Atomically-precise dopant-controlled single cluster catalysis for electrochemical nitrogen reduction.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 32873783.
- Also identified by DOI 10.1038/s41467-020-18080-w and PMC identifier 7463028.
- Licence recorded as CC BY.
- The licence permits redistribution, so the abstract is shown in full and the full text is available from the publisher.
Abstract
The ability to precisely engineer the doping of sub-nanometer bimetallic clusters offers exciting opportunities for tailoring their catalytic performance with atomic accuracy. However, the fabrication of singly dispersed bimetallic cluster catalysts with atomic-level control of dopants has been a long-standing challenge. Herein, we report a strategy for the controllable synthesis of a precisely doped single cluster catalyst consisting of partially ligand-enveloped Au<sub>4</sub>Pt<sub>2</sub> clusters supported on defective graphene. This creates a bimetal single cluster catalyst (Au<sub>4</sub>Pt<sub>2</sub>/G) with exceptional activity for electrochemical nitrogen (N<sub>2</sub>) reduction. Our mechanistic study reveals that each N<sub>2</sub> molecule is activated in the confined region between cluster and graphene. The heteroatom dopant plays an indispensable role in the activation of N<sub>2</sub> via an enhanced back donation of electrons to the N<sub>2</sub> LUMO. Moreover, besides the heteroatom Pt, the catalytic performance of single cluster catalyst can be further tuned by using Pd in place of Pt as the dopant.