Pyrite is the most common sulfur-bearing iron mineral in Earth surface environments. Pyrite is extensively utilized as a catalyst in the advanced oxidation processes (AOPs) for wastewater treatment due to its impressive reductive capacity and high Fe(II) content. However, it is still controversial whether pyrite could play a truly favorable role in the decontamination processes, as most of the pyrite-based AOPs are susceptible to water matrices and prone to deactivation during reactions. Elucidating mechanisms of the pyrite-mediated reactive oxygen species (ROS) generation is crucial for addressing the aforementioned question, but this topic has rarely been systematically summarized so far. In this Critical Review, we first elaborate on the fundamental mechanisms of the pyrite-mediated ROS generation in anoxic/aerobic environments. Afterward, detailed discussions are presented on how the intrinsic nature of pyrite, the secondary iron/sulfur species formed during the oxidation processes, and the conventional water chemistry parameters influence the pyrite-mediated ROS generation process. Furthermore, we summarize the enhancing mechanisms of the recently developed pyrite-based AOPs. Especially, the research focus and experimental design are compared between studies targeting the geo-environmental processes and the environmental engineering systems, since some overlooked but important mechanisms should be mutually informative across different disciplines to advance the comprehension of the environmental behavior of pyrite. Finally, the perspectives and proposals are briefly outlined to stimulate future discussion and interest in developing more rational pyrite-based environmental remediation technologies.

中文翻译：

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黄铁矿非生物氧化过程中活性氧化物质的产生：起源、影响因素、环境修复应用


黄铁矿是地球表面环境中最常见的含硫铁矿物。黄铁矿因其令人印象深刻的还原能力和高 Fe（II） 含量而被广泛用作废水处理高级氧化过程 （AOP） 中的催化剂。然而，黄铁矿是否能在净化过程中发挥真正有利的作用仍然存在争议，因为大多数基于黄铁矿的 AOP 容易受到水基质的影响，并且在反应过程中容易失活。阐明黄铁矿介导的活性氧 （ROS） 生成的机制对于解决上述问题至关重要，但到目前为止，这一主题很少被系统地总结。在这篇批判性综述中，我们首先详细阐述了在缺氧/好氧环境中黄铁矿介导的 ROS 生成的基本机制。之后，详细讨论了黄铁矿的内在本质、氧化过程中形成的次生铁/硫物质以及常规水化学参数如何影响黄铁矿介导的 ROS 生成过程。此外，我们总结了最近开发的基于黄铁矿的 AOPs 的增强机制。特别是，在针对地环境过程和环境工程系统的研究之间比较了研究重点和实验设计，因为一些被忽视但重要的机制应该在不同学科之间相互提供信息，以促进对黄铁矿环境行为的理解。最后，简要概述了这些观点和建议，以激发未来的讨论和对开发更合理的基于黄铁矿的环境修复技术的兴趣。