<br>La2O3 的球磨可调整晶体结构、活性氧以及自由基和非自由基光催化途径,ACS Applied Materials & Interfaces

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La2O3 的球磨可调整晶体结构、活性氧以及自由基和非自由基光催化途径
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2024-04-09 , DOI: 10.1021/acsami.3c15677
Xuewen Luo _{1,

2} , Lei Xu _{1,

2} , Leba Yang _{1,

2} , Jiawen Zhao _{1,

2} , Tewodros Asefa ₃ , Rongliang Qiu _{1,

2} , Zhujian Huang _{1,

2}

Affiliation

使用金属氧化物催化剂的非自由基光催化是一种重要的高级氧化过程，可以去除各种新兴的环境污染物，例如四环素。本文合成了四种具有不同氧空位密度和晶体特征的六方La ₂ O ₃光催化剂，然后通过球磨进一步处理。发现这些La ₂ O ₃光催化剂的球磨增加了其表面上的氧空位的量，从而增加了它们产生的¹ O ₂物质的量。这些La ₂ O ₃光催化剂对TC的光催化降解取决于其上存在的氧空位。此外，具有强 (101) 衍射峰的物质主要通过¹ O ₂和^OH物质从水系统中去除四环素，而具有弱 (101) 衍射峰的物质主要通过¹ O ₂和直接电子转移 (DET) 来去除四环素。）过程。还通过密度泛函理论计算研究了它们的总体催化性能。此外，发现通过含有强(101)衍射峰的La ₂ O ₃光催化剂由四环素产生的有机产物比由含有弱(101)衍射峰的La ₂ O ₃光催化剂产生的有机产物毒性更低。这项研究还提供了令人信服的证据，证明 La ₂ O ₃的结构决定了其产生的物种，并最终介导光催化反应途径（即，自由基与非自由基）来降解新兴的环境污染物。

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Ball Milling of La2O3 Tailors the Crystal Structure, Reactive Oxygen Species, and Free Radical and Non-Free Radical Photocatalytic Pathways

Non-free radical photocatalysis with metal oxide catalysts is an important advanced oxidation process that enables the removal of various emerging environmental pollutants, such as tetracycline. Here, four hexagonal La₂O₃ photocatalysts with different densities of oxygen vacancy and crystalline features are synthesized and then further treated by ball milling. Ball milling of these La₂O₃ photocatalysts is found to increase the amount of oxygen vacancies on their surfaces and thereby the amount of ¹O₂ species produced by them. The photocatalytic degradation of TC by these La₂O₃ photocatalysts depends on the oxygen vacancies present on them. Furthermore, the ones with a strong (101) diffraction peak remove tetracycline from water systems largely with ¹O₂ and ^•OH species, whereas those with a weak (101) diffraction peak do so mainly via ¹O₂ and direct electron transfer (DET) process. Their overall catalytic properties are also studied by density functional theory calculations. Moreover, the organic products produced from tetracycline by La₂O₃ photocatalysts containing a strong (101) diffraction peak are found to be less toxic than those produced by La₂O₃ photocatalysts containing a weak (101) diffraction peak. This study also provides convincing evidence that the structures of La₂O₃ determine the species that is produced by it and that end up mediating photocatalytic reaction pathways (i.e., free radical versus non-free radical) to degrade an emerging environment pollutant.

更新日期：2024-04-09

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