Performance of the nitrogen reduction reaction on metal bound g-C₆N₆: a combined approach of machine learning and DFT

Abstract

Developing a cost-effective and environmentally benign substitute for the energy-intensive Haber-Bosch process for the production of ammonia is a global challenge. Electrocatalytic nitrogen reduction reaction (NRR) under ambient condition through...

Tuning the Coordination Environment of Single‐Atom Iron Catalysts Towards Effective Nitrogen Reduction

“…The comparison analysis suggests these Fe SACs have strong stability under ambient conditions. The binding strength is pretty comparable to the reported B/C 2 N [24] and TMÀ C 6 N 6 , [25] again demonstrating the property of their high stability. More characteristics regarding Fe SACs can be found in Table S1.…”

“…Therefore, when it comes to designing catalysts for a specific ChemCatChem reaction, a structure parameter reflecting the key structural change needs to be integrated into the search for effective descriptors. Datta et al [25] employed a combined approach of machine learning (ML) and DFT to search for effective eNRR descriptors and identified the covalent radius and the d-band center of SAC TM as most correlated descriptors. Enlighted by this, a comprehensive descriptor, including the electronic and structural parameters, can be proposed with the aid of large database and ML.…”

First‐principles Calculations Reveal Frictional Advantage for C2N/C6N6 van der Waals Heterostructures

“…In order to treat the exchange correlation functional, Perdew‐Burke‐Ernzerhof (PBE) within a generalized gradient approximation (GGA) has been taken into account. The two different structures of polymeric carbon nitride family, namely, C 2 N and C 6 N 6 have been taken for their versatile applications in various fields [23–26] . The computational cell of heterostructure is composed of 2×2 supercell of C 6 N 6 and $${\sqrt{3}\times \sqrt{3}}$$ supercell of C 2 N with 20 Å vacuum along Z‐direction to avoid the interaction between periodic images.…”

“…The two different structures of polymeric carbon nitride family, namely, C 2 N and C 6 N 6 have been taken for their versatile applications in various fields. [23][24][25][26] The computational cell of heterostructure is composed of 2 × 2 supercell of C 6 N 6 and ffi ffi ffi 3 p � ffi ffi ffi 3 p supercell of C 2 N with 20 Å vacuum along Zdirection to avoid the interaction between periodic images. The thermal stability of the heterostructure C 2 N/C 6 N 6 measured by ab initio molecular dynamics (AIMD) using VASP simulation package for the time period of 15 ps at 300 K, shows good agreement of DFT optimized and AIMD equilibrated structures.…”

Single-Atom Low-Valent Alkaline-Earth-Metal Catalysts for Electrochemical Nitrogen Reduction with an Acceptance–Backdonation Mechanism

“…Therefore, it is worthwhile to explore sustainable development strategies and efficient catalysts for ammonia synthesis. , Here, the electrocatalytic nitrogen reduction reaction (NRR) is an efficient approach for ammonia synthesis but also faces major issues, including large overpotential and low faradaic efficiency . Recently, single-atom catalysts (SACs), which exhibit high atom utilization, special electronic structure, tunable coordination, and outstanding catalytic activity, have been widely used as electrocatalysts in the NRR. − Generally, SACs include p-block nonmetal- and main-group-metal-based SACs, − d-block transition-metal-based SACs, , and f-block rare-earth-metal-based SACs, , which can effectively reduce inert N 2 through the classical electron “acceptance–donation” mechanism by p orbitals, d orbitals, and synergistic d and f orbitals,, respectively. However, the practical application of SACs in the NRR still has the problems of low activity and low selectivity, which makes it difficult to satisfy the industrial targets. ,, Hence, it is significant to develop highly effective SACs for NRR with good stability, high activity, and selectivity.…”