Unveiling the Active Site of Metal-Free Nitrogen-doped Carbon for Electrocatalytic Carbon Dioxide Reduction

Efficient Fabrication of Diverse Mesostructured Materials from the Self-Assembly of Pyrrole-Containing Block Copolymers and Their Confined Chemical Transformation

“…As the carbonization temperature was increased from 600 to 800 °C, the content of pyridinic N decreased from 19.6 to 12.6%, that of pyrrolic N decreased from 34.4 to 25.4%, and that of graphitic N increased from 46 to 62% (Figure S19c). This trend is consistent with the reported works on N-doped carbon, in which increasing the temperature facilitated the formation of graphitic N, while the less stable pyrrolic N and pyridinic N would be consumed. , The high nitrogen doping could endow the carbon materials with the potential for the hydrogen evolution reaction, supercapacitors, CO 2 adsorption, oxygen reduction reaction, and other fields.…”

Surface and interface chemistry in metal‐free electrocatalysts for electrochemical CO2 reduction

“…(B) Free energy pathways and limiting potentials as functions of Δ G (*COOH) for the CO 2 RR to CO and the HER. Reproduced with permission: Copyright 2020, Cell Reports Physical Science 62 . CO 2 RR, CO 2 reduction reaction; DFT, density function theoretical; HER, hydrogen evolution reaction…”

“…The carbon atoms at the edges next to graphitic N induced CO formation over the HER, while carbon atoms next to pyridinic N facilitate the HER (Figure 3B). 62 The CO 2 RR mechanism of N-doped graphene was studied from thermodynamics and kinetics by using the quantum mechanics of constant electrode potential, which found the carbon atoms on the edge of graphene and near the graphitic N atoms as the active sites. The CO 2 RR performance for N-doped carbon materials can be improved by adjusting the form of N doping to obtain more graphitic N rather than pyridinic N. 117 These results indicated that a specific defect could have distinct effects on different materials and reactions.…”

“…Reproduced with permission: Copyright 2020, Cell Reports Physical Science. 62 CO 2 RR, CO 2 reduction reaction; DFT, density function theoretical; HER, hydrogen evolution reaction only the electronic structure of defect sites and the adsorption/desorption behavior of key intermediates but also defect source, type, number, location, and various materials in which the defect is located. From the surface point of view, the electronic structure of surface defects has been changed, which is conducive to adjusting the physical and chemical properties of MFEs, altering the adsorption behavior of the reactants, and further regulating the binding/adsorption energy of specific intermediates.…”

Nitrogen-doped porous carbon nanosheets as a robust catalyst for tunable CO2 electroreduction to syngas

“…33–35 In particular, the doping of nitrogen (N) atoms with a larger atomic size can introduce more defect sites into the carbon skeleton, which changes the charge density and spin polarisation of the adjacent carbon atoms. 36,37 These catalytic-active N sites can both enhance CO 2 adsorption and improve mass transfer efficiency to promote product selectivity. 38 In addition, the well-developed porosity not only further improves the catalytic activity area, but also provides a large number of space-accessible mass transmission channels to achieve the optimal CO 2 RR performance.…”