Oral Presentation Royal Australian Chemical Institute National Congress 2026

Stabilizing Phthalocyanine Catalysts via Cobalt–Copper Dual-Metal COFs for CO2-to-Methanol Electrocatalysis (136756)

Mengxin Liu 1 , Yijiao Jiang 1 , Yuming Wu 1
  1. Macquarie University, Marsfield, NSW, Australia

Electrochemical CO2 reduction to methanol (MeOH) represents an attractive pathway for renewable fuel production and carbon neutrality; however, molecular phthalocyanine (Pc) catalysts typically suffer from poor stability and low MeOH selectivity at high cathodic potential due to aggregation and structural degradation. Previous studies highlight that molecular phthalocyanine catalysts with single metal centers or single functional modifications (e.g., amino functionalized) are inherently limited in achieving both high methanol selectivity and long-term stability for electrochemical CO2 reduction. Motivated by these limitations, the present work successfully fabricated a dual-metal-centered covalent organic framework (COF) incorporating cobalt (Co-) and copper (Cu-) Pc to simultaneously integrate complementary catalytic functions and structural stabilization. Compared with molecular CoPc(NH2)4 and a single-metal CoPc COF, the dual metal CoPc–CuPc COF exhibits enhanced performance, which deliver a stable MeOH Faradaic efficiency of approximately 40 % at -1.0 V vs RHE, accompanied by a substantially increased current density (45 mA∙cm–2), outperforming both molecular CoPc(NH2)4 and the single-metal CoPc COF counterpart. This originates from COF immobilization, which increases the density of accessible catalytic sites while effectively suppressing molecular aggregation and catalyst leaching, thereby improving structural stability during electrolysis. This work demonstrates COF engineering as an effective strategy to stabilize molecular phthalocyanine catalysts and increase active site utilization, providing a promising platform for durable electrochemical CO2-to-MeOH conversion.