Cheng Zhihua, Xiao Yukun, Wu Wenpeng, Zhang Xinqun, Fu Qiang, Zhao Yang, Qu Liangti
Key Laboratory of Cluster Science, Ministry of Education of China, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 100081, People's Republic of China.
Department of Chemistry & Department of Mechanical Engineering, Tsinghua University, Beijing 100084, People's Republic of China.
ACS Nano. 2021 Jul 27;15(7):11417-11427. doi: 10.1021/acsnano.1c01024. Epub 2021 Jul 2.
Generally, electrocatalytic hydrogen evolution reaction (HER) by water splitting is a pH-dependent reaction, which limits the widespread harvesting of hydrogen energy. Herein, we present a simple way for chemical bonding of MoS (002) planes and α-MoC {111} planes to form in-plane heterostructures capable of efficient pH-universal HER. Due to the lattice strain from mismatched lattice parameters between α-MoC and MoS, this catalyst changes the electronic configuration of the MoS and thus acquires the favorable proton adsorption and desorption activity, suggested by the platinum (Pt)-like free Gibbs energy. Consequently, only a low 78 mV overpotential is needed to achieve the current density of 10 mA cm in acidic solution along with a favorable Tafel kinetic process with a Tafel slope of 38.7 mV dec. Owing to the synergistic interaction between MoS (002) planes and α-MoC {111} planes with strong water dissociation activities, this catalyst also exhibits high HER performances beyond that of Pt in neutral and alkaline. This work proves the advances of in-plane heterostructures and illustrates the production of low-cost but highly efficient pH-universal HER catalytic materials, promising for future sustainable hydrogen energy.
一般来说,通过水分解进行的电催化析氢反应(HER)是一个依赖于pH值的反应,这限制了氢能的广泛获取。在此,我们提出了一种简单的方法,用于将MoS(002)平面与α-MoC{111}平面进行化学键合,以形成能够实现高效pH通用析氢反应的面内异质结构。由于α-MoC和MoS之间晶格参数不匹配产生的晶格应变,这种催化剂改变了MoS的电子构型,从而获得了良好的质子吸附和解吸活性,这由类似铂(Pt)的自由吉布斯能表明。因此,在酸性溶液中,仅需78 mV的低过电位就能实现10 mA cm的电流密度,同时具有良好的塔菲尔动力学过程,塔菲尔斜率为38.7 mV dec。由于MoS(002)平面与具有强水解离活性的α-MoC{111}平面之间的协同相互作用,这种催化剂在中性和碱性条件下也表现出高于Pt的高析氢反应性能。这项工作证明了面内异质结构的先进性,并展示了低成本但高效pH通用析氢反应催化材料的制备,对未来可持续氢能具有重要意义。