Hierarchical Self-assembly of Well-Defined Louver-Like P-Doped Carbon Nitride Nanowire Arrays with Highly Efficient Hydrogen Evolution.
Hierarchical Self-assembly of Well-Defined Louver-Like P-Doped Carbon Nitride Nanowire Arrays with Highly Efficient Hydrogen Evolution.
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具有高效析氢能力的明确百叶窗状磷掺杂碳氮化碳纳米线阵列的分层自组装
DOI：
10.1007/s40820-020-0399-1
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发表时间：
2020-02-17
影响因子：
26.6
通讯作者：
Huang GF
中科院分区：
文献类型：
--
作者：
Li B;Si Y;Fang Q;Shi Y;Huang WQ;Hu W;Pan A;Fan X;Huang GF
自组装纳米结构阵列结合了纳米结构的固有特性以及阵列的稳定性的优点，在先进材料领域具有很大的吸引力。然而，由于均匀成核的普遍发生和非共价相互作用的困难，在没有模板或衬底的情况下，精确地自下而上地合成纳米结构阵列是相当具有挑战性的。在这里，我们首次报道了通过氢键调节非共价相互作用，通过超分子自组装方法精确地合成了定义良好的百叶窗状掺磷氮化碳纳米线阵列(L-PCN)。通过这种策略，CN纳米线在外框内与分离物和空间位置对准，实现了超稳定性和优异的光电性能。值得注意的是，这种自组装的L-PCN表现出了1872.9μ−1g−1的优异的可见光驱动析氢活性，与块体CN相比， ~ 提高了25.6倍，并且具有很高的光稳定性。此外，在420 ± 15 nm处获得了6.93%的表观量子效率。实验结果和第一性原理计算表明，L PCN光催化活性的显著提高可以归因于结构拓扑和掺杂剂的协同作用。这些发现表明，我们能够利用氢键工程设计出具有理想性能的特定层次化纳米结构。
Self-assembled nanostructure arrays integrating the advantages of the intrinsic characters of nanostructure as well as the array stability are appealing in advanced materials. However, the precise bottom-up synthesis of nanostructure arrays without templates or substrates is quite challenging because of the general occurrence of homogeneous nucleation and the difficult manipulation of noncovalent interactions. Herein, we first report the precisely manipulated synthesis of well-defined louver-like P-doped carbon nitride nanowire arrays (L-PCN) via a supramolecular self-assembly method by regulating the noncovalent interactions through hydrogen bond. With this strategy, CN nanowires align in the outer frame with the separation and spatial location achieving ultrastability and outstanding photoelectricity properties. Significantly, this self-assembly L-PCN exhibits a superior visible light-driven hydrogen evolution activity of 1872.9 μmol h−1g−1, rendering a ~ 25.6-fold enhancement compared to bulk CN, and high photostability. Moreover, an apparent quantum efficiency of 6.93% is achieved for hydrogen evolution at 420 ± 15 nm. The experimental results and first-principles calculations demonstrate that the remarkable enhancement of photocatalytic activity of L-PCN can be attributed to the synergetic effect of structural topology and dopant. These findings suggest that we are able to design particular hierarchical nanostructures with desirable performance using hydrogen-bond engineering.
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影响因子：
3
作者：
Grimme, Stefan
通讯作者：
Grimme, Stefan
影响因子：
16.6
作者：
Kawasaki S;Takahashi R;Yamamoto T;Kobayashi M;Kumigashira H;Yoshinobu J;Komori F;Kudo A;Lippmaa M
通讯作者：
Lippmaa M
AgCl/Ag/g-C3N4杂化复合材料的制备、可见光驱动光催化活性及机理
影响因子：
26.6
作者：
Bao Y;Chen K
通讯作者：
Chen K
具有碳空位的多孔石墨氮化碳纳米片可显着提高光催化产氢能力
影响因子：
19
作者：
Liang, Qinghua;Li, Zhi;Yang, Quan-Hong
通讯作者：
Yang, Quan-Hong
影响因子：
3.7
作者：
Kresse, G;Furthmuller, J
通讯作者：
Furthmuller, J