ACS Appl Mater Interfaces. 2018 May 2;10(17):14735-14743. doi: 10.1021/acsami.8b02231. Epub 2018 Apr 17.
Oxidant-regulated polymerization of dopamine was exploited, for the first time, for effective surface engineering of the well-defined cylindrical pores of nuclear track-etched membranes (NTEMs) to develop novel catalytic membrane reactor. First, in the presence of a strong oxidant, controlled synthesis of polydopamine (PDA) with tunable particle size was achieved, allowing a homogeneous deposition to the confined pore channels of NTEMs. The PDA interfaces rich in catechol and amine groups provided enhanced hydrophilicity to promote mass transport across the membrane and abundant nucleation sites for formation and stabilization of metallic nanoparticles (NPs). In-situ reductive growth of multiple metallic NPs, including Pd, Ag, and Au, was then achieved inside the cylindrical pores of NTEMs. Using the functionalized membrane as a catalytic reactor, efficient reduction of 4-nitrophenol (4-NP) was demonstrated in a flow-through mode. Moreover, after dissolution removal of the NTEMs, self-sustained one-dimensional (1D) PDA/M (M = Pd, Ag, or Au) hybrid nanotubes (NTs), with determined aspect ratio and a length reaching up to 10 μm, were obtained for catalysis of 4-NP in a batch reaction mode. This study established a facile and versatile method, by rational tuning of the polymerization behavior of dopamine, for effective modification of confined microscale/nanoscale cavities with different surface characteristics. The integration of PDA chemistry with NTEMs would provide more opportunities for development of novel catalytic membrane reactors as well as for the tailored synthesis of functional 1D nanotubes for broadened applications.
首次利用多巴胺的氧化聚合反应对核径迹蚀刻膜(NTEMs)的规则圆柱形孔进行有效的表面工程化,以开发新型催化膜反应器。首先,在强氧化剂存在的条件下,实现了具有可调粒径的聚多巴胺(PDA)的可控合成,从而使 PDA 均匀沉积到 NTEMs 的受限孔道中。富含儿茶酚和胺基团的 PDA 界面提供了增强的亲水性,以促进跨膜的质量传递,并为金属纳米颗粒(NPs)的形成和稳定提供了丰富的成核位点。然后,在 NTEMs 的圆柱形孔内原位实现了多种金属 NPs(包括 Pd、Ag 和 Au)的还原生长。在功能化膜作为催化反应器的情况下,在流动模式下高效地还原了 4-硝基苯酚(4-NP)。此外,在 NTEMs 溶解去除后,自维持的一维(1D)PDA/M(M=Pd、Ag 或 Au)混合纳米管(NTs)得以获得,其具有确定的纵横比,长度可达 10μm,用于在批式反应模式下催化 4-NP。该研究通过合理调控多巴胺的聚合行为,建立了一种简便且通用的方法,可有效修饰具有不同表面特性的受限微尺度/纳米尺度空腔。PDA 化学与 NTEMs 的集成将为新型催化膜反应器的开发以及功能 1D 纳米管的定制合成提供更多机会,以拓宽其应用范围。