Yao Aonan, Jiao Xiuling, Chen Dairong, Li Cheng
National Engineering Research Center for Colloidal Materials and School of Chemistry and Chemical Engineering, Shandong University, 250100 Jinan, China.
ACS Appl Mater Interfaces. 2020 Apr 22;12(16):18437-18445. doi: 10.1021/acsami.9b22242. Epub 2020 Mar 26.
Self-detoxifying fabrics are desirable forms for protection against chemical warfare agents (CWAs). Zirconium-based metal-organic frameworks (Zr-MOFs) have emerged as one of the fastest catalysts for nerve-agent hydrolysis, but there is still a lack of reliable methods to integrate them onto fibrous supports, and instantaneous detoxification remains challenging for MOF/fiber composites. Herein, we report a bio-inspired polydopamine (PDA)-mediated strategy for the preparation of Zr-MOF (UiO-66-NH)-coated nanofiber membranes, which are capable of photothermally catalyzing the degradation of CWA simulants. UiO-66-NH nanocrystalline coating with high mass loading, perfect coverage, and good adhesion is readily formed on polyamide (PA)-6 nanofibers with the precoated PDA layer. The prepared PA-6@PDA@UiO-66-NH nanofibers display almost an order of magnitude higher turnover frequency (TOF) for the hydrolysis of the nerve agent simulant dimethyl 4-nitrophenylphosphate (DMNP) when irradiated under simulated solar light, with a half-life of only 0.5 min. Such a hydrolysis rate is significantly higher compared to that of the corresponding UiO-66-NH powder and UiO-66-NH/fiber composites reported so far. This strategy may be easily generalized to other MOF/fiber pairs to achieve even higher performance and opens up new opportunities for solar photothermal catalysis in CWA protection.
自解毒织物是抵御化学战剂(CWA)的理想防护形式。锆基金属有机框架(Zr-MOFs)已成为神经毒剂水解速度最快的催化剂之一,但仍缺乏将它们整合到纤维载体上的可靠方法,并且MOF/纤维复合材料的即时解毒仍然具有挑战性。在此,我们报道了一种受生物启发的聚多巴胺(PDA)介导的策略,用于制备Zr-MOF(UiO-66-NH)包覆的纳米纤维膜,该膜能够光热催化CWA模拟物的降解。在预涂覆有PDA层的聚酰胺(PA)-6纳米纤维上,很容易形成具有高质量负载、完美覆盖和良好附着力的UiO-66-NH纳米晶体涂层。制备的PA-6@PDA@UiO-66-NH纳米纤维在模拟太阳光照射下,对神经毒剂模拟物4-硝基苯基磷酸二甲酯(DMNP)的水解显示出几乎高一个数量级的周转频率(TOF),半衰期仅为0.5分钟。与迄今为止报道的相应UiO-66-NH粉末和UiO-66-NH/纤维复合材料相比,这种水解速率明显更高。该策略可以很容易地推广到其他MOF/纤维对,以实现更高的性能,并为CWA防护中的太阳光热催化开辟新的机会。