Joyner Jarin, Oliveira Eliezer F, Yamaguchi Hisato, Kato Keiko, Vinod Soumya, Galvao Douglas S, Salpekar Devashish, Roy Soumyabrata, Martinez Ulises, Tiwary Chandra S, Ozden Sehmus, Ajayan Pulickel M
Department of Material Science and NanoEngineering, Rice University, Houston, Texas 77005, United States.
Materials Physics and Applications Division, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States.
ACS Appl Mater Interfaces. 2020 Mar 18;12(11):12629-12638. doi: 10.1021/acsami.9b17713. Epub 2020 Mar 9.
The development of novel efficient and robust electrocatalysts with sufficient active sites is one of the key parameters for hydrogen evolution reactions (HER) catalysis, which plays a key role in hydrogen production for clean energy harvesting. Recently, two-dimensional (2D) materials, especially those based upon transition metal dichalcogenides such as molybdenum disulfide (MoS), have gained attention for the catalysis of hydrogen production because of their exceptional properties. Innovative strategies have been developed to engineer these material systems for improvements in their catalytic activity. Toward this aim, the facile growth of MoS clusters by sulfurization of molybdenum dioxide (MoO) particles supported on reduced graphene oxide (rGO) foams using the chemical vapor deposition (CVD) method is reported. This approach created various morphologies of MoS with large edges and defect densities on the basal plane of rGO supported MoS structures, which are considered as active sites for HER catalysis. In addition, MoS nanostructures on the surface of the porous rGO network show robust physical interactions, such as van der Waals and π-π interactions between MoS and rGO. These features result in an improved process to yield a suitable HER catalyst. In order to gain a better understanding of the improvement of this MoS-based HER catalyst, fully atomistic molecular dynamics (MD) simulations of different defect geometries were also performed.
开发具有足够活性位点的新型高效且稳定的电催化剂是析氢反应（HER）催化的关键参数之一，析氢反应在清洁能源收集制氢过程中起着关键作用。最近，二维（2D）材料，尤其是基于过渡金属二硫属化物（如二硫化钼（MoS））的材料，因其优异的性能而在制氢催化方面受到关注。人们已经开发出创新策略来设计这些材料体系，以提高其催化活性。为此，报道了使用化学气相沉积（CVD）方法通过硫化负载在还原氧化石墨烯（rGO）泡沫上的二氧化钼（MoO）颗粒来轻松生长MoS簇。这种方法在rGO负载的MoS结构的基面产生了具有大边缘和缺陷密度的各种MoS形态，这些被认为是HER催化的活性位点。此外，多孔rGO网络表面的MoS纳米结构表现出强大的物理相互作用，如MoS与rGO之间的范德华相互作用和π-π相互作用。这些特性导致了一种改进的方法来制备合适的HER催化剂。为了更好地理解这种基于MoS的HER催化剂的改进，还进行了不同缺陷几何形状的全原子分子动力学（MD）模拟。
