Heterogeneous Fenton reactions offer the opportunities to overcome iron sludge accumulation and limited recyclability of existing homogeneous Fenton process, but the sharp attenuation in their reactivity at near-neutral and even higher pH conditions, still remains a formidable challenge. In this work, we report a versatile and robust approach to create a local acidic microenvironment on BiOI with graphene oxide bonding, enabling the heterogeneous Fenton (BiOI@rGO/H2O2) system to sustainably degrade organic pollutants over a wide pH range (3.0–10.0). Notably, BiOI@rGO exhibits a superior catalytic activity (∼100 % removal) and robust durability (over ten cycles) in degrading bisphenol A and tetracycline, even in real wastewater scenarios. Furthermore, immobilizing the BiOI@rGO on carbon felt to establish a continuous flow-through device achieves a stable treatment performance with a degradation efficiency exceeding 98 % for micropollutants over a continuous operation. This work provides a paradigm for constructing an acidic microenvironment on the catalyst to surmount the pH limitations of the heterogeneous Fenton reactions for advanced water purification.

中文翻译：

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扩大用于污染物降解的 Fenton 类反应的 pH 范围：酸性微环境的影响


非均相 Fenton 反应为克服铁污泥积累和现有均相 Fenton 工艺的有限可回收性提供了机会，但它们在接近中性甚至更高 pH 值的条件下的反应性急剧衰减仍然是一个艰巨的挑战。在这项工作中，我们报道了一种通用且强大的方法，通过氧化石墨烯键在 BiOI 上创建局部酸性微环境，使异质 Fenton （BiOI@rGO/H2O2） 系统能够在较宽的 pH 范围 （3.0–10.0） 内可持续降解有机污染物。值得注意的是，即使在实际废水场景中，BiOI@rGO在降解双酚 A 和四环素方面也表现出卓越的催化活性（∼100% 去除率）和强大的耐久性（超过 10 次循环）。此外，将BiOI@rGO固定在碳毡上以建立连续流通装置，可实现稳定的处理性能，在连续运行中对微污染物的降解效率超过 98%。这项工作为在催化剂上构建酸性微环境提供了一种范例，以克服非均相 Fenton 反应的 pH 限制，以实现高级水净化。