneous generation of active and dormant species is observed, and the reaction process is described as [FTO] + [catalyst] → [active species] + [dormant species]. This reaction fitting curve also conforms to the Boltzmann (R 2 ≥ 0.993). The effect of different types of olefins on catalytic evolution and product properties is investigated. The existence of multiple α-olefins inhibits the formation of the second inactivate species found in 1-decene polymerization. However, the multiple isomeric olefins further enhance the possibility of dormant species generation, because of the promotion of β-H concentration in catalytic system, leading to the higher activation energy (19.597kJ/mol) than pure 1-decene (10.949kJ/mol). Based on those findings, a possible mechanism in ansa-zirconocene catalyzed to prepare high-viscosity poly-alpha-olefin from Fischer-Tropsch mixed α-olefins is proposed.
研究领域:
高分子化学
·
催化化学
·
石油化学
·
材料科学
·
工业化学
·
反应机理
·
流变性能
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Jun Mou,Xingqi Fan,Fei Liu,Xiaodan Wang,Tianxiang Zhao,Peng Chen,Ziwei Li,Chunliang Yang,Jianxin Cao
The direct conversion of CO 2 hydrogenation to lower olefins via methanol as an intermediate is of great significance, but challenges still remain. Herein, we present a binary Mn 2 O 3 -ZnO oxide, which is responsible for catalytic hydrogenation of CO 2 to methanol. After combination of Mn 2 O 3 -ZnO and SAPO-34 molecular sieve, the catalytic reaction displays a markable increase. CO 2 adsorption by alkaline nature, followed by oxygen vacancy activation and synergistic hydrogenation over the binary Mn 2 O 3 -ZnO oxide are the prerequisites for the tandem reaction. However, the tandem spacing between oxide and molecular sieve plays a crucial role, because the suitable intimacy can induce enhanced methanol formation as intermediate via tandem dynamics effect, causing an apparent limitation for reverse water gas shift reaction at high temperature. The optimum mass ratio of 3:1 for two phases demonstrates that more components of binary oxide are needed to improve the rate of CO 2 hydrogenation to methanol, aiming to balance the two-step tandem reaction. Finally, under conditions of 380 ℃, 3 MPa and 3600 mL/g cat /h, 20%Mn 2 O 3 -ZnO/SAPO-34 tandem catalyst is obtained by physical ball milling after 15 min, with excellent stability, sulfur tolerance and catalytic performance with CO 2 conversion at almost 30%, lower olefins selectivity of 80.2% (propylene/ethylene = 5.6:1), and single-pass yield of 10.7%.
研究领域:
催化化学
·
能源化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2022
·Vol. 13
·期 1
·1-8
·
IF 17.694
Zhang Peixin,Yang Lifeng,Liu Xing,Wang Jun,Suo Xian,Chen Liyuan,Cui Xili,Xing Huabin
Selective paraffin capture from olefin/paraffin mixtures could afford high-purity olefins directly, but suffers from the issues of low separation selectivity and olefin productivity. Herein, we report an ultramicroporous material (PCP-IPA) with parallel-aligned linearly extending isophthalic acid units along the one-dimensional channel, realizing the efficient production of ultra-high purity C 2 H 4 and C 3 H 6 (99.99%). The periodically expanded and parallel-aligned aromatic-based units served as a paraffin nano-trap to contact with the exposed hydrogen atoms of both C 2 H 6 and C 3 H 8 , as demonstrated by the simulation studies. PCP-IPA exhibits record separation selectivity of 2.48 and separation potential of 1.20 mol/L for C 3 H 8 /C 3 H 6 (50/50) mixture, meanwhile the excellent C 2 H 6 /C 2 H 4 mixture separation performance. Ultra-high purity C 3 H 6 (99.99%) and C 2 H 4 (99.99%) can be directly obtained through fixed-bed column from C 3 H 8 /C 3 H 6 and C 2 H 6 /C 2 H 4 mixtures, respectively. The record C 3 H 6 productivity is up to 15.23 L/kg from the equimolar of C 3 H 8 /C 3 H 6 , which is 3.85 times of the previous benchmark material, demonstrating its great potential for those important industrial separations.
研究领域:
化学工程
·
材料科学
·
分离技术
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yibo Tang,Jiayin Liang,Jiabing Chen,Mengheng Wang,Xinying Liu,Xiaojun Lu
Na- and Mn-promoted Co 2 C-based catalysts have demonstrated promise for the one-step conversion of syngas to olefins via Fischer-Tropsch synthesis to olefins (FTO). However, their consistently low activity limits their industrial applications. Here, we designed a compound catalyst comprising a CoMn composite catalyst and ZSM-5 zeolite, achieving 4.9 times the activity compared to the sole Co 2 C catalyst without compromising olefin selectivity. CO– and H 2 -TPD studies, in-situ DRIFT experiment, and DFT calculation revealed that the surface acidity of ZSM-5 modulated the strong electron effect of Na, subsequently strengthening H 2 adsorption on the Co 2 C catalyst surface. The H-assisted CO dissociation was therefore promoted and the catalyst activity was boosted. Meanwhile, Co 2 C as active site was unaffected, maintaining high selectivity to olefins. Constructing an interface between Co 2 C and ZSM-5 in the compound catalyst is proven to be a successful strategy for enhancing the activity of Co 2 C-based catalysts for FTO.
研究领域:
催化化学
·
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）