Highly dispersed Pd nanoclusters anchored on CNx-modified SiO2 for selective hydrogenation of nitrile-butadiene rubber

IF 3.5 3区材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY

Journal of Materials Science Pub Date : 2024-11-26 DOI:10.1007/s10853-024-10444-7

Kewen Zhang, Benwei Fan, Shidong Wang, Hongwei Zhang, Qunhong Liu, Xiaojun Bao, Pei Yuan

{"title":"Highly dispersed Pd nanoclusters anchored on CNx-modified SiO2 for selective hydrogenation of nitrile-butadiene rubber","authors":"Kewen Zhang, Benwei Fan, Shidong Wang, Hongwei Zhang, Qunhong Liu, Xiaojun Bao, Pei Yuan","doi":"10.1007/s10853-024-10444-7","DOIUrl":null,"url":null,"abstract":"<div><p>Heterogeneous hydrogenation is an effective way to improve the performance of unsaturated polymers, but the preparation of supported catalysts with high metal dispersion and stability remains challenging. Herein, we synthesize a SiO<sub>2</sub>-based support wrapping with carbon nitride on the surface (CN<sub><i>x</i></sub>@SiO<sub>2</sub>) via the thermal polycondensation of melamine, on which Pd nanoclusters with highly exposed active sites are formed and stably anchored via the strong interaction between N and Pd. The thermal temperature affects the properties of CN<sub><i>x</i></sub>, which further modulates the electronic and structural state of Pd nanoclusters. The Pd/CN<sub><i>x</i></sub> @SiO<sub>2</sub>-500 catalyst, prepared at 500 °C with an optimal CN<sub><i>x</i></sub> structure (<i>g</i>-C<sub>3</sub>N<sub>4</sub>) and high nitrogen content, features highly dispersed and electron-rich Pd nanoclusters (1.3 nm). This catalyst exhibits a hydrogenation activity of 98.0% for nitrile rubber, with a selectivity of 100% for C=C bonds. This work provides a facile method to prepare Pd catalysts with high activity and stability, paving the way for the upgrading of unsaturated polymers via hydrogenation.</p><h3>Graphical abstract</h3><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":645,"journal":{"name":"Journal of Materials Science","volume":"59 46","pages":"21265 - 21276"},"PeriodicalIF":3.5000,"publicationDate":"2024-11-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Materials Science","FirstCategoryId":"88","ListUrlMain":"https://link.springer.com/article/10.1007/s10853-024-10444-7","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}

引用次数: 0

Abstract

Heterogeneous hydrogenation is an effective way to improve the performance of unsaturated polymers, but the preparation of supported catalysts with high metal dispersion and stability remains challenging. Herein, we synthesize a SiO₂-based support wrapping with carbon nitride on the surface (CN_x@SiO₂) via the thermal polycondensation of melamine, on which Pd nanoclusters with highly exposed active sites are formed and stably anchored via the strong interaction between N and Pd. The thermal temperature affects the properties of CN_x, which further modulates the electronic and structural state of Pd nanoclusters. The Pd/CN_x @SiO₂-500 catalyst, prepared at 500 °C with an optimal CN_x structure (g-C₃N₄) and high nitrogen content, features highly dispersed and electron-rich Pd nanoclusters (1.3 nm). This catalyst exhibits a hydrogenation activity of 98.0% for nitrile rubber, with a selectivity of 100% for C=C bonds. This work provides a facile method to prepare Pd catalysts with high activity and stability, paving the way for the upgrading of unsaturated polymers via hydrogenation.

Graphical abstract

查看原文本刊更多论文

求助全文

约1分钟内获得全文求助全文

来源期刊

Journal of Materials Science 工程技术-材料科学：综合

CiteScore

7.90

自引率

4.40%

发文量

1297

审稿时长

2.4 months

期刊介绍： The Journal of Materials Science publishes reviews, full-length papers, and short Communications recording original research results on, or techniques for studying the relationship between structure, properties, and uses of materials. The subjects are seen from international and interdisciplinary perspectives covering areas including metals, ceramics, glasses, polymers, electrical materials, composite materials, fibers, nanostructured materials, nanocomposites, and biological and biomedical materials. The Journal of Materials Science is now firmly established as the leading source of primary communication for scientists investigating the structure and properties of all engineering materials.