Nanocomposites of tantalum-based pyrochlore and indium hydroxide showing high and stable photocatalytic activities for overall water splitting and carbon dioxide reduction.

Nanocomposites of tantalum-based pyrochlore and indium hydroxide showing high and stable photocatalytic activities for overall water splitting and carbon dioxide reduction.
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DOI:
10.1002/anie.201408868
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发表时间:
2014-12
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通讯作者:
M. Hsieh;Guan Wu;Wei-Guang Liu;W. Goddard;Chia‐Min Yang
M. Hsieh;Guan Wu;Wei-Guang Liu;W. Goddard;Chia‐Min Yang
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文献类型:
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作者:
M. Hsieh;Guan Wu;Wei-Guang Liu;W. Goddard;Chia‐Min Yang

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采用水热法制备了钽基烧绿石纳米颗粒和氢氧化铟的纳米复合材料,用于紫外光催化分解水、甲醇光重整制氢、最佳催化剂的总水分解活性是钽酸钠的20倍以上,CO2分解活性是Degussa P25 TiO2的3倍还原此外,该催化剂是非常稳定的,同时产生化学计量的产品H2(或CO)和O2在整个长期的光催化反应。在去除In(OH)3后,烧绿石纳米颗粒对纯水和甲醇水溶液的制氢反应仍具有很高的活性。实验研究和密度泛函理论计算表明,烧绿石纳米颗粒催化水还原产生H2,而In(OH)3是水氧化产生O2的主要活性组分。
Nanocomposites of tantalum-based pyrochlore nanoparticles and indium hydroxide were prepared by a hydrothermal process for UV-driven photocatalytic reactions including overall water splitting, hydrogen production from photoreforming of methanol, and CO2 reduction with water to produce CO. The best catalyst was more than 20 times more active than sodium tantalate in overall water splitting and 3 times more active than Degussa P25 TiO2 in CO2 reduction. Moreover, the catalyst was very stable while generating stoichiometric products of H2 (or CO) and O2 throughout long-term photocatalytic reactions. After the removal of In(OH)3, the pyrochlore nanoparticles remained highly active for H2 production from pure water and aqueous methanol solution. Both experimental studies and density functional theory calculations suggest that the pyrochlore nanoparticles catalyzed the water reduction to produce H2, whereas In(OH)3 was the major active component for water oxidation to produce O2.