铁基双金属/石墨烯的制备及其吸附与可见光Fenton降解染料的性能和机理研究

To overcome the difficult problems about disposal of organic dyes sewage with high concentration, bimetallic iron nanoparticles (FeM) with highly efficient adsorption activities were chosen as visible-light heterogeneous Fenton catalyst in this project. To solve the dispersity, structural stability and catalytic properties, it would be an effective measure to integrate the magnetic FeM nanoparticles with Graphene (G) possessing excellent conductivity. Consequently, the pH using range of visible-light Fenton catalyst can be widened and the leaching of iron ions can be decreased. Meanwhile, the magnetic properties of FeM/G nanocomposite can facilitate to solve the difficult problems of separation and recycling as catalysts. The main investigation emphases are placed on the following problems: Based on first-principles density functional theory, effect of FeM introduction on the configuration and electronic properties of G; Design and preparation of FeM/G nanocomposite; Influence of the design mechanism of FeM/G on the rule of adsorption properties; To reveal the synergistic adsorption mechanism, the discussions are performed on the chemical reactions of organic dyes on the surface of FeM/G nanocomposite, as well as the adsorption kinetics and adsorption isotherm of organic dyes on the surface of FeM/G nanocomposite; Analyzing the influence of structure of visible-light Fenton catalyst on the using efficiency of H2O2 and mineralization effect and discovering the reaction process and catalysis mechanism of organic dyes degraded by Fenton reaction catalyst. Accordingly, this research can provide necessary reference experiments and theoretical support for developing the novel visible-light Fenton catalyst.

针对高浓度有机染料废水处理难度大的课题，本项目选择具有高还原性和吸附性的铁基双金属（FeM）纳米粒子作为可见光异相Fenton催化剂，通过与具有优良导电性的石墨烯（G）复合，提高FeM的分散性、结构稳定性和催化性能，拓宽催化剂使用pH范围，减少铁离子的溶出。同时应用FeM/G的磁性能解决催化剂难分离回收、循环使用的难题。重点研究基于第一性原理密度泛函理论，引入FeM对石墨烯几何结构和电子结构的影响；研究FeM/G纳米材料的设计与制备；研究FeM/G的构建原理，影响吸附性能的规律；探讨染料分子在FeM/G材料表面的化学反应，结合吸附动力学和吸附等温式，揭示FeM/G的协同吸附机制；解析光Fenton催化剂的结构对H2O2利用率的影响和矿化效果，探索FeM/G催化光Fenton反应降解染料的反应历程和催化机理。为开发新型可见光Fenton催化剂提供可借鉴的实验和理论支持。

针对高浓度有机染料废水处理难度大的课题，本项目选择具有高还原性和吸附性的铁基双金属（FeM）纳米粒子作为可见光异相Fenton催化剂，通过与具有优良导电性的石墨烯（G）复合，提高FeM的分散性、结构稳定性和催化性能，拓宽催化剂使用pH范围，减少铁离子的溶出。同时应用FeM/G的磁性能解决催化剂难分离回收、循环使用的难题。重点研究基于第一性原理密度泛函理论，引入FeM对石墨烯几何结构和电子结构的影响；研究FeM/G纳米材料的设计与制备；研究FeM/G的构建原理，影响吸附性能的规律；探讨染料分子在FeM/G材料表面的化学反应，结合吸附动力学和吸附等温式，揭示FeM/G的协同吸附机制；解析光Fenton催化剂的结构对H2O2利用率的影响和矿化效果，探索FeM/G催化光Fenton反应降解染料的反应历程和催化机理。为开发新型可见光Fenton催化剂提供可借鉴的实验和理论支持。项目书中制备的FeM纳米粒子吸附有机染料后再利用为催化剂由于其高的反应性、低的离子浸出、优异的长期稳定性、普适性和可重复使用性在污水处理领域中的应用前景是非常可观的。对深度处理高浓度染料污水十分有效，为今后环境修复领域的未来工程应用开辟了巨大的可能性。