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引用次数: 0
摘要
调节金属-金属(M-M')和金属-支撑物之间的物理和化学相互作用是提高金属纳米颗粒(NPs)催化活性的理想方法。作为概念验证,我们在此报告了镍-金(Ni-Au)合金纳米粒子的制备方法,该方法是将金属前驱体与 Mg(OH)2 一起浸渍到席夫碱基网络聚合物(SNP)框架中,然后在 800 °C 的 N2 大气中进行热解,从而制备出附着在 N 掺杂的纳米多孔碳(NPC)上的镍-金(Ni73Au27@MgO-NPC)。富含镍的 Ni73Au27@MgO-NPC 具有高稳定性和异质性,表现出更高的催化活性,其周转频率分别为 29 272 h-1(对硝基苯酚的氢化)、93 843 h-1(甲基橙的降解)和 2 218 h-1(二苯乙烯的环氧化)。催化活性的增强与金、镍和富含氧化镁/氮的纳米多孔碳异质结构中电子密度的同步增强有关,详细的 X 射线光电子能谱研究证明了这一点。
Impacting the Surface Chemistry of NiAu by Immobilizing on MgO/N-Rich Nanoporous Carbon Heterostructures for Boosting Catalytic Activities.
Tuning the physical and chemical interaction between metal-metal' (M-M') and metal-support is an ideal way to realize enhanced catalytic activity of metal nanoparticles (NPs). As a proof of concept, herein we report the fabrication of nickel-gold (Ni-Au) alloy nanoparticles attached to N-doped nanoporous carbon (NPC) intervened with MgO (Ni73Au27@MgO-NPC), achieved through the impregnation of metal precursors into Schiff-base network polymer (SNP) framework along with Mg(OH)2 and pyrolysis at 800 °C in N2 atmosphere. With high stability and heterogeneity, the nickel rich Ni73Au27@MgO-NPC exhibited higher catalytic activities with turnover frequencies of 29,272 h-1 (hydrogenation of p-nitrophenol), 93,843 h-1 (degradation of methyl orange), and 2,218 h-1 (epoxidation of stilbene), compared to commercial 10 wt % Pd/C. Enhanced catalytic activity is correlated to the synchronized electron density enhancement in Au, by Ni and MgO/N-rich nanoporous carbon heterostructures, as evident from detailed X-ray photoelectron spectroscopic studies.
期刊介绍:
ChemPlusChem is a peer-reviewed, general chemistry journal that brings readers the very best in multidisciplinary research centering on chemistry. It is published on behalf of Chemistry Europe, an association of 16 European chemical societies.
Fully comprehensive in its scope, ChemPlusChem publishes articles covering new results from at least two different aspects (subfields) of chemistry or one of chemistry and one of another scientific discipline (one chemistry topic plus another one, hence the title ChemPlusChem). All suitable submissions undergo balanced peer review by experts in the field to ensure the highest quality, originality, relevance, significance, and validity.