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吸附分离 1

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客体适应性行为 1

工程成就 1

煤制烯烃；煤间接液化；煤直接液化；煤制天然气；生命周期；碳排放 1

超微孔金属-有机框架材料 1

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Selective epoxidation of linear terminal olefins with metalloporphyrins under mild conditions

Xiaoguang BAI, Yuanbin SHE

《化学科学与工程前沿（英文）》 2009年第3卷第3期页码 310-313 doi: 10.1007/s11705-009-0168-7

摘要： The epoxidation of linear terminal olefins with metalloporphyrins in the presence of dioxygen and isobutyraldehyde under ambient temperature and atmospheric pressure was investigated. The results show that all olefins could be smoothly converted to epoxides with high selectivities (70%-90%). For the metalloporphyrins with different catalytic activities within 1-hexene epoxidation in the order of Fe>Mn>Co, T( -Cl)PPFe(Ⅲ)Cl was most effective, with a 41.7% yield and 80.2% selectivity of 1,2-epoxyhexane. Various amounts of catalyst were investigated, and it was found that with only 10 ppm catalyst the yield of 1,2-epoxyhexane and turnover number (TON) could reach up to 41.9% and 41859, respectively.

关键词： metalloporphyrins olefins dioxygen epoxidation

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Confinement effects in methanol to olefins catalysed by zeolites: A computational review

German Sastre

《化学科学与工程前沿（英文）》 2016年第10卷第1期页码 76-89 doi: 10.1007/s11705-016-1557-3

摘要： Small pore zeolites, containing 8-rings as the largest, are widely employed as catalysts in the process of methanol-to-olefins (MTO). Reactants and products diffuse with constraints through 8-rings and this is one of the reaction bottlenecks related to zeolite micropore topology. Small pore zeolites and silicon-aluminophosphates(SAPOs) containing cavities, where olefins are mainly formed through the hydrocarbon pool (HP) mechanism, are frequently tested for MTO. Shape selectivity of transition states within the side-chain methylation will be reviewed as this is one of the controlling steps of the MTO process, with particular attention to the role of hexamethylbenzene (HMB) and heptamethylbenzenium cation (HeptaMB ), which are the most tipically detected reaction intermediates, common to the paring and side-chain routes within the HP mechanism. The relative stability of these and other species will be reviewed in terms of confinement effects in different cage-based zeolites. The role of the different alkylating agents, methanol, dimethyl ether (DME), and surface methoxy species (SMS) will also be reviewed from the computational viewpoint.

关键词： small pore zeolites SAPOs methanol-to-olefins hydrocarbon pool mechanism alkylation of polymethylbenzenes

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Light olefins synthesis from С

Anton SHALYGIN, Evgenii PAUKSHTIS, Evgenii KOVALYOV, Bair BAL’ZHINIMAEV

《化学科学与工程前沿（英文）》 2013年第7卷第3期页码 279-288 doi: 10.1007/s11705-013-1338-1

摘要： A two-step process was employed to convert methane or ethane to light olefins via the formation of an intermediate monoalkyl halide. A novel K RuOCl /TiO catalyst was tested for the oxidative chlorination of methane and ethane. The catalyst had high selectivity for methyl and ethyl chlorides, 80% and 90%, respectively. During the oxychlorination of ethane at ≥250°C, the formation of ethylene as a reaction product along with ethyl chloride was observed. In situ Fourier transform infrared studies showed that the key intermediate for monoalkyl chloride and ethylene formation is the alkoxy group. The reaction mechanism for the oxidative chlorination of methane and ethane over the Ru-oxychloride catalyst was proposed. The novel fiber glass catalyst was also tested for the dehydrochlorination of alkyl chlorides to ethylene and propylene. Very high selectivities (up to 94%–98%) for ethylene and propylene formation as well as high stability were demonstrated.

