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[Display omitted] • The synergistic effect of natural minerals for persulfate activation were reviewed. • The mechanism of persulfate activation and contaminants degradation were summarized. • We pointed out that the major challenges and direction of mineral-based catalysts. • This review is meaningful for the high-value-added application and functional specialization of minerals. The severity of environmental pollution poses a serious threat to human health, and especially organic pollution is more complex and difficult to treat compared to heavy metal pollution. Nowadays, the persulfate-based advanced oxidation processes receive more and more attention due to high efficiency, strong controllability, easy operation, and economic competitiveness, which is generally employed for the efficient degradation of organic contaminants. Natural minerals possess the characteristics of low-cost, easy availability, environmental friendliness, non-toxic, special structural effects, etc., which have played a critical role and could be the promising alternative to traditional catalysts for persulfate activation. First, this review retrospects the research status of natural minerals and mineral-based catalysts for persulfate activation to degrade organic contaminants, i.e., pyrite, mackinawite, copper sulfide, kaolinite, and montmorillonite. Then, the mechanisms of persulfate activation by natural minerals and mineral-based catalysts to generate the reactive oxygen species including SO 4 •−, •OH, •O 2 −, 1O 2 , and surface reactive complex for contaminants degradation are systematically summarized. Finally, we discussed the further application of natural minerals in activating persulfate as well as the future research frontiers for practical environmental remediation, i.e., the synthesis and characterization of mineral-based catalysts dominated by non-radical pathway, the large-scale application of PDS with low-cost, the surface modification of mineral-based catalysts with amphiphilicity, as well as the more efficient catalysts possessing nano-restricted domain catalytic effect. The development and expansion of novel and efficient mineral-based catalysts with enhanced synergistic effects would provide new opportunities for persulfate activation in environmental remediation. [ABSTRACT FROM AUTHOR]

• Oxygen-vacancy-rich Co 3 O 4 /illite can activate peroxymonosulfate (PMS) efficiently. • Modulating crystallization of Co 3 O 4 by illite resulted in rich oxygen vacancies. • Theoretical calculations were employed to elucidate catalytic mechanism for PMS. • Rich oxygen vacancies accelerated electron-transfer and reduced adsorption energy. • S O 4 - • , OH and 1O 2 were generated and functioned in Co 3 O 4 /illite/PMS system. Natural illite microsheets were firstly utilized to induce oxygen vacancies into ultrafine cobalt oxide (Co 3 O 4) for highly efficient Fenton-like catalysis via activation of peroxymonosulfate (PMS). The results indicated that presence of illite microsheets regulated multi-directional crystallization of Co 3 O 4 nanospheres and resulted in reduced grain size and crystallinity. The smaller grain size provided more reactive edge sites for PMS catalysis. The numerous indistinct lattice boundaries caused by reduced crystallinity created abundant oxygen vacancies. Density functional theory (DFT) calculations illustrated that presence of oxygen vacancies significantly reduced adsorption energy and accelerated electron transfer, which further faciliated PMS activation. The oxygen vacancy-rich Co 3 O 4 /illite exhibited superior catalytic efficiency in real water matrix. Apart from sulfate and hydroxyl radicals, singlet oxygen generated from oxygen vacancy-based reaction pathway also played a significant role in atrazine degradation. This strategy provided a new insight for future designing of natural mineral-based catalysts for efficient wastewater treatment via Fenton-like process. [ABSTRACT FROM AUTHOR]