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The chain-condensation reaction and its reversible reaction are the key controlling elementary reactions of the copolymerization mechanism for the studied system,while the chain initiation elementary reactions are not the key controlling elementary reactions of the copolymerization mechanism for the studied system.

其中,链引发及其逆反应对D4/APAEDMS的本体共聚反应没有直接调控作用,而链缩合及其逆反应是本体系反应机理不同于纯活性阴离子聚合或逐步聚合反应机理的关键原因。

For the reaction of benzaldehyde, malononitrile and α-naphthol, the ionic liquid can be recycled at least 3 times without the significant loss of activity.

以对氯苯甲醛、丙二腈和α-萘酚为模板反应,离子液体可重复使用3次,其催化活性没有明显降低,同时还探讨了该反应体系下的可能反应机理。

Oxygen was found to be the best oxidant and almost no reaction was observed without adding any oxidant.

发现氧气是该反应较好的氧化剂,而没有氧化剂存在时,几乎没有羰基化反应发生。

Various alcohols are tolerable under the present conditions including benzylic alcohols,allylic alcohols as well as simple aliphatic alcohols.

普通烷基醇如环己醇,甚至最简单的甲醇和乙醇也能顺利反应,产率中等。在这个反应中,磷钨酸能够顺利回收,并在此被用于催化反应,活性没有降低。

Dealcoholization temperature markedly influences the surface area and porosity of the resultant MAO-supports. When the support was pretreated at lower or higher temperature, the corresponding MAO-support shows very low surface area;2.XRD and IR analyses indicate that MAO has reacted with the residual ethanol in the supports, which is an important manner to get MAO fixed on the carrier. Morever, XPS analyse indicates that MAO can also be coordinated with MgCl_2, which is another way to get MAO fixed on the support;3.ICP and EDX analyses indicate that dealcoholization temperature not only determined the element content on the solid catalyst, but also influences the element distribution on the carrier;4.The activities of the supported phenoxy-imine catalysts and the properties of resultant polymers are strongly dependent on the dealcoholization temperature. The support (MSP-5) obtained by treating MgCl_2·2.56C_2H_5OH at 160℃for 4 h, then modified by MAO is very effective for immobilizing complex 3, the resultant solid catalyst (MSPC-5) shows very high activity in ethylene polymerization, and its kinetics of polymerization is stable during the reaction process. Finally, PEs with spherical morphology and high bulk density (over 0.35g/ml) were obtained, without reactor fouling;5.In this work, polymerization conditions such as alkylaluminums, Al/Zr ratio, temperature and H_2 had a pronounced effect on the activity of MSPC-5 and properties of PE;(3). New MgCl_2-Supported Single-Site Catalysts for Ethylene PolymerizationIn this work, a kind of new MgCl_2 support was obtained by anhydrous MgCl_2 co-milled with solid MAO, and it is a creative contribution. Then some single-site catalysts were supported on the new MgCl_2 support, and the resulted solid catalysts were tested in ethylene polymerization, the results indicated that:1.XRD and IR analyses indicate that MAO does be coordinated with MgCl_2, which is in good agreement with the results obtained by XPS;2.co-mlling time had no obvious effect on the texture of support after 12 hours;3.In this work, MgCl_2 was co-milled with solid MAO for different hours, and then complex 3 was supported on these co-milled supports. It was found that co-milling time markedly influences the activity of solid catalysts, but it had negligible effect on the kinetic profile and the properties of resultant PE.

XPS研究结果表明,MAO不仅仅只和乙醇作用,MAO还与MgCl_2本身有一定的作用,这是一个极为重要的发现;3、通过ICP和EDX表征,发现载体的脱醇温度直接影响着元素在固体催化剂中的含量及分布;4、脱醇温度极大地影响着负载苯氧基亚胺类催化剂的活性和聚合物的性能,特别是原始载体经160℃活化4小时制备得到的固体催化剂MSPC-5的活性明显高于其他脱醇温度条件下制得的固体催化,并且催化剂寿命长,表现出稳定的动力学行为,最终获得了高堆密度(大于0.35g/ml)的球形聚乙烯颗粒;5、本文选择MSPC-5为研究对象,考察了聚合反应参数对催化剂的活性及其聚合物的影响,研究发现:不同的烷基铝对催化剂具有非常重要的影响,特别足TIBA对MSPC-5的助催化活性最高,烷基铝的加入量有一个较佳值,聚合温度为80度时活性最高,H_2的加入使催化剂的活性明显降低且聚合物的分子量也减小;、新型氯化镁载体负载单活性中心催化剂催化乙烯聚合本文创造性采用固体MAO与无水氯化镁直接进行共研磨,制备出了一种的新型的氯化镁载体,并将该载体用于多种单活性中心催化剂的负载化研究,研究表明:1、通过BET、XRD的表征,再次证实了MAO与MgCl_2之间具有直接作用,与XPS的研究结果相一致;2、当研磨时间高于12小时时,延长研磨时间对载体的结构没有显著的影响;3、将配合物3负载于共研磨时间不同的一系列载体上,乙烯聚合结果表明,尽管共研磨时间对负载催化剂的活性具有明显的影响,但是它对聚合物的性能以及催化剂的影响不明显。

