Abstract:
In the contemporary context, executing light-oxidant- and reductant-driven reactions in solution-phase processes remains challenging mainly due to the lack of general tools for understanding the reactive potential of nano-functional catalysts. In this study, dual-active nanometals (Au and Cu doped with Au) capped within soy lecithin (SL), were developed and characterized, combining flexibility with the catalytic advantages and stability of liquid-phase catalysts. The as-synthesized SL-Au (LG) and SL-Au-Cu (LGC) catalysts were efficiently degraded rhodamine B (RB, 100%) in the presence of H2O2 under light irradiation (350 W lamp) at wide pH range (3-7) within 4.5 h and p-nitrophenol (p-NP, >90% degradation at pH 7) in the presence of NaBH4 under normal stirring with slower kinetics (∼72 h). RB degradation followed a pseudo-second-order kinetic model with a higher r2, and p-NP degradation followed first-order kinetics. The active sites embedded within the structural order of SL arrangement displayed elevated catalytic activity, which was further enhanced by the movement of intermediate/excited states and charged elements within the metal suspended in the phospholipid (LG and LGC). The self-regulating tunability of the physicochemical characteristics of these catalysts provides a convenient and generalizable platform for the transformation of modern dual-active (redox) catalysts into dynamic homogeneous equivalents.
摘要:
在当代语境中,在液相过程中执行光氧化剂和还原剂驱动的反应仍然具有挑战性,主要是由于缺乏了解纳米功能催化剂反应潜力的通用工具。在这项研究中,双活性纳米金属(Au和掺杂Au的Cu)覆盖在大豆卵磷脂(SL)中,被开发和表征,结合灵活性和液相催化剂的催化优势和稳定性。合成的SL-Au(LG)和SL-Au-Cu(LGC)催化剂有效降解了罗丹明B(RB,100%)在4.5h内宽pH范围(3-7)和对硝基苯酚(p-NP,>90%的降解在pH7)在NaBH4的存在下,在缓慢的动力学搅拌(〜72小时)。RB降解遵循具有较高r2的伪二级动力学模型,p-NP降解遵循一级动力学。嵌入SL排列的结构顺序中的活性位点显示出提高的催化活性,通过悬浮在磷脂中的金属(LG和LGC)内的中间/激发态和带电元素的运动进一步增强。这些催化剂的物理化学特性的自我调节可调性为现代双活性(氧化还原)催化剂转化为动态均相当量提供了方便且可推广的平台。