Hierarchical Porous Co9S8/Nitrogen-Doped Carbon@MoS2 Polyhedrons as pH Universal Electrocatalysts for Highly Efficient Hydrogen Evolution Reaction

4 years ago

Hierarchical Porous Co9S8/Nitrogen-Doped Carbon@MoS2 Polyhedrons as pH Universal Electrocatalysts for Highly Efficient Hydrogen Evolution Reaction

Hongmei Li, Li Shao, Chong Xu, Xiancai Jiang, Xing Qian, Shaowei Huang, Linxi Hou, Changli Zhu

The development of highly active and stable earth-abundant electrocatalysts to reduce or eliminate the reliance on noble-metal based ones for hydrogen evolution reaction (HER) over a broad pH range remains a great challenge. Herein, hierarchical porous Co₉S₈/N-doped carbon@MoS₂ (Co₉S₈/NC@MoS₂) polyhedrons have been synthesized by a facile hydrothermal approach using highly conductive Co/NC polyhedrons composed of cobalt nanoparticles embedded in N-doped carbon matrices as both the structural support and cobalt source. The Co/NC polyhedrons were prepared by direct carbonization of Co-based zeolitic imidazolate framework (ZIF-67) in Ar atmosphere. Benefiting from the prominent synergistic effect of N-doped carbon enhancing the conductivity of the hybrid, MoS₂ and Co₉S₈ providing abundant catalytically active sites as well as the well-defined polyhedral structure promoting mechanical stability, the as-synthesized Co₉S₈/NC@MoS₂ shows excellent HER activity and good stability over a broad pH range, with onset overpotentials of 4, 38, and 45 mV, Tafel slopes of 60.3, 68.8, and 126.1 mV dec^–1, and overpotentials of 67, 117, and 261 mV at 10 mA cm^–2 in 1.0 M KOH, 0.5 M H₂SO₄, and 1.0 M phosphate buffer solution (PBS), respectively. This work provides a general and promising approach for the design and synthesis of inexpensive and efficient pH-universal HER electrocatalysts.

Publisher URL: http://dx.doi.org/10.1021/acsami.7b06384

DOI: 10.1021/acsami.7b06384