Nitrogen and sulfur co-doped CeO2 nanorods for efficient photocatalytic VOCs degradation

Nitrogen and sulfur co-doped CeO2 nanorods for efficient photocatalytic VOCs degradation
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氮硫共掺杂CeO2纳米棒可有效光催化降解VOCs

DOI:
10.1039/d2cy00934j
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发表时间:
2022
影响因子:
5
通讯作者:
T.
T.
中科院分区:
化学2区
文献类型:
--
作者:
Yang;H.;Jia;L.;Haraguchi;J.;Wang;Y.;Xu;B.;Zhang;Q.;Nan;Z.;Zhang;M.;Ohno;T.

文献摘要

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二氧化铈及其衍生物是一种环境友好型、可持续发展的光催化剂,具有很强的氧储存/释放能力、良好的光稳定性和较高的成本效益。本文成功制备了具有规则纳米棒形貌的氮硫同步掺杂氧化铈(NS-CeO2),该掺杂仅由一个前驱体一步煅烧处理即可获得。乙醛在NS-CeO2上的光氧化性能明显优于未掺杂的氧化铈。密度泛函理论(DFT)计算证实,氮和硫掺杂后,暴露在表面的氧原子被部分取代,导致在费米能级附近产生新的杂质能级,NS-CeO2的带隙减小。同时,氧空位浓度的增加形成了掺杂过渡态,可以作为有效的电子捕获中心。此外,由于这种过渡态有效地限制了电子与空穴的复合,进一步表现出对界面电荷分离的中介作用,从而进一步提高了NS-CeO2的光催化性能。本文提出了一种合成可降解挥发性有机化合物的非金属掺杂ceo2基半导体光催化剂的有效策略。
Ceria and its derivatives are environmentally-friendly and sustainable photocatalysts with a strong oxygen storage/release ability, good photostability, and high cost-effectiveness. In this work, nitrogen and sulfur synchronously doped ceria (NS-CeO2) with a regular nanorod morphology was successfully prepared, in which doping was obtained just from one precursor and by one-step calcination treatment. The photooxidation performance of acetaldehyde on NS-CeO2 was significantly better than that on undoped ceria. As confirmed by density functional theory (DFT) calculations, the oxygen atoms exposed on the surface were partially replaced after doping with nitrogen and sulfur, resulting in the generation of new impurity level states near the Fermi level and reduction of the bandgap of NS-CeO2. Meanwhile, the increased concentration of oxygen vacancies formed a doping transition state which can act as an effective electron capture center. In addition, this transition state further exhibits a mediation role in interfacial charge separation due to its effective restriction of the recombination of electrons and holes, which can further improve the photocatalytic performance of NS-CeO2. Herein, an effective strategy for synthesizing non-metal doped CeO2-based semiconductor photocatalysts that can degrade volatile organic compounds is proposed.