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Ultrafine PdRu Nanoparticles Immobilized in Metal–Organic Frameworks for Efficient Fluorophenol Hydrodefluorination under Mild Aqueous Conditions
CCS Chemistry ( IF 11.2 ) Pub Date : 2021-09-04 , DOI: 10.31635/ccschem.021.202101230
Wenqian Yang 1 , Qinglin Liu 1 , Jun Yang 1 , Jiahui Xian 1 , Yinle Li 1 , Guangqin Li 1 , Cheng-Yong Su 1
Affiliation  

Fluorinated organic compounds are of great importance to modern industries, while their release to the environment is inevitable, causing extreme environmental pollution and the subsequent hazardous effect on ecosystems. This is because the degradation of fluorinated compounds under mild conditions remains a challenging task due to the strong C–F bond strength. In this study, we report preparation of [email protected] through immobilizing ultrafine PdRu alloy nanoparticles with a mean diameter of ∼2 nm into the metal–organic framework (MOF), MIL-101(Cr), which was highly active and stable in the hydrodefluorination of 4-fluorophenol (4-FP) under mild aqueous conditions. The optimized catalyst Pd0.5Ru0.5@MIL-101 achieved impressive hydrogenation performance with a 98.5% conversion of 4-FP and a 97.7% selectivity of cyclohexanol, much better than the single metal-doped [email protected] and [email protected] catalysts. The excellent catalytic behavior contributed to the synergistic effect of combining the PdRu alloying effect and the MOF nanospace confinement effect, providing a promising strategy to develop highly efficient hydrodefluorination catalysts to assist environmental restoration and green ecology.



中文翻译:

固定在金属-有机骨架中的超细 PdRu 纳米颗粒用于温和水性条件下的高效氟苯酚加氢脱氟

含氟有机化合物对现代工业具有重要意义,但其排放到环境中是不可避免的,会造成严重的环境污染和随之而来的对生态系统的危害。这是因为氟化合物在温和条件下的降解仍然是一项具有挑战性的任务,因为它具有很强的 C-F 键强度。在这项研究中,我们报告了通过将平均直径约为 2 nm 的超细 PdRu 合金纳米粒子固定到金属有机框架 (MOF) MIL-101(Cr) 中来制备 [电子邮件保护],它在4-氟苯酚 (4-FP) 在温和水性条件下的加氢脱氟。优化后的催化剂 Pd 0.5 Ru 0.5@MIL-101 以 98.5% 的 4-FP 转化率和 97.7% 的环己醇选择性实现了令人印象深刻的氢化性能,远优于单一金属掺杂的 [电子邮件保护] 和 [电子邮件保护] 催化剂。优异的催化行为有助于结合 PdRu 合金化效应和 MOF 纳米空间限制效应的协同效应,为开发高效加氢脱氟催化剂以辅助环境修复和绿色生态提供了有前景的策略。

更新日期:2021-09-06
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