Journal of Colloid and Interface Science ( IF 9.4 ) Pub Date : 2022-12-29 , DOI: 10.1016/j.jcis.2022.12.145 Jinyuan Liu 1 , Qichang Peng 1 , Ruizhe Yang 1 , Bin Wang 2 , Xiaolin Zhang 3 , Rong Wang 1 , Xingwang Zhu 4 , Ming Cheng 1 , Hui Xu 1 , Huaming Li 1
Iron-cobalt dual single-atom anchoring on nitrogen-doped graphene (FexCoy-NG) improves the efficiency of migration and separation of photo-generated carriers. In this work, the perylene diimide (PDI) is self-assembled on the FexCoy-NG to form the FexCoy-NG/PDI composites by π-π interaction, which is reported for the first time. The bisphenol A (BPA) degradation of optimized 20% Fe0.2Co0.8-NG/PDI are nearly 100%, and the degradation rate is 1.5 and 12.7 times that of the self-assembled PDI and commercial-grade PDI. The high degradation performance by FexCoy-NG/PDI are mainly due to: (i) regulating the proportion of Fe-Co dual active sites content, so that it can achieve the synergistic interaction to facilitate the transfer of electrons in the catalytic reaction. (ii) PDI is uniformly dispersed by adding the FexCoy-NG, which increases the specific surface area of composites to adsorb more pollutants. Free radical trapping experiments and electron spin-resonance spectroscopy characterization confirmed that the O2–, OH, 1O2 and h+ are the main reactive species (RSs) for BPA degradation. Under the attack of RSs, BPA completes the processes of hydroxylation, demethylation, aromatization, ring-opening, and finally complete mineralization into CO2 and H2O. These results revealed that Fe0.2Co0.8-NG/PDI photocatalysts may be efficiently applied for the remediation of phenol contaminated natural waters.
中文翻译:
将 Fe、Co 共掺杂石墨烯与 PDI 超分子结合以促进光催化活性:电子转移的故事
铁钴双单原子锚定在氮掺杂石墨烯 (Fe x Co y -NG) 上提高了光生载流子的迁移和分离效率。本工作首次报道了苝二酰亚胺(PDI)在Fe x Co y -NG上通过π-π相互作用自组装形成Fe x Co y -NG/PDI复合材料。优化后的20% Fe 0.2 Co 0.8 -NG/PDI对双酚A(BPA)的降解率接近100%,降解率分别是自组装PDI和商品级PDI的1.5倍和12.7倍。Fe x Co y的高降解性能-NG/PDI主要是由于:(i)调节了Fe-Co双活性位点含量的比例,从而达到协同作用,促进催化反应中电子的转移。(ii) 通过添加 Fe x Co y -NG使 PDI 均匀分散,增加复合材料的比表面积以吸附更多的污染物。自由基捕获实验和电子自旋共振光谱表征证实了O 2 –、OH、1 O 2和 h +是 BPA 降解的主要活性物质 (RSs)。在RSs的作用下,BPA完成羟基化、去甲基化、芳构化、开环等过程,最终完全矿化成CO 2和H 2 O。这些结果表明Fe 0.2 Co 0.8 -NG/PDI光催化剂可以有效应用用于修复受苯酚污染的天然水域。