Environmental photochemistry in hematite-oxalate system: Fe(III)-Oxalate complex photolysis and ROS generation
Environmental photochemistry in hematite-oxalate system: Fe(III)-Oxalate complex photolysis and ROS generation
复制标题
赤铁矿-草酸盐体系中的环境光化学：Fe(III)-草酸盐络合物光解和ROS生成
DOI：
10.1016/j.apcatb.2020.119645
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发表时间：
2021-04
期刊：
影响因子：
--
通讯作者：
Zhang Lizhi
中科院分区：
文献类型：
--
作者：
Xu Tianyuan;Fang Yumin;Tong Tianyi;Xia Yabei;Liu Xiao;Zhang Lizhi
草酸盐与铁(氢)氧化物一起，通过光化学产生活性氧物种(ROS)，在环境净化中发挥着重要作用。然而，对固-液界面光分解行为的反应机理了解甚少。本文通过络合、光解和ROS生成实验研究了赤铁矿-草酸盐体系的光化学性质。结果表明，在光照作用下，吸附在赤铁矿表面的草酸盐以非还原溶解的方式被分离。然后，Fe(III)-草酸盐络合物在赤铁矿表面或溶液中的光解遵循光解机理，其中每个Fe(III)-草酸盐络合物导致两个CO_2自由基点−的形成。在Fe~(3+)-O_x均相体系中，由光解离机制引起的氧自由基点−/自由基点OOH和自由基点OH量远高于经典的分子内配体-金属电荷转移机制。在赤铁矿-Ox体系中，磺胺(5 mg/L)在2 h内的光降解和矿化率分别达到95%和59%。这些发现有助于利用自然环境中的铁(氢)氧化物和草酸盐进行环境修复。
Oxalates, together with iron (hydr)oxides, play important roles in environmental decontamination by photochemical generation of reactive oxygen species (ROS). However, comprehending reaction mechanism about photolytic behaviors across solid-liquid interface is scarce. Here, the photochemical properties of hematite-oxalate system were investigated from complexation, photolysis, and ROS generation tests. Results implied adsorbed oxalate on hematite surface was detached via non-reductive dissolution by irradiating light. Then, the photolysis of Fe(III)-oxalate complexes on hematite surface or dissolved in solution was followed by photodissociation mechanism, in which per Fe(III)-oxalate complex led to two CO2radical dot−formation. Moreover, O2radical dot−/radical dotOOH andradical dotOH amounts induced by photodissociation mechanism were much higher than that by classic intramolecular ligand-to-metal charge transfer mechanism in Fe3+-Ox homogeneous system. The photo-degradation and mineralization of sulfadimidine (5 mg/L) reached 95 % and 59 % within 2 h using hematite-Ox system. These findings can help in implementing environmental remediation by utilizing iron (hydr)oxides and oxalate in natural environment.
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