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

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.