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Electroreduction of CO2 to CO powered by renewable electricity is a possible alternative to synthesizing CO from fossil fuel. However, it is very hard to achieve high current density at high faradaic efficiency (FE). Here, the first use of N,P‐co‐doped carbon aerogels (NPCA) to boost CO2 reduction to CO is presented. The FE of CO could reach 99.1 % with a partial current density of −143.6 mA cm−2, which is one of the highest current densities to date. NPCA has higher electrochemical active area and overall electronic conductivity than that of N‐ or P‐doped carbon aerogels, which favors electron transfer from CO2 to its radical anion or other key intermediates. By control experiments and theoretical calculations, it is found that the pyridinic N was very active for CO2 reduction to CO, and co‐doping of P with N hinder the hydrogen evolution reaction (HER) significantly, and thus the both current density and FE are very high. [ABSTRACT FROM AUTHOR]

Electrochemical reduction of CO2 into energy‐dense chemical feedstock and fuels provides an attractive pathway to sustainable energy storage and artificial carbon cycle. Herein, we report the first work to use atomic Ir electrocatalyst for CO2 reduction. By using α‐Co(OH)2 as the support, the faradaic efficiency of CO could reach 97.6 % with a turnover frequency (TOF) of 38290 h−1 in aqueous electrolyte, which is the highest TOF up to date. The electrochemical active area is 23.4‐times higher than Ir nanoparticles (2 nm), which is highly conductive and favors electron transfer from CO2 to its radical anion (CO2.−). Moreover, the more efficient stabilization of CO2.− intermediate and easy charge transfer makes the atomic Ir electrocatalyst facilitate CO production. Hence, α‐Co(OH)2‐supported atomic Ir electrocatalysts show enhanced CO2 activity and stability. High‐density atomic Ir supported on α‐Co(OH)2 had outstanding performance for CO2 reduction to CO. The faradaic efficiency can reach 97.6 % with a TOF of 38 290 h−1. The high catalytic activity is attributed to more active sites for CO2 adsorption and activation and the higher efficiency in stabilizing the CO2.− intermediate. [ABSTRACT FROM AUTHOR]