Du Rongrong, Zhu Hongyang, Zhao Hongyao, Lu Hao, Dong Chang, Liu Mengting, Yang Fu, Yang Jun, Wang Jun, Pan Jianming
School of Environmental and Chemical Engineering, Jiangsu University of Science and Technology, Zhenjiang, 212003, China.
School of Environmental and Chemical Engineering, Jiangsu University of Science and Technology, Zhenjiang, 212003, China; Jiangsu Provincial Key Laboratory of Environmental Science and Engineering, Suzhou University of Science and Technology, China.
Environ Res. 2023 Apr 1;222:115365. doi: 10.1016/j.envres.2023.115365. Epub 2023 Jan 25.
Environmental governance by photothermal materials especially for the separation of organic pollutants and regeneration of freshwater afford growing attention owing to their special solar-to-heat properties. Here, we construct a special functional nanosphere composed of an internal silica core coated by a thin carbon layer encapsulated plasmonic bimetallic FeCoO spinel (SiO@CoFe/C) by a facile self-assembled approach and tuned calcination. Through combining the advantage of bimetallic Fe-Co and carbon layer, this obtained nanosphere affords improved multiple environmental governing functions including peroxymonosulfate (PMS) activation to degrade pollutants and photothermal interfacial solar water evaporation. Impressively, fined bimetal (FeCo) species (20 nm) acted as main catalytic substance were distributed on the N-doping carbon thin layer, which favors electron transfer and reactive accessibility of active metals. The increasing treatment temperature of catalysts caused the optimization of the surface active metal species and tuning catalytic properties in the AOPs. Besides, the incorporation of Co in the SiO@CoFe/C-700 could enable the improved PMS activation efficiency compared to SiO@Fe/C-700 and the mixed SiO@Co/C-700 and SiO@Fe/C-700, hinting a synergetic promotion effect. The bimetal coupled catalyst SiO@CoFe/C-700 affords enhanced photothermal properties compared to SiO@Co/C-700. Furthermore, photothermal catalytic PMS activation using optimal SiO@CoFe/C-700 was further explored in addressing stubborn pollutants including oxytetracycline, sulfamethoxazole, 2, 4-dichlorophenol, and phenol. The free radical quenching control suggests that both the sulfate radical, hydroxyl radical, superoxide radical, and singlet oxygen species are involved in the degradation, while the hydroxyl radical and singlet oxygen play a dominant role. Furthermore, the implementation of a solar-driven interfacial water evaporation model using SiO@CoFe/C-700 was further studied to obtain freshwater regeneration (1.26 kg m h, 76.81% efficiency), indicating the comprehensive ability of the constructed nanocomposites for treating complicated environmental pollution including organics removal and freshwater regeneration.
光热材料的环境治理，尤其是用于有机污染物的分离和淡水的再生，因其特殊的太阳能-热能转换特性而受到越来越多的关注。在此，我们通过一种简便的自组装方法和调控煅烧，构建了一种特殊的功能纳米球，其内部为二氧化硅核，表面包覆一层薄碳层，碳层包裹着等离子体双金属FeCoO尖晶石（SiO@CoFe/C）。通过结合双金属Fe-Co和碳层的优势，这种纳米球具有多种改善的环境治理功能，包括过一硫酸盐（PMS）活化以降解污染物以及光热界面太阳能水蒸发。令人印象深刻的是，作为主要催化物质的精细双金属（FeCo）物种（20纳米）分布在氮掺杂碳薄层上，这有利于电子转移和活性金属的反应可及性。催化剂处理温度的升高导致表面活性金属物种的优化，并调节了高级氧化过程中的催化性能。此外，与SiO@Fe/C-700以及混合的SiO@Co/C-700和SiO@Fe/C-700相比，SiO@CoFe/C-700中Co的引入能够提高PMS活化效率，这暗示了协同促进作用。与SiO@Co/C-700相比，双金属耦合催化剂SiO@CoFe/C-700具有增强的光热性能。此外，还进一步探索了使用最佳的SiO@CoFe/C-700进行光热催化PMS活化以处理包括土霉素、磺胺甲恶唑、2,4-二氯苯酚和苯酚在内的顽固污染物。自由基猝灭控制表明，硫酸根自由基、羟基自由基、超氧自由基和单线态氧物种都参与了降解过程，而羟基自由基和单线态氧起主导作用。此外，还进一步研究了使用SiO@CoFe/C-700的太阳能驱动界面水蒸发模型以实现淡水再生（1.26 kg m h，76.81%的效率），这表明所构建的纳米复合材料具有处理包括有机物去除和淡水再生在内的复杂环境污染的综合能力。
