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Insight into the Role of TiO2 Facets in Photocatalytic Selective Oxidation of p-Xylene
ACS Catalysis ( IF 11.3 ) Pub Date : 2024-03-26 , DOI: 10.1021/acscatal.4c00543
Xiaowen Sun 1, 2 , Zhendong Feng 2, 3 , Shengyang Wang 2 , Qing-Nan Wang 2 , Pengfei Zhang 2 , Rengui Li 2 , Can Li 2, 3
ACS Catalysis ( IF 11.3 ) Pub Date : 2024-03-26 , DOI: 10.1021/acscatal.4c00543
Xiaowen Sun 1, 2 , Zhendong Feng 2, 3 , Shengyang Wang 2 , Qing-Nan Wang 2 , Pengfei Zhang 2 , Rengui Li 2 , Can Li 2, 3
Affiliation
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The crystal facets of semiconductors often have critical effects on photocatalytic reactions. The spatial charge separation between different facets in TiO2 reveals a preferential accumulation of photogenerated holes on the {001} facet; thereby, the activation of the C–H bond predominantly occurs on the {001} facet. However, the dissociative adsorption of initially generated p-methylbenzyl alcohol (p-MBY) forms alcoholate species, which impedes the interaction between p-xylene and the {001} facet, and thus blocks the photocatalytic reaction of p-xylene oxidation on {001}-72%. On the other hand, H3PO4 predominantly adsorbs on the {001} facet, with an adsorption energy higher than p-MBY (−5.15 vs −3.90 eV). Therefore, adding H3PO4 can prevent the dissociative adsorption of p-MBY on the {001} facet. The addition of H3PO4 also significantly improves the injection efficiency of photogenerated holes into p-xylene and suppresses the generation of ·O22–, thereby enhancing the conversion and selectivity. Consequently, the addition of H3PO4 obtains a selectivity as high as 94.8% to the primary products at 15.2% conversion on {001}-72%. The results demonstrate that facet engineering for a semiconductor-based photocatalyst can regulate the charge separation, charge injection, and adsorption behavior of intermediates, which is an effective strategy to accomplish high performance of photocatalytic reactions.
中文翻译：
深入了解 TiO2 面在对二甲苯光催化选择性氧化中的作用
半导体的晶面通常对光催化反应具有关键影响。 TiO 2不同晶面之间的空间电荷分离揭示了光生空穴在{001}晶面上的优先积累；因此，C-H键的激活主要发生在{001}面上。然而，最初生成的对甲基苯甲醇（p -MBY）的解离吸附形成醇化物，阻碍了对二甲苯与{001}面之间的相互作用，从而阻碍了对二甲苯氧化在{001上的光催化反应}-72%。另一方面，H 3 PO 4主要吸附在{001}面上，吸附能高于p -MBY（-5.15 vs -3.90 eV）。因此，添加H 3 PO 4可以防止p -MBY在{001}面上的解离吸附。 H 3 PO 4的添加还显着提高了光生空穴向对二甲苯的注入效率，并抑制·O 2 2–的生成，从而提高了转化率和选择性。因此，添加H 3 PO 4可获得高达94.8%的初级产物选择性，{001}-72%的转化率为15.2%。结果表明，半导体光催化剂的面工程可以调节中间体的电荷分离、电荷注入和吸附行为，这是实现高性能光催化反应的有效策略。
更新日期：2024-03-26
中文翻译：
深入了解 TiO2 面在对二甲苯光催化选择性氧化中的作用
半导体的晶面通常对光催化反应具有关键影响。 TiO 2不同晶面之间的空间电荷分离揭示了光生空穴在{001}晶面上的优先积累；因此，C-H键的激活主要发生在{001}面上。然而，最初生成的对甲基苯甲醇（p -MBY）的解离吸附形成醇化物，阻碍了对二甲苯与{001}面之间的相互作用，从而阻碍了对二甲苯氧化在{001上的光催化反应}-72%。另一方面，H 3 PO 4主要吸附在{001}面上，吸附能高于p -MBY（-5.15 vs -3.90 eV）。因此，添加H 3 PO 4可以防止p -MBY在{001}面上的解离吸附。 H 3 PO 4的添加还显着提高了光生空穴向对二甲苯的注入效率，并抑制·O 2 2–的生成，从而提高了转化率和选择性。因此，添加H 3 PO 4可获得高达94.8%的初级产物选择性，{001}-72%的转化率为15.2%。结果表明，半导体光催化剂的面工程可以调节中间体的电荷分离、电荷注入和吸附行为，这是实现高性能光催化反应的有效策略。
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