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

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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

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高度分散的钯纳米团簇锚定在cnx修饰的SiO2上，用于丁腈橡胶的选择性加氢

非均相加氢是提高不饱和聚合物性能的有效途径，但制备具有高分散性和稳定性的负载型催化剂仍是一个挑战。在此，我们通过三聚氰胺的热缩聚合成了一种表面有氮化碳的二氧化硅支撑包膜（CNx@SiO2），在其表面形成了具有高度暴露活性位点的Pd纳米团簇，并通过N和Pd之间的强相互作用稳定地锚定。热温度影响CNx的性质，进而调控钯纳米团簇的电子和结构状态。在500℃下制备的Pd/CNx @SiO2-500催化剂具有最佳CNx结构（g-C3N4）和高氮含量，具有高度分散和富电子的Pd纳米团簇（1.3 nm）。该催化剂对丁腈橡胶的加氢活性为98.0%，对C=C键的选择性为100%。本研究为制备高活性、稳定的钯催化剂提供了一种简便的方法，为不饱和聚合物的加氢升级铺平了道路。图形抽象

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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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.

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