摘要
Herein,a one-step co-pyrolysis protocol was adopted for the first time to prepare a novel pyrogenic carbon-Cu^(0)/Fe_(3)O_(4)heteroatoms (FCBC) in CO_(2)ambiance to discern the roles of each component in PDS activation.During co-pyrolysis,CO_(2)catalyzed formation of reducing gases by biomass which facilitated reductive transformation of Fe^(3+)and Cu^(2+)to Cu^(0)and Fe_(3)O_(4),respectively.According to the analysis,the resulting metal (oxide) catalyzed graphitization of biocharand decomposition of volatile substances resulting in an unprecedented surface area (1240 m^(2)/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 Fe_(3)O_(4)(50%) and Cu^(0)/Fe_(3)O_(4)(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,^(1)O_(2)) pathways.Regarding FCBC,Cu^(0)can continuously react with Fe^(3+)in Fe_(3)O_(4)to generate larger quantities of Fe^(2+),and both Cu^(0)and Fe^(2+)activated PDS to yield sulfate radicals which was quickly converted to hydroxyl radical.Besides,Cu^(0)/Cu^(2+)could complex with PDS to form a metastable complex,which particularly contributed to1O_(2)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.
基金
supported by the National Natural Science Foundation of China (Nos. 41771349, 41977117, 41977085)
Qing-Lan Project of Yangzhou University (2020)
High-level Talent Support Plan of Yangzhou University (2019)
the Key Research and Development Program of Zhejiang Province (No. 2019C02053)
Foreign Expert Recruitment Program of Jiangsu Province (No. BX2020050)。
