Systematic screening of transition metal dual-atom-doped phthalocyanine electrocatalysts for the oxygen reduction reaction

Electrocatalysis is emerging as a promising technology for dealing with the energy crisis and environmental challenges. Phthalocyanines doped with two transition metal atoms (Tm₂-Pc) show outstanding ORR catalytic activity and offer several catalytic sites. However, a systematic investigation of the ORR catalytic efficacy of Tm₂-Pc monolayers with varying central metal atoms is lacking, hindering the establishment of design principles for this family of materials. Our research findings demonstrate that the d-band center, HOMO-LUMO, and adsorption energy are significant factors in the evaluation of catalysts. The ORR efficacy of Tm₂-Pc is dependent on the interaction strength between the adsorbate and Tm₂-Pc. With overpotentials of just 0.28 eV and 0.27 eV, respectively, Mn₂-Pc and Ru₂-Pc show good stability and outstanding catalytic activity. This work provides a theoretical foundation for the creation of high-performance catalysts by revealing the ORR catalytic mechanism of Tm₂-Pc.