<br>用于制氢的 MoS2 光电极：调节高度均匀超薄纳米晶体中的 S 空位含量,ACS Applied Materials & Interfaces

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用于制氢的 MoS2 光电极：调节高度均匀超薄纳米晶体中的 S 空位含量
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2023-07-05 , DOI: 10.1021/acsami.3c02192
Nuria Jiménez-Arévalo ₁ , Jinan H Al Shuhaib ₁ , Rodrigo Bautista Pacheco ₁ , Dario Marchiani ₂ , Mahmoud M Saad Abdelnabi _{2,

3} , Riccardo Frisenda ₂ , Marco Sbroscia ₂ , Maria Grazia Betti ₂ , Carlo Mariani ₂ , Yolanda Manzanares-Negro ₄ , Cristina Gómez Navarro _{4,

5} , Antonio J Martínez-Galera _{1,

5} , José Ramón Ares ₁ , Isabel J Ferrer _{1,

5} , Fabrice Leardini _{1,

5}

Affiliation

调节MoS ₂层的电催化性能可以通过不同的途径来实现，例如减少其厚度、在MoS ₂薄片中创建边缘以及引入S-空位。我们通过使用特殊的盐辅助化学气相沉积 (CVD) 方法生长 MoS ₂电极来结合这三种方法。该过程允许超薄 MoS ₂纳米晶体（1-3 层厚，几纳米宽）的生长，原子力显微镜和扫描隧道显微镜证明了这一点。与剥离或微晶MoS ₂层相比，纳米级MoS ₂层的这种形态在拉曼和光致发光光谱中引起一些特定特征。此外，可以在CVD生长期间通过使用Ar/H ₂混合物作为载气来调节层中的S空位含量。具有亚毫米空间分辨率的详细光学微透射率和微反射光谱、微拉曼和X射线光电子能谱测量表明，所获得的样品在cm ²范围内的面积上呈现出优异的均匀性。使用相对较大面积（0.8 cm ² ）的电极研究了这些MoS ₂层的电化学和光电化学性质。所制备的MoS ₂阴极表现出出色的法拉第效率以及在酸性溶液中的长期稳定性。此外，我们证明存在最佳数量的S空位来提高MoS ₂的电化学和光电化学性能。

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MoS2 Photoelectrodes for Hydrogen Production: Tuning the S-Vacancy Content in Highly Homogeneous Ultrathin Nanocrystals

Tuning the electrocatalytic properties of MoS₂ layers can be achieved through different paths, such as reducing their thickness, creating edges in the MoS₂ flakes, and introducing S-vacancies. We combine these three approaches by growing MoS₂ electrodes by using a special salt-assisted chemical vapor deposition (CVD) method. This procedure allows the growth of ultrathin MoS₂ nanocrystals (1–3 layers thick and a few nanometers wide), as evidenced by atomic force microscopy and scanning tunneling microscopy. This morphology of the MoS₂ layers at the nanoscale induces some specific features in the Raman and photoluminescence spectra compared to exfoliated or microcrystalline MoS₂ layers. Moreover, the S-vacancy content in the layers can be tuned during CVD growth by using Ar/H₂ mixtures as a carrier gas. Detailed optical microtransmittance and microreflectance spectroscopies, micro-Raman, and X-ray photoelectron spectroscopy measurements with sub-millimeter spatial resolution show that the obtained samples present an excellent homogeneity over areas in the cm² range. The electrochemical and photoelectrochemical properties of these MoS₂ layers were investigated using electrodes with relatively large areas (0.8 cm²). The prepared MoS₂ cathodes show outstanding Faradaic efficiencies as well as long-term stability in acidic solutions. In addition, we demonstrate that there is an optimal number of S-vacancies to improve the electrochemical and photoelectrochemical performances of MoS₂.

更新日期：2023-07-05

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