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DFT mechanistic study of the H2‐assisted chain transfer copolymerization of propylene and p‐methylstyrene catalyzed by zirconocene complex 下载免费PDF全文
Cheng‐Gen Zhang Shu‐Yuan Yu Liaoyun Zhang Huayi Li Zhi‐Xiang Wang 《Journal of polymer science. Part A, Polymer chemistry》2015,53(4):576-585
DFT computations have been performed to investigate the mechanism of H2‐assisted chain transfer strategy to functionalize polypropylene via Zr‐catalyzed copolymerization of propylene and p‐methylstyrene (pMS). The study unveils the following: (i) propylene prefers 1,2‐insertion over 2,1‐insertion both kinetically and thermodynamically, explaining the observed 1,2‐insertion regioselectivity for propylene insertion. (ii) The 2,1‐inserion of pMS is kinetically less favorable but thermodynamically more favorable than 1,2‐insertion. The observation of 2,1‐insertion pMS at the end of polymer chain is due to thermodynamic control and that the barrier difference between the two insertion modes become smaller as the chain length becomes longer. (iii) The pMS insertion results in much higher barriers for subsequent either propylene or pMS insertion, which causes deactivation of the catalytic system. (iv) Small H2 can react with the deactivated [Zr]?pMS?PPn facilely, which displace functionalized pMS?PPn chain and regenerate [Zr]? H active catalyst to continue copolymerization. The effects of counterions are also discussed. © 2014 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2015 , 53, 576–585 相似文献
54.
The use of soft X-rays in a neutrahzer represents an alternative technique that could replace conventional radioactive sources.In this study,we evaluated the charging characteristics of a soft X-ray aerosol neutralize!".In addition,the results from the evaluation of the soft X-ray charger were compared with results obtained using a neutralizer incorporating an 241Am radioactive source.The tandem differential mobility analyzer technique was used previously to determine the size-dependent positive,negative,and neutral charge fractions of a soft X-ray neutralizer.This technique was used to show that the neutral fractions obtained using the soft X-ray charger agreed well with the predictions of bipolar diffusion charging theory,and that the soft X-ray charger could be used as a neutralizer for a scanning mobility particle sizer system. 相似文献
55.
Experimental Mechanics - Insufficient data are available to fully understand the effects of metal additive manufacturing (AM) defects for widespread adoption of the emerging technology.... 相似文献
56.
Nai-Heng Chang 《Applicable analysis》2018,97(10):1771-1796
In this paper, we study the Cauchy problem for magnetic fluid of spin-liquid type with Mermin-Ho relation in the three-dimensional space and prove global existence and uniqueness of solutions. The proof is based on the equivalence relation between smooth solutions of the spin-liquid model and the systems of Schrödinger equations with Abelian gauge field. The Sobolev spaces with fractional derivatives are also used in our estimates. 相似文献
57.
Four kinds of red phosphorescent organic light-emitting devices were fabricated and compared to investigate the effect of interfacial layers for hole transport and electron injection. 1 nm-thick LiF in the device A and C and 1 nm-thick Cs2CO3 in the device B and D were deposited as an electron injection layer between the anode and the electron transport layer, and 5 nm-thick layer of dipyrazion[2,3-f:2′,2′-h]quinoxaline-2,3,6,7,10,11-hexacarbonitrile[HATCN] was inserted as a hole transport interfacial layer between the hole injection layer and the hole transport layer only in the device C and D. Under a luminance of 1000 cd/m2, the power efficiencies were 7.6 lm/W and 8.5 lm/W in the device A and B, and 8.6 lm/W and 13.4 lm/W in the device C and D. The quantum efficiency of the device D was 15.8% under 1000 cd/m2 which was somewhat lower than those of the device A and C, but a little higher than that of the device B. The luminance of the device D was much higher than those of the other devices at a given votage. The luminance of the device D at 7 V was 23,710 cd/m2, which was 13.0, 3.4, and 4.0 times higher than those of the device A, B, and C at the same voltage, respectively. 相似文献
58.
Sung Hwan Koo Dong Jun Li Taeyeong Yun Dong Sung Choi Kyung Eun Lee Gil Yong Lee Youngtak Oh Joonwon Lim Suchithra Padmajan Sasikala Ho Jin Lee In Ho Kim Hong Ju Jung Rishabh Jain Sang Ouk Kim 《Particle & Particle Systems Characterization》2019,36(7)
Efficient water electrolysis catalyst is highly demanded for the production of hydrogen as a sustainable energy fuel. It is reported that cobalt derived nanoparticle (CoS2, CoP, CoS|P) decorated reduced graphene oxide (rGO) composite aerogel catalysts for highly active and reliable hydrogen evolution reaction electrocatalysts. 7 nm level cobalt derived nanoparticles are synthesized over graphene aerogel surfaces with excellent surface coverage and maximal expose of active sites. CoS|P/rGO hybrid aerogel composites show an excellent catalytic activity with overpotential of ≈169 mV at a current density of ≈10 mA cm?2. Accordingly, efficient charge transfer is attained with Tafel slope of ≈52 mV dec?1 and a charge transfer resistance (Rct) of ≈12 Ω. This work suggests a viable route toward ultrasmall, uniform nanoparticles decorated graphene surfaces with well‐controlled chemical compositions, which can be generally useful for various applications commonly requiring large exposure of active surface area as well as robust interparticle charger transfer. 相似文献
59.
Kai He Tsegaye TadesseTsega Xi Liu Jiantao Zai Xin‐Hao Li Xuejiao Liu Wenhao Li Nazakat Ali Xuefeng Qian 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(34):12029-12035
The modulation of electron density is an effective option for efficient alternative electrocatalysts. Here, p‐n junctions are constructed in 3D free‐standing FeNi‐LDH/CoP/carbon cloth (CC) electrode (LDH=layered double hydroxide). The positively charged FeNi‐LDH in the space‐charge region can significantly boost oxygen evolution reaction. Therefore, the j at 1.485 V (vs. RHE) of FeNi‐LDH/CoP/CC achieves ca. 10‐fold and ca. 100‐fold increases compared to those of FeNi‐LDH/CC and CoP/CC, respectively. Density functional theory calculation reveals OH? has a stronger trend to adsorb on the surface of FeNi‐LDH side in the p‐n junction compared to individual FeNi‐LDH further verifying the synergistic effect in the p‐n junction. Additionally, it represents excellent activity toward water splitting. The utilization of heterojunctions would open up an entirely new possibility to purposefully regulate the electronic structure of active sites and promote their catalytic activities. 相似文献
60.
Robin F. Weitkamp Beate Neumann Hans‐Georg Stammler Berthold Hoge 《Angewandte Chemie (International ed. in English)》2020,59(14):5494-5499
We report on the first examples of isolated silanol–silanolate anions, obtained by utilizing weakly coordinating phosphazenium counterions. The silanolate anions were synthesized from the recently published phosphazenium hydroxide hydrate salt with siloxanes. The silanol–silanolate anions are postulated intermediates in the hydroxide‐mediated polymerization of aryl and alkyl siloxanes. The silanolate anions are strong nucleophiles because of the weakly coordinating character of the phosphazenium cation, which is perceptible in their activity in polysiloxane depolymerization. 相似文献