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石榴状核壳结构的Ni-NSs@MSNSs作为用于二环戊二烯加氢的高活性、高稳定性、快速磁分离且可多次循环使用的纳米催化剂。

Pomegranate-like Core-Shell Ni-NSs@MSNSs as a High Activity, Good Stability, Rapid Magnetic Separation, and Multiple Recyclability Nanocatalyst for DCPD Hydrogenation.

作者信息

Gao Xia, Zhang Huanhuan, Guan Jingying, Shi Daxin, Wu Qin, Chen Kang-Cheng, Zhang Yaoyuan, Feng Caihong, Zhao Yun, Jiao Qingze, Li Hansheng

机构信息

Beijing Key Laboratory for Chemical Power Source and Green Catalysis, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, 100081 Beijing, China.

School of Chemical Engineering and Materials Science, Beijing Institute of Technology, 519085 Zhuhai, China.

出版信息

ACS Omega. 2021 Apr 21;6(17):11570-11584. doi: 10.1021/acsomega.1c00779. eCollection 2021 May 4.

Abstract

A novel pomegranate-like Ni-NSs@MSNSs nanocatalyst was successfully synthesized via a modified Stöber method, and its application in the hydrogenation of dicyclopentadiene (DCPD) was firstly reported. The Ni-NSs@MSNSs possessed a high specific area (658 m/g) and mesoporous structure (1.7-3.3 nm). The reaction of hydrogenation of DCPD to -tetrahydrodicyclopentadiene (-THDCPD) was used to evaluate the catalytic performance of the prepared materials. The distinctive pomegranate-like Ni-NSs@MSNSs core-shell nanocomposite exhibited superior catalytic activity (TOF = 106.0 h and STY = 112.7 g·L·h) and selectivity (98.9%) than conventional Ni-based catalysts (experimental conditions: Ni/DCPD/cyclohexane = 1/100/1000 (w/w), 150 °C, and 2.5 MPa). Moreover, the Ni-NSs@MSNSs nanocatalyst could be rapidly and conveniently recycled by magnetic separation without appreciable loss. The Ni-NSs@MSNSs also exhibited excellent thermal stability (≥750 °C) and good recycling performance (without an activity and selectivity decrease in four runs). The superior application performance of the Ni-NSs@MSNSs nanocatalyst was mainly owing to its unique pomegranate-like structure and core-shell synergistic confinement effect.

摘要

通过改进的Stöber方法成功合成了一种新型石榴状Ni-NSs@MSNSs纳米催化剂,并首次报道了其在双环戊二烯(DCPD)加氢反应中的应用。Ni-NSs@MSNSs具有高比表面积(658 m/g)和介孔结构(1.7 - 3.3 nm)。以DCPD加氢生成四环戊二烯(-THDCPD)的反应来评估所制备材料的催化性能。独特的石榴状Ni-NSs@MSNSs核壳纳米复合材料表现出比传统镍基催化剂更高的催化活性(TOF = 106.0 h和STY = 112.7 g·L·h)和选择性(98.9%)(实验条件:Ni/DCPD/环己烷 = 1/100/1000 (w/w),150 °C,2.5 MPa)。此外,Ni-NSs@MSNSs纳米催化剂可通过磁分离快速方便地回收,且无明显损失。Ni-NSs@MSNSs还表现出优异的热稳定性(≥750 °C)和良好的循环性能(四次循环中活性和选择性均无下降)。Ni-NSs@MSNSs纳米催化剂优异的应用性能主要归因于其独特的石榴状结构和核壳协同限制效应。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8552/8153983/efdd50deee9b/ao1c00779_0014.jpg

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