Photocatalytic conversion of carbon dioxide into methanol using zinc-copper-M(III) (M = aluminum, gallium) layered double hydroxides

Photocatalytic conversion of carbon dioxide into methanol using zinc-copper-M(III) (M = aluminum, gallium) layered double hydroxides
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DOI:
10.1016/j.jcat.2011.01.004
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发表时间:
2011-04-01
影响因子:
7.3
通讯作者:
Izumi, Yasuo
Izumi, Yasuo
中科院分区:
化学1区
文献类型:
--
作者:
Ahmed, Naveed;Shibata, Yoshiyuki;Izumi, Yasuo

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合成了由锌和/或铜的氢氧化物组成的有序层状双氢氧化物(LDHs),并与铝或镓结合。然后将这些LDH化合物用作光催化剂,以在UV-可见光下使用氢气将气态CO2(2.3kPa)转化为甲醇或CO。Zn-Al LDH对于CO2光还原是最活跃的,并且主要产物是以620 nmol h(-1)g(cat)(-1)的速率形成的CO,而甲醇是通过在LDH光催化剂中包含Cu而形成的主要产物,例如,生成速率为170 nmol h(-1)g(cat)(-1)。当使用Zn-Al(转化率为0.16-0.11%)和Zn-Ga LDH催化剂(转化率为0.02-0.03%)时,通过包含Cu分别从5.9摩尔%和39摩尔%提高到26摩尔%和68摩尔%。特定的相互作用的Cu网站与CO2光谱建议,使耦合与质子和光生电子形成甲醇。(C)2011 Elsevier Inc. All rights reserved.
Ordered layered double hydroxides (LDHs) consisting of zinc and/or copper hydroxides were synthesized and combined with aluminum or gallium. These LDH compounds were then applied as photocatalysts to convert gaseous CO2 (2.3 kPa) to methanol or CO under UV-visible light using hydrogen. Zn-Al LDH was the most active for CO2 photoreduction and the major product was CO formed at a rate of 620 nmol h(-1) g(cat)(-1), whereas methanol was the major product formed by the inclusion of Cu in the LDH photocatalysts, e.g., at a formation rate of 170 nmol h(-1) g(cat)(-1), using Zn-Cu-Ga photocatalyst. The methanol selectivity improved by the inclusion of Cu from 5.9 to 26 mol% and 39 to 68 mol%, respectively, when Zn-Al (the conversion 0.16-0.11%) and Zn-Ga LDH catalysts were used (the conversion 0.02-0.03%). Specific interaction of Cu sites with CO2 was spectroscopically suggested to enable coupling with protons and photogenerated electrons to form methanol. (C) 2011 Elsevier Inc. All rights reserved.