Beijing Key Laboratory of Microstructure and Properties of Solids, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing, 100124, China.
Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, 100049, China.
Small. 2022 Apr;18(16):e2107238. doi: 10.1002/smll.202107238. Epub 2022 Mar 15.
Metallic MoS (i.e., 1T-MoS ) is considered as the most promising precious-metal-free electrocatalyst with outstanding hydrogen evolution reaction (HER) performance in acidic media comparable to Pt. However, sluggish kinematics of HER in alkaline media and its inability for the oxygen evolution reaction (OER), hamper its development as bifunctional catalysts. The instability of 1T-MoS further impedes its applications for scaling up, calling an urgent need for simple synthesis to produce stable 1T-MoS . In this work, the challenge of 1T-MoS synthesis is first addressed using a direct one-step hydrothermal method by adopting ascorbic acid. 1T-MoS with flower-like morphology is obtained, and transition metals (Ni, Co, Fe) are simultaneously doped into 1T-MoS . Ni-1T-MoS achieves an enhanced bifunctional catalytic activity for both HER and OER in alkaline media, where the key role of Ni doping as single atom is proved to be essential for boosting HER/OER activity. Finally, a Ni-1T-MoS ||Ni-1T-MoS electrolyzer is fabricated, reaching a current density of 10 mA cm at an applied cell voltage of only 1.54 V for overall water splitting.
金属 MoS(即 1T-MoS)被认为是最有前途的无贵金属电催化剂,在酸性介质中具有与 Pt 相当的出色析氢反应(HER)性能。然而,碱性介质中 HER 的动力学缓慢及其对析氧反应(OER)的不适应,阻碍了其作为双功能催化剂的发展。1T-MoS 的不稳定性进一步阻碍了其应用的扩大化,因此迫切需要简单的合成方法来制备稳定的 1T-MoS。在这项工作中,首先采用一步水热法,通过使用抗坏血酸,解决了 1T-MoS 的合成挑战。得到了具有花状形态的 1T-MoS,并且过渡金属(Ni、Co、Fe)同时被掺杂到 1T-MoS 中。Ni-1T-MoS 在碱性介质中对 HER 和 OER 均表现出增强的双功能催化活性,证明了 Ni 掺杂作为单原子的关键作用对于提高 HER/OER 活性是必不可少的。最后,制备了 Ni-1T-MoS||Ni-1T-MoS 电解槽,在仅 1.54 V 的施加电池电压下,达到了 10 mA cm 的电流密度,实现了整体水分解。