Ni-La/AC甲醇气相羰基化催化剂失活行为的研究

采用等容浸渍法制备了Ni-La/AC双金属催化剂,在连续流动固定床反应装置中,于260℃、1.5 MPa、CO/CH3OH/CH3I摩尔比20/19/17、.5 g-cath.mol-1条件下考察了催化剂的稳定性,并通过BET、XRD、TPR和ICP等技术手段对甲醇气相羰基化反应失活前后Ni-La/AC催化剂进行了表征,考察了催化剂在反应过程中的结构变化和失活行为。结果表明:La组分的引入促进了Ni在催化剂表面的分散,提高了反应的初活性。但是在长时间运转条件下,羰基化活性中心Ni晶粒发生聚集,成为积碳的活性中心,堵塞了部分催化剂微孔,使得催化剂比表面积减小导致催化剂失活。失活催化剂再生后,比表面积有所回升,但Ni晶粒明显增大,反应过程中失活速率加快。此外,活性金属镍的流失以及Ni、La在催化剂上分布的变化也是催化剂失活的原因之一。     

中变催化剂失活典型事例剖析

通过2起中变催化剂失活的事件，从理论上剖析其根源，并探讨防范的对策。     

Revised Model of Strain in Ceria–Zirconia-Encapsulated Precious-Metal Particles

A previously proposed model of strain in ceria–zirconia-encapsulated precious-metal particles is revised to reflect several new observations: encapsulation of unstrained Pt particles, quantitative relation between partial reduction and the change in ceria–zirconia cell parameters, temperature/time dependence of strain relaxation/imposition in encapsulated Pd and Rh particles, and strained PdO. According to the revised model, the main cause of strain is partial oxidation of the precious metal (rather than the change in oxygen content of ceria–zirconia, as originally suggested).     

Hydrodechlorination of 3-chloropyridine and chlorobenzene in methanol solution over alkali-modified zirconia-supported palladium catalysts

The liquid-phase hydrodechlorination of 3-chloropyridine and chlorobenzene has been studied over alkali-modified zirconia-supported palladium catalysts. The modification of the ZrO₂ with alkali metal carbonates improves the catalytic activity of the final palladium catalyst. Therefore, the larger the ionic radii (Li⁺ < Na⁺ < K⁺), the greater the catalytic activity (TOF) of the palladium catalyst. For 3-chloropyridine, hydrodechlorination proceeds without catalyst deactivation. This is explained as the result of the interaction of reaction products (pyridine and HCl) forming pyridinium chloride, thus avoiding the detrimental effect of HCl on the palladium particles. Catalytic hydrodechlorination of chlorobenzene over Pd catalysts exhibits an initial catalytic activity (TOF) much lower than that of 3-chloropyridine and the Pd catalysts deactivate as the reaction proceeds. Finally, chlorobenzene hydrodehalogenation has also been carried out in the presence of an equimolecular amount of pyridine resulting in a decrease in the initial reaction rate on the one hand, but also in an increase in final conversion on the other.     

合成直链烷基苯环境友好固体酸催化剂的研究 Ⅲ .催化剂失活原因分析

采用固定床反应器,对催化剂的稳定性进行了初步评价。在120℃、空速相同、液固反应条件下,高苯烯比时催化剂的稳定性明显高于低苯烯比时;在苯烯比和空速相同、液固反应条件下,相对低温反应时,催化剂的稳定性明显高于高温反应。IR分析结果表明,同新鲜和反应后未失活的催化剂相比,失活后催化剂的活性组分特征衍射峰消失,出现的新的特征衍射峰可能同—CH基的振动有关。TG分析结果表明,失活后催化剂在空气流中焙烧,失重幅度比新鲜催化剂大。     

Interoceptive Sensitivity and Self-Reports of Emotional Experience.

People differ in the extent to which they emphasize feelings of activation or deactivation in their verbal reports of experienced emotion, termed arousal focus (AF). Two multimethod studies indicate that AF is linked to heightened interoceptive sensitivity (as measured by performance on a heartbeat detection task). People who were more sensitive to their heartbeats emphasized feelings of activation and deactivation when reporting their experiences of emotion over time more than did those who were less sensitive. This relationship was not accounted for by several other variables, including simple language effects. Implications for the role of interoception in experienced emotion and the validity of self-reported emotion are discussed. (PsycINFO Database Record (c) 2010 APA, all rights reserved)     

HRP-12型负载杂多酸催化剂的失活原因及预防措施

采用XRD、NMR、IR、MS等手段对长链烷基苯合成中失活负载型杂多酸催化剂进行了表征,结果表明,催化剂的失活主要是由于表面结焦引起的,原料中的双烯、烷基芳烃杂质以及反应生成的副产物重烷基苯是引起催化剂结焦的主要原因,对原料进行脱双烯和脱芳烃精制、提高苯烯比以及用苯洗涤催化剂等措施能够有效抑制催化剂的失活。     

膦化合物对加氢催化剂的影响

丁辛醇装置丁醛加氢催化剂在装置扩能投产以后热点上移 (失活 )的速率较快 ,针对催化剂老化的原因进行分析、判断 ,找出原因 ,采用相应的解决措施 ,可延长催化剂使用寿命 ,增加装置效益     

LY-8602系列催化剂的失活原因及对策

通过催化剂的评价及表征，对LY-8602系列催化剂在低硫裂解汽油加氢时的失活原因进行了研究，结果表明，其活性下降主要是催化剂的活性中心相Co-Mo-s遭到破坏，使催化剂表面的具有加氢活性的Mo^4 峰减小所致。采用新研制的高活性加氢催化剂LY-9702与LY-8602构成复合床催化剂，可以使加氢产品合格。     

Partial Oxidation of Methane to Syngas over Calcined Ni–Mg/Al Layered Double Hydroxides

The catalytic partial oxidation of CH₄ to syngas was carried out over an Ni–Mg/Al mixed-oxide catalyst prepared from layered double hydroxide-type precursors. The catalysts were characterized by XRD, TPR, UV-DRS, XRF, BET and CHNS analysis. The effects of the catalyst composition and the calcination temperature on the catalytic performance and the extent of catalyst deactivation were investigated. Ni–Mg/Al oxide catalysts converted CH₄ into syngas efficiently with high selectivity. The catalyst performance was strongly related to the Ni particle size and the calcination temperature. The catalysts that were calcined at higher temperature exhibited a better catalytic performance. In conclusion, the NiAl₂O₄ spinel phase had a positive effect on the stability of the catalyst.