关键词： oxychlorination methane ethane light olefins ruthenium catalyst

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Benzene alkylation with long chain olefins catalyzed by ionic liquids: a review

QIAO Congzhen, CAI Yonghong, GUO Quanhui

《化学科学与工程前沿（英文）》 2008年第2卷第3期页码 346-352 doi: 10.1007/s11705-008-0045-9

摘要： The introduction of ionic liquids to alkylation process gives a choice for “green production” in the petrochemical and detergent industry. A lot of papers and patents have been published using chloroaluminate ionic liquid as a novel catalyst for alkylation with high reactivity and easy separation from reactants. These included the acidity, characterization, determination and catalysis technologies in batch and continuous operation mode for different scales. According to published data and several results of pilot alkylation,including the authors’ experience,the prospect of chloroaluminate ionic liquids for commercials was also discussed. It has been pointed out that there still are many difficulties and challenges to be overcome for commercial application of the ionic liquid catalyst.

关键词： different petrochemical characterization introduction chloroaluminate

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Continuous reaction performances of benzene alkylation with long chain olefins catalyzed by ionic liquid

QIAO Congzhen, LI Chengyue

《化学科学与工程前沿（英文）》 2008年第2卷第1期页码 69-73 doi: 10.1007/s11705-008-0014-3

摘要： Based on a compulsive mixing-reacting-separating-recycling small experimental setup,the continuous reaction performances of benzene alkylation with long chain olefins catalyzed by [BMIM]Cl-AlCl ionic liquid were investigated. Three different situations including normal continuous operation mode (reagent materials), sidetrack feeding from different axial positions along the static mixing reactor (reagent materials) and normal continuous alkylation using industrial paraffin and olefins materials were examined. Even under the relatively hypecritical reaction conditions, the single pass conversion of pure 1-dodecene could reach to nearly 100.0%, and the selectivity of 2-phenyl isomer was higher than 37.7%. Although the positions along the reactor for sidetrack feeding were different, the 100.0% single pass conversion of 1-dodecene was also attained before the outlet of the reactor. The refined industrial olefins as raw material could meet with the requirements of continuous alkylation. The influences of impurities such as di-olefins and non-benzene aromatics on the catalytic activity and stability should be studied further.

关键词： stability different hypecritical compulsive mixing-reacting-separating-recycling non-benzene

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Effect of temperature in the conversion of methanol to olefins (MTO) using an extruded SAPO-34 catalyst

Ignacio Jorge Castellanos-Beltran, Gnouyaro Palla Assima, Jean-Michel Lavoie

《化学科学与工程前沿（英文）》 2018年第12卷第2期页码 226-238 doi: 10.1007/s11705-018-1709-8

摘要： The methanol-to-olefin (MTO) reaction was investigated in a bench-scale, fixed-bed reactor using an extruded catalyst composed of a commercial SAPO-34 (65 weight percentage, wt-%) embedded in an amorphous SiO matrix (35 wt-%). The texture properties, acidity and crystal structure of the pure SAPO-34 and its extruded form (E-SAPO-34) were analyzed and results indicated that the extrusion step did not affect the properties of the catalyst. Subsequently, E-SAPO-34 was tested in a temperature range between 300 and 500 °C, using an aqueous methanol mixture (80 wt-% water content) fed at a weight hour space velocity (WHSV) of 1.21 h . At 300 °C, a low conversion was observed combined with catalyst deactivation, which was ascribed to oligomerization and condensation reactions. The coke analysis showed the presence of diamandoid hydrocarbons, which are known to be inactive molecules in the MTO process. At higher temperatures, a quasi-steady state was reached during a 6 h reaction where the optimal temperature was identified at 450 °C, which incidentally led to the lowest coke deposition combined with the highest H/C ratio. Above 450 °C, surges of ethylene and methane were associated to a combination of H-transfer and protolytic cracking reactions. Finally, the present work underscored the convenience of the extrusion technique for testing catalysts at simulated scale-up conditions.

