胶体喷射制备CQDs-Fe双助光催化材料及降解含-CN化合物机理

Cyanide organic matter is the most danger matters to the people and environment in the China due to its high toxicity. In the recent studies, many methods were used to solve this problem, such as distillation method, biochemical method, burning method, oxidation method, radiation method, liquid film method, active carbon adsorption, ion exchange method and so on. However, those method may bring in some other solid waste and the cyanide organic can not completely degradation. .As we all know, SP2-CQDs is the best matter to the photocatalysis process because its nontoxic characteristic and wide spectrum depleting characteristic. Therefore, in this study, we synthesis a new CQDs-Fe electrode by colloid jet printing basic on SP2-CQDs collosol, α-FeO(OH) collosol and TiO2 collosol. What’s more, micro piezoelectric field and was been used to enhance the photocatalysis process and transfer of the activated hydrogen. The activated hydrogen may give an reducing atmosphere to hinder the production of the NOx. This process could control the oriented conversion of the N element. Some of the useful method were used to control the CO2 turn into CO32-. The seed crystal nucleus was been used to incorporation with CO32- to produce  carbonate-precipitation. At last, a new photocatalytic degradation of organic carbon detoxification system was been set to study the photocatalytic mechanism of this process.

针对含-CN化合物处理中毒性迁移、固废和温室气体等局限性，基于光诱导电子迁移反应为设计思路，提出CQDs-Fe双助光催化电极降解含-CN化合物固碳-解毒新方法，一方面利用碳量子点和铁化合物强化催化材料对可见光的吸收能力；另一方面调节溶液环境和反应条件实现固碳-解毒协同机制。拟从电极制备、固碳-解毒反应机制等方面深入研究，应用绿色、宽谱捕光的碳量子点（SP2-CQDs）和铁配位中心作为光电子转移剂改性纳米TiO2溶胶，籍用胶体喷射技术制备CQDs-Fe双助光催化电极，碱性体系微压电场协助催化降解含-CN化合物固碳-解毒。引入造孔剂优化孔道结构，胶体喷射成型完善电极的制备；通过反应参数和电场调控，实现碳、氮元素的定向迁移，达到降解含-CN化合物固碳-解毒，借助仪器研究反应过程中碳-碳键、碳-氮键及光电子的传递转化过程，阐明协同体系下C、N形态转化过程中电子迁移历程。

本项目按计划针对含-CN化合物的抗生素左氧氟沙星、四环素和无机氰化物进行了水溶液中电、光双助催化转化过程研究。首先基于量子点和铁基化合物掺杂相关元素制备了系列催化剂，利用3D打印技术制备成宏观尖端电极；进一步研究发现微观纳米结构的尖端效应更具有分离和稳定电荷作用。在电场、光源和机械力作用下对复杂化合物中的氮元素和碳元素的形态进行分析，验证了弱碱性条件下引入硫酸根自由基、单线氧自由基降解优于羟基自由基降解效果，同时利于碳元素转化为碳酸根，并进一步碳酸盐固碳-解毒；同时，氮元素利于转化为氮气（pH：7-9），避免NOx温室气体释放。再者对于水质调控方面，弱酸性条件下，六价铬等有毒金属离子共存，也为固碳和氮转化提供有力条件。而在有氯离子等卤素存在时，表现出氮元素转化为氮气的趋势。综合考虑作用机理，复杂化合物中的C-C,C-N键在氧化自由基的作用下逐步无机矿化，与催化剂的微观结构、形貌和溶液组分相关。另外，利用密度泛函和分子动力学，从吸附能角度确定了在过渡金属离子氧化物尖端和弱碱性条件下，电子密度更大，揭示了通过铁基氧化物和碳基组分结构优化，调控作用点并促进电子逸出功和传输速率，从而利于碳酸盐和氮气的定向转化机制,该结果对水质深度处理具有重要意义。