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负载在氮掺杂炭黑上的钯金合金纳米颗粒作为用于乌尔曼偶联和硝基苯酚加氢反应的高活性催化剂。

PdAu alloy nanoparticles supported on nitrogen-doped carbon black as highly active catalysts for Ullmann coupling and nitrophenol hydrogenation reactions.

作者信息

Han Fengyan, Xia Jiawei, Zhang Xinglong, Fu Yongsheng

机构信息

Key Laboratory for Soft Chemistry and Functional Materials of Ministry Education, Nanjing University of Science and Technology Nanjing 210094 China.

College of Science, Institute of Materials Physics and Chemistry, Nanjing Forestry University Nanjing 210037 China

出版信息

RSC Adv. 2019 Jun 5;9(31):17812-17823. doi: 10.1039/c9ra01685f. eCollection 2019 Jun 4.

DOI:10.1039/c9ra01685f
PMID:35520540
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9064667/
Abstract

Noble metal-based catalysts have been proven to be active for catalytic organic reactions. The selectivity and conversion can be improved by integration with proper carrier materials, and further modulated by tuning the composition as well as the electronic structure of the active noble metals. Compared with unsupported monometallic catalysts, the synergistic interactions between neighboring metals and the combined effects between the carrier materials and the active components often give rise to positive influences on the enhancement of the catalytic efficiency and selectivity. In this work, we report a facile process for the fabrication of nitrogen-doped carbon black (NCB) supported PdAu bimetallic nanoparticles (NPs) with a uniform dispersion and narrow size distribution. The PdAu/NCB catalyst with a Pd/Au mole ratio of 1/1 shows the highest activity towards both Ullmann coupling reactions of aryl halides and the hydrogenation reaction of nitrophenols. Moreover, this bimetallic catalyst also exhibits a superior recycling durability to that of monometallic Pd/NCB and Au/NCB catalysts. The enhanced catalytic performance of the bimetallic catalyst is mainly due to the large BET specific surface area (125.45 m g) and the synergy between the individual components of the catalyst.

摘要

贵金属基催化剂已被证明对催化有机反应具有活性。通过与合适的载体材料结合可以提高选择性和转化率,并通过调整活性贵金属的组成以及电子结构进一步进行调控。与无载体的单金属催化剂相比,相邻金属之间的协同相互作用以及载体材料与活性组分之间的综合效应通常对提高催化效率和选择性产生积极影响。在这项工作中,我们报道了一种简便的方法来制备具有均匀分散和窄尺寸分布的氮掺杂炭黑(NCB)负载的钯金双金属纳米颗粒(NPs)。钯金摩尔比为1/1的PdAu/NCB催化剂对芳基卤化物的乌尔曼偶联反应和硝基苯酚的氢化反应均表现出最高活性。此外,这种双金属催化剂还表现出比单金属Pd/NCB和Au/NCB催化剂更优异的循环耐久性。双金属催化剂催化性能的增强主要归因于较大的BET比表面积(125.45 m²/g)以及催化剂各组分之间的协同作用。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/17ab/9064667/96d0588ba0f6/c9ra01685f-f6.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/17ab/9064667/68725fd346ed/c9ra01685f-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/17ab/9064667/151b78f001a0/c9ra01685f-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/17ab/9064667/96d0588ba0f6/c9ra01685f-f6.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/17ab/9064667/050119fc837e/c9ra01685f-s1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/17ab/9064667/b46c939372d6/c9ra01685f-f1.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/17ab/9064667/6704f27edb57/c9ra01685f-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/17ab/9064667/1fc96b4865c3/c9ra01685f-s2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/17ab/9064667/68725fd346ed/c9ra01685f-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/17ab/9064667/151b78f001a0/c9ra01685f-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/17ab/9064667/96d0588ba0f6/c9ra01685f-f6.jpg

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