一个强大的吡唑酸金属有机框架集成全氟辛酸浓度和降解

Rong-Ran Liang, Yubin Fu, Zongsu Han, Yihao Yang, Vladimir I. Bakhmutov, Zhaoyi Liu, Joshua Rushlow, Hong-Cai Zhou
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摘要

全氟辛酸(PFOA)由于其生物蓄积性和致癌性对人类健康构成重大威胁。目前的补救策略通常侧重于吸附或降解,忽视了综合方法的潜力。在此,我们提出了一种吡甲酸盐金属有机框架(MOF), PCN-1003,具有一维开放通道的片层结构。PCN-1003在水溶液中表现出优异的稳定性,在很宽的pH范围内(1 - 12),实现了有效的PFOA吸附(642 mg g−1)。机理研究表明,PFOA -乙酸交换过程占主导地位,代表了这种机制的一个显著例子,并使PFOA有效吸收。值得注意的是,与之前报道的方法相比,PCN-1003在更低的温度(90°C)下极大地促进了PFOA的降解,具有大约三倍的催化加速效应,这归因于PCN-1003内PFOA和受限环境的协同作用。该研究率先将PFOA的浓度与单一MOF的降解结合起来,为处理被全氟烷基和多氟烷基物质污染的水提供了一条有前途的途径。坚固的吡唑酸盐金属有机骨架既可作为全氟辛酸的吸附剂,又可作为温和条件下降解的催化剂,为捕获和破坏单氟烷基和多氟烷基物质提供了一种综合方法。
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A robust pyrazolate metal–organic framework for integrated perfluorooctanoic acid concentration and degradation
Perfluorooctanoic acid (PFOA) poses a substantial threat to human health due to its bioaccumulation and carcinogenic nature. Current remediation strategies typically focus on either adsorption or degradation, neglecting the potential of an integrated approach. Herein, we present a pyrazolate metal–organic framework (MOF), PCN-1003, featuring a lamellar structure with one-dimensional open channels. PCN-1003 exhibits exceptional stability across a wide pH range (1–12) in aqueous solutions, achieving efficient PFOA adsorption (642 mg g−1). Mechanistic studies revealed that a PFOA–acetate exchange process dominates, representing a remarkable example of such a mechanism and enabling efficient PFOA uptake. Notably, PCN-1003 greatly facilitates PFOA degradation at a much lower temperature (90 °C) than observed in previously reported methods, with an approximately threefold catalytic acceleration effect, attributed to the coordination of PFOA and the confined environment within PCN-1003. This study pioneers integrated PFOA concentration and degradation using a single MOF, presenting a promising avenue for treating water contaminated with per- and polyfluoroalkyl substances. A robust pyrazolate metal–organic framework acts as both an adsorbent for perfluorooctanoic acid and a catalyst for degradation under mild conditions, providing an integrated approach for the capture and destruction of per- and polyfluoroalkyl substances.
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