In Situ Synthesis of Few-Layered g-C3N4 with Vertically Aligned MoS2 Loading for Boosting Solar-to-Hydrogen Generation
In Situ Synthesis of Few-Layered g-C3N4 with Vertically Aligned MoS2 Loading for Boosting Solar-to-Hydrogen Generation
复制标题
原位合成多层 g-C3N4 并垂直排列 MoS2 负载以促进太阳能制氢
DOI：
10.1002/smll.201703003
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发表时间：
2018-01-18
期刊：
影响因子：
13.3
通讯作者：
Liu, Shengzhong (Frank)
中科院分区：
文献类型：
--
作者：
Bian, Hui;Ji, Yujin;Liu, Shengzhong (Frank)
在人工光催化析氢中，有效的入射光子吸收和高的电荷重组率是影响整体效率的关键因素。本文首次采用传统的固相合成方法合成了具有垂直排列MoS_2负载的稀层g-C_3N_4(MoS_2/C_3N_4)。选择硫脲和层状MoO_3作为前驱体，在氮气气氛下反应原位生成产物。根据准傅里叶变换红外反射光谱和X射线衍射仪的测量，确定了详细的反应过程，确定了该反应的形成途径。两个前体单元MoS2和C3N4通过MON键相连，这些键起到电子接收器/导体和产氢中心的作用。用密度泛函理论确定了界面位为电子聚集区。根据光电化学结果，MoS2/C3N4可以达到0.05 mA cm(-2)的电流，几乎是裸g-C3N4或MoS2/C3N4-R参比样品的十倍。本工作的发现不仅为合成一系列指定的样品铺平了道路，而且也为深入了解固相反应奠定了基础。
In artificial photocatalytic hydrogen evolution, effective incident photon absorption and a high-charge recombination rate are crucial factors influencing the overall efficiency. Herein, a traditional solid-state synthesis is used to obtain, for the first time, novel samples of few-layered g-C3N4 with vertically aligned MoS2 loading (MoS2/C3N4). Thiourea and layered MoO3 are chosen as precursors, as they react under nitrogen atmosphere to in situ produce the products. According to the quasi-Fourier transform infrared reflectance and X-ray diffraction measurements, the detailed reaction process is determined to proceed through the confirmed formation pathway. The two precursor units MoS2 and C3N4 are linked by MoN bonds, which act as electronic receivers/conductors and hydrogen-generation sites. Density functional theory is also carried out, which determines that the interface sites act as electron-accumulation regions. According to the photoelectrochemical results, MoS2/C3N4 can achieve a current of 0.05 mA cm(-2), which is almost ten times higher than that of bare g-C3N4 or the MoS2/C3N4-R reference samples. The findings in the present work pave the way to not only synthesize a series of designated samples but also thoroughly understand the solid-state reaction.