Rational Design of a N,S Co‐Doped Supermicroporous CoFe–Organic Framework Platform for Water Oxidation

It remains a challenge to rational design of a new metal-organic framework (MOF) as highly efficient direct electrocatalysts for the oxygen evolution reaction (OER). Herein, we developed a simple and effective method to explore a new pillared-layered MOF with syringic acid as a promising OER electrocatalyst. The isostructural mono-, heterobimetallic MOF and N,S co-doped MOF by mixing thiourea were quickly synthesized in a high yield under solvothermal condition. Moreover, the optimized N,S co-doped MOF exhibits the lowest overpotential of 254 mV at 10 mA cm^-2 on a glass carbon electrode and a small Tafel slope of 50 mV dec^-1 , especially, this catalyst also possesses long-term electrochemical durability for at least 16 h. According to the characterization, the incorporation of N and S atoms into this heterobimetallic CoFe-based MOF could modify its pore structure, tune the electronic structure, accordingly, improve the mass and electron transportation, and facilitate the formation of active species, as a consequence, the improved activity of this new N,S co-doped MOF for OER should be mainly be ascribed to higher electrochemical activation toward the active species via in situ surface modification during the OER process.