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Infrared Light-Driven CO2 Overall Splitting at Room Temperature
Joule ( IF 39.8 ) Pub Date : 2018-03-20 , DOI: 10.1016/j.joule.2018.02.019
Liang Liang , Xiaodong Li , Yongfu Sun , Yuanlong Tan , Xingchen Jiao , Huanxin Ju , Zeming Qi , Junfa Zhu , Yi Xie

To date, infrared (IR) light constituting almost 50% of the solar energy has never been utilized, owing to an insurmountable contradiction between IR light utilization and CO2 photoreduction. To break through this limitation, we designed an ultrathin intermediate-band semiconductor, and hence first realized IR-driven CO2 overall splitting on a single material without using any sacrificial reductants. Taking the synthetic ultrathin cubic-WO3 layers as an example, theoretical calculations disclose that the created oxygen vacancies reaching a critical density results in an intermediate band, verified by synchrotron-radiation valence-band spectra, photoluminescence spectra, UV-vis-NIR spectra, and synchrotron-radiation IR reflectance spectra. As a result, the oxygen-deficient WO3 atomic layers display IR-driven CO2 overall splitting to CO and O2, while their catalytic activity proceeds without deactivation even after 3 days. Also, the higher oxygen vacancy concentration favors CO2 adsorption and activation into COOH* radical, affirmed by CO2 temperature-programmed desorption spectra and in situ FTIR spectra, hence guaranteeing increased CO and O2 formation rates.



中文翻译:

室温下红外光驱动的CO 2整体分解

迄今为止,由于IR光的利用与CO 2的光还原之间存在无法克服的矛盾,所以几乎没有利用构成太阳能的近50%的红外(IR)光。为了克服此限制,我们设计了超薄中带半导体,因此首先在不使用任何牺牲还原剂的情况下,在单一材料上实现了红外驱动的CO 2整体分解。取合成的超薄立方WO 3以计算层为例,理论计算表明,所产生的氧空位达到临界密度会产生中间带,并通过同步辐射价带光谱,光致发光光谱,UV-vis-NIR光谱和同步辐射IR反射光谱进行验证。结果,缺氧的WO 3原子层显示出IR驱动的CO 2整体分裂成CO和O 2,而它们的催化活性甚至在3天后仍未失活。同样,较高的氧空位浓度有利于CO 2吸附和活化成COOH *自由基,这是由CO 2温度编程的解吸光谱和原位证实的FTIR光谱,从而保证增加的CO和O 2形成速率。

更新日期:2018-03-20
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