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Published on: December 6, 2021
Transition Metal-Embedded C4N4 Octahedral Rings as Highly Efficient Electrocatalysts for NO to NH3 Conversion: A
Hong Wang1, Yunfei Ma1, Jinkun Bai1
1School of Physics and Materials Science, Changji University, Changji 831100, China.
None:
The increasing pollution of nitric oxide (NO) along with the growing demand for ammonia (NH3) has brought the electrochemical NO reduction reaction (NORR) toward NH3 into the spotlight in the field of pollution control and green synthesis. In this study, 24 transition metal (TM) monatomic catalysts (TM-C4N4, TM = Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Y, Zr, Nb, Mo, Rh, Pd, Ag, Hf, Ta, W, Re, Os, Ir, Pt, Au) are systematically characterized by high-throughput first-principles calculations to assess their potential to convert NO to NH3. Based on a five-step screening strategy, Cr-C4N4 is identified as the most promising catalytic system in terms of key indicators of adsorption strength, reaction barrier, and product selectivity. Cr-C4N4 not only has the lowest limiting potential (UL = -0.10 eV) but also reveals excellent thermodynamic stability and high selectivity for the generation of NH3. The intrinsic correlation between the key physicochemical descriptors and ΔG*NO is demonstrated by combining machine learning and the SISSO algorithm. This work provides theoretical guidance for the efficient design of C4N4-supported single-atom catalysts in electrochemical NO to NH3 conversion.
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