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Fine-Tuning Surface Properties of Perovskites via Nanocompositing with Inert Oxide toward Developing Superior Catalysts for Advanced Oxidation

机译：通过与惰性氧化物纳米复合对钙钛矿的表面性质进行微调，以开发用于高级氧化的高级催化剂

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摘要

Cost-effective, stable, and highly efficient heterogeneous catalyst is the key challenge for wastewater treatment based on Fenton-like advanced oxidation processes. Perovskite oxides offer new opportunities because of their versatile compositions and flexible physiochemical properties. Herein, a new strategy is proposed that is different from the frequently used alien-metal doping, to tune surface properties of perovskite oxides by nanocompositing perovskite with inert oxide, resulting in improved activity and stability for catalytic oxidation. By in situ modification of LaFeO3 with inert La2O3 oxide through one-pot synthesis, several important surface properties such as surface defects, H2O2 adsorption capacity, Fe2+ concentration, and charge-transfer rate were improved, as well as resistance against iron leaching. In performance evaluation, among the various materials, La1.15FeO3 (L1.15FO) composite shows the highest Fenton activity (0.0402 min(-1)) for activating H2O2 to oxidize methyl orange, 2.5 times that of the pristine LaFeO3. Notably, in situ electron paramagnetic resonance analysis and radical scavenging tests unveil a faster generation of singlet oxygen as the dominant reactive species over L1.15FO, consequently a novel non-radical activation mechanism is proposed. Such improved performance is assigned to the strong coupling effect between the nanosized LaFeO3 and La2O3 in the hybrids, which fine-tune the surface properties of LaFeO3 perovskite as superior Fenton catalysts.
机译：具有成本效益，稳定和高效的非均相催化剂是基于类似Fenton的高级氧化工艺的废水处理的主要挑战。钙钛矿氧化物因其多功能的组成和灵活的理化特性而提供了新的机会。在此，提出了一种新的策略，该策略不同于经常使用的外来金属掺杂，其通过将钙钛矿与惰性氧化物纳米复合来调节钙钛矿氧化物的表面性质，从而提高了催化氧化的活性和稳定性。通过一锅法合成用惰性La2O3氧化物原位修饰LaFeO3，改善了一些重要的表面性能，例如表面缺陷，H2O2吸附容量，Fe2 +浓度和电荷转移速率，以及抗铁浸出性。在性能评估中，在各种材料中，La1.15FeO3（L1.15FO）复合材料显示出最高的Fenton活性（0.0402 min（-1）），用于活化H2O2氧化甲基橙，是原始LaFeO3的2.5倍。值得注意的是，原位电子顺磁共振分析和自由基清除测试揭示了单线态氧比L1.15FO更快地生成为主要反应性物种，因此，提出了一种新颖的非自由基活化机理。这种改善的性能归因于纳米LaFeO3和La2O3在杂化物中的强耦合作用，从而微调了LaFeO3钙钛矿作为卓越的Fenton催化剂的表面性能。

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  • 来源
    《Advanced Functional Materials》 |2018年第44期|1804654.1-1804654.12|共12页
  • 作者

    Li Jiang; Miao Jie; Duan Xiaoguang; Dai Jie; Liu Qiwei; Wang Shaobin; Zhou Wei; Shao Zongping;

  • 作者单位

    Nanjing Tech Univ, Coll Chem Engn, State Key Lab Mat Oriented Chem Engn, Nanjing 210009, Jiangsu, Peoples R China;

    Nanjing Tech Univ, Coll Chem Engn, State Key Lab Mat Oriented Chem Engn, Nanjing 210009, Jiangsu, Peoples R China;

    Curtin Univ, Dept Chem Engn, Perth, WA 6845, Australia;

    Nanjing Tech Univ, Coll Chem Engn, State Key Lab Mat Oriented Chem Engn, Nanjing 210009, Jiangsu, Peoples R China;

    Nanjing Tech Univ, Coll Chem Engn, State Key Lab Mat Oriented Chem Engn, Nanjing 210009, Jiangsu, Peoples R China;

    Curtin Univ, Dept Chem Engn, Perth, WA 6845, Australia;

    Nanjing Tech Univ, Coll Chem Engn, State Key Lab Mat Oriented Chem Engn, Nanjing 210009, Jiangsu, Peoples R China;

    Nanjing Tech Univ, Coll Chem Engn, State Key Lab Mat Oriented Chem Engn, Nanjing 210009, Jiangsu, Peoples R China;

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  • 正文语种 eng
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  • 关键词

    advanced oxidation; Fenton-like reaction; nanocompositing; perovskite; singlet oxygen;

    机译：高级氧化;芬顿样反应;纳米复合;钙钛矿;单氧;

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