Highly Ordered Nitrogen-Rich Mesoporous Carbon Nitrides and Their Superior Performance for Sensing and Photocatalytic Hydrogen Generation

Highly Ordered Nitrogen-Rich Mesoporous Carbon Nitrides and Their Superior Performance for Sensing and Photocatalytic Hydrogen Generation
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DOI:
10.1002/anie.201702386
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发表时间:
2017-07-10
影响因子:
16.6
通讯作者:
Vinu, Ajayan
Vinu, Ajayan
中科院分区:
化学1区
文献类型:
--
作者:
Mane, Gurudas P.;Talapaneni, Siddulu N.;Vinu, Ajayan

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介孔氮化碳(MCN)具有独特的半导体和基本性能,在光催化和传感等许多应用中都很有用。大多数MCN的合成都集中在利用基于三嗪的前驱体采用纳米硬模板方法制备理论上预测的带隙为2.7 eV的C3N4化学测量。然而,MCN在半导体应用中的性能仅限于具有小带隙的MCN框架,这将与在CN框架中添加更多的N有关,但这仍然是一个巨大的挑战。在这里,我们报道了一种高氮含量的前体,3-氨基-1,2,4-三唑,它可以形成新的和有序的三维MCN,具有C3N5化学计量(MCN-8),这是迄今为止尚未预测的,并且具有低带隙能量(2.2 eV)。这种新型材料在不添加任何掺杂剂的情况下,不仅在可见光照射下具有801 mmol h -2的优异光催化水解性能,而且对有毒酸具有优异的传感性能。
Mesoporous carbon nitrides (MCN) are fascinating materials with unique semiconducting and basic properties that are useful in many applications including photocatalysis and sensing. Most syntheses of MCN focus on creating theoretically predicted C3N4 stoichiometry with a band gap of 2.7 eV using a nano-hard templating approach with triazine-based precursors. However, the performance of the MCN in semiconducting applications is limited to the MCN framework with a small band gap, which would be linked with the addition of more N in the CN framework, but this remains a huge challenge. Here, we report a precursor with high nitrogen content, 3-amino-1,2,4- triazole, that enables the formation of new and wellordered 3D MCN with C3N5 stoichiometry (MCN-8), which has not been predicted so far, and a low-band-gap energy (2.2 eV). This novel class of material without addition of any dopants shows not only a superior photocatalytic water-splitting performance with a total of 801 mmol of H-2 under visible-light irradiation for 3 h but also excellent sensing properties for toxic acids.