化学
催化作用
苯酚
选择性
苯
化学工程
纳米颗粒
超分子化学
纳米技术
三聚氰胺
微型多孔材料
热稳定性
多孔性
结晶学
有机化学
材料科学
晶体结构
工程类
作者
Ting Zhang,Di Zhang,Xinghua Han,Ting Dong,Xinwen Guo,Chunshan Song,Rui Si,Wei Liu,Yuefeng Liu,Zhongkui Zhao
摘要
Developing single-atom catalysts with porous micro-/nanostructures for high active-site accessibility is of great significance but still remains a challenge. Herein, we for the first time report a novel template-free preassembly strategy to fabricate porous hollow graphitic carbonitride spheres with single Cu atoms mounted via thermal polymerization of supramolecular preassemblies composed of a melamine-Cu complex and cyanuric acid. Atomically dispersed Cu-N3 moieties were unambiguously confirmed by spherical aberration correction electron microscopy and extended X-ray absorption fine structure spectroscopy. More importantly, this material exhibits outstanding catalytic performance for selective oxidation of benzene to phenol at room temperature, especially showing phenol selectivity (90.6 vs 64.2%) and stability much higher than those of the supported Cu nanoparticles alone, originating from the isolated unique Cu-N3 sites in the porous hollow structure. An 86% conversion of benzene, with an unexpectedly high phenol selectivity of 96.7% at 60 °C for 12 h, has been achieved, suggesting a great potential for practical applications. This work paves a new way to fabricate a variety of single-atom catalysts with diverse graphitic carbonitride architectures.
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