Reinventing MoS2 Co-catalytic Fenton reaction: Oxygen-incorporation mediating surface superoxide radical generation
Reinventing MoS2 Co-catalytic Fenton reaction: Oxygen-incorporation mediating surface superoxide radical generation
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DOI：
10.1007/s12274-021-3848-3
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发表时间：
2021-09
期刊：
影响因子：
9.9
通讯作者：
X. Tan;Wenhui Ding;Zhenying Jiang;Linxiao Sun;Yuxiong Huang
中科院分区：
文献类型：
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作者：
X. Tan;Wenhui Ding;Zhenying Jiang;Linxiao Sun;Yuxiong Huang
深入了解过氧化氢（H2 O2）的分解和活性氧（ROS）在催化剂表面的生成机理一直是芬顿/类芬顿反应在环境中应用的关键问题。我们在这里报告了一种新的方法来激活H2 O2在共催化芬顿系统与氧结合的二硫化钼，即MoS 2 − xOx纳米片。MoS 2 −xOxnanosheets辅助的助催化芬顿系统表现上级对新兴抗生素污染物（例如，磺胺甲恶唑）。结合密度泛函理论（DFT）计算和实验研究，我们证明了氧的掺入可以提高MoS 2 − xOx纳米片的本征电导率，加速表面/界面电荷转移，从而进一步导致H2 O2的有效活化。此外，通过调节MoS 2 − xOx纳米片中的氧比例，我们能够调节ROS的产生，并进一步引导H2 O2定向转化为表面结合的超氧自由基（·O2表面−）。它揭示了工程化系统中ROS的产生和转化（例如，芬顿，类芬顿反应）高效降解持久性污染物。
To better understand the mechanisms of hydrogen peroxide (H2O2)’s decomposition and reactive oxygen species (ROS)’s formation on the catalyst’s surface is always a critical issue for the environmental application of Fenton/Fenton-like reaction. We here report a new approach to activate H2O2in a co-catalytic Fenton system with oxygen incorporated MoS2, namely MoS2−xOxnanosheets. The MoS2−xOxnanosheets assisted co-catalytic Fenton system exhibited superior degradation activity of emerging antibiotic contaminants (e.g., sulfamethoxazole). Combining density functional theory (DFT) calculation and experimental investigation, we demonstrated that oxygen incorporation could improve the intrinsic conductivity of MoS2−xOxnanosheets and accelerate surface/interfacial charge transfer, which further leads to the efficacious activation of H2O2. Moreover, by tuning the oxygen proportion in MoS2−xOxnanosheets, we are able to modulate the generation of ROS and further direct the oriented-conversion of H2O2to surface-bounded superoxide radical (·O2 surface−). It sheds light on the generation and transformation of ROS in the engineered system (e.g., Fenton, Fenton-like reaction) for efficient degradation of persistent pollutants.