Tetrahedral W 4 cluster confined in graphene-like C 2 N enables electrocatalytic nitrogen reduction from theoretical perspective

Zhang, Jin; Fang, Cong; Li, Yang; An, Wei

doi:10.1088/1361-6528/ac5bb9

Tetrahedral W ₄ cluster confined in graphene-like C ₂ N enables electrocatalytic nitrogen reduction from theoretical perspective

Journal Article · 25 March 2022 · Nanotechnology

DOI:https://doi.org/10.1088/1361-6528/ac5bb9· OSTI ID:1982444

Zhang, Jin; Fang, Cong; Li, Yang;

Abstract Exploring the format of active site is essential to further the understanding of an electrocatalyst working under ambient conditions. Herein, we present a DFT study of electrocatalytic nitrogen reduction (eNRR) on W₄tetrahedron embedded in graphene-like C₂N (denoted as W₄@C₂N). Our results demonstrate that N-affinity of active sites on W₄dominate over single-atom site, rendering *NH₂ + (H⁺ + e^-) →*NH₃invariably the potential-determining step (PDS) of eNRR via consecutive or distal route (U_L = -0.68 V) to ammonia formation. However, *NHNH₂ + (H⁺ + e^-) →*NH₂NH₂has become the PDS (U_L = -0.54 V) via enzymatic route towards NH₂NH₂formation and thereafter desorption, making W₄@C₂N a potentially promising catalyst for hydrazine production from eNRR. Furthermore, eNRR is competitive with hydrogen evolution reaction (U_L = -0.78 V) on W₄@C₂N, which demonstrated sufficient thermal stability and electric property for electrode application.

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)

Sponsoring Organization:: USDOE Office of Science (SC)

DOE Contract Number:: SC0012704

OSTI ID:: 1982444

Journal Information:: Nanotechnology, Vol. 33, Issue 24; ISSN 0957-4484

Publisher:: IOP Publishing

Country of Publication:: United States

Language:: English

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