Shahnazarova Gubakhanim, Al Hoda Al Bast Nour, Ramirez Jessica C, Nogues Josep, Esteve Jaume, Fraxedas Jordi, Serra Albert, Esplandiu Maria J, Sepulveda Borja
Catalan Institute of Nanoscience and Nanotechnology (ICN2), CSIC and BIST, Campus UAB, Bellaterra, E-08193 Barcelona, Spain.
Universitat Autònoma de Barcelona, 08193 Cerdanyola del Vallès, Barcelona, Spain.
Mater Horiz. 2024 May 7;11(9):2206-2216. doi: 10.1039/d3mh01935g.
The generation of reactive oxygen species (ROS) the Fenton reaction has received significant attention for widespread applications. This reaction can be triggered by zero-valent metal nanoparticles by converting externally added HO into hydroxyl radicals (˙OH) in acidic media. To avoid the addition of external additives or energy supply, developing self-sustained catalytic systems enabling onsite production of HO at a neutral pH is crucial. Here, we present novel galvanic nanocells (GNCs) based on metallic Fe/Au bilayers on arrays of nanoporous silica nanostructures for the generation of self-sustained Fenton reactions. These GNCs exploit the large electrochemical potential difference between the Fe and Au layers to enable direct HO production and efficient release of Fe in water at neutral pH, thereby triggering the Fenton reaction. Additionally, the GNCs promote Fe/Fe circulation and minimize side reactions that passivate the iron surface to enhance their reactivity. The capability to directly trigger the Fenton reaction in water at pH 7 is demonstrated by the fast degradation and mineralization of organic pollutants, by using tiny amounts of catalyst. The self-generated HO and its transformation into ˙OH in a neutral environment provide a promising route not only in environmental remediation but also to produce therapeutic ROS and address the limitations of Fenton catalytic nanostructures.
通过芬顿反应产生活性氧物种(ROS)已在广泛应用中受到了极大关注。该反应可由零价金属纳米颗粒引发,即在酸性介质中通过将外部添加的H₂O₂转化为羟基自由基(˙OH)来实现。为避免添加外部添加剂或能量供应,开发能够在中性pH下原位产生活性氧物种的自持催化系统至关重要。在此,我们展示了基于纳米多孔二氧化硅纳米结构阵列上的金属铁/金双层的新型原电池纳米单元(GNCs),用于产生自持芬顿反应。这些GNCs利用铁层和金层之间的大电化学势差,在中性pH下实现直接产生活性氧物种以及铁在水中的有效释放,从而引发芬顿反应。此外,GNCs促进铁/铁循环,并最大限度地减少使铁表面钝化的副反应,以提高其反应活性。通过使用少量催化剂对有机污染物的快速降解和矿化,证明了在pH 7的水中直接引发芬顿反应的能力。在中性环境中自生的活性氧物种及其向˙OH的转化不仅为环境修复提供了一条有前景的途径,而且为产生治疗性ROS以及解决芬顿催化纳米结构的局限性提供了途径。