Dealcoholization temperature markedly influences the surface area and porosity of the resultant MAO-supports. When the support was pretreated at lower or higher temperature, the corresponding MAO-support shows very low surface area; 2.XRD and IR analyses indicate that MAO has reacted with the residual ethanol in the supports, which is an important manner to get MAO fixed on the carrier. Morever, XPS analyse indicates that MAO can also be coordinated with MgCl_2, which is another way to get MAO fixed on the support; 3.ICP and EDX analyses indicate that dealcoholization temperature not only determined the element content on the solid catalyst, but also influences the element distribution on the carrier; 4.The activities of the supported phenoxy-imine catalysts and the properties of resultant polymers are strongly dependent on the dealcoholization temperature. The support (MSP-5) obtained by treating MgCl_2·2.56C_2H_5OH at 160℃for 4 h, then modified by MAO is very effective for immobilizing complex 3, the resultant solid catalyst (MSPC-5) shows very high activity in ethylene polymerization, and its kinetics of polymerization is stable during the reaction process. Finally, PEs with spherical morphology and high bulk density (over 0.35g/ml) were obtained, without reactor fouling; 5.In this work, polymerization conditions such as alkylaluminums, Al/Zr ratio, temperature and H_2 had a pronounced effect on the activity of MSPC-5 and properties of PE;(3). New MgCl_2-Supported Single-Site Catalysts for Ethylene Polymerization In this work, a kind of new MgCl_2 support was obtained by anhydrous MgCl_2 co-milled with solid MAO, and it is a creative contribution. Then some single-site catalysts were supported on the new MgCl_2 support, and the resulted solid catalysts were tested in ethylene polymerization, the results indicated that: 1.XRD and IR analyses indicate that MAO does be coordinated with MgCl_2, which is in good agreement with the results obtained by XPS; 2.co-mlling time had no obvious effect on the texture of support after 12 hours; 3.In this work, MgCl_2 was co-milled with solid MAO for different hours, and then complex 3 was supported on these co-milled supports. It was found that co-milling time markedly influences the activity of solid catalysts, but it had negligible effect on the kinetic profile and the properties of resultant PE.

XPS研究结果表明,MAO不仅仅只和乙醇作用,MAO还与MgCl_2本身有一定的作用,这是一个极为重要的发现; 3、通过ICP和EDX表征,发现载体的脱醇温度直接影响着元素在固体催化剂中的含量及分布; 4、脱醇温度极大地影响着负载苯氧基亚胺类催化剂的活性和聚合物的性能,特别是原始载体经160℃活化4小时制备得到的固体催化剂MSPC-5的活性明显高于其他脱醇温度条件下制得的固体催化,并且催化剂寿命长,表现出稳定的动力学行为,最终获得了高堆密度(大于0.35g/ml)的球形聚乙烯颗粒; 5、本文选择MSPC-5为研究对象,考察了聚合反应参数对催化剂的活性及其聚合物的影响,研究发现:不同的烷基铝对催化剂具有非常重要的影响,特别足TIBA对MSPC-5的助催化活性最高,烷基铝的加入量有一个较佳值,聚合温度为80度时活性最高,H_2的加入使催化剂的活性明显降低且聚合物的分子量也减小;、新型氯化镁载体负载单活性中心催化剂催化乙烯聚合本文创造性采用固体MAO与无水氯化镁直接进行共研磨,制备出了一种的新型的氯化镁载体,并将该载体用于多种单活性中心催化剂的负载化研究,研究表明: 1、通过BET、XRD的表征,再次证实了MAO与MgCl_2之间具有直接作用,与XPS的研究结果相一致; 2、当研磨时间高于12小时时,延长研磨时间对载体的结构没有显著的影响; 3、将配合物3负载于共研磨时间不同的一系列载体上,乙烯聚合结果表明,尽管共研磨时间对负载催化剂的活性具有明显的影响,但是它对聚合物的性能以及催化剂的影响不明显。

