School of Civil and Environmental Engineering, Harbin Institute of Technology Shenzhen, Shenzhen, 518055, China.
School of Civil and Environmental Engineering, Harbin Institute of Technology Shenzhen, Shenzhen, 518055, China.
Chemosphere. 2024 Jan;346:140538. doi: 10.1016/j.chemosphere.2023.140538. Epub 2023 Oct 28.
To enhance the polarization distribution of electron cloud density on the catalyst surface, we have introduced a novel bimetallic-substituted dual-reaction center (DRC) catalyst (FeCo-γ-AlO) comprising iron (Fe) and cobalt (Co) for the decomplexation and mineralization of heavy metal complex Ni-EDTA in this study. Compared to the catalysts doped solely with Fe or Co, the bimetal-doped catalyst offered several advantages, including enhanced electron cloud polarization distribution, additional electron transfer pathway, and improved capacity of free radical generation. Through DFT calculations and EPR tests, we have elucidated the influences of the catalyst's adsorption toward Ni-EDTA and its decomplexation products on the electron transfer between the pollutant and the catalyst. The competition between the pollutants and HO affects the generation of free radicals in both electron-rich Fe and Co centers as well as electron-deficient Al center. Building on these findings, we have proposed a plausible removal mechanism of Ni-EDTA using the heterogeneous Fenton-like catalyst FeCo-γ-AlO. This study sheds light on the potential of FeCo-γ-AlO as a DRC catalyst and emphasizes the significance of pollutant characteristics in determining the catalyst's performance.
为了增强催化剂表面电子云密度的极化分布,我们引入了一种新型的双金属取代的双反应中心(DRC)催化剂(FeCo-γ-AlO),用于重金属络合物 Ni-EDTA 的解络和矿化。与仅掺杂 Fe 或 Co 的催化剂相比,双金属掺杂催化剂具有几个优点,包括增强的电子云极化分布、额外的电子转移途径和提高的自由基生成能力。通过 DFT 计算和 EPR 测试,我们阐明了催化剂对 Ni-EDTA 及其解络产物的吸附对污染物和催化剂之间电子转移的影响。污染物和 HO 之间的竞争会影响富电子 Fe 和 Co 中心以及缺电子 Al 中心中自由基的生成。在此基础上,我们提出了使用非均相类 Fenton 催化剂 FeCo-γ-AlO 去除 Ni-EDTA 的可能机制。本研究揭示了 FeCo-γ-AlO 作为 DRC 催化剂的潜力,并强调了污染物特性在确定催化剂性能方面的重要性。