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Perovskite Oxynitride Solid Solutions of LaTaON2‐CaTaO2N with Greatly Enhanced Photogenerated Charge Separation for Solar‐Driven Overall Water Splitting
Advanced Science ( IF 14.3 ) Pub Date : 2020-11-25 , DOI: 10.1002/advs.202003343
Yawei Wang 1 , Yuyang Kang 2 , Huaze Zhu 2 , Gang Liu 2, 3 , John T S Irvine 4 , Xiaoxiang Xu 1
Affiliation  

The search for solar‐driven photocatalysts for overall water splitting has been actively pursued. Although metal oxynitrides with metal d0/d10‐closed shell configuration are very promising candidates in terms of their visible light absorption, they usually suffer from serious photo‐generated charge recombination and thus, little photoactivity. Here, by forming their solid solutions of LaTaON2 and CaTaO2N, which are traditionally considered to be inorganic yellow‐red pigments but have poor photocatalytic activity, a class of promising solar‐driven photocatalysts La1‐xCaxTaO1+yN2‐y (0 ≤ x, y ≤ 1) are explored. In particular, the optimal photocatalyst with x = 0.9 has the ability of realizing overall water splitting with stoichiometric H2/O2 ratio under the illumination of both AM1.5 simulated solar light and visible light. The modulated key parameters including band structure, Ta bonding environment, defects concentration, and band edge alignments revealed in La0.1Ca0.9TaO1+yN2‐y have substantially promoted the separation of photogenerated charge carriers with sufficient energetics for water oxidation and reduction reactions. The results obtained in this study provide an important candidate for designing efficient solar‐driven photocatalysts for overall water splitting.

中文翻译:


LaTaON2-CaTaO2N 的钙钛矿氮氧化物固溶体具有大大增强的光生电荷分离能力,用于太阳能驱动的整体水分解



人们一直在积极寻找用于整体水分解的太阳能光催化剂。尽管具有金属 d 0 /d 10闭壳结构的金属氮氧化物在可见光吸收方面是非常有前途的候选者,但它们通常会遭受严重的光生电荷复合,因此光活性很低。在此,通过形成LaTaON 2和CaTaO 2 N(传统上被认为是无机黄红色颜料但光催化活性较差)的固溶体,一类有前途的太阳能驱动光催化剂La 1‐ x Ca x TaO 1+y探索 N 2‐ y (0 ≤ x , y ≤ 1)。特别是, x =0.9的最佳光催化剂在AM1.5模拟太阳光和可见光照射下均能够实现化学计量H 2 /O 2比例的整体水分解。 La 0.1 Ca 0.9 TaO 1+ y N 2‐ y中揭示的调制关键参数,包括能带结构、Ta键合环境、缺陷浓度和能带边缘排列,极大地促进了光生电荷载流子的分离,具有足够的能量用于水的氧化和还原反应。本研究获得的结果为设计用于整体水分解的高效太阳能驱动光催化剂提供了重要的候选者。
更新日期:2021-01-20
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