Rapid microwave synthesis of Ru-supported partially carbonized conductive metal–organic framework for efficient hydrogen evolution

Abstract

Precise adjustment of the electronic structure of conductive MOFs load materials plays an important role in the design of electrocatalysts. In this paper, a hydrogen evolution catalyst in the full pH range was prepared by using a rapid microwave method to partially carbonize conductive MOFs materials and quickly anchoring small metal Ru nanoparticles on them. • Ru@p-Co 3 HHTP 2 is quickly prepared by a microwave solid-phase pyrolysis method. • Partial carbonization and SMSI in microwave improves stability and reactivity. • This catalyst has excellent hydrogen evolution performance in the full pH range. • DFT calculations and experiments revealed the synergy between Ru and p-Co 3 HHTP 2 . Conductive metal organic frameworks (MOFs) have limited their long-term development in the actual electrocatalytic test process due to their low activity and poor stability. Here, for the first time, ultra-small Ru nanoparticles supported by a novel conductive MOF material (Co 3 HHTP 2 ) were synthesized simply and quickly (60 s) using only a household microwave oven. In this process, the conductive MOF is partially carbonized, strong metal carrier interaction (SMSI) is generated, and Ru nanoparticles are firmly attached to the carrier to form Ru@p-Co 3 HHTP 2 . The Ru@p-Co 3 HHTP 2 -3.2% catalyst has excellent hydrogen evolution performance in the full pH range. Density functional theory calculations (DFT) result shows that the partial carbonization of the conductive MOF and the presence of SMSI promote the charge transfer at the interface between Ru nanoparticles and Co 3 HHTP 2 , which not only synergistically accelerates the water dissociation step and reduces the hydrogen adsorption energy, but also enhances the stability of the catalyst.