Visible-light-driven Photocatalytic Activation of Peroxymonosulfate by K+-reformed Polymeric Carbon Nitride for Effective Sulfamethoxazole Decomposition
Visible-light-driven Photocatalytic Activation of Peroxymonosulfate by K+-reformed Polymeric Carbon Nitride for Effective Sulfamethoxazole Decomposition
复制标题
DOI：
10.1016/j.colsurfa.2022.128816
复制
发表时间：
2022-03
期刊：
影响因子：
--
通讯作者：
Yin Tian;Zechong Guo;Guoshuai Liu;Ming Liu;Can Yang;Hua Zou
中科院分区：
文献类型：
--
作者：
Yin Tian;Zechong Guo;Guoshuai Liu;Ming Liu;Can Yang;Hua Zou
基于SO4·-的高级氧化工艺(SR-AOP)是解决难降解污染物造成的严重污染风险的有效修复策略。在本研究中，我们报道了利用K+诱导的结构重塑(KPCN)高结晶度来实现PMS的可见光驱动光催化活化(VL-PCA)。KPCN+PMS+VL体系(对应的动力学常数为0.1452×m in-1)比PCN+PMS+VL体系(0.0263×m in-1)对磺胺甲恶唑的降解有显著的促进作用，活性物种清除剂和电子顺磁共振实验表明，·O2-、1O2、·OH和SO4·-是促进磺胺甲恶唑降解的主要反应物种.KPCN晶体半导体保持了原始PCN的长程原子有序组态和非线性光学(NLO)响应特性。KPCN独特的NLO效应使其能够产生更多的光生载流子，并最大限度地减少电子-空穴对复合，从而显示出PMS对SMX降解具有优越的VL-PCA性能。本研究通过调控PCN的无序结构和相缺陷，对C3N4基PMS光催化活性的提高进行了概念验证，为开发基于氮化碳的高效VL-PCA催化剂提供了启示。
The SO4•–radical based advanced oxidation process (SR-AOP) is the effective remediation strategy for addressing the concern of severe pollution risk caused by recalcitrant pollutants. In this study, we report the visible-light-driven photocatalytic activation (VL-PCA) of PMS by using K+-induced structure remodeling high crystallinity of (KPCN). The degradation of sulfamethoxazole (SMX) by KPCN+PMS+VL system (the corresponding kinetic constant is 0.1452 min–1) was enhanced remarkably compared with PCN+PMS+VL system (0.0263 min–1).•O2–,1O2, •OH and SO4•–radicals were the dominant reactive species for the enhanced decomposition of SMX, evidently demonstrated by reactive species scavenger and electron paramagnetic resonance (EPR) experiments. The KPCN crystalline semiconductors maintain the properties of long-range atomic order configuration and nonlinear optical (NLO) response of pristine PCN. The unique NLO effects of KPCN enable it to produce more photogenerated carriers and minimize the electron-hole pair recombination, which exhibit superior VL-PCA performance of PMS toward SMX degradation. This study gives a proof-in-concept demonstration of the increased activity of the C3N4-based PMS photocatalytic-activator by regulating the disordered structure and phase defects of PCN, shedding light on the development of highly efficient VL-PCA catalysts based on carbon nitride.