Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2021-09-09 , DOI: 10.1016/j.apcatb.2021.120694 Qishi Si 1 , Wanqian Guo 1 , Huazhe Wang 1 , Banghai Liu 1 , Shanshan Zheng 1 , Qi Zhao 1 , Haichao Luo 1 , Nanqi Ren 1 , Tao Yu 2
In this study, a lateral heterostructures material (LCCN) of carbon quantum dot (CQDs) and carbon nitride (CN) was designed via the thermal polymerization of freeze-dried precursor. The special lateral heterostructures (LHSs) increased the bond length of O–O to fleetly active dissolved oxygen (DO), which exhibits 14-fold increased for tetracycline (TC) visible-light degradation compared to CN. In addition, the electrons of activated DO came from both TC and LCCN, which trapped the oxygen to generate multitudinous superoxide radical (•O2–), while the hole (h+) showed a negligible role in photocatalytic system. A rapid electron transfer channel was speculated between TC and photocatalyst by experiments and density functional theory. Furthermore, DFT and LC/MS predicted four degradation pathways of TC with the Fukui index (f0), and LCCN exhibited a favorable hinder on various environmental interferences. This work presented a novel perspective for the relationship of pollutant and material in photocatalysis.
中文翻译:
双功能碳量子点/g-C3N4 具有面内电子缓冲液,可在可见光下强烈降解四环素:紧密吸附和平稳电子转移
在这项研究中,通过冷冻干燥前驱体的热聚合设计了碳量子点 (CQDs) 和氮化碳 (CN) 的横向异质结构材料 (LCCN)。特殊的横向异质结构 (LHS) 增加了 O-O 与快速活性溶解氧 (DO) 的键长,与 CN 相比,四环素 (TC) 可见光降解增加了 14 倍。此外,活化的 DO 的电子来自 TC 和 LCCN,它们捕获氧以生成大量超氧自由基 (•O 2 – ),而空穴 (h +) 在光催化体系中的作用可以忽略不计。通过实验和密度泛函理论推测了TC和光催化剂之间的快速电子转移通道。此外,DFT 和 LC/MS 用福井指数 (f 0 )预测了 TC 的四种降解途径,并且 LCCN 对各种环境干扰表现出有利的阻碍。这项工作为光催化中污染物与材料的关系提供了新的视角。