Yang Jiaqi, Yang Yu, Gao Kexuan, Graham Nigel J D, Hou Li-An
State Key Laboratory of Water Environment Simulation, School of Environment, Beijing Normal University, Beijing, 100875, China.
State Key Laboratory of Water Environment Simulation, School of Environment, Beijing Normal University, Beijing, 100875, China.
Environ Res. 2025 Oct 1;282:122051. doi: 10.1016/j.envres.2025.122051. Epub 2025 Jun 4.
Regulation of the types and content of reactive oxygen species (ROS) in advanced oxidation processes (AOPs) is regarded as a challenging task. Herein, the features of sulfur-vacancy (Sv) and nitrogen-vacancy (Nv), and cobalt (Co)/molybdenum (Mo)-bimetallic constituents were simultaneously incorporated into a novel Co-N@MoS-COOH catalyst through a simple hydrothermal calcination method. The adsorption of oxygen (O) and peroxymonosulfate (PMS) was promoted by Sv/Nv, whereby the generation of superoxide radical (O·) and singlet oxygen (O) species was induced, and the energy barrier for the formation of high-valent cobalt-oxo species (Co(IV)=O) was reduced. The decomposition of PMS was enhanced by a bimetal (Mo/Co) electronic pump and the O·, O, and Co(IV)=O active species degraded tetracycline (TC) together to achieve an efficient degradation rate (initial K = 0.490 min). The degradation intermediates and potential degradation pathways were identified, and the leaching of Co was within the acceptable range of environmental standards. Incorporation of the catalyst into a microfilter membrane achieved a 100 % degradation of TC at an ultra-high membrane flux (1803.4 LMH/bar). This study provided new insights into the types of ROS regulated by bi-vacancy and bimetallic catalysts in AOP systems, with the intention of promoting a more sustainable and resource-efficient treatment technology.
调控高级氧化过程(AOPs)中活性氧物种(ROS)的类型和含量被视为一项具有挑战性的任务。在此,通过简单的水热煅烧方法,将硫空位(Sv)和氮空位(Nv)以及钴(Co)/钼(Mo)双金属成分的特性同时引入到一种新型的Co-N@MoS-COOH催化剂中。Sv/Nv促进了氧气(O)和过一硫酸盐(PMS)的吸附,从而诱导了超氧自由基(O·)和单线态氧(O)物种的生成,并降低了高价钴氧物种(Co(IV)=O)形成的能垒。双金属(Mo/Co)电子泵增强了PMS的分解,并且O·、O和Co(IV)=O活性物种共同降解四环素(TC)以实现高效降解速率(初始K = 0.490 min)。确定了降解中间体和潜在的降解途径,并且Co的浸出在环境标准的可接受范围内。将该催化剂掺入微滤膜中,在超高膜通量(1803.4 LMH/bar)下实现了TC的100%降解。本研究为AOP系统中双空位和双金属催化剂调控的ROS类型提供了新的见解,旨在推动一种更可持续和资源高效的处理技术。