Metal‐Free Nitrogen‐Doped Mesoporous Carbon for Electroreduction of CO₂ to Ethanol

Abstract

CO electroreduction is a promising technique for satisfying both renewable energy storage and a negative carbon cycle. However, it remains a challenge to convert CO into C2 products with high efficiency and selectivity. Herein, we report a nitrogen-doped ordered cylindrical mesoporous carbon as a robust metal-free catalyst for CO electroreduction, enabling the efficient production of ethanol with nearly 100 % selectivity and high faradaic efficiency of 77 % at -0.56 V versus the reversible hydrogen electrode. Experiments and density functional theory calculations demonstrate that the synergetic effect of the nitrogen heteroatoms and the cylindrical channel configurations facilitate the dimerization of key CO* intermediates and the subsequent proton-electron transfers, resulting in superior electrocatalytic performance for synthesizing ethanol from CO .

A Core–Shell‐Structured Silver Nanowire/Nitrogen‐Doped Carbon Catalyst for Enhanced and Multifunctional Electrofixation of CO2

“…However, as ingle catalyst showing activity in both solvent types is still rare, to the best of our knowledge.W ed eveloped ac ore-shell-structured AgNW/NC700 composite using aA gn anowire( NW) core encapsulated by aN -doped carbon (NC) shell at 700 8C. [10][11][12][13][14][15] In particular, Ag-based catalysts could selectivelyc onvertC O 2 into CO, which is widely used as syngasi nc hemical industry. Under mild conditions, up to 96 %faradaic efficiency of CO, 95 %yield of Ibuprofen and 92 %y ield of propylene carbonate could be obtained in the electrochemical CO 2 direct reduction,c arboxylation and cycloaddition,respectively,using the same AgNWs/NC700 catalyst.…”

“…Although CO 2 is recognized as the main greenhouse gas,i ti sa lso ac heap, abundant, and nontoxic C 1 resource, which could be used for the productiono f many valuablem aterials. [10][11][12][13][14][15] In particular, Ag-based catalysts could selectivelyc onvertC O 2 into CO, which is widely used as syngasi nc hemical industry. [1][2][3] Electrochemical reduction of CO 2 has attracted wide attention because it can convert and store renewable energy resources, such as solar and wind energies, in the form of chemical energy.…”

“…As seen from Figure 3a and Figure S6, AgNW/NC700 shows as ignificantly higher current density of À22.8 mA cm À2 than the À13.1 mA cm À2 for AgNW/NC800, À7.1 mA cm À2 for AgNW/ NC600,a nd À5.2 mA cm À2 for AgNWsw ith the same catalyst loading at À1.15 V RHE in the CO 2 -purged solution. Considering that N-dopedc arbon materials were also reported as efficient electro-catalysts for CO 2 reduction, [10][11][12] controlled potential electrolysisw as also performed with the NC700 catalyst. [19] Only LSV resultsc ould not conclusively distinguish between the CO 2 reduction and the hydrogen evolution reactions duringC O 2 electroreduction of our catalyst, because theser eactions alwaysc ompetitively occur during electrolysis,p articularly in aqueous solutions.…”

Superior Selectivity and Tolerance towards Metal‐Ion Impurities of a Fe/N/C Catalyst for CO2 Reduction

“…The higher content of Ni nS MFe compared with SMFeSCN implies that SMFe is more defective, [30] which is consistent with the TEM, XRD, and Raman analyses. [31][32][33] The concentrationso fd ifferent Ns peciesw ere determined by calculating the area beneath the correspondingp eak (results are shown in Ta ble S1 in the Supporting Information). [31][32][33] The concentrationso fd ifferent Ns peciesw ere determined by calculating the area beneath the correspondingp eak (results are shown in Ta ble S1 in the Supporting Information).…”

Role of Heteroatoms in S,N‐Codoped Nanoporous Carbon Materials in CO2 (Photo)electrochemical Reduction

“…[11] studied as eries of mesoporousN -doped carbon materialsw ith highly uniformc ylindrical pore structures. Songe tal.…”