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Tubular g-C3N4 Isotype Heterojunction: Enhanced Visible-Light Photocatalytic Activity through Cooperative Manipulation of Oriented Electron and Hole Transfer

机译:管状g C3N4同型异质结:通过定向电子和空穴传输的合作操纵增强的可见光光催化活性。

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摘要

A tubular g-C3N4 isotype heterojunction (TCNH) photocatalyst was designed for cooperative manipulation of the oriented transfer of photogenerated electrons and holes to pursue high catalytic performance. The adduct of cyanuric acid and melamine (CA.M) is first hydrothermally treated to assemble into hexagonal prism crystals; then the hybrid precursors of urea and CA.M crystals are calcined to form tubular g-C3N4 isotype heterojunctions. Upon visible-light irradiation, the photogenerated electrons transfer from g-C3N4 (CA.M) to g-C3N4 (urea) driven by the conduction band offset of 0.05 eV, while the photogenerated holes transfer from g-C3N4 (urea) to g-C3N4 (CA.M) driven by the valence band offset of 0.18 eV, which renders oriented transfer of the charge carriers across the heterojunction interface. Meanwhile, the tubular structure of TCNH is favorable for oriented electron transfer along the longitudinal dimension, which greatly decreases the chance of charge carrier recombination. Consequently, TCNH exhibits a high hydrogen evolution rate of 63 mu mol h(-1) (0.04 g, lambda > 420 nm), which is nearly five times of the pristine g-C3N4 and higher than most of the existing g-C3N4 photocatalysts. This study demonstrates that isotype heterojunction structure and tubular structure can jointly manipulate the oriented transfer of electrons and holes, thus facilitating the visible-light photocatalysis.
机译:设计了管状g-C3N4同型异质结(TCNH)光催化剂,用于协同操纵光生电子和空穴的定向转移,以追求高催化性能。首先对氰尿酸和三聚氰胺的加合物(CA.M)进行水热处理,以组装成六方柱状晶体;然后,对六聚体进行结晶。然后将尿素和CA.M晶体的混合前体煅烧以形成管状g-C3N4同型异质结。在可见光照射下,光生电子在0.05 eV的导带偏移的驱动下从g-C3N4(CA.M)转移到g-C3N4(尿素),而光生空穴从g-C3N4(尿素)转移到g -C3N4(CA.M)由0.18 eV的价带偏移驱动,这使电荷载流子在异质结界面上定向转移。同时,TCNH的管状结构有利于沿纵向方向的定向电子转移,大大降低了电荷载流子复合的机会。因此,TCNH的氢释放速率很高,为63μmol h(-1)(0.04 g,λ> 420 nm),几乎是原始g-C3N4的五倍,并且比大多数现有的g-C3N4光催化剂要高。 。这项研究表明,同型异质结结构和管状结构可以共同操纵电子和空穴的定向转移,从而促进可见光的光催化作用。

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