硫氮共掺杂碳负载钴团簇的制备及其催化活化过一硫酸盐的研究

Synthesis of cobalt clusters anchored on S/N co-doped carbon for catalytic peroxymonosulfate activation

杂原子掺杂对碳负载金属团簇的过一硫酸盐(PMS)催化性能具有潜在的提升作用,但相关研究尚有限.本文采用热分解碳化法合成了一种硫氮共掺杂碳负载钴团簇材料SNC@CoNC,并对其进行了深入的表征和催化性能研究.结果表明,硫杂原子的引入显著增强了催化剂的活性和稳定性.在投加30 mg·L^(-1)SNC@CoNC和500μmol·L^(-1)PMS时,5 min内罗丹明B (RhB, 25μmol·L^(-1))的去除率达96%以上.与钴纳米颗粒催化剂、常用金属/非金属催化剂及许多先前报道的催化剂相比,SNC@CoNC展现出更优越的催化活性.此外,SNC@CoNC对水中共存阴离子和天然有机质展现出良好的耐受性,在pH=3~9范围内能有效催化PMS降解各类有机污染物.自由基猝灭、电子顺磁共振和电化学实验表明,SNC@CoNC主要通过电子转移为主的非自由基路径催化PMS降解RhB.

Investigating the influence of heteroatom doping on the catalytic efficacy of peroxymonosulfate(PMS)in carbon-supported metal clusters remains relatively uncharted.This study specifically focuses on synthesizing sulfur and nitrogen co-doped carbon-supported cobalt clusters(SNC@CoNC)via thermal pyrolysis carbonization.It aims to examine their characteristic and catalytic performance.Our findings reveal that upon the introduction of sulfur heteroatoms,there is a significant enhancement in both activity and stability of the catalyst.Notably,the inclusion of 30 mg·L^(-1) SNC@CoNC and 500μmol·L^(-1) PMS resulted in a degradation rate exceeding 96%for Rhodamine B(RhB,25μmol·L^(-1))within 7 min.Comparative assessments against cobalt nanoparticle catalysts,traditional metal/nonmetallic catalysts,and previously documented counterparts underscore the superior catalytic activity of SNC@CoNC.Furthermore,SNC@CoNC demonstrates exceptional resistance to inorganic anions and natural organic matter in water,effectively catalyzing the degradation of diverse organic pollutants by PMS across a pH range of 3 to 9.In-depth investigations encompassing radical quenching,electron paramagnetic resonance,and electrochemical experiments elucidate that SNC@CoNC primarily facilitates the degradation of RhB by PMS through a nonradical pathway,predominantly driven by electron transfer mechanisms.