关键词： MTO SAPO-34 temperature extrusion coke light alkanes

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靶向生产低碳烯烃的催化裂化技术——反应机理、生产方案和工艺展望 Review

许友好, Yanfen Zuo, Wenjie Yang, Xingtian Shu, Wei Chen, Anmin Zheng

《工程（英文）》 2023年第30卷第11期页码 100-109 doi: 10.1016/j.eng.2023.02.018

摘要：

Light olefins are important organic building blocks in the chemicals industry. The main low-carbon olefin production methods, such as catalytic cracking and steam cracking, have considerable room for improvement in their utilization of hydrocarbons. This article provides a thorough overview of recent studies on catalytic cracking, steam cracking, and the conversion of crude oil processes. To maximize the production of light olefins and reduce carbon emissions, the perceived benefits of various technologies are examined. Taking olefin generation and conversion as a link to expand upstream and downstream processes, a targeted catalytic cracking to olefins (TCO) process is proposed to meet current demands for the transformation of oil refining into chemical production. The main innovations of this process include a multiple feedstock supply, the development of medium-sized catalysts, and a diameter-transformed fluidized-bed reactor with different feeding schemes. In combination with other chemical processes, TCO is expected to play a critical role in enabling petroleum refining and chemical processes to achieve low carbon dioxide emissions.

关键词： Light olefins Steam cracking Catalytic cracking TCO process Oil processing revolution

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surfactant-assisted synthesis of mesoporous SSZ-39 zeolite with enhanced catalytic performance in the methanol-to-olefins

Hao Xu, Chi Lei, Qinming Wu, Qiuyan Zhu, Xiangju Meng, Daniel Dai, Stefan Maurer, Andrei-Nicolae Parvulescu, Ulrich Müller, Fengshou Xiao

《化学科学与工程前沿（英文）》 2020年第14卷第2期页码 267-274 doi: 10.1007/s11705-019-1845-9

摘要： SSZ-39 zeolite with AEI framework structure is a good catalyst candidate for the methanol-to-olefins (MTO) reaction. However, the diffusion limitation and coke formation often results in fast deactivation of the SSZ-39 zeolite catalyst. One solution for this challenge is to introduce mesoporosity in the SSZ-39 zeolite. Herein, we report the synthesis of mesoporous SSZ-39 zeolite using an organosilane surfactant, , -dimethyl- -(3-(trimethoxysilyl)propyl)octan-1-aminium chloride, as a mesopore template and , -dimethyl- -2,6-dimethylpiperidinium as a micropore template. The obtained zeolites were characterized by X-ray diffraction, N sorption, scanning electron microscopy, temperature programmed desorption of ammonia, and magic angle spinning nuclear magnetic resonance of Al. The results show that the mesoporous SSZ-39 zeolite has high crystallinity, meso/microporosity, high surface area, cuboid morphology, and abundant acidic sites. More importantly, this mesoporous SSZ-39 zeolite exhibits enhanced catalyst lifetime in the MTO reaction due to the presence of mesoporosity for fast mass transfer, compared with a conventional SSZ-39 zeolite without mesoporosity.

关键词： SSZ-39 zeolite mesopores organosilane surfactant MTO reaction soft template mass transfer

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甲醇制烯烃技术——DMTO技术

叶茂, 田鹏, 刘中民

《工程（英文）》 2021年第7卷第1期页码 17-21 doi: 10.1016/j.eng.2020.12.001

关键词：工程成就

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新型煤化工的生命周期碳排放趋势分析

武娟妮,张岳玲,田亚峻,谢克昌

《中国工程科学》 2015年第17卷第9期页码 69-74

摘要：

近年来新型煤化工的发展势头强劲，不仅使煤转化过程的碳排放有大幅增长的趋势，更会带动整个产业链碳排放的增长。为了全面认识新型煤化工发展给气候变化带来的潜在影响，本文采用生命周期评价的方法，以煤制烯烃、煤间接液化、煤直接液化、煤制天然气作为新型煤化工的代表，分析了从煤炭生产到产品消费的整个产业链的碳排放现状和趋势。结果显示，从生命周期的角度认识煤化工发展带来的碳排放潜力，中期新型煤化工生命周期CO₂eq（CO₂当量）排放量是现状的10倍，远期甚至达到现状的21倍，新型煤化工发展呈现过热势头，这给我国的碳减排目标带来不容忽视的压力，其中尤以煤制天然气、煤经甲醇制烯烃和间接液化发展潜力较大；分析表明，整个产业链的碳排放主要来自于煤转化过程，约占54 %~63 %，然而该环节排放的CO₂纯度较高，适于碳捕集、利用和封存(CCUS)，可以显著降低新型煤化工快速发展给气候变化带来的影响；其次，新型煤化工上下游产业链碳排放约占37 %~46 %，其中用电导致的间接排放占7 %~15 %，可通过推广超临界和超超临界发电技术以及高压和超高压输电技术减排。

