Engineering dual photocatalytic sites on an S-scheme MoS2@Co3O4 heterostructure for coupled PMS activation and hydrogen production

IF 4.4 3区 化学 Q2 CHEMISTRY, PHYSICAL
Zenghao Liu , Hongjie Zhu , Yanshuo Fan , Jiakai Ma , Youyou Hu , Yan Feng , Haitao Zhao , Yao-Yao Wang , Hui-Juan Wang
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引用次数: 0

Abstract

The wide use of antibiotics poses serious ecological risks due to its environmental persistence and bioaccumulation. Although sulfate radical-based advanced oxidation processes (SR-AOPs) via peroxymonosulfate (PMS) activation exhibit promise for antibiotics elimination, practical applications is limited by excessive oxidant consumption, proton accumulation, and inefficient energy utilization. Herein, we report an S-scheme MoS2@Co3O4 heterojunction that couples Co3O4-mediated PMS activation with MoS2-driven H2 evolution. The built-in electric field at the MoS2@Co3O4 interface directs photogenerated electrons to MoS2, enabling proton reduction at H2 production rate of 2.7 mmol g−1 h−1. Simultaneously, the photocatalysis process accelerates Co3+/Co2+ cycle in Co3O4, enabling sustained PMS activation and radical generation. Under visible-light irradiation the coupled system achieves 97.77% TC degradation within 45 min. By converting reaction-generated protons into H2, this dual-channel charge-transfer mechanism mitigates effluent acidification and obviates the need for subsequent alkaline dosing. This work provides an energy-compensated process that transforms conventional energy-intensive wastewater treatment into a sustainable system capable of simultaneous pollutant removal and energy recovery, offering new insights into multifunctional environmental catalysts.

Abstract Image

在S-scheme MoS2@Co3O4异质结构上设计双光催化位点用于耦合PMS活化和制氢
抗生素的广泛使用由于其环境持久性和生物蓄积性造成了严重的生态风险。尽管通过过氧单硫酸盐(PMS)活化的硫酸盐自由基高级氧化过程(SR-AOPs)显示出消除抗生素的希望,但实际应用受到过多氧化剂消耗,质子积累和低效能量利用的限制。在此,我们报告了一个s方案MoS2@Co3O4异质结,将co3o4介导的PMS激活与mos2驱动的H2演化耦合在一起。MoS2@Co3O4界面处的内置电场将光生电子引导到MoS2上,使质子还原H2的产氢速率为2.7 mmol g−1 h−1。同时,光催化过程加速了Co3O4中Co3+/Co2+的循环,实现了PMS的持续活化和自由基的生成。在可见光照射下,耦合系统在45 min内实现了97.77%的TC降解。通过将反应产生的质子转化为H2,这种双通道电荷转移机制减轻了废水酸化,并避免了后续碱性投加的需要。这项工作提供了一个能量补偿过程,将传统的能源密集型废水处理转变为能够同时去除污染物和能量回收的可持续系统,为多功能环境催化剂提供了新的见解。
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来源期刊
CiteScore
7.90
自引率
7.00%
发文量
580
审稿时长
48 days
期刊介绍: JPPA publishes the results of fundamental studies on all aspects of chemical phenomena induced by interactions between light and molecules/matter of all kinds. All systems capable of being described at the molecular or integrated multimolecular level are appropriate for the journal. This includes all molecular chemical species as well as biomolecular, supramolecular, polymer and other macromolecular systems, as well as solid state photochemistry. In addition, the journal publishes studies of semiconductor and other photoactive organic and inorganic materials, photocatalysis (organic, inorganic, supramolecular and superconductor). The scope includes condensed and gas phase photochemistry, as well as synchrotron radiation chemistry. A broad range of processes and techniques in photochemistry are covered such as light induced energy, electron and proton transfer; nonlinear photochemical behavior; mechanistic investigation of photochemical reactions and identification of the products of photochemical reactions; quantum yield determinations and measurements of rate constants for primary and secondary photochemical processes; steady-state and time-resolved emission, ultrafast spectroscopic methods, single molecule spectroscopy, time resolved X-ray diffraction, luminescence microscopy, and scattering spectroscopy applied to photochemistry. Papers in emerging and applied areas such as luminescent sensors, electroluminescence, solar energy conversion, atmospheric photochemistry, environmental remediation, and related photocatalytic chemistry are also welcome.
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