石墨相氮化碳基光催化剂激活过硫酸盐体系对莠去津污染水体的修复效能和机理研究

Graphite carbon nitride photocatalyst is simple to be prepared and environmental friendly, which not only owns excellent photocatalytic degradation ability, but also has broad application prospects in photocatalytic activation of persulfate for polluted water remediation. However, at present, there are few reports about photocatalytic activation of persulfate by graphite carbon nitride for water remediation, and there is no report on atrazine treatment based on this system. Meanwhile, the corresponding activation mechanism and degradation process are not clear yet. This project intends to prepare graphite carbon nitride-based photocatalyst, and as an activator to activate persulfate, forming a composite system combine photocatalysis and persulfate, which can degrade and mineralize atrazine thoroughly. We aim to studied the property of graphite carbon nitride with different morphology, different dope elements and plasmonic tungsten oxide for persulfate activation. The deactivation process and reaction mechanism were studied by density functional theory, free radical quenching and detection, and intermediate product analysis. At the same time, the actual water samples were simulated to study the effects of various environmental factors and analyze their reaction mechanism. This study is expected to provide scientific basis for the efficient and sustainable removal of atrazine and the remediation and treatment of atrazine-contaminated water under actual environmental conditions.

石墨相氮化碳基光催化剂具有优异的光催化降解能力，同时制备过程简单、环境友好，在光催化激活过硫酸盐修复污染水体具有广阔的应用前景。但是目前关于石墨相氮化碳光催化激活过硫酸盐进行水体修复的相关报道还不多见，而用该体系处理莠去津尚未见报道，其相应的激活机理和降解过程尚不清晰。本项目拟制备多种石墨相氮化碳基光催化剂，并且用于激活过硫酸盐，形成光催化和过硫酸盐相结合的复合体系，彻底降解莠去津，使之彻底矿化。研究不同形貌结构和元素杂化类型和含量的石墨相氮化碳，等离子体型氧化钨的负载的石墨相氮化碳基复合材料激活过硫酸盐去除莠去津的性能。结合密度泛函理论，自由基猝灭与检测、中间产物分析等充分研究去激活过程和反应机理。同时取实际水样进行模拟实验，研究各种环境因子的影响，分析其作用机制。本研究有望为莠去津的高效可持续性去除，以及实际环境条件下的莠去津污染水体的修复和治理提供科学依据。

石墨相氮化碳具有制备过程简单、环境友好，结构稳定，容易进行调控等特点，基于石墨相氮化碳的光催化反应体系用于活化过硫酸盐降解莠去津具有较为现实的研究意义。石墨相氮化碳光催化剂性能提升的关键是如何产生更多的光生电荷，并且高效分离以便进行氧化还原反应。因此，本项目通过同质结的构建、小分子修饰、元素杂化、异质结构建兼形貌调控以及多场结合的方法，或者多种手段结合并行的方式，增强石墨相氮化碳基光催化剂的光催化性能。同时采用多种表征手段对所制备的石墨相氮化碳基光催化剂进行系统的分析与研究。系统研究了环境因素对石墨相氮化碳基光催化活化过硫酸盐降解莠去津的影响，并且详细分析其影响机理；结合基于第一性原理的密度泛函理论，深入剖析石墨相氮化碳基光催化的结构特性与其光催化性能之间的构效关系，通过自由基猝灭与检测、中间产物分析等充分研究激活过程和反应机理。这些研究思路和方法为制备高效的石墨相氮化碳基光催化剂以及用于莠去津等有机农药污染水体的治理与修复提供新的思路和实践依据，有利于推动光催化技术的实际应用与推广。

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