化学
气凝胶
石墨烯
铀
氧化物
异质结
X射线光电子能谱
光谱学
吸收光谱法
肖特基势垒
光电子学
化学工程
纳米技术
材料科学
光学
有机化学
二极管
物理
量子力学
工程类
冶金
作者
Tao Chen,Pan He,Tong Liu,Li Zhou,Mingxin Li,Kaifu Yu,Qi Meng,Jie Lian,Wenkun Zhu
出处
期刊:Inorganic Chemistry
[American Chemical Society]
日期:2022-08-01
卷期号:61 (32): 12759-12771
被引量:49
标识
DOI:10.1021/acs.inorgchem.2c01850
摘要
Encapsulation of nano-semiconductor materials in three-dimensional (3D) adsorbents to build a typical semiconductor-adsorbent heterostructure is a forward-looking strategy for photo-assisted uranium extraction. Here, we develop 3D MXene-derived TiO2(M)@reduced graphene oxide (RGO) aerogel for photo-assisted uranium extraction. Theoretical simulations demonstrate that oxygen vacancies on TiO2(M) tailor the energy level structure and enhance the electron accumulation at gap states of TiO2(M), thereby further realizing the spatial separation efficiency of electron-hole pairs by the Schottky junction. By virtue of the in situ X-ray photoelectron spectroscopy spectrum, we identify that photogenerated electrons generated over TiO2(M) were transferred to graphene oxide aerogel by the Schottky junction. Accordingly, TiO2 (M)@RGO aerogel presents a considerable removal efficiency for U(VI) with a removal ratio of 95.7%. Relying on the X-ray absorption spectroscopy technique, we distinguish the evolution of 2H2O-2Oax-U-5Oeq into H2O-2Oax-U-3Oeq from dark to light conditions, further confirming the reduction of high-valent uranium. This strategy may open a paradigm for developing novel heterojunctions as photocatalysts for selective U(VI) extraction.
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