Sharma Mamta Devi, Mahala Chavi, Basu Mrinmoyee
Department of Chemistry, BITS Pilani, Pilani Campus, Rajasthan-333031, India.
Inorg Chem. 2020 Apr 6;59(7):4377-4388. doi: 10.1021/acs.inorgchem.9b03445. Epub 2020 Mar 9.
Two-dimensional layered transition metal dichalcogenides, MoSe and MoS, have drawn potential attention in the field of water splitting. Coupling of MoS and MoSe provides a sustainable route to improve the electrocatalytic activity for the hydrogen evolution reaction (HER). Here, the heterostructures of thin sheets (ts) of MoSe and MoS are combined to develop the MoSe-ts@MoS-ts heterostructure via multiple-step methodology. First, thin sheets of MoSe are synthesized following the stepwise hydrothermal method. After the successful synthesis of MoSe-ts, MoS-ts is synthesized on it to develop the heterostructure: MoSe-ts@MoS-ts. By tuning the amount of MoS-ts and MoSe-ts in the heterostructure separately, the optimum condition is obtained for HER. The unique heterostructure is efficient for HER under wide pH conditions like 1 M KOH, pH-7 phosphate buffer, 3.5% saline water, and finally 0.5 M HSO. MoSe-ts@MoS-ts can generate 10 mA/cm current density under the application of -0.186 V vs RHE with a low Tafel value of 71 mV/decade. The formation of the heterojunction plays an essential role in facilitating charge transportation. Furthermore, the heterostructure provides the more active sites for the adsorption of hydrogen to generate H. An excess amount of any of the bare counter parts in the heterostructure leads to a decrease in electrocatalytic efficiency because of the lowered heterojuction formation. MoSe-ts@MoS-ts has very high stability during the electrocatalytic reaction, which is determined from 1000 consecutive cycles and a 24 h prolonged scan. MoSe-ts@MoS-ts can generate 147 μmol of H in ∼50 min of reaction time with 100% Faradaic efficiency.
二维层状过渡金属二硫属化物MoSe₂和MoS₂在水分解领域引起了潜在关注。MoS₂和MoSe₂的耦合为提高析氢反应(HER)的电催化活性提供了一条可持续途径。在此,通过多步方法将MoSe₂和MoS₂的薄片(ts)异质结构组合起来,开发出MoSe₂-ts@MoS₂-ts异质结构。首先,按照逐步水热法合成MoSe₂薄片。在成功合成MoSe₂-ts后,在其上合成MoS₂-ts以形成异质结构:MoSe₂-ts@MoS₂-ts。通过分别调整异质结构中MoS₂-ts和MoSe₂-ts的量,获得了HER的最佳条件。这种独特的异质结构在1 M KOH、pH = 7的磷酸盐缓冲液、3.5%的盐水以及最终0.5 M H₂SO₄等宽pH条件下对HER都很有效。MoSe₂-ts@MoS₂-ts在相对于可逆氢电极(RHE)施加-0.186 V电压时可产生10 mA/cm²的电流密度,塔菲尔值低至71 mV/decade。异质结的形成在促进电荷传输方面起着至关重要的作用。此外,该异质结构为氢气吸附以生成H₂提供了更多活性位点。异质结构中任何一种裸片过量都会由于异质结形成减少而导致电催化效率降低。MoSe₂-ts@MoS₂-ts在电催化反应过程中具有非常高的稳定性,这通过1000次连续循环和24小时的长时间扫描得以确定。MoSe₂-ts@MoS₂-ts在约50分钟的反应时间内可以产生147 μmol的H₂,法拉第效率为100%。