One-step preparation of a novel graphitic biochar/Cu0/Fe3O4 composite using CO2-ambiance pyrolysis to activate peroxydisulfate for dye degradation
2023
Yuan, Yangfan | Zhang, Changai | Zhao, Chenhao | Wang, Bing | Wang, Xiaozhi | Gao, Bin | Wang, Shengsen | Rinklebe, Jörg
Herein, a one-step co-pyrolysis protocol was adopted for the first time to prepare a novel pyrogenic carbon-Cu⁰/Fe₃O₄ heteroatoms (FCBC) in CO₂ ambiance to discern the roles of each component in PDS activation. During co-pyrolysis, CO₂ catalyzed formation of reducing gases by biomass which facilitated reductive transformation of Fe³⁺ and Cu²⁺ to Cu⁰ and Fe₃O₄, respectively. According to the analysis, the resulting metal (oxide) catalyzed graphitization of biocharand decomposition of volatile substances resulting in an unprecedented surface area (1240 m²/g). The resulting FCBC showed greater structural defects and less electrical impedance. Batch experiments indicated that Rhodamine B (RhB) degradation by FCBC (100%) was superior to Fe₃O₄ (50%) and Cu⁰/Fe₃O₄ (76.4%) in persulfate (PDS) system, which maintained reasonable efficiency (75.6%-63.6%) within three cycles. The reactive oxygen species (ROS) associated with RhB degradation was identified by an electron paramagnetic resonance and confirmed by scavenging experiments. RhB degradation invoked both (sulfate and dominantly hydroxyl) radical and non-radical (singlet oxygen, ¹O₂) pathways. Regarding FCBC, Cu⁰ can continuously react with Fe³⁺ in Fe₃O₄ to generate larger quantities of Fe²⁺, and both Cu⁰ and Fe²⁺ activated PDS to yield sulfate radicals which was quickly converted to hydroxyl radical. Besides, Cu⁰/Cu²⁺ could complex with PDS to form a metastable complex, which particularly contributed to ¹O₂ generation. These cascade reactions by FCBC were reinforced by carbonyl group of biochar and favorable electron transfer ability. This work highlighted a new approach to prepare a magnetic and environment-benign heterogonous catalyst to remove organic pollutants in water.
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