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. Performance enhancing MOF: A new N,S co‐doped CoFe‐based metal–organic framework (MOF) obtained by a facile one‐pot solvothermal method shows highly efficient OER performance owing to its unique hierarchical porous structure and the introduction of N and S atoms into this heterobimetallic MOF, which improves its electronic conductivity and increases active reaction sites.