π-π conjugation driving peroxymonosulfate activation for pollutant elimination over metal-free graphitized polyimide surface
π-π conjugation driving peroxymonosulfate activation for pollutant elimination over metal-free graphitized polyimide surface
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γ-γ共轭驱动过一硫酸盐活化，消除无金属石墨化聚酰亚胺表面的污染物
DOI：
10.1016/j.jhazmat.2021.125191
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发表时间：
2021
影响因子：
13.6
通讯作者：
Lyu Lai
中科院分区：
文献类型：
--
作者：
Cao Wenrui;Luo Yongxiang;Cai Xuanying;Wang Shuguang;Hu Chun;Lyu Lai
采用改进的水热聚合工艺合成了一种新型的无金属催化剂，该催化剂由典型的花状石墨化聚酰亚胺(g-PI)组成，在较宽的pH范围(3−11)内通过活化过一硫酸盐(PMS)表现出良好的污染物去除性能。该催化剂对攻击内分泌干扰物双酚A(BPA)特别有效，双酚A可以在短时间内完全降解。根据表征结果，g-PI是由丰富的芳香族骨架和基于C-O-C键的π偶联物和N-杂化环组成的，它们在后续的污染物降解中起着至关重要的作用。在g-PI/PMS/BPA体系中，富含π键的双酚A通过π-π相互作用优先吸附到催化剂表面，并伴随着活化能的降低而生成表面吸附的双酚A*。该物种可被PMS直接攻击和降解，不需要自由基过程，从而节省了PMS中间活化过程所需的能量。另一方面，从污染物中获得的电子迅速转移到O中心，驱动PMS激活产生自由基。协同界面工艺为实际废水净化提供了极大的潜力。
A novel metal-free catalyst consisting of typical flower-like graphitized polyimide (g-PI) is first synthesized via an enhanced hydrothermal polymerization process, and it exhibits excellent performance for pollutant removal through peroxymonosulfate (PMS) activation over a wide pH range (3−11). The catalyst is especially effective for attacking the endocrine disruptor bisphenol A (BPA), which can be completely degraded in a short time. Based on the results of characterization, g-PI is consisted of abundant aromatic frameworks with π conjugates based on C-O-C linkages and N-hybrid rings, which play essential roles in the subsequent degradation of pollutants. In the g-PI/PMS/BPA system, BPA (rich in π bonds) is preferentially adsorbed to the catalyst surface through π-π interactions, accompanied by a decrease in its activation energy to produce surface-adsorbed BPA*. This species can be directly attacked and degraded by PMS without the need for the radical processes, which saves the energy required for the intermediate activation process of PMS. On the other hand, the electrons obtained from pollutants are rapidly transferred to the O center, driving PMS activation to generate free radicals. The synergetic interface process offers excellent potential for practical wastewater purification.