Bandgap engineering of ultrathin graphene-like carbon nitride nanosheets with controllable oxygenous functionalization

Bandgap engineering of ultrathin graphene-like carbon nitride nanosheets with controllable oxygenous functionalization
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具有可控含氧功能化的超薄石墨烯类氮化碳纳米片的带隙工程

DOI:
10.1016/j.carbon.2016.11.030
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发表时间:
2017-03
期刊:
影响因子:
10.9
通讯作者:
Guoxiu Wang
Guoxiu Wang
中科院分区:
材料科学2区
文献类型:
--
作者:
Zhenyuan Teng;Hongying Lv;Chengyin Wang;Huaiguo Xue;Huan Pang;Guoxiu Wang

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寻找有效的带隙工程方法以增加载流子寿命是设计半导体光电子器件和光催化系统的关键。超薄类石墨烯氮化碳纳米片在光催化方面具有广阔的应用前景,但目前还没有广泛调节其带隙的制备策略。本文首次采用改进的hummer方法,结合浓硫酸质子化和高锰酸钾辅助剥离、水合肼还原,实现了可控氧功能化(相对质量比为0.523% ~ 19.9%)的超薄二维氮化碳纳米片的高产率合成。本文首次在分子水平上阐述了不同酸处理大块g- c3n4时的质子化和插层行为。研究首次发现,引入氧基可以将类石墨烯氮化碳纳米片的带隙从2.54 eV调节到3.07 eV,并显著提高了光载流子的寿命。我们的研究可能为各种氮化碳纳米复合材料的设计和构建开辟新的前景,并为其他二维功能材料的带隙工程提供详细的指导,以获得更广泛的应用。
Seeking effective approaches of bandgap engineering with increased carrier lifetime is critical for designing semiconductor photoelectronic devices and photocatalysis systems. Ultrathin graphene-like carbon nitride nanosheets have shown promising prospect in photocatalysis, whereas no preparation strategy for adjusting their bandgap in a wide range has ever been reported. Here in, high yield-rate synthesis of ultrathin two-dimensional carbon nitride nanosheets with controllable oxygenous functionalization (the relative mass ratio of oxygen ranges from 0.523% to 19.9%) was firstly achieved by an improved hummer's method combining concentrated sulfuric acid protonation and potassium permanganate assisted exfoliation, and reduction employing hydrazine hydrate. Protonation and intercalation behavior of different acids in the treatment of bulk-g-C3N4was elaborated at molecule level for the first time. Introduced oxygenous groups are firstly found to have the capability for adjusting the bandgap of graphene-like carbon nitride nanosheets from 2.54 eV to 3.07 eV and significantly increased the lifetime of the photo carriers. Our strategy may open a new vista for design and construction of various carbon nitride nanocomposites and give detailed instructions in bandgap engineering of other two-dimensional functional materials for wider applications.
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