Eisen Constantin, Ge Lingcong, Santini Elena, Chin Jia Min, Woodward Robert T, Reithofer Michael R
Institute of Inorganic Chemistry, Faculty of Chemistry, University of Vienna Währinger Straße 42 1090 Vienna Austria
Institute of Material Chemistry and Research, Faculty of Chemistry, University of Vienna Währinger Straße 42 1090 Vienna Austria
Nanoscale Adv. 2022 Nov 21;5(4):1095-1101. doi: 10.1039/d2na00799a. eCollection 2023 Feb 14.
Highly active and selective heterogeneous catalysis driven by metallic nanoparticles relies on a high degree of stabilization of such nanomaterials facilitated by strong surface ligands or deposition on solid supports. In order to tackle these challenges, N-heterocyclic carbene stabilized gold nanoparticles (NHC@AuNPs) emerged as promising heterogeneous catalysts. Despite the high degree of stabilization obtained by NHCs as surface ligands, NHC@AuNPs still need to be loaded on support structures to obtain easily recyclable and reliable heterogeneous catalysts. Therefore, the combination of properties obtained by NHCs and support structures as NHC bearing "functional supports" for the stabilization of AuNPs is desirable. Here, we report the synthesis of hyper-crosslinked polymers containing benzimidazolium as NHC precursors to stabilize AuNPs. Following the successful synthesis of hyper-crosslinked polymers (HCP), a two-step procedure was developed to obtain HCP·NHC@AuNPs. Detailed characterization not only revealed the successful NHC formation but also proved that the NHC functions as a stabilizer to the AuNPs in the porous polymer network. Finally, HCP·NHC@AuNPs were evaluated in the catalytic decomposition of 4-nitrophenol. In batch reactions, a conversion of greater than 99% could be achieved in as little as 90 s. To further evaluate the catalytic capability of HCP·NHC@AuNP, the catalytic decomposition of 4-nitrophenol was also performed in a flow setup. Here the catalyst not only showed excellent catalytic conversion but also exceptional recyclability while maintaining the catalytic performance.
由金属纳米颗粒驱动的高活性和选择性多相催化依赖于通过强表面配体或沉积在固体载体上实现的此类纳米材料的高度稳定性。为了应对这些挑战,N-杂环卡宾稳定的金纳米颗粒(NHC@AuNPs)作为有前景的多相催化剂出现。尽管NHC作为表面配体获得了高度稳定性,但NHC@AuNPs仍需要负载在载体结构上以获得易于回收且可靠的多相催化剂。因此,将NHC获得的性质与作为负载NHC的“功能载体”用于稳定AuNPs的载体结构相结合是很有必要的。在此,我们报道了含有苯并咪唑鎓作为NHC前体以稳定AuNPs的超交联聚合物的合成。在成功合成超交联聚合物(HCP)之后,开发了一种两步法来获得HCP·NHC@AuNPs。详细表征不仅揭示了NHC的成功形成,还证明了NHC在多孔聚合物网络中作为AuNPs的稳定剂发挥作用。最后,对HCP·NHC@AuNPs进行了4-硝基苯酚催化分解的评估。在间歇反应中,短短90秒内转化率就可超过99%。为了进一步评估HCP·NHC@AuNP的催化能力,还在流动装置中进行了4-硝基苯酚的催化分解。在此,该催化剂不仅表现出优异的催化转化率,还具有出色的可回收性,同时保持了催化性能。