宽光谱响应范围的氮化碳纳米片的制备及其光催化产氢性能研究

Preparation of carbon nitride nanosheets with wide spectral response range and photocatalytic hydrogen production properties

  • 摘要: 以块体氮化碳 (CN) 为前驱物,采用氧化剥离制备氧化型氮化碳纳米片 (o-CN NSs),将o-CN NSs还原制得了还原型氮化碳纳米片 (r-CN NSs)。o-CN NSs和r-CN NSs厚度均约2 nm,且都保留了纯CN的庚嗪环骨架结构;相比于o-CN NSs,r-CN NSs具有更小的禁带宽度 (2.62 eV)、更宽的光响应范围 (485 nm) 和更高的产氢速率((1700 μmol/(g·h));r-CN NSs的光催化产氢速率是CN的8.5倍、o-CN NSs的2.1倍。经过20 h的循环测试,r-CN NSs的光催化产氢速率没有衰减,具备良好的光催化稳定性。实验和理论分析表明,r-CN NSs是边缘基团为氨基的纳米片结构,氨基的引入改善了纳米片的结晶性,提高了电子和空穴的分离效率、拓宽了纳米片的光响应范围,从而导致光催化性能增强。

     

    Abstract: Oxidized carbon nitride nanosheets (o-CN NSs) was prepared by oxidative stripping with bulk carbon nitride (CN) as the precursor, and then reduced carbon nitride nanosheet (r-CN NSs) was prepared via reduced o-CN NSs. The thickness of o-CN NSs and r-CN NSs are both about 2 nm and retain the heptazine ring skeleton structure of pure CN. Compared with o-CN NSs, r-CN NSs has a smaller band gap (2.62 eV), wider photoresponse range (485 nm) and higher H2 evolution rates (1700 μmol/(g·h)). The H2 evolution rates of r-CN NSs is 8.5 times of CN and 2.1 times of o-CN NSs. After a 20 h cycle test, the photocatalytic hydrogen production efficiency of r-CN NSs has no attenuation, has well photocatalytic stability. Experimental and theoretical analyses reveal that r-CN NSs is nanosheet structure with amino group at the edge. The introduction of amino group improves the crystallinity of nanosheets, improves the separation efficiency of electrons and holes, broadens the photoresponse range of nanosheets, thus resulting in the enhanced photocatalytic performance.

     

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