Uncovering Original Z Scheme Heterojunctions of COF/MOx (M = Ti, Zn, Zr, Sn, Ce, and Nb) with Ascendant Photocatalytic Selectivity for Virtually 99.9% NO-to-NO3− Oxidation,Advanced Functional Materials

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Uncovering Original Z Scheme Heterojunctions of COF/MOx (M = Ti, Zn, Zr, Sn, Ce, and Nb) with Ascendant Photocatalytic Selectivity for Virtually 99.9% NO-to-NO3− Oxidation
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2023-06-19 , DOI: 10.1002/adfm.202303851
Yujiao Zhang ₁ , Zhao Hu ₁ , Heng Zhang ₁ , Hu Li ₁ , Song Yang ₁

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Novel Covalent organic skeleton/metal oxide (COF/MO_x; M = Ti, Zn, Zr, Sn, Ce, Nb) Z scheme heterojunction is constructed to achieve highly selective oxidation of nitric oxide (NO). Under visible-light irradiation, the optimized COF/TiO₂ (CF/TS0.05) catalyst showed an excellent NO removal rate (64.5%), resulting from the improvement of light absorption performance, the separation efficiency of photoexcited electron-hole pairs, and O₂ activation due to the uniform coating of COF. Meanwhile, the electrons are captured by the adsorbed oxygen to effectively render into superoxide radicals as the main active species, and the corresponding holes are retained at the complex interface due to the hydrophobic COF coating, which extremely reduced the ability of activated water to produce hydroxyl radicals and limited the production of intermediate nitrogen dioxide (NO₂), thereby improving the oxidation selectivity toward nitrate (NO₃⁻) at 99.9% in the Z scheme heterojunction. More importantly, other COF/MO_x catalysts also exhibited superior selectivity and activity, meaning that this scheme is credited with universality. In short, this study reveals that the generation of only one main reactive oxygen species is enhanced by reasonable control of electron-hole pair in the new Z scheme heterojunction to significantly increase photocatalytic performance and selectivity.

中文翻译：

揭示 COF/MOx（M = Ti、Zn、Zr、Sn、Ce 和 Nb）的原始 Z 方案异质结，光催化选择性几乎达到 99.9% NO 至 NO3− 氧化

构建新型共价有机骨架/金属氧化物（COF/MO _{x ；M = Ti、Zn、Zr、Sn、Ce、Nb）Z方案异质结以实现一氧化氮（NO）的高选择性氧化。}在可见光照射下，优化后的COF/TiO ₂ (CF/TS0.05)催化剂表现出优异的NO去除率(64.5%)，这得益于光吸收性能、光生电子空穴对分离效率的提高、由于COF的均匀涂层，O _2活化。同时，电子被吸附的氧捕获，有效地转化为超氧自由基作为主要活性物种，而相应的空穴由于疏水性COF涂层而被保留在复合物界面上，极大地降低了活化水产生羟基的能力自由基并限制了中间体二氧化氮（NO ₂ ）的产生，从而将Z方案异质结中对硝酸盐（NO ₃^- ）的氧化选择性提高到99.9%。更重要的是，其他COF/MO _x催化剂也表现出优异的选择性和活性，这意味着该方案具有普适性。简而言之，这项研究表明，通过合理控制新型Z方案异质结中的电子-空穴对，仅增强一种主要活性氧的产生，从而显着提高光催化性能和选择性。

更新日期：2023-06-19

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