Boosting CO₂ Electroreduction on N,P‐Co‐doped Carbon Aerogels

Abstract

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.

Spontaneously producing syngas from MFC-MEC coupling system based on biocompatible bifunctional metal-free electrocatalyst

“…S11), it still display the highest ECSA-normalized current density (Table S2), suggesting the active sites on NP-C have a higher intrinsic activity to CDRR than that on the singledoped N-C and P-C, which could partially explain the superior CDRR on NP-C than that on the single-doped P-C and N-C as well as undoped C. The higher intrinsic activity of active sites on NP-C might be derived from the co-doping of N and P hetero-atoms, which was in agreement with the previous reports [40][41][42]. Because the active site and mechanism were very similar to previous studies [42], the focus of this study was the feasibility of the device, and there was no further in-depth study of the mechanism. Moreover, the low ECSA of N-C can par- ARTICLES .…”

Single‐Atom Electrocatalysts from Multivariate Metal–Organic Frameworks for Highly Selective Reduction of CO2 at Low Pressures

“…Given the existence of competitive HER process,t he limiting potential difference between CO 2 RR and HER (U L (CO 2 )-U L (H 2 ); U L = ÀDG 0 /e) has been further calculated and employed as the descriptor of CO selectivity, where more positive value of U L (CO 2 )-U L (H 2 )r epresents ah igher CO 2 RR selectivity than hydrogen evolution. [35,54,55] As shown in Figure 4c Figure S27). Thec alculations conclude that the CO 2 RR will be much more difficult at low CO 2 partial pressures from the viewpoint of thermodynamics.T herefore, this raises ahigher demand for both activity and selectivity of the electrocatalysts,t oward addressing this challenging goal.…”

Non‐N‐Doped Carbons as Metal‐Free Electrocatalysts

“…Along with the monodoped carbon catalysts discussed above, co‐doping of carbon materials with two or more different heteroatoms can further enhance the catalytic performance of the carbon catalysts by increasing the total number of active sites and through possible synergistic effects. [ 47 ] So far, co‐doping studies have been focused on co‐doping of N‐doped carbon materials with a second element, such as B, [ 69–76 ] S, [ 77–88 ] P, [ 89–106 ] and, to a less extent, Cl, [ 107 ] and Si. [ 108,109 ] A few reports on the co‐doping of carbon materials with three elements, such as N–P–S, [ 110,111 ] N–P–B, [ 112,113 ] N–P–F, [ 114 ] and N–S–F, [ 115 ] have recently appeared.…”

“…Recently, the N,P co‐doped carbon catalyst has also been used for electroreduction of CO 2 to CO. [ 97,98 ] Specifically, Chen et al. firstly presented the use of the N,P co‐doped carbon aerogel (NPCA) to boost CO 2 reduction to CO.…”