论文标题

用二维材料对石墨烯海绵电极的功能化,用于定制电催化活性,以朝着新兴的特定污染物

Functionalization of graphene sponge electrodes with two-dimensional materials for tailored electrocatalytic activity towards specific contaminants of emerging concern

论文作者

Lumbaque, Elisabeth Cuervo, Baptista-Piresa, Luis, Radjenovic, Jelena

论文摘要

低成本石墨烯海绵电极用二维(2D)材料(即唯一的唯一和六边形氮化硼(HBN))使用一步,一个水热自组装方法来官能化。唯一和HBN修饰的石墨烯海绵阳极和N掺杂的石墨烯海绵阴极被用来用于在单通路,通过模式下流动的新兴关注的模型持续污染物的电化学降解,并使用支持电解质的低传导性。用2D材料的还原石墨烯(RGO)涂层的功能化导致电极电催化性能以及与靶污染物的相互作用的特定修饰。例如,添加HBN通过范德华和π-π相互作用促进了更多疏水有机污染物的吸附。与非官能化的石墨烯海绵阳极相比,用唯一的石墨烯海绵阳极的官能化增强了氧化剂物种(如H2O2和O3)的产生,并产生了更高浓度的羟基自由基(HO),从而增强了目标污染物的去除。用选择性自由基清除剂进行的实验表明,在电化学降解中,表面结合的羟基自由基(HOADS)和单线氧(1O2)的关键作用。该研究表明,用2D材料的石墨烯海绵电极的功能化可以增强其电催化活性并调节与特定有机污染物的相互作用,从而为设计用于去除特定污染物组的电极开辟了新的可能性。

Low-cost graphene sponge electrodes were functionalized with two-dimensional (2D) materials, i.e., borophene and hexagonal boron nitride (hBN), using a one-step, hydrothermal self-assembly method. Borophene and hBN-modified graphene sponge anode and N-doped graphene sponge cathode were employed for electrochemical degradation of model persistent contaminants of emerging concern in one-pass, flow through mode, and using low-conductivity supporting electrolyte. Functionalization of the reduced graphene oxide (RGO) coating with 2D materials led to specific modifications in the electrode electrocatalytic performance and interactions with the target contaminants. For instance, addition of hBN promoted the adsorption of more hydrophobic organic contaminants via van der Waals and π-π interactions. Functionalization of the graphene sponge anode with borophene enhanced the generation of oxidant species such as H2O2 and O3 and yielded an order of magnitude higher concentration of hydroxyl radicals (HO) compared with the non-functionalized graphene sponge anode, thus enhancing the removal of target contaminants. Experiments conducted with the selective radical scavengers indicated the key role of surface-bound hydroxyl radicals (HOads) and singlet oxygen (1O2) in electrochemical degradation. The study demonstrates that functionalization of graphene sponge electrodes with 2D materials can enhance their electrocatalytic activity and modulate the interaction with specific organic contaminants, thus opening new possibilities for designing electrodes tailored to remove specific groups of pollutants.

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