School of Environmental Science and Engineering, Tianjin University/Tianjin Key Lab of Biomass/Wastes Utilization, Tianjin 300072, China.
School of Environmental Science and Engineering, Tianjin University/Tianjin Key Lab of Biomass/Wastes Utilization, Tianjin 300072, China; School of Mechanical Engineering, Tianjin University of Commerce, Tianjin 300134, China.
J Colloid Interface Sci. 2022 Feb 15;608(Pt 2):1983-1998. doi: 10.1016/j.jcis.2021.10.150. Epub 2021 Oct 30.
Active sites on catalyst surface play significant roles in oxidative species formation. The work focused on the regulation of main active sites on catalyst surface and oxidative species formation. Herein, sewage sludge (SS)-red mud (RM) complex biochar (SRCB) and N-functionalized SRCB (NSRCB) were served as activators of peroxymonosulfate (PMS) for sulfanilamide (SMX) degradation. Specially, NSRCB-1 showed excellent catalytic performance with 97.5% removal of SMX within 110 min. Additionally, the effects of N incorporation on the reconstruction of N species, conversion of intrinsic Fe species and ketonic CO groups in SRCB were studied systematically. Both radical (hydroxyl radicals (OH), sulfate radicals (SO) and superoxide radical (O)) and non-radical (electron transfer and singlet oxygen (O)) pathways were confirmed by quenching experiments, electron paramagnetic resonance (EPR) testing and electrochemical measurements. Ketonic CO groups, pyridinic N and pyrrolic N were responsible for non-radical pathway in SMX degradation process. Besides, Fe(II) modulated by N-doping was the main actives site for radicals generation. The contribution of active sites on catalyst surface to oxidative species formation provided fundamental basis for practical water treatment in PMS process.
催化剂表面的活性位在氧化物种的形成中起着重要作用。这项工作集中于调节催化剂表面的主要活性位和氧化物种的形成。在此,污水污泥(SS)-赤泥(RM)复合生物炭(SRCB)和 N 功能化 SRCB(NSRCB)被用作过一硫酸盐(PMS)的活化剂,用于磺胺甲恶唑(SMX)的降解。特别是,NSRCB-1 表现出优异的催化性能,在 110 分钟内可去除 97.5%的 SMX。此外,还系统研究了 N 掺入对 SRCB 中 N 物种的重构、内在 Fe 物种的转化和酮羰基的影响。通过猝灭实验、电子顺磁共振(EPR)测试和电化学测量证实了自由基(羟基自由基(OH)、硫酸根自由基(SO)和超氧自由基(O))和非自由基(电子转移和单线态氧(O))途径。酮羰基、吡啶 N 和吡咯 N 是 SMX 降解过程中非自由基途径的主要作用位点。此外,N 掺杂调节的 Fe(II)是产生自由基的主要活性位。催化剂表面的活性位对氧化物种形成的贡献为 PMS 工艺在实际水处理中的应用提供了基础。