Department of Advanced Materials Chemistry, Korea University, Sejong 339-700, Republic of Korea.
Institute for Application of Advanced Materials, Jeonju University, Chonju, Chonbuk 55069, Republic of Korea.
ACS Nano. 2023 Feb 14;17(3):2968-2979. doi: 10.1021/acsnano.2c11528. Epub 2023 Jan 19.
Ternary alloying of transition metal dichalcogenides (TMDs) has the potential for altering the electronic structure of materials to suit electrochemical applications. Herein, we synthesized (MoWV)Se nanosheets at various compositions a colloidal reaction. The mole fraction of V atoms () was successfully increased up to 0.8, producing a metallic phase that is highly durable against hydration. Furthermore, we synthesized (MoW)Se nanosheets over the entire composition range. The atomic mixing of the ternary alloys is more random than that of the constitutional binary alloys, as supported by first-principles calculations. Compared to binary alloying, ternary alloying more effectively enhanced the electrocatalytic activity for acidic hydrogen evolution reaction (HER). The HER performance increased upon increasing to 0.44, and thereafter, it declined at higher primarily owing to surface oxidation. The analysis of Gibbs free energy for H adsorption revealed that ternary alloying strongly activates the basal plane for the HER. VSe contains numerous sites favorable for H adsorption, facilitating the composition-dependent HER. These results provide a pioneering strategy for designing multicomponent TMD catalysts that maximize the advantages of each component.
过渡金属二硫属化物（TMDs）的三元合金化有可能改变材料的电子结构，以适应电化学应用。在此，我们通过胶体反应合成了具有不同组成的（MoWV）Se 纳米片。V 原子的摩尔分数（）成功增加到 0.8，产生了一种对水合作用高度稳定的金属相。此外，我们在整个组成范围内合成了（MoW）Se 纳米片。原子混合的三元合金比组成二元合金更随机，这得到了第一性原理计算的支持。与二元合金化相比，三元合金化更有效地提高了酸性析氢反应（HER）的电催化活性。随着增加到 0.44，HER 性能增加，此后，由于表面氧化，在更高时下降。对 H 吸附的吉布斯自由能分析表明，三元合金化强烈激活了 HER 的基面。VSe 包含许多有利于 H 吸附的位点，促进了组成依赖性 HER。这些结果为设计最大限度发挥各组分优势的多组分 TMD 催化剂提供了一种开创性策略。