关键词：煤制烯烃；煤间接液化；煤直接液化；煤制天然气；生命周期；碳排放

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茂金属催化剂催化烯烃聚合反应的研究 ——聚合物的聚集行为和热性能 Letter

吴长江, Minqiao Ren, Liping Hou, Shuzhang Qu, Xinwei Li, Cui Zheng, Jian Chen, 王伟

《工程（英文）》 2023年第30卷第11期页码 93-99 doi: 10.1016/j.eng.2023.07.001

摘要：

Olefin solution polymerization can be used to obtain high-performance polyolefin materials that cannot be obtained via other polymerization processes. Polyolefin elastomers (POE) are a typical example. Due to cost, only a few linear α-olefins (e.g., 1-butene, 1-hexene, and 1-octene) are used as comonomers in solution polymerization in industry. However, α-olefin comonomers with other structures may have different effects on polymerization in comparison with common linear ones. Moreover, the properties of the corresponding materials may differ significantly. In this work, copolymers of ethylene with linear and end-cyclized α-olefins are synthesized using a metallocene catalyst. The copolymerization of ethylene with linear α-olefins results in a higher turn-over frequency (TOF) and lower incorporation than copolymerization with end-cyclized α-olefins, which may indicate that end-cyclized α-olefins have a higher coordination probability and lower insertion rate. In this reaction, the comonomer is distributed randomly in the polymer chain and efficiently destroys crystallization. End-cyclized α-olefins exhibit a much stronger crystallization destructive capacity (CDC) in the copolymer than linear α-olefins, possibly because linear α-olefins act mainly in the radial direction of the main chain of the polymer, while end-cyclized α-olefins act mainly in the axial direction of the main chain.

关键词： Metallocene catalyst Ethylene copolymerization Comonomer distribution Crystallization destructive capacity

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具有客体适应型孔道的阴离子柱撑超微孔材料实现顺-/反-烯烃高效分离

张照强, 崔希利, 姜小明, 丁琦, 崔稷宇, 张袁斌, Youssef Belmabkhout, Karim Adil, Mohamed Eddaoudi, 邢华斌

《工程（英文）》 2022年第11卷第4期页码 82-88 doi: 10.1016/j.eng.2021.10.013

摘要：

顺-/反-烯烃异构体在石油化工行业具有重要应用价值，然而其极为相似的物理化学性质为节能高效的分离纯化技术的开发带来了巨大的挑战。本文设计的阴离子柱撑超微孔金属-有机框架材料，即ZU-36-Ni和ZU-36-Fe，首次实现了基于分子筛分效应的顺-/反-2-丁烯高效分离。ZU-36-Ni 具有智能的客体适应型孔道结构，其对反-2-丁烯呈现出高吸附容量（2.45 mmol∙g⁻¹）并对顺-2-丁烯高效排阻，可从混合气中分离获得99.99%的高纯度顺-2-丁烯气体。密度泛函理论计算表明：当反-2-丁烯进入孔道时，ZU-36-Ni 的有机配体在主-客体相互作用下可定向旋转，从而导致孔穴扩张并使孔道更加适应反-2-丁烯形状及尺寸，加之ZU-36-Ni 具有可匹配反-2-丁烯三维尺寸的最优孔穴维度，使得反-2-丁烯可以被高效吸附。ZU-36-Ni的适应性行为可最大限度地强化ZU-36-Ni 和反-2-丁烯的主-客体作用，不仅有利于提升反-2-丁烯的优先吸附及动力学扩散行为，同时可实现对顺-2-丁烯的高效分子筛分。本工作为拓展孔穴工程在先进智能或适应型多孔材料在客体分子辨识领域的应用提供了新思路。

关键词：吸附分离顺-/反-丁烯超微孔金属-有机框架材料孔工程客体适应性行为