基于光降解四环素类抗生素废水的过渡金属磷化物/氮化碳复合材料的可控制备及其光解行为与机理研究

According to the national demand for safe drinking water, this project uses green and environmentally friendly photocatalytic oxidation technology to treat tetracycline antibiotics (TCs), which are low concentration, high hazard and difficult to biodegrade in water. Based on the mechanism of active radical oxidation in the process of semiconductor photodegradation of this kind of pollutants, aiming at the problems of high cost and low efficiency of photocatalyst at present, the transition metal phosphides/graphitic carbon nitride (TMPs/g-C3N4) composite was constructed by two-step method (solvothermal-phosphating) , which was applied to the photocatalytic degradation of TCs. The relationship between the composition, structure, crystal phase, morphology, photoabsorption property, adsorption property, photocatalytic activity and stability of TMPs/g-C3N4 composites was studied. The intermediate products, active species, electron transport mechanism and degradation kinetics/thermodynamics process of TMPs/g-C3N4 composites during the degradation of TCs were elucidated, and an efficient and stable photolysis model was established. The research results of this project provide a useful design idea and model for the construction of practical photodegradation system, and have important research value and guiding significance for the prevention and control of TCs pollutants at the same time.

本项目从饮用水安全的国家重大需求出发，利用绿色环保的光催化氧化技术处理水中低浓度、高危害且难生物降解的四环素类抗生素（TCs）。基于半导体光降解该类污染物过程中活性自由基氧化的机理，针对当前光催化剂成本高、效率低等问题，拟通过两步法（溶剂热-磷化法）构建过渡金属磷化物/氮化碳（TMPs/g-C3N4）复合材料，用于高效光催化降解TCs。探究g-C3N4与TMPs在复合过程中所建立的微观机制及相互作用规律；研究复合材料的成分、结构、晶相、形貌与光吸收性能、吸附性能、光催化性能及稳定性之间的内在联系；阐明TMPs/g-C3N4复合材料在降解TCs过程中的中间产物、活性物种、电子传输机制及降解动力学/热力学行为过程，建立其高效、稳定的光解模型。该项目的研究成果为构筑可实用化光降解体系提供了有益的设计思路和模型，同时对TCs污染物的防治具有重要的研究价值和指导意义。

本项目从饮用水安全的国家重大需求和纳米技术的关键问题出发，利用过渡金属磷化物(TMPs)作助催化剂修饰氮化碳(g-C3N4)形成复合材料，并将其应用于在可见光下光降解四环素类抗生素(TCs)的性能研究。探索g-C3N4与TMPs复合过程的微观机制及相互作用规律；研究所复合材料的成分组成、结构、晶相、形貌与光吸收性能、吸附性能、光催化性能以及稳定性之间的内在联系；研究TMPs/g-C3N4光降解过程中的动力学/热力学行为；研究TMPs 与g-C3N4材料之间在光催化降解过程中电子的传输机制及界面传递行为；阐明TMPs/g-C3N4复合材料在降解水中TCs污染物的中间产物和活性物种探索光催化剂降解TCs的机理，构建其光降解模型，为高效光催化降解酚类废水奠定科学基础。项目成果对抗生素类污染物防治具有重要的科学意义。