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Bridging the g-C3N4 Interlayers for Enhanced Photocatalysis
ACS Catalysis ( IF 11.3 ) Pub Date : 2016-03-11 00:00:00 , DOI: 10.1021/acscatal.5b02922 Ting Xiong 1 , Wanglai Cen 2 , Yuxin Zhang 3 , Fan Dong 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2016-03-11 00:00:00 , DOI: 10.1021/acscatal.5b02922 Ting Xiong 1 , Wanglai Cen 2 , Yuxin Zhang 3 , Fan Dong 1
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Graphitic carbon nitride (g-C3N4) has been widely investigated and applied in photocatalysis and catalysis, but its performance is still unsatisfactory. Here, we demonstrated that K-doped g-C3N4 with a unique electronic structure possessed highly enhanced visible-light photocatalytic performance for NO removal, which was superior to Na-doped g-C3N4. DFT calculations revealed that K or Na doping can narrow the bandgap of g-C3N4. K atoms, intercalated into the g-C3N4 interlayer via bridging the layers, could decrease the electronic localization and extend the π conjugated system, whereas Na atoms tended to be doped into the CN planes and increased the in-planar electron density. On the basis of theoretical calculation results, we synthesized K-doped g-C3N4 and Na-doped g-C3N4 by a facile thermal polymerization method. Consistent with the theoretical prediction, it was found that K was intercalated into the space between the g-C3N4 layers. The K-intercalated g-C3N4 sample showed increased visible-light absorption, efficient separation of charge carriers, and strong oxidation capability, benefiting from the narrowed band gap, extended π conjugated systems, and positive-shifted valence band position, respectively. Despite that the Na-doped g-C3N4 exhibited narrowed bandgap, the high recombination rate of carriers resulted in the reduced photocatalytic performance. Our discovery provides a promising route to manipulate the photocatalytic activity simply by introducing K atoms in the interlayer and gains a deep understanding of doping chemistry with congeners. The present work could provide new insights into the mechanistic understanding and the design of electronically optimized layered photocatalysts for enhanced solar energy conversion.
中文翻译：
桥接gC 3 N 4中间层以增强光催化作用
石墨碳氮化物（gC 3 N 4）已被广泛研究并应用于光催化和催化，但其性能仍不令人满意。在这里，我们证明了具有独特电子结构的掺K的gC 3 N 4具有显着增强的可见光光催化除NO的性能，这优于掺Na的gC 3 N 4。DFT计算表明，K或Na掺杂可以缩小gC 3 N 4的带隙。K原子，嵌入gC 3 N 4中中间层通过桥接各层，可以降低电子定位并扩展π共轭体系，而Na原子倾向于被掺杂到CN平面中，并增加了平面内电子密度。在理论计算结果的基础上，采用简便的热聚合法合成了掺钾的gC 3 N 4和掺钠的gC 3 N 4。与理论预测一致，发现K插入在gC 3 N 4层之间的空间中。K嵌入的gC 3 N 4样品显示出增加的可见光吸收，有效的电荷载流子分离和强大的氧化能力，分别得益于变窄的带隙，扩展的π共轭体系和价移的价带位置。尽管Na掺杂的gC 3 N 4表现出窄的带隙，但是载流子的高重组率导致光催化性能降低。我们的发现为简单地通过在中间层中引入K原子提供了一种有前途的途径来操纵光催化活性，并获得了对同族元素掺杂化学的深刻理解。本工作可以为机械理解和电子优化分层光催化剂的设计提供新的见解，以提高太阳能的转化率。
更新日期：2016-03-11
中文翻译：
桥接gC 3 N 4中间层以增强光催化作用
石墨碳氮化物（gC 3 N 4）已被广泛研究并应用于光催化和催化，但其性能仍不令人满意。在这里，我们证明了具有独特电子结构的掺K的gC 3 N 4具有显着增强的可见光光催化除NO的性能，这优于掺Na的gC 3 N 4。DFT计算表明，K或Na掺杂可以缩小gC 3 N 4的带隙。K原子，嵌入gC 3 N 4中中间层通过桥接各层，可以降低电子定位并扩展π共轭体系，而Na原子倾向于被掺杂到CN平面中，并增加了平面内电子密度。在理论计算结果的基础上，采用简便的热聚合法合成了掺钾的gC 3 N 4和掺钠的gC 3 N 4。与理论预测一致，发现K插入在gC 3 N 4层之间的空间中。K嵌入的gC 3 N 4样品显示出增加的可见光吸收，有效的电荷载流子分离和强大的氧化能力，分别得益于变窄的带隙，扩展的π共轭体系和价移的价带位置。尽管Na掺杂的gC 3 N 4表现出窄的带隙，但是载流子的高重组率导致光催化性能降低。我们的发现为简单地通过在中间层中引入K原子提供了一种有前途的途径来操纵光催化活性，并获得了对同族元素掺杂化学的深刻理解。本工作可以为机械理解和电子优化分层光催化剂的设计提供新的见解，以提高太阳能的转化率。
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