Oxygen-Deficient Zirconia (ZrO2-x): A New Material for Solar Light Absorption.

Oxygen-Deficient Zirconia (ZrO2-x): A New Material for Solar Light Absorption.
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DOI:
10.1038/srep27218
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发表时间:
2016-06-06
期刊:
影响因子:
4.6
通讯作者:
Yu JS
Yu JS
中科院分区:
综合性期刊3区
文献类型:
--
作者:
Sinhamahapatra A;Jeon JP;Kang J;Han B;Yu JS

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在这里,我们提出了缺氧黑色ZrO2−x作为一种新的材料,具有约1.5 eV的低带隙,通过控制镁热还原5% H2/Ar的白色ZrO2,宽带隙(~5 eV)半导体,通常不被考虑用于太阳能光吸收。这是第一次表明,在白色ZrO2失效的情况下,太阳能光吸收率显著增加,甲醇-水的太阳能光诱导制氢活性显著,稳定性可达30天。通过对黑色ZrO2−x的XPS和DFT计算表明,在价带和导带附近形成新的能态,导致黑色ZrO2−x的光学性质发生剧烈变化,主要原因是在HR-TEM和HR-SEM图像上可以清楚地看到大量氧空位或表面缺陷的产生。目前使用Mg和H2还原法制备太阳光辅助光催化活性黑色ZrO2−x的方法温和,但效率高。
Here, we present oxygen-deficient black ZrO2−x as a new material for sunlight absorption with a low band gap around ~1.5 eV, via a controlled magnesiothermic reduction in 5% H2/Ar from white ZrO2, a wide bandgap(~5 eV) semiconductor, usually not considered for solar light absorption. It shows for the first time a dramatic increase in solar light absorbance and significant activity for solar light-induced H2 production from methanol-water with excellent stability up to 30 days while white ZrO2 fails. Generation of large amounts of oxygen vacancies or surface defects clearly visualized by the HR-TEM and HR-SEM images is the main reason for the drastic alteration of the optical properties through the formation of new energy states near valence band and conduction band towards Fermi level in black ZrO2−x as indicated by XPS and DFT calculations of black ZrO2−x. Current reduction method using Mg and H2 is mild, but highly efficient to produce solar light-assisted photocatalytically active black ZrO2−x.