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大环修饰树枝状大分子稳定的Pt-Pd双金属纳米催化剂的合成及氢化应用

Synthesis and hydrogenation application of Pt-Pd bimetallic nanocatalysts stabilized by macrocycle-modified dendrimer.

作者信息

Jin Zhijun, Xiao Haiyan, Zhou Wei, Zhang Dongqiao, Peng Xiaohong

机构信息

Department of Polymer Science and Engineering, South China University of Technology, Guangzhou 510640, People's Republic of China.

出版信息

R Soc Open Sci. 2017 Dec 13;4(12):171414. doi: 10.1098/rsos.171414. eCollection 2017 Dec.

DOI:10.1098/rsos.171414
PMID:29308263
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC5750030/
Abstract

Different generations of poly(propylene imine) (G -PPI) terminated with N-containing 15-membered triolefinic macrocycle (G M) ( = 2, 3, 4, 5) were prepared. The bimetallic nanoparticle catalysts G M-(Pt /Pd ) ( = 0, 3, 5, 7, 10) were prepared by the synchronous ligand-exchange reaction between G M and the complexes of Pt(PPh) and Pd(PPh). The structure and catalytic properties of G M-(Pt /Pd ) were characterized via Fourier transform infrared spectroscopy, H nuclear magnetic resonance spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy, high-resolution transmission electron microscopy, energy-dispersive spectroscopy and inductively coupled plasma atomic emission spectroscopy. The novel bimetallic Pd-Pt nanoparticle catalysts stabilized by dendrimers (DSNs) present higher catalytic activities for the hydrogenation of dimeric acid (DA) than that of nitrile butadiene rubber (NBR). It can be concluded that bimetallic Pd-Pt DSNs possess alloying and synergistic electronic effects on account of the hydrogenation degree (HD) of DA and NBR. Furthermore, the HD of DA and NBR shows a remarkable decrease with the incremental generations () of G M-(Pt/Pd) ( = 2, 3, 4, 5).

摘要

制备了以含氮的15元三烯烃大环（GM）封端的不同代数的聚（丙烯亚胺）（G -PPI）（ = 2、3、4、5）。通过GM与Pt(PPh)和Pd(PPh)配合物之间的同步配体交换反应制备了双金属纳米颗粒催化剂GM-(Pt /Pd )（ = 0、3、5、7、10）。通过傅里叶变换红外光谱、氢核磁共振光谱、X射线衍射、X射线光电子能谱、高分辨率透射电子显微镜、能量色散光谱和电感耦合等离子体原子发射光谱对GM-(Pt /Pd )的结构和催化性能进行了表征。由树枝状大分子稳定的新型双金属Pd-Pt纳米颗粒催化剂（DSNs）对二聚酸（DA）加氢的催化活性高于丁腈橡胶（NBR）。根据DA和NBR的氢化度（HD）可以得出结论，双金属Pd-Pt DSNs具有合金化和协同电子效应。此外，随着GM-(Pt/Pd)（ = 2、3、4、5）代数（）的增加，DA和NBR的HD显著降低。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e819/5750030/28a1d599db3b/rsos171414-g14.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e819/5750030/cb73eb6a659c/rsos171414-g5.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e819/5750030/c6a7f8cae9ab/rsos171414-g8.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e819/5750030/2c8d82654655/rsos171414-g9.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e819/5750030/516315a3bc9b/rsos171414-g10.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e819/5750030/3b40761d5265/rsos171414-g11.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e819/5750030/7313f80a68b5/rsos171414-g12.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e819/5750030/6528fba69f64/rsos171414-g13.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e819/5750030/28a1d599db3b/rsos171414-g14.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e819/5750030/20ba43984813/rsos171414-g1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e819/5750030/f5ac007723ce/rsos171414-g2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e819/5750030/f8141d367db8/rsos171414-g3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e819/5750030/508433c96d9c/rsos171414-g4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e819/5750030/cb73eb6a659c/rsos171414-g5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e819/5750030/34a4b1e265ba/rsos171414-g6.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e819/5750030/b204dfdbdf47/rsos171414-g7.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e819/5750030/c6a7f8cae9ab/rsos171414-g8.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e819/5750030/2c8d82654655/rsos171414-g9.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e819/5750030/516315a3bc9b/rsos171414-g10.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e819/5750030/3b40761d5265/rsos171414-g11.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e819/5750030/7313f80a68b5/rsos171414-g12.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e819/5750030/6528fba69f64/rsos171414-g13.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e819/5750030/28a1d599db3b/rsos171414-g14.jpg

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