2023
DOI: 10.1021/acsami.3c08853
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Curvature Effect of Pyridinic N-Modified Carbon Atom Sites for Electrocatalyzing CO2 Conversion to CO

Abstract: Carbon material is considered a promising electrocatalyst for the CO2 reduction reaction (CO2RR); especially, N-doped carbon material shows high CO Faradic efficiency (FECO) when using pyridinic N species as the active site. However, in the past decade, more efforts were focused on the preparation of various carbon nanostructures containing abundant pyridinic N species and few researchers studied the electronic structure modulation of the pyridinic N site. The curvature of the carbon substrate is an easily con… Show more

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Cited by 14 publications
(4 citation statements)
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“…Although there is little difference in their (H 2 O 2 /HO 2 − ) formation free energies, the volcano plots in the form of H 2 O 2 can provide a more general mechanism. 45 Compared to the other models, the energy of the edge B1 site is 4.15 eV, which approaches the ideal standard free energy of 4.22 eV (the Δ G OOH* of 4.22 eV corresponds to the thermodynamic equilibrium potential, U 0 = 0.70 V 43 ). The U limited of the edge B1 site is 0.64 V, which is nearly the lowest potential of 0.70 V. The appropriate adsorption energy and low U limited demonstrate that the highest catalytic activity for H 2 O 2 occurs at the edge B1.…”
Section: Resultsmentioning
confidence: 83%
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“…Although there is little difference in their (H 2 O 2 /HO 2 − ) formation free energies, the volcano plots in the form of H 2 O 2 can provide a more general mechanism. 45 Compared to the other models, the energy of the edge B1 site is 4.15 eV, which approaches the ideal standard free energy of 4.22 eV (the Δ G OOH* of 4.22 eV corresponds to the thermodynamic equilibrium potential, U 0 = 0.70 V 43 ). The U limited of the edge B1 site is 0.64 V, which is nearly the lowest potential of 0.70 V. The appropriate adsorption energy and low U limited demonstrate that the highest catalytic activity for H 2 O 2 occurs at the edge B1.…”
Section: Resultsmentioning
confidence: 83%
“…For an ideal model, the reaction free energies ( G ) for all electron-transfer steps are zero when the applied potential equals the equilibrium potential. 45 Compared to the C and N atoms in different models, the edge B atom in the B-centered AB stacking model (edge B1) achieves the highest reaction rate under the same conditions because its G is 0.06 eV, which is nearly zero (Fig. 7b and Table S4, ESI†).…”
Section: Resultsmentioning
confidence: 96%
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“…Through comparing the kinetics for the four catalysts (Figure d), the BS-C-3 has a Tafel slope of 66.7 mV dec –1 which surpasses those of S–C (84.7 mV dec –1 ), BS-C-1 (72.3 mV dec –1 ), and BS-C-2 (73.1 mV dec –1 ), demonstrating the faster kinetics of BS-C-3 in 2e – ORR. , The electrochemical active surface area (ECSA) was applied to measure the density of active sites (Figures e and S14). Though with the highest catalytic performance, the BS-C-3 shows the lowest ECSA (1.09 μF cm –2 ), indicating the lower site density, which well supports that the better catalytic performance of BS-C-3 is originated from the higher intrinsic activity of B–S pairs rather than the large number of active sites. , At high and low frequencies, the BS-C-3 has the smallest semicircle and the highest slope, indicating the small charge-transfer resistance and faster mass diffusion, respectively, in the electrochemical impedance spectroscopy (EIS) spectra (Figure f) . The small resistance of BS-C-3 is due to its lowest B and S content, which has less influence on the charge transfer.…”
Section: Resultsmentioning
confidence: 99%