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CO2 electroreduction is a promising technique for the management of the global carbon balance by low-grade renewable electricity. However, the lack of highly efficient and selective catalysts has hampered the development of this area. Herein, we report a poly-phenylenediamine-derived atomically dispersed Ni catalyst as a highly efficient and selective electrocatalyst for the conversion of CO2 to CO. The catalyst facilitates efficient production of CO with high faradaic efficiency (FE) (90%) and a large current density of 11.6 mA cm−2 at −0.8 V compared to a reversible hydrogen electrode (RHE). An excellent turnover frequency (TOF) of 3079 h−1 for the electroreduction of CO2 was also achieved at −0.8 V vs. RHE.

Ni– and Co–porphyrin multilayers on reduced graphene oxide (rGO) sheets are reported as novel bifunctional catalysts for the oxygen evolution reaction (OER) and the oxygen reduction reaction (ORR)., Ni– and Co–porphyrin multilayers on reduced graphene oxide (rGO) sheets are reported as novel bifunctional catalysts for the oxygen evolution reaction (OER) and the oxygen reduction reaction (ORR). After binding with organic porphyrin molecules, the catalytically-active Ni2+ and Co2+ ions are periodically constructed onto the rGO surfaces via the layer-by-layer (LBL) assembly technique. The resulting catalysts exhibit good performance towards both OER and ORR, which is achieved with accurate control of the composition and thickness of the multilayer structures. This work highlights the potential for the fabrication of efficient electrocatalysts via molecular design.