Hydrothermal synthesis of CuV2O6 supported on mesoporous SiO2 as SO3 decomposition catalysts for solar thermochemical hydrogen production

Hydrothermal synthesis of CuV2O6 supported on mesoporous SiO2 as SO3 decomposition catalysts for solar thermochemical hydrogen production
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DOI:
10.1016/j.ijhydene.2014.06.162
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发表时间:
2014-12
影响因子:
7.2
通讯作者:
T. Kawada;Hiroaki Yamashita;Qingxin Zheng;M. Machida
T. Kawada;Hiroaki Yamashita;Qingxin Zheng;M. Machida
中科院分区:
工程技术2区
文献类型:
--
作者:
T. Kawada;Hiroaki Yamashita;Qingxin Zheng;M. Machida

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研究了以三维有序介孔SiO_2(CuV/SiO_2)为载体的水热合成CuV_2O_6催化剂对太阳能热化学制氢中的关键步骤SO3分解的催化活性。在较低的水热温度(≤200℃)下,生成了复合氧化物水合物Cu3O(V2O7)·H2O和氧化物氢氧化物水合物Cu3(OH)2V2O7·(H2O)2。在600℃空气中焙烧后,氧化物水合物相主要生成Cu2V2O7。相比之下,在250℃(CuV/SiO_2@250)下的水热合成直接从氢氧化物水合物中结晶出CuV_2O_6,尽管其非常大的颗粒(∼5和μm)不适合催化应用。在600℃下测得的SO3分解活性与CuV2O6的产率和分散度有关,在200℃时水热合成活性最高,CuV/SiO_2@250在650℃时催化活性最高,这是因为CuV2O6的熔融相穿透了介孔二氧化硅,从而改善了活性相的分散性。
Hydrothermal synthesis of CuV2O6supported on 3-D ordered mesoporous SiO2(CuV/SiO2) was studied to evaluate the catalytic activity for SO3decomposition, which is a key step in solar thermochemical hydrogen production. A composite oxide hydrate, Cu3O(V2O7)·H2O, and an oxide hydroxide hydrate, Cu3(OH)2V2O7·(H2O)2, were formed at lower hydrothermal temperatures (≤200 °C). The oxide hydrate phase mainly yielded Cu2V2O7after calcination at 600 °C in air. By contrast, the hydrothermal synthesis at 250 °C (CuV/SiO2@250) directly crystallized CuV2O6from the oxide hydroxide hydrate, although its very large particle size (∼5 μm) is not suitable for the catalytic application. The SO3decomposition activity measured at 600 °C was associated with the yield as well as the dispersion of CuV2O6, giving rise to the maximum for the hydrothermal synthesis at 200 °C. CuV/SiO2@250 achieved the highest catalytic activity at the reaction temperature of 650 °C, because the melting phase of CuV2O6penetrated mesoporous SiO2and thus improved the dispersion of the active phase.