Cobalt (0/II) incorporated N-doped porous carbon as effective heterogeneous peroxymonosulfate catalyst for quinclorac degradation
Cobalt (0/II) incorporated N-doped porous carbon as effective heterogeneous peroxymonosulfate catalyst for quinclorac degradation
复制标题
钴 (0/II) 掺氮多孔碳作为有效的非均相过一硫酸盐催化剂，用于二氯喹啉酸降解
DOI：
10.1016/j.jcis.2019.12.067
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发表时间：
2020
影响因子：
9.9
通讯作者：
Zhong Mei-e
中科院分区：
文献类型：
--
作者：
Zhou Nan;Zu Junning;Yang Lihua;Shu Xiaoqing;Guan Jindiao;Deng Yaocheng;Gong Daoxin;Ding Chunxia;Zhong Mei-e
以乙二胺四乙酸和钴盐为原料，通过一步热分解制备了Co（0/II）掺杂的N掺杂多孔碳（Co/N单键C）催化剂。纳米Co粒子由金属和氧化态Co组成，在石墨烯类薄膜型N掺杂碳载体中分散良好。钴物种在过一硫酸盐（PMS）活化中起主导作用，产生硫酸根和羟基自由基。N掺杂的多孔碳通过增强电子转移协同影响催化性能。由此产生的Co/N单键C是一种高效的多相催化剂PMS活化，并使显着增强的二氯喹啉酸（QNC）的降解。通常，使用0.08 g L−1Co/N单键C和20 mmol L− 1 PMS可实现93%的QNC（50 mg L−1）去除。QNC的降解动力学数据符合准一级动力学模型，相关系数（R2）大于0.99。反应机理的研究表明，在Co/N单键-C单键-PMS体系中，羟基自由基（HOradical dot）和硫酸根自由基（SO 4 radical dot−）是主要的活性物种，QNC的降解主要是脱羟基和单键OH取代单键COOH的过程.这种Co/N单键C催化剂有望用于高级氧化工艺去除持久性有机污染物。
A cobalt(0/II)-incorporatedN-doped porous carbon (Co/Nsingle bondC) catalyst was prepared via one-step thermal decomposition of ethylene-diamine tetra-acetic acid and a Co salt. Fine Co nanoparticles composed of metallic and oxidized Co species were formed and well dispersed in the graphene-like film-typeN-doped carbon support. The Co species played a dominant role in peroxymonosulfate (PMS) activation to generate sulfate and hydroxyl radicals. TheN-doped porous carbon synergistically affected the catalytic performance by enhancing electronic transfer. The resulting Co/Nsingle bondC was a highly efficient heterogeneous catalyst for PMS activation and enabled considerably enhanced quinclorac (QNC) degradation. Typically, 93% QNC (50 mg L−1) removal was achieved with 0.08 g L−1Co/Nsingle bondC and 20 mmol L−1PMS. The QNC degradation kinetic data fitted a pseudo-first-order kinetic model well, with a correlation coefficient (R2) higher than 0.99. Investigation of the reaction mechanism suggested that hydroxyl (HOradical dot) and sulfate (SO4radical dot−) radicals were the predominant active species in the Co/Nsingle bondCsingle bondPMS system and QNC degradation mainly involved dehydroxylation and substitution of single bondOH for single bondCOOH. This Co/Nsingle bondC catalyst is promising for use in advanced oxidation processes for the removal of persistent organic pollutants.