期刊
CHEMOSPHERE
卷 287, 期 -, 页码 -出版社
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.chemosphere.2021.131933
关键词
Hydrothermal carbons; Ferrihydrite; Graphitization degree; H2O2 consumption; Fe(III)/Fe(II) redox cycling
资金
- National Natural Science Foundation of China [41872044]
- Postdoctoral Innovative Talent Support Program Project [BX20190330]
- China Postdoctoral Science Foundation [2019M663137]
- International Partnership Programme of the International Cooperation Bureau, Chinese Academy of Sciences [132744KYSB20200001_o]
- Science and Technology Planning of Guangdong Province, China [2020B1212060055]
The study found that HTC with abundant carbon-centered persistent free radicals (PFRs) can directly reduce Fe(III) to Fe(II), thereby decreasing Fe(III) consumption of H2O2 and improving the utilization efficiency of H2O2. HTC with low graphitization degree containing more PFRs significantly enhances the Fenton catalytic activity of Fh.
As the heterogeneous Fenton reactions are always restricted by the unsatisfied reduction efficiency of Fe(III) and ineffective consumption of H2O2, many strategies have been developed. In this work, we prepared hydrothermal carbons (HTC) with different graphitization degrees using glucose under different hydrothermal times, and then they were combined with ferrihydrite (Fh). Interestingly, although 30%HTC/Fh has much better BPA degradation efficiency than Fh (26 times larger of calculated degradation rate constants), the decomposition rate of H2O2 in the former system is lower. The generated Fe(II) of HTC/Fh is much higher than that of Fh during the heterogeneous Fenton reactions, and the degradation of BPA is almost unaffected by p-benzoquinone (scavenger of superoxide radicals (O-2(center dot-))) while greatly inhibited by isopropanol (scavenger of hydroxyl radicals (HO center dot)). These results indicate that HTC act as electron donors due to the abundant carbon-centered persistent free radicals (PFRs) to directly reduce Fe(III) to Fe(II) and therefore decrease the H2O2 consumption by Fe(III), which subsequently inhibits the generation of less active O(2)(center dot-)and promote the utilization efficiency of H2O2. HTC with a low graphitization degree contain more PFRs for Fe(III) reducing, significantly enhancing the Fenton catalytic activity of Fh.
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