第一作者：Ran Gao
通讯作者：洪俊明 教授
通讯单位：华侨大学化工学院
DOI:10.1016/j.seppur.2024.126339
高级氧化工艺广泛使用普鲁士蓝类似物（PBAs）催化剂。然而，金属离子浸出限制了它们在类似芬顿体系中的应用，造成环境污染和长期性能下降。本研究采用共沉淀-煅烧法制备了立方体铁锰双金属 PBA 催化剂。在悬浮流实验中，在最佳条件下，亚甲基蓝（MB）在 90 分钟内的降解率超过 99.92%。基于密度泛函理论（DFT）分析和液相色谱-质谱（LC-MS）结果，提出了铁锰双金属成分的协同效应和甲基溴的降解途径。在回收实验中，金属离子浸出和催化剂结构破坏大大降低了催化剂的活性。为了克服 PBA 材料的金属浸出问题，研究人员构建了一种类似芬顿的连续流系统。将装有铁锰双金属催化剂的棉球与煅烧牡蛎壳固定床反应器相连。在 60 小时的连续进流实验中，废水中甲基溴的平均降解率达到 95.81%，比单催化剂连续进流系统高出 25.42%。实验和表征验证了使用改性牡蛎壳提高反应效果的机理。这种牡蛎壳能有效吸附反应过程中浸出的铁和锰金属离子，这些被吸附的金属离子通过异相芬顿反应进一步促进甲基溴的过一硫酸盐（PMS）氧化，这种反应被称为再芬顿反应。这项研究为 PBA 催化剂在高级氧化过程中的实际应用提供了一种新策略。
Fig. 1. (A) XRD spectra of FFM and FFM-PBA. (B) FTIR spectra of FFM and FFM-PBA. (C) BET curve of FFM-PBA. (D-E) The SEM images of FFM-PBA. (F) The EDS elemental mapping images of FFM-PBA.
Fig. 2. (A) Degradation efficiency of different systems. (B) K value of different systems. (C) Degradation efficiency of different PBA systems. (D) K value of different PBA systems. (E) Effect of catalyst dosage. (F) Effect of PMS dosage. (G) Effect of different initial pH. (H) Effect of different anions. (I) Effect of different water bodies. Conditions: Catalyst = 200 mg•L−1, MB = 10.0 mg•L−1, PMS = 0.2 mM, pH = 7.
Fig. 3. (A) Effect of different quenchers; (B) DMPO-SO4-•, DMPO-OH•; (C) DMPO- •O2–; (D) TMPO-1O2; (E-F) Fe2p spectrum before and after reaction; (G-H) Fe2p spectrum before and after reaction. Conditions: Catalyst = 200 mg•L−1, MB = 10.0 mg•L−1, PMS = 0.2 mM, pH = 7.
Fig. 4. (A) Chemical structure of MB; (B) HOMO of MB; (C) Fukui index distribution of MB.
Fig. 5. (A) Cyclic experiment; (B) The SEM images of used FFM-PBA; (C) Degradation effect of FFM-PBA/PMS system on other pollutants. Conditions: Catalyst = 200 mg•L−1, MB = 10.0 mg•L−1, PMS = 0.2 mM, pH = 7.
Fig. 6. (A) Diagram of fixed bed continuous flow reactor based on FFM-PBA; (B) MB removal efficiency and effluent pH in catalyst/oyster shells/PMS system; (C) MB removal efficiency and effluent pH in only catalyst/PMS system. Conditions: MB = 10 mg•L−1, input flow rate = 500 mL/h, 0.1 mol•L−1 PMS input flow rate = 15 mL/h, pH = 7.
Ran Gao, Zhi Huang, Jielong Xu, Yuwei Xue, Ting Zhang, Qian Zhang, Jiefeng Xiao, Junming Hong, Pollutant degradation by Fenton-like system with Prussian blue analogs (PBAs) on cotton and modified oyster shell: Via re-Fenton reaction, Separation and Purification Technology, 2024, https://doi.org/10.1016/j.seppur.2024.126339
声明：本公众号仅分享前沿学术成果，无商业用途。如涉及侵权，请立刻联系公众号后台或发送邮件，我们将及时修改或删除！
邮箱：Environ2022@163.com
欢迎大家将《水处理文献速递》加为星标
即时获取前沿学术成果
若有帮助，请点击“在看”分享！
投稿、转载请扫描下方二维码联系小编吧
