General synthesis of carbon and oxygen dual-doped graphitic carbon nitride via copolymerization for non-photochemical oxidation of organic pollutant
General synthesis of carbon and oxygen dual-doped graphitic carbon nitride via copolymerization for non-photochemical oxidation of organic pollutant
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共聚碳氧双掺杂石墨氮化碳的通用合成用于有机污染物的非光化学氧化
DOI：
10.1016/j.jhazmat.2020.122578
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发表时间：
2020
影响因子：
13.6
通讯作者：
Hu Chun
中科院分区：
文献类型：
--
作者：
Zhu Yue;Chen Zhenhuan;Gao Yaowen;Hu Chun
地球资源丰富、环境友好且耐用的催化剂对于有机污染物的修复至关重要，石墨碳氮化物（g-C3 N4）是用于该应用的有前途的非金属材料。然而，由于g-C3 N4的化学惰性，如果没有光照射，其催化氧化效率低。本文以尿素为g-C3 N4前驱体，抗坏血酸（AA）为碳源和氧源，通过共聚反应合成了碳氧双掺杂g-C3 N4，并诱导了电子结构的重构。通过用其他有机前驱体代替AA，成功地制备了一系列C和O双掺杂的g-C3 N4，证明了所开发方法的通用性。结果表明，以AA为有机前驱体的C和O双掺杂g-C3 N4（CN-AA 0.3）在无光照条件下，与纯g-C3 N4和单氧掺杂g-C3 N4相比，表现出明显增强的过硫酸盐活化降解有机污染物的催化活性.实验和理论结果表明，贫电子的C原子和富电子的O原子作为PMS活化的同时PMS氧化和还原的活性位点。该工作为合成具有重构电子结构的非金属双掺杂g-C3 N4提供了一种通用的方法，刺激了g-C3 N4基材料的开发，用于各种环境应用。
Earth-abundant, environmental-benign and durable catalysts are of paramount importance for remediation of organic pollutants, and graphitic carbon nitride (g-C3N4) is a promising nonmetallic material for this application. However, the catalytic oxidation on g-C3N4suffers from low efficiency because of its chemical inertness if not irradiated with light. Herein, we develop a facile copolymerization strategy for the synthesis of carbon and oxygen dual-doped g-C3N4using urea as g-C3N4precursor and ascorbic acid (AA) as carbon and oxygen sources, which induces electronic structure reconfiguration. By replacing AA with other organic precursors, a series of C and O dual-doped g-C3N4are successfully prepared, demonstrating the generality of the developed methodology. As a demonstration, the C and O dual-doped g-C3N4using AA as the organic precursor (CN-AA0.3) exhibits pronouncedly enhanced catalytic activity in peroxymonosulfate (PMS) activation for organic pollutant degradation without light irradiation compared with pristine g-C3N4and single oxygen-doped g-C3N4. Experimental and theoretical results revealed the electron-poor C atoms and electron-rich O atoms as active sites for PMS activation in terms of simultaneous PMS oxidation and reduction. This work offers a universal approach to synthesize nonmetal dual-doped g-C3N4with reconfigured electronic structure, stimulating the development of g-C3N4-based materials for diverse environmental applications.