.png){kind=icon}
.png){kind=icon}
Return
Auene-Supported Transition-Metal Single-Atom Catalysts for Promising Electrocatalytic Nitrogen Reduction
.png){kind=icon}
PRE
AI
L
J
DOI：10.1002/chem.71194.png)
.png){kind=icon}
Original request for help.png){kind=icon}
Share.png){kind=icon}
Save
Abstract
En 中文
The electrochemical nitrogen reduction reaction (NRR) provides a sustainable route to ammonia synthesis, but its efficiency is hindered by the inert N≡N bond and competing hydrogen evolution reaction (HER). Herein, we systematically screened 25 transition-metal (TM) single-atom catalysts (SACs) supported on goldene, denoted as TM@Auene, using density functional theory (DFT). Sixteen TM@Auene systems capable of end-on N2 adsorption were evaluated across distal, alternating, and mixed NRR pathways. Mo@Auene and Re@Auene exhibited high NRR catalytic activity with low limiting potentials of −0.04 and −0.10 V, respectively, associated with effective N2 activation through synergistic σ-donation and π*-back-donation. A volcano-type relationship was established between NRR activity and occupied d-electron number, positioning Mo and Re near the optimum. HER competition was assessed, with Nb@Auene, Mo@Auene, W@Auene, Re@Auene, and Os@Auene showing favorable NRR selectivity. For Mo@Auene and Re@Auene, Pourbaix diagram analysis and ab initio molecular dynamics (AIMD) simulations provide preliminary support for electrochemical stability and short-timescale structural integrity under NRR-relevant conditions. These results identify Mo@Auene as a promising NRR candidate and highlight Auene-supported SACs as a descriptor-guided platform for catalyst design.
Keywords:
Auene
density functional theory
electrochemical nitrogen reduction reaction
single-atom catalysts
Journal
C
IF:
3.7
Papers:
1.1K
Citations:
20
Organization
Cited Papers