The Pivotal Role of Selenium Vacancies in Defective FeSe2@MoO3 for Efficient Peroxymonosulfate Activation: Experimental and DFT Calculation,ACS ES&T Engineering

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The Pivotal Role of Selenium Vacancies in Defective FeSe2@MoO3 for Efficient Peroxymonosulfate Activation: Experimental and DFT Calculation
ACS ES&T Engineering ( IF 7.4 ) Pub Date : 2023-07-19 , DOI: 10.1021/acsestengg.3c00195
Fei Wang _{1,

2} , Ya Gao _{1,

2} , Hongyu Chu _{1,

2} , Yuwei Wei _{1,

2} , Chong-Chen Wang _{1,

2} , Shan-Shan Liu _{1,

2} , Guangchi Liu _{1,

2} , Huifen Fu _{1,

2} , Peng Wang _{1,

2} , Chen Zhao _{1,

2}

Affiliation

The presence of selenium vacancies (V_Se) in metal selenides enables the activation of peroxymonosulfate (PMS) for efficient water purification. However, the mechanisms of interactions of V_Se with PMS and organic pollutant removal are unclear. Hence, we precisely prepared a series of FeSe₂@MoO₃ composites with V_Se for effective activation of PMS for the removal of various organic pollutants. The roles of V_Se are explored via density functional theory (DFT) calculations: (i) regulating the electron distribution of Fe and Mo orbitals in FeSe₂@MoO₃ for enhancing the PMS adsorption and (ii) promoting the conversion of transition metallic redox pairs (Fe³⁺/Fe²⁺ and Mo⁶⁺/Mo⁵⁺/Mo⁴⁺). The as-prepared FeSe₂@MoO₃-8 exhibits excellent catalytic performance via PMS activation in which nearly 100% removal efficiencies of various organic pollutants are achieved within 2–10 min. The quenching experiments, electronic spin resonance (ESR), and probe tests demonstrated that the multiple reactive species like SO₄^•–, O₂^•–, ^•OH, and ¹O₂ contributed to the removal of 2,4-D. Finally, FeSe₂@MoO₃-8 was attached to the polyvinylidene difluoride (PVDF) membrane for continuous and efficient removal of 2,4-D, in which the removal efficiency and total organic carbon removal efficiency of 2,4-D were > 90% and >70% within 12 h of operation.

中文翻译：

缺陷 FeSe2@MoO3 中硒空位对于有效过一硫酸盐活化的关键作用：实验和 DFT 计算

_{金属硒化物中硒空位 (V Se} )的存在能够激活过一硫酸盐 (PMS)，从而有效净化水。_{然而，V Se}与 PMS 和有机污染物去除相互作用的机制尚不清楚。因此，我们精确制备了一系列具有V _Se的FeSe₂ @MoO ₃复合材料，用于有效激活PMS以去除各种有机污染物。通过密度泛函理论（DFT）计算探索了V _Se的作用：（i）调节 FeSe ₂ @MoO ₃中 Fe 和 Mo 轨道的电子分布，以增强 PMS 吸附；（ii）促进过渡金属氧化还原的转化对(Fe ³⁺ /Fe ²⁺和Mo ⁶⁺ /Mo ⁵⁺ /Mo ⁴⁺ )。所制备的 FeSe ₂ @MoO ₃ -8 通过 PMS 活化表现出优异的催化性能，在 2-10 分钟内实现了各种有机污染物近 100% 的去除效率。猝灭实验、电子自旋共振（ESR）和探针测试表明，多种活性物质如SO ₄^•–、O ₂^•–、^• OH 和¹ O ₂有助于去除2,4-D。最后将FeSe ₂ @MoO ₃ -8附着在聚偏二氟乙烯（PVDF）膜上，连续高效去除2,4-D，其中2,4-D去除效率和总有机碳去除效率>运行 12 小时内达到 90% 和> 70%。

更新日期：2023-07-19

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