The results show that:First, concentration of hydrogen peroxide have the most obvious influence to oil yield and carbon black yield,with the increase of concentration of hydrogen peroxide the oil yield first increase then decrease,when concentration of hydrogen peroxide is 8.19% or so,the oil yield reach to the biggest value, and with the increase of concentration of hydrogen peroxide carbon black yield decrese;Then,reaction time have more obvious influence to oil yield and carbon black yield,oil yield increase but carbon black yield decrease with the increase of reaction time;Thirdly,reaction tempreture have some influence to oil yield and carbon black yield,samely,oil yield increase but carbon black yield decrease with the increase of reaction tempreture;Finally,reaction pressure does almost no influence on oil yield and carbon black yield.

研究结果表明:过氧化氢质量浓度对产油率和炭黑产率的影响最为显著,产油率随过氧化氢质量浓度的提高先提高后降低,在过氧化氢质量浓度为8.19%左右时达到最大值,炭黑产率随过氧化氢质量浓度的提高而降低;反应时间对产油率和炭黑产率的影响也比较显著,产油率随反应时间的增加而提高,炭黑产率随反应时间的增加而降低;反应温度对产油率和炭黑产率也有一定的影响,产油率随反应温度的提高而相应地提高,炭黑产率随反应温度的提高而降低;在本文实验范围内,反应压力对产油率和炭黑产率基本上没有影响。

Furthermore,the adsorption of acetylene on the Ni(111)surface is investigatedby DV-Xα method,as well as its migration pathway from the aligned bridgesite,the favorite adsorption site for ethylene,to the cross-bridge site.Afterstudying several reaction pathways of C2H2 on Ni(111),we find that acetylene,as the product of dehydrogenated ethylene,will migrate from the alignedbridge site to the cross-bridge site with a very small energy barrier,0.02eV.

给出了乙炔在各个吸附位的吸附结构,并在假定乙烯在脱氢前没有迁移的基础上,对各种可能的反应途径作了模拟研究,发现乙炔在平行桥位的吸附结构不稳定,通过1.24的平移和30度的旋转的耦合,迁移到垂直桥位,迁移过程中只有0.02eV的势垒。

It's no wonder that only people with rich aesthetic appreciation experiences have a physiological or psychological demand for tachisme, because in their eyes, what they expect most is a kind of pleasant sensation on aesthetic appreciation. They have seen too many delicate paintings, so their eyes are very particular and slashing. Especially, they can't bear ordinary paintings without mien. It has become impossible for those quotidian and easy descriptions about the reality without sound and colors to catch their eyes, to say nothing of touching their heartstrings. In their eyes, a good artwork "shall not get separated from the thought course of the reality to make an immediate response to various experiences and feelings in the life, and express them in a surprising manner with a breath-taking vigor, even make a crazy demonstration."

朱健甫:这也难怪,只有有着丰富的审美经验者,他才会对抽象绘画有一种生理和心理的需求,因为在他们眼睛里最为期盼的是一种审美快感,他们看了太多的精美绘画,因而眼睛是十分挑剔与苛刻的,尤其不能容忍平凡,没有声色的存在,对于那些司空见惯的对现实简单的描述,已不能打动他们的眼球,更无法触动他们的心灵,在他们看来,好的艺术品:&既不能脱离现实的思维进程,将生活中的种种经验与感受即刻的作出反应,并将它以出乎意料的方式表达出来,用一种摄人心魄的气势,做甚至是癫狂的展示。&

On the other hand, steam can be used to restrain the side reaction such as hydrogen transfer reaction so as to increase the yield of light olefins by diluting the concentration of the reactant. In addition, minor steam can react with the feed hydrocarbon resulting in the decrease of coke and the formation of active hydrogen without the increase of hydrogen gas and light saturates that is not desirable.

另一方面,水蒸气不仅仅具有降低烃分压的作用,抑制了氢转移反应等副反应,对于低碳烯烃的产率有好的影响,而且在反应过程中,少量参与了反应,与烃类发生了水煤气反应,生成了活泼氢,不仅降低了焦碳的产率,并且没有提高氢气、低碳烷烃等不希望得到的产物。

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