Catalytic Reduction of N2O by CO on Single-Atom Catalysts Au/C2N and Cu/C2N: A First-Principles Study
Abstract
:1. Introduction
2. Results and Discussion
2.1. Geometric and Electronic Properties of Cu/C2N and Au/C2N
2.2. Mechanism of Catalytic N2O Reduction
2.2.1. Mechanism I: N2O Adsorption Mechanism
Au/C2N-Catalyzed N2O Reduction
Cu/C2N-Catalyzed N2O Reduction
2.2.2. Mechanism II: CO Adsorption Mechanism
Au/C2N-Catalyzed N2O Reduction
Cu/C2N-Catalyzed N2O Reduction
3. Computational Methods
4. Conclusions
Supplementary Materials
Author Contributions
Funding
Data Availability Statement
Acknowledgments
Conflicts of Interest
References
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Au/C2N | Cu/C2N | |||||
---|---|---|---|---|---|---|
ΔEcorr | ΔHcorr | ΔGcorr | ΔEcorr | ΔHcorr | ΔGcorr | |
R | 0.00 | 0.00 | 0.00 | 0.00 | 0.00 | 0.00 |
IS1a | −0.05 | −0.06 | −0.09 | −0.02 | −0.01 | −0.11 |
TS1a | 0.90 | 1.04 | 0.74 | 1.07 | 1.25 | 0.80 |
MS1a | 0.84 | 0.91 | 0.40 | 0.63 | 0.71 | 0.20 |
MS2a | 0.98 | 1.07 | 0.47 | 0.81 | 0.89 | 0.34 |
MS3a | 0.83 | 0.93 | 0.60 | 0.56 | 0.63 | 0.29 |
TS2a | 1.13 | 1.21 | 0.95 | 0.99 | 1.04 | 0.83 |
MS4a | −3.69 | −3.62 | −3.97 | −4.13 | −4.15 | −3.80 |
IS1b | −0.32 | −0.28 | −0.28 | −0.90 | −0.84 | −0.92 |
MS1b | −0.43 | −0.40 | −0.14 | −1.10 | −1.05 | −0.96 |
TS1b | 1.87 | 1.90 | 2.08 | 0.72 | 0.75 | 0.86 |
MS2b | −3.48 | −3.44 | −3.30 | −3.58 | −3.49 | −3.54 |
FS | −3.40 | −3.34 | −3.25 | −3.40 | −3.34 | −3.25 |
Atom/ Molecule | Charges/e | |||||||
---|---|---|---|---|---|---|---|---|
Isolated Systems | IS1a | TS1a | MS1a | MS2a | MS3a | TS2a | MS4a | |
Au | 0.548 | 0.551 | 0.705 | 0.734 | 0.739 | 0.736 | 0.708 | 0.561 |
O(N2O) | −0.278 | −0.291 | −0.466 | −0.478 | −0.474 | −0.474 | −0.475 | −0.275 |
N(a) | 0.420 | 0.435 | 0.141 | 0.013 | ||||
N(b) | −0.143 | −0.140 | −0.112 | −0.016 | ||||
N2O | 0 | 0.004 | −0.437 | |||||
C | 0.08 | 0.080 | 0.102 | 0.543 | ||||
O(CO) | −0.08 | −0.088 | −0.164 | −0.261 | ||||
CO | 0 | −0.008 |
Atom/ Molecule | Charges of the Systems/e | |||||||
---|---|---|---|---|---|---|---|---|
Isolated Systems | IS1a | TS1a | MS1a | MS2a | MS3a | TS2a | MS4a | |
Cu | 0.622 | 0.639 | 0.785 | 0.809 | 0.807 | 0.806 | 0.725 | 0.685 |
O(N2O) | −0.278 | −0.306 | −0.515 | −0.530 | −0.526 | −0.527 | −0.504 | −0.265 |
N(a) | 0.420 | 0.449 | 0.148 | 0.006 | ||||
N(b) | −0.143 | −0.120 | −0.095 | −0.006 | ||||
N2O | 0 | 0.023 | −0.462 | |||||
C | 0.08 | 0.080 | 0.156 | 0.538 | ||||
O(CO) | −0.08 | −0.086 | −0.123 | −0.237 | ||||
CO | 0 | 0.006 |
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Su, S.; Ma, J.; Liu, Z.; Holiharimanana, D.; Sun, H. Catalytic Reduction of N2O by CO on Single-Atom Catalysts Au/C2N and Cu/C2N: A First-Principles Study. Catalysts 2023, 13, 578. https://doi.org/10.3390/catal13030578
Su S, Ma J, Liu Z, Holiharimanana D, Sun H. Catalytic Reduction of N2O by CO on Single-Atom Catalysts Au/C2N and Cu/C2N: A First-Principles Study. Catalysts. 2023; 13(3):578. https://doi.org/10.3390/catal13030578
Chicago/Turabian StyleSu, Shengyang, Junmei Ma, Zhenhua Liu, Domoina Holiharimanana, and Hao Sun. 2023. "Catalytic Reduction of N2O by CO on Single-Atom Catalysts Au/C2N and Cu/C2N: A First-Principles Study" Catalysts 13, no. 3: 578. https://doi.org/10.3390/catal13030578