Molecular-Level Understanding of Selectively Photocatalytic Degradation of Ammonia via Copper Ferrite/N-Doped Graphene Catalyst under Visible Near-Infrared Irradiation

Molecular-Level Understanding of Selectively Photocatalytic Degradation of Ammonia via Copper Ferrite/N-Doped Graphene Catalyst under Visible Near-Infrared Irradiation
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可见近红外辐射下铁氧体铜/氮掺杂石墨烯催化剂选择性光催化降解氨的分子水平理解

DOI:
10.3390/catal8100405
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发表时间:
2018-09
期刊:
影响因子:
3.9
通讯作者:
Li Luo
Li Luo
中科院分区:
化学3区
文献类型:
--
作者:
Hang Zhang;Yang Zhou;Shou-Qing Liu;Qin-Qin Gu;Ze-Da Meng;Li Luo

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开发具有分子识别功能的光催化剂在环境领域的特定应用中是非常有趣和期望的。采用表面光电压谱、X射线粉末衍射、透射电镜、拉曼光谱、紫外-可见近红外漫反射光谱和X射线光电子能谱等方法对铜铁氧体/氮掺杂石墨烯(CuFe 2 O 4/NG)复合催化剂进行了表征。CuFe 2 O 4/NG催化剂在可见近红外光照射下,可识别氨-罗丹明B(RhB)混合溶液中的氨,并选择性降解氨。当NH3-N浓度为100.0 mg/L,RhB浓度为50 mg/L时,6 h时NH3-N的降解率达到92.6%,而RhB的降解率仅为39.3%。拉曼光谱和X射线光电子能谱表明,氨吸附在CuFe 2 O 4上,而RhB吸附在NG上。气相色谱法检测氨氧化产物,结果表明光催化氧化过程中有N2生成。机理研究表明,光生电子按照Z-方案构型流向N掺杂石墨烯以还原溶解在溶液中的O2,而光生空穴直接将氨氧化为氮气。
Developing photocatalysts with molecular recognition function is very interesting and desired for specific applications in the environmental field. Copper ferrite/N-doped graphene (CuFe2O4/NG) hybrid catalyst was synthesized and characterized by surface photovoltage spectroscopy, X-ray powder diffraction, transmission electron microscopy, Raman spectroscopy, UV–Vis near-infrared diffuse reflectance spectroscopy and X-ray photoelectron spectroscopy. The CuFe2O4/NG catalyst can recognize ammonia from rhodamine B (RhB) in ammonia-RhB mixed solution and selectively degrade ammonia under visible near-infrared irradiation. The degradation ratio for ammonia reached 92.6% at 6 h while the degradation ratio for RhB was only 39.3% in a mixed solution containing 100.0 mg/L NH3-N and 50 mg/L RhB. Raman spectra and X-ray photoelectron spectra indicated ammonia adsorbed on CuFe2O4 while RhB was adsorbed on NG. The products of oxidized ammonia were detected by gas chromatography, and results showed that N2 was formed during photocatalytic oxidization. Mechanism studies showed that photo-generated electrons flow to N-doped graphene following the Z-scheme configuration to reduce O2 dissolved in solution, while photo-generated holes oxidize directly ammonia to nitrogen gas.
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