Thermally polymerizable phthalocyanine realizes a metal–nitrogen-doped carbon material featuring a defined single-atom catalyst motif with CO2RR activity

Abstract

Metal–nitrogen-doped carbon materials (MNCs) exhibit good electrocatalytic performance owing to the intrinsic advantages of carbon-based materials and the presence of isolated and stabilized metal atoms coordinated by nitrogen sites. However, conventional high-temperature pyrolysis of precursor molecules make it difficult to control the coordination structure precisely. To address this issue, here we report a new synthesis strategy for MNCs. Specifically, we design and synthesize Ni-phthalocyanine functionalized with ethynyl groups as solid-state thermal polymerization points. After depositing the Ni-phthalocyanine precursor on a carbon support and performing a thermal treatment, the resultant carbon composite material features a Ni–N₄ coordination structure derived from the precursor, and enhanced porosity. This material demonstrates high catalytic activity for the CO₂ reduction reaction (CO₂RR). Our synthetic approach is applicable to various precursor molecules and carbon supports, paving the way for the further development of MNC-based electrode catalysts.