Chun Hu

Efficient elimination of emerging contaminants (ECs) from complex water matrices remains a challenge for peroxymonosulfate (PMS)-based advanced oxidation processes, which typically require high PMS dosages and suffer from poor oxidant utilization. Here, we report a Fenton-like flow reactor (FFR) composed of stacked layers of immobilized catalysts (Co-carbon nanotube/carbon fiber, Co-CNT/CF). Unlike conventional PMS-activating batch reactors, the FFR harnesses in situ-generated concentration and potential gradients to induce a spontaneous galvanic effect (GE). This macroscale GE enables self-sustained PMS activation, dissolved oxygen reduction, and radical generation without external energy input, thereby overcoming mass transfer limitations inherent to batch reactors. Additionally, it endows the FFR with exceptional adaptability under a wide range of EC concentration, salinity, natural organic matter (NOM), and pH. Notably, increasing wastewater conductivity boosted the treatment capacity by several times, achieving the removal of nearly 100% ECs at a flux rate >1000 mL min^–1. Furthermore, the enhanced microcosmic charge transfer at the catalyst/wastewater interface enabled extremely low PMS usage (≤0.08 mM) and high utilization efficiency (77.5–96.3%). This work introduces a gradient-driven, galvanic-enabled PMS activation pathway that establishes a new design paradigm for cost-effective and energy-saving continuous-flow water purification technologies.

Traditional photocatalytic systems for pollutant removal depend on exogenous oxidants or sacrificial agents, hampering sustainability. Herein, we report an exogenous reagent‐free dual‐substrate cooperative strategy. Without adding external chemicals (e.g., methanol, sulfite), the target pollutant phenol is directly used as an endogenous electron donor to drive the reduction of Cr(VI) and its own degradation over a thermally exfoliated graphitic carbon nitride (CN‐T) catalyst. Phenol fulfills two critical roles in this system: (i) it is oxidized and degraded by photogenerated holes (h ⁺ ), and (ii) it transfers electrons to CN‐T, enhancing Cr(VI) reduction by photogenerated electrons (e ⁻ ). Kinetic studies, DFT calculations, and EPR spectroscopy reveal that phenol adsorbs on CN‐T via π‐π stacking and hydrogen bonding, facilitating electron transfer from its HOMO to the CN‐T LUMO. This process suppresses e ⁻ ‐h ⁺ recombination and promotes Cr(VI) reduction. In the coexisting system, CN‐T achieved 76.4% Cr(VI) reduction and 99.8% phenol degradation, with a 6.4‐fold higher Cr(VI) reduction rate constant than in the single pollutant system. Substituted phenols (4‐methylphenol, 4‐chlorophenol, p‐nitrophenol) strongly correlate with electronic descriptors (Hammett constant, E _HOMO ), establishing a robust quantitative structure‐activity relationship (QSAR) for predictive synergistic co‐removal. This work advances photocatalytic redox coupling and provides a “waste‐to‐waste” strategy for sustainable complex wastewater.

抗生素在水体中的持久性残留可对人类健康及生态环境构成潜在威胁。然而，现有处理技术受限于高能耗及溶解性有机碳(DOC)对降解效率的抑制作用。为此，本研究成功制备了一种Fe/Al双金属络合修饰的石墨烯类材料包覆零价铁(Fe/Al-GC@Fe⁰)复合材料。该材料在常温常压，无需外加任何能量的条件，实现了水中痕量抗生素左氧氟沙星、磺胺甲基嘧啶、磺胺甲恶唑、四环素和环丙沙星的高效快速降解。这得益于催化剂表面显著的Fe-π相互作用，Fe/Al-GC@Fe⁰形成了由富电子Fe微区和缺电子石墨碳(GC)微区构成的强静电场，并表现出优异的电子传导性能。这种独特的电子结构促使反应过程中抗生素分子在缺电子GC微区与H₂O/O₂在富电子Fe微区发生协同配位，通过Fe-π相互作用引发显著的表面电荷重排。该过程显著增强了界面电场强度，进而触发类电化学反应机制，最终实现对实际水体中痕量抗生素的高效选择性去除。

Toxic organic pollutants and heavy metals (HMs) present in aquatic environments have been a global challenge for water purification, which is often difficult to address even with massive resources and energy consumption. Herein, a new strategy is proposed to achieve simultaneous pollutant removal and Ag recovery in an expanded water self-purification system based on Mo-SnS₂ quantum dots (MSS QDs) with dual-reaction-center (DRC). The innovative discovery is that the electrons of pollutants are finally utilized by Ag⁺ and dissolved oxygen through the constructed interfacial process without any sacrificial agent or additional energy consumption. Especially for antibiotics, one of the typical emerging contaminants (ECs), the degradation rate reaches 100% in a very short time. In N₂ environment, the Ag recovery rate even reaches 94%. It is estimated that the cost of wastewater treatment is only $0.01/m³ (USD), and it even comes with huge benefits from Ag recovery in this expanded water self-purification system. This work provides novel technical references for developing multifunctional and low-consumption water purification technologies in response to the United Nations Sustainable Development Goals.