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“Uncapped” metal–organic framework (MOF) dispersions driven by O2 plasma towards superior oxygen evolution electrocatalysis
Journal of Materials Chemistry A ( IF 11.9 ) Pub Date : 2022-09-16 , DOI: 10.1039/d2ta05387j
Shan Ding, Yuxiang Zhang, Fengqian Lou, Muhammad Kashif Aslam, Yuntong Sun, Ming Li, Jingjing Duan, Yibing Li, Sheng Chen

The lack of solution processability of metal–organic frameworks (MOFs) has been a major obstacle hampering their practical applications. At present, a common belief is that the solution processability of MOFs can only be improved by functionalization with foreign stabilizers. In this work, we firstly predicted through density functional theory (DFT) that in case of a slight excess of the oxygen percentage of MOFs (∼15%), the ionization of additional hydroxyl groups on the surface of MOFs can greatly enhance the solution dispersibility of MOFs through electrostatic stabilization. We consequently demonstrated a general protocol for manipulating MOFs' solution processability through O2 plasma treatment (0–40 min), which can continuously adjust their surface charge in aqueous dispersions (zeta potentials: −13.3–−29.4 mV). This has resulted in a class of “uncapped” MOF aqueous colloids. Further size fractionation of these MOFs in aqueous colloids has produced small-sized MOFs with superior electrocatalytic performance towards the oxygen evolution reaction (overpotential of 258 mV at 10 mA cm−2, small Tafel slope of 19 mV dec−1, and strong durability up to 100 h).

中文翻译:

由 O2 等离子体驱动的“未封端”金属有机框架 (MOF) 分散体实现卓越的析氧电催化

金属有机框架(MOF)缺乏溶液加工性一直是阻碍其实际应用的主要障碍。目前普遍认为MOFs的溶液加工性能只能通过外来稳定剂的功能化来提高。在这项工作中,我们首先通过密度泛函理论(DFT)预测,在 MOFs 的氧百分比略微过量(~15%)的情况下,MOFs 表面额外羟基的电离可以大大提高溶液的分散性MOFs 通过静电稳定。因此,我们展示了一种通过 O 2操纵 MOF 溶液可加工性的通用协议等离子体处理(0-40 分钟),它可以连续调节它们在水分散体中的表面电荷(zeta 电位:-13.3--29.4 mV)。这导致了一类“未加盖”的 MOF 水性胶体。这些 MOF 在水性胶体中的进一步尺寸分级产生了对析氧反应具有优异电催化性能的小尺寸 MOF(在 10 mA cm -2时为 258 mV 的过电位,19 mV dec -1的小 Tafel 斜率和强耐久性至 100 小时)。
更新日期:2022-09-16
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