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Visible light-driven photocatalytically active g-C3N4 material for enhanced generation of H2O2
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2018-03-12 , DOI: 10.1016/j.apcatb.2018.03.035
Zedong Zhu , Honghui Pan , Muthu Murugananthan , Jianyu Gong , Yanrong Zhang

Reduced g-C3N4 material was prepared by a thermal treatment of g-C3N4 in presence of NaBH4 under N2 atmosphere. The prepared catalyst material was characterized by using elemental analyzer, FTIR and XPS and the analysis showed that the reduction treatment created nitrogen vacancies followed by a formation of functional group CN owing to a break-up reaction in the pyridine nitride of a s-triazine-C3N4. The findings of UV–vis DRS and DFT calculation revealed that the formed functional group CN results in a narrowed energy band gap owing to positive shift in the conduction band as well as valence band. The downshift observed in the valence band level made the catalyst material with a feature of visible light-driven water oxidation capacity, that was confirmed by the electron and hole sacrifice and OH trapping-EPR techniques. The intermediate energy level within the band gap of g-C3N4 originated from the vacancies caused an extended absorption, especially to the visible region. The analysis of PL emission spectrum confirmed that the reduction treatment could facilitate the spatial separation of photo-excited electron and hole, and enhance the charge transfer as well. RDE studies showed that the selective production of H2O2 by two-electron reduction of O2 was a predominant reaction step using the reduced g-C3N4. The reduced g-C3N4 prepared at 370 °C exhibited an efficient visible light driven catalytic performance on H2O2 production (170 μmol/L h−1) from pure H2O and O2 at ambient atmosphere in the absence of organic electron donors. The solar-to-H2O2 chemical conversion efficiency and apparent quantum yield approached to ∼0.26%, ∼4.3%, respectively. In addition, the experimental results obtained on recycling of the prepared g-C3N4 evidenced the photocatalytic stability of the material.



中文翻译:

可见光驱动的光催化活性gC 3 N 4材料,用于增强H 2 O 2的产生

降低GC 3 Ñ 4材料通过利用GC进行热处理制备3 Ñ 4中的NaBH存在4氮气氛下2气氛。使用元素分析仪,FTIR和XPS对制得的催化剂材料进行了表征,分析表明,还原处理产生了氮空位,随后由于s-三嗪的吡啶氮化物中的分解反应而形成了官能团C N。 -C 3 N 4。UV-vis DRS和DFT计算的结果表明,形成的官能团C由于导带和价带的正向偏移,N导致能带隙变窄。在价带水平上观察到的下降使催化剂材料具有可见光驱动的水氧化能力,这一点已通过电子和空穴牺牲以及OH捕集-EPR技术得到了证实。gC 3 N 4的带隙内的中间能级由空位引起,引起了吸收的扩展,尤其是到可见光区域的吸收。PL发射光谱的分析证实,还原处理可以促进光激发电子和空穴的空间分离,并且还增强电荷转移。RDE研究表明H 2 O 2的选择性产生O 2的两电子还原反应是使用还原后的gC 3 N 4的主要反应步骤。在370°C下制备的还原gC 3 N 4表现出有效的可见光驱动的催化性能,该反应性能是在环境气氛下,在不存在有机物的情况下,由纯H 2 O和O 2产生H 2 O 2(170μmol/ L h -1)的过程。电子供体。太阳到H 2 O 2的化学转化效率和表观量子产率分别达到〜0.26%,〜4.3%。此外,回收制得的gC 3的实验结果N 4证明了该材料的光催化稳定性。

更新日期:2018-03-12
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