UiO-66-NH2 Metal–Organic Framework (MOF) Nucleation on TiO2, ZnO, and Al2O3 Atomic Layer Deposition-Treated Polymer Fibers: Role of Metal Oxide on MOF Growth and Catalytic Hydrolysis of Chemical Warfare Agent Simulants,ACS Applied Materials & Interfaces

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UiO-66-NH2 Metal–Organic Framework (MOF) Nucleation on TiO2, ZnO, and Al2O3 Atomic Layer Deposition-Treated Polymer Fibers: Role of Metal Oxide on MOF Growth and Catalytic Hydrolysis of Chemical Warfare Agent Simulants
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2017-12-13 00:00:00 , DOI: 10.1021/acsami.7b15397
Dennis T. Lee ₁ , Junjie Zhao ₁ , Christopher J. Oldham ₁ , Gregory W. Peterson ₂ , Gregory N. Parsons ₁

Affiliation

Metal–organic frameworks (MOFs) chemically bound to polymeric microfibrous textiles show promising performance for many future applications. In particular, Zr-based UiO-66-family MOF-textiles have been shown to catalytically degrade highly toxic chemical warfare agents (CWAs), where favorable MOF/polymer bonding and adhesion are attained by placing a nanoscale metal-oxide layer on the polymer fiber preceding MOF growth. To date, however, the nucleation mechanism of Zr-based MOFs on different metal oxides and how product performance is affected are not well understood. Herein, we provide new insight into how different inorganic nucleation films (i.e., Al₂O₃, ZnO, or TiO₂) conformally coated on polypropylene (PP) nonwoven textiles via atomic layer deposition (ALD) influence the quality, overall surface area, and the fractional yield of UiO-66-NH₂ MOF crystals solvothermally grown on fiber substrates. Of the materials explored, we find that TiO₂ ALD layers lead to the most effective overall MOF/fiber adhesion, uniformity, and a rapid catalytic degradation rate for a CWA simulant, dimethyl p-nitrophenyl phosphate (DMNP) with t_1/2 = 15 min, 580-fold faster than the catalytic performance of untreated PP textiles. Interestingly, compared to ALD TiO₂ and Al₂O₃, ALD ZnO induces a larger MOF yield in solution and mass loading on PP fibrous mats. However, this larger MOF yield is ascribed to chemical instability of the ZnO layer under MOF formation condition, leading to Zn²⁺ ions that promote further homogeneous MOF growth. Insights presented here improve understanding of compatibility between active MOF materials and substrate surfaces, which we believe will help advanced MOF composite materials for a variety of useful functions.

中文翻译：

TiO ₂，ZnO和Al ₂ O ₃原子层沉积处理过的聚合物纤维上的UiO-66-NH ₂金属有机骨架（MOF）成核：金属氧化物对MOF生长和化学战剂模拟物的催化水解的作用

化学结合到聚合物微纤维纺织品上的金属有机骨架（MOF）在许多未来应用中显示出令人鼓舞的性能。特别是，基于Zr的UiO-66族MOF纺织品已显示出催化降解高毒性化学战剂（CWA）的作用，其中通过在聚合物上放置纳米级金属氧化物层可实现良好的MOF /聚合物键合和粘合MOF增长之前的光纤。然而，迄今为止，对基于Zr的MOF在不同金属氧化物上的成核机理以及如何影响产品性能的了解尚不十分清楚。在此，我们提供了有关不同的无机成核膜（即Al ₂ O ₃，ZnO或TiO _2）如何变化的新见解。）通过原子层沉积（ALD）保形地涂覆在聚丙烯（PP）非织造织物上会影响溶剂热生长在纤维基材上的UiO-66-NH ₂ MOF晶体的质量，总表面积和分数产率。在探索的材料中，我们发现TiO ₂ ALD层可导致最有效的整体MOF /纤维粘附性，均匀性和CWA模拟物二甲基对硝基苯基磷酸二甲酯（DMNP）的t _1/2 =的快速催化降解速率。15分钟，比未处理的PP纺织品的催化性能快580倍。有趣的是，与ALD TiO ₂和Al ₂ O _3相比，ALD ZnO在溶液和PP纤维毡的质量负载中诱导出更高的MOF产量。然而，更高的MOF产量归因于在MOF形成条件下ZnO层的化学不稳定性，导致Zn ²⁺离子促进了进一步的MOF均匀生长。此处介绍的见解可增进对活性MOF材料与基材表面之间兼容性的理解，我们相信这将有助于先进的MOF复合材料实现多种有用功能。

更新日期：2017-12-13

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