Powerful CO₂ electroreduction performance with N–carbon doped with single Ni atoms

Abstract

A single-atom dispersed Ni doping strategy to boost the performance of N–C materials for CO2RR by the pyrolysis of a metal–organic molecule complex was reported and revealed.

Understanding the Origin of Highly Selective CO2 Electroreduction to CO on Ni,N‐doped Carbon Catalysts

“…This high selectivity is in agreement with many recent literature reports of selective CO production in Ni,N-doped carbon materials (summary of past reported Ni-N-C catalysts in SI Table 2). [13][14][15][16][17][18][19][20][21] Thep artial current density towards CO increases with applied electrode potential and reaches 21 mA cm À2 at À1.1 Vvs. RHE before the onset of hydrogen evolution which results in aplateau in j CO and an increase of j tot to 40 mA cm À2 at À1.3 Vv s. RHE ( Figure 3B).…”

“…[11,12] Among these materials,Ni-N-C has been reported by many groups to have Faradaic efficiencies toward CO exceeding 90 %. [13][14][15][16][17][18][19][20][21] The proposed active site structure for Ni-N-C is atomically dispersed Ni-N x sites,ahypothesis that has been made based on evidence from electron microscopy, [13] hard X-ray absorption spectroscopy, [18] and density functional theory. [17] This active site determination closely matches the conclusions of the ORR literature for the Fe-N-C system where activity is attributed to FeN 4 C x sites that bear strong structure resemblance to typical molecular catalysts such as metal porphyrins and metal phthalocyanines.…”

“…TheN i-N-C for CO 2 Rr eports have,h owever, varied in their assignment of Ni oxidation state,c oordination number, and bonding environment, and have not shown conclusive evidence of nitrogen-nickel bonding. [13][14][15][16][17][18][19][20][21] In addition, previous reports have focused far more on characterizing Ni in the single atom form with less attention to the role of Ni aggregates in controlling the catalytic performance of Ni-N-C materials.T hus,o pen challenges remain in confirming that nickel-nitrogen bonding occurs in these materials,a nd in conclusively attributing catalytic activity to these dispersed Ni species.…”

Emerging Metal Single Atoms in Electrocatalysts and Batteries

“…[155] Carbonaceous materials are the commonly used substrates, including graphene sheets, [156][157][158][159] carbon nanotubes, [160,161] and porous carbon frameworks. [162][163][164][165] For instance, the dispersion of Ni SAs into NG (Ni-NG) sheets, without the involvement of Ni nanoparticles, was reported to serve as the active sites for catalyzing CO 2 reduction to carbon monoxide (CO) ( Figure 6). [158] Owing to the abundant Ni sites in graphene vacancies and the effects induced by Ni SAs with neighboring nitrogen coordination, the as-obtained electrocatalysts presented a very high selectivity, reaching 95%, and an excellent long-life stability.…”

Atomic Ni Species Anchored N‐Doped Carbon Hollow Spheres as Nanoreactors for Efficient Electrochemical CO2 Reduction

“…Electrochemical CO 2 reduction is a promising alternative to transform CO 2 to useful fuels, which can be operated in mild reaction condition, such as room temperature, atmospheric pressure and neutral solution . However, molecular CO 2 is very stable and the hydrogen evolution reaction (HER) as competitive reaction usually preferentially occurs during the potential range of electrochemical CO 2 reduction . The challenge for the electrochemical CO 2 reduction is the high overpotential and low faradaic efficiency .…”