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Unravelling the water oxidation mechanism on NaTaO3-based photocatalysts
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2020/03/12 , DOI: 10.1039/c9ta14235e Qian Ding 1, 2, 3, 4, 5 , Yang Liu 1, 2, 3, 4, 5 , Tao Chen 1, 2, 3, 4, 5 , Xiaoyu Wang 6, 7, 8, 9 , Zhaochi Feng 1, 2, 3, 4, 5 , Xiuli Wang 1, 2, 3, 4, 5 , Michel Dupuis 6, 7, 8, 9 , Can Li 1, 2, 3, 4, 5
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2020/03/12 , DOI: 10.1039/c9ta14235e Qian Ding 1, 2, 3, 4, 5 , Yang Liu 1, 2, 3, 4, 5 , Tao Chen 1, 2, 3, 4, 5 , Xiaoyu Wang 6, 7, 8, 9 , Zhaochi Feng 1, 2, 3, 4, 5 , Xiuli Wang 1, 2, 3, 4, 5 , Michel Dupuis 6, 7, 8, 9 , Can Li 1, 2, 3, 4, 5
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Understanding the detailed kinetics and mechanisms of water oxidation is crucial because water oxidation is the bottleneck reaction in overall water splitting. Here, we investigated photocatalytic water oxidation on NaTaO3-based photocatalysts. With in situ FT-IR spectroscopy, two new water oxidation intermediates with IR absorption peaks centered at 1058 and 935 cm−1 were observed and assigned to Ta(VI)![[double bond, length as m-dash]](https://www.rsc.org/images/entities/char_e001.gif)
O and Ta(O2) peroxo species, respectively. With H218O as the reactant and NaTa16O3 as the photocatalyst, both 16O18O and 18O2 were evolved continuously from overall water splitting as analyzed by mass spectroscopy (MS), demonstrating that the lattice O atoms in NaTaO3-based photocatalysts participate in the formation of O2 during the reaction. DFT results are consistent with the formation of TaO, 16O18O and 18O18O intermediates and products, while predicting that several water oxidation pathways are thermodynamically accessible for water oxidation on NaTaO3. Based on these observations, we propose a three-step two-site mechanism for photocatalytic water oxidation on NaTaO3-based photocatalysts in which lattice oxygen plays a key role. The elucidation of the present mechanism should help in broadly understanding water oxidation on semiconductor-based photocatalysts.
中文翻译：
阐明NaTaO3基光催化剂的水氧化机理
了解水氧化的详细动力学和机理至关重要，因为水氧化是整个水分解过程中的瓶颈反应。在这里，我们研究了基于NaTaO 3的光催化剂上的光催化水氧化。使用原位FT-IR光谱，观察到两个新的水氧化中间体，其IR吸收峰集中在1058和935 cm -1处，分别分配给过氧化Ta（VI）O和Ta（O 2）物种。以H 2 18 O为反应物，NaTa 16 O 3为光催化剂，两者均为16 O 18 O和18 O如通过质谱法（MS）分析的，从总的水分解连续地演化出2个，表明基于NaTaO 3的光催化剂中的晶格O原子在反应期间参与O 2的形成。DFT结果与TaO， 16 O 18 O和18 O 18 O中间体和产物的形成相一致，同时预测NaTaO 3上水氧化的热氧化途径是热力学可及的。基于这些观察，我们提出了NaTaO 3上光催化水氧化的三步两点机理。基光催化剂，其中晶格氧起关键作用。对本机制的阐明应有助于广泛地理解基于半导体的光催化剂上的水氧化。
更新日期：2020-04-08
O and Ta(O2) peroxo species, respectively. With H218O as the reactant and NaTa16O3 as the photocatalyst, both 16O18O and 18O2 were evolved continuously from overall water splitting as analyzed by mass spectroscopy (MS), demonstrating that the lattice O atoms in NaTaO3-based photocatalysts participate in the formation of O2 during the reaction. DFT results are consistent with the formation of TaO, 16O18O and 18O18O intermediates and products, while predicting that several water oxidation pathways are thermodynamically accessible for water oxidation on NaTaO3. Based on these observations, we propose a three-step two-site mechanism for photocatalytic water oxidation on NaTaO3-based photocatalysts in which lattice oxygen plays a key role. The elucidation of the present mechanism should help in broadly understanding water oxidation on semiconductor-based photocatalysts.
中文翻译：
阐明NaTaO3基光催化剂的水氧化机理
了解水氧化的详细动力学和机理至关重要，因为水氧化是整个水分解过程中的瓶颈反应。在这里，我们研究了基于NaTaO 3的光催化剂上的光催化水氧化。使用原位FT-IR光谱，观察到两个新的水氧化中间体，其IR吸收峰集中在1058和935 cm -1处，分别分配给过氧化Ta（VI）
O和Ta（O 2）物种。以H 2 18 O为反应物，NaTa 16 O 3为光催化剂，两者均为16 O 18 O和18 O如通过质谱法（MS）分析的，从总的水分解连续地演化出2个，表明基于NaTaO 3的光催化剂中的晶格O原子在反应期间参与O 2的形成。DFT结果与TaO， 16 O 18 O和18 O 18 O中间体和产物的形成相一致，同时预测NaTaO 3上水氧化的热氧化途径是热力学可及的。基于这些观察，我们提出了NaTaO 3上光催化水氧化的三步两点机理。基光催化剂，其中晶格氧起关键作用。对本机制的阐明应有助于广泛地理解基于半导体的光催化剂上的水氧化。
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