Anhui Province Key Laboratory of Advanced Catalytic Materials and Reaction Engineering, School of Chemistry and Chemical Engineering, Hefei University of Technology, Tunxi Road 193, Hefei 230009, China.
Anhui Province Key Laboratory of Advanced Catalytic Materials and Reaction Engineering, School of Chemistry and Chemical Engineering, Hefei University of Technology, Tunxi Road 193, Hefei 230009, China.
J Hazard Mater. 2020 May 5;389:121844. doi: 10.1016/j.jhazmat.2019.121844. Epub 2019 Dec 7.
Nonprecious bimetallic molybdenum and iron embedded into N-doped carbon (MoFe-NC) hybrids were designed and fabricated by pyrolysis of mixed precursors and then immobilized on poly (vinylidene fluoride) (PVDF) films via a phase inversion process to obtain novel catalytic membranes (MoFe-NC@PVDF) for toxic Cr reduction. The catalytic membranes are highly active for aqueous Cr reduction using formic acid (FA) as a sacrificial electron donor under mild conditions. The results demonstrated that the parameters of synthesis process can efficiently adjust the morphology and textural properties of the as-synthesized MoFe-NC@PVDF membrane, and thus have a significant impact on the catalytic behavior. Cr reduction rates significantly increased with increasing FA concentrations (0.234-0.936 M) and reaction temperature (5-35℃), but declined with the increase of Cr concentrations (5-40 mg/L) and pH values of solution (1.87-4.62). Mo-N, Fe-N, and C-N are the active sites, boosting the dissociation of FA molecules into active H* species for effective catalytic reduction of Cr. The catalytic PVDF membrane exhibited distinct porous structure and numerous interaction sites, which not only stabilized metallic nanoparticles, but also promoted mass transfer across the membrane. This cost-effective catalytic membrane provides a new approach toward the treatment of Cr-containing water.
非贵金属双金属钼铁嵌入氮掺杂碳(MoFe-NC)杂化物是通过混合前体的热解设计和制备的,然后通过相转化过程固定在聚偏二氟乙烯(PVDF)膜上,以获得用于有毒 Cr 还原的新型催化膜(MoFe-NC@PVDF)。在温和条件下,使用甲酸(FA)作为牺牲电子供体,催化膜对水溶液中的 Cr 还原具有高活性。结果表明,合成过程的参数可以有效地调节合成的 MoFe-NC@PVDF 膜的形态和结构特性,从而对催化行为产生重大影响。随着 FA 浓度(0.234-0.936 M)和反应温度(5-35℃)的增加,Cr 还原率显著提高,但随着 Cr 浓度(5-40 mg/L)和溶液 pH 值(1.87-4.62)的增加而降低。Mo-N、Fe-N 和 C-N 是活性位点,促进 FA 分子解离成活性 H*物种,从而有效催化 Cr 的还原。催化 PVDF 膜具有独特的多孔结构和众多相互作用位点,不仅稳定了金属纳米颗粒,而且促进了跨膜的质量传递。这种具有成本效益的催化膜为处理含 Cr 水提供了一种新方法。