Solid waste-azo dye degradation closed loop: bridging coal gangue recycling and azo dye removal

Chunjie Huang, Wenkang Qi, Yutong Yang, Ying Zhang, Jianwen Lu, Qiuxia Ye, Xingyong Xue, Yaocong Han, Qiaoqiao Su, Dongping Wei, Lihong Lan
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Abstract

To address the dual challenges of coal gangue utilization and azo dye wastewater treatment, this study developed cobalt-loaded geopolymer microsphere catalysts (Co@CGM) through the resource utilization of coal gangue for peroxymonosulfate (PMS) activation, achieving efficient degradation of azo dyes sunset yellow (SY) and amaranth red (AR). Single-factor experiments demonstrated that Co@CGM exhibited exceptional catalytic performance at ultra-low PMS concentrations (0.25–0.50 mmol/L), achieving degradation efficiencies of 99.38% for SY and 99.91% for AR within 30 min for 100 mL solutions at 50 mg/L concentration. Stability tests revealed that Co@CGM maintained significant PMS activation effectiveness through five degradation cycles, demonstrating strong acid-base resistance (pH=3–9) and excellent anion interference resistance (Cl, NO3, H2PO4, etc.). Quenching experiments and electron paramagnetic resonance spectrometer (EPR) analysis confirmed that singlet oxygen (1O2) served as the primary reactive species driving the rapid degradation process in both SY and AR systems. Liquid chromatography-mass spectrometer (LC-MS) analysis identified intermediate products and proposed degradation pathways for both dyes. This work successfully developed an eco-friendly functional material through coal gangue waste recycling, achieving the goal of “treating waste with waste” in azo dye wastewater remediation.

Graphical abstract

固体废物-偶氮染料降解闭环:架起煤矸石回收与偶氮染料去除的桥梁
为了解决煤矸石利用和偶氮染料废水处理的双重挑战,本研究通过对煤矸石资源利用进行过氧单硫酸盐(PMS)活化,开发了钴负载地聚合物微球催化剂(Co@CGM),实现了偶氮染料日落黄(SY)和苋菜红(AR)的高效降解。单因素实验表明Co@CGM在超低PMS浓度(0.25-0.50 mmol/L)下表现出优异的催化性能,在50 mg/L浓度的100 mL溶液中,30 min内对SY和AR的降解效率分别达到99.38%和99.91%。稳定性测试表明,Co@CGM在5个降解循环中保持了显著的PMS活化效果,具有较强的酸碱耐受性(pH= 3-9)和优异的阴离子抗干扰性(Cl−、NO3−、H2PO4−等)。猝灭实验和电子顺磁共振谱(EPR)分析证实,单线态氧(1O2)是驱动SY和AR体系快速降解过程的主要反应物质。液相色谱-质谱仪(LC-MS)分析确定了两种染料的中间产物并提出了降解途径。通过对煤矸石废弃物的回收利用,成功开发了一种生态友好型功能材料,实现了偶氮染料废水修复中“以废治废”的目标。图形抽象
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