A Homo-Triatomic Molybdenum Cluster Catalyst Enables Synergistic Optimization of Multi-Step Sulfur Reduction Chemistry.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 41603195.
- Also identified by DOI 10.1002/adma.72365.
- No licence information is recorded for this record.
- Because redistribution is not established, this page shows the abstract only. Follow the links below for the full text.
Abstract
The isolated single-active sites of single-atom catalysts (SACs) often suffer from simultaneously maintaining the optimal adsorption states of multiple lithium polysulfide intermediates in sulfur redox reactions of Li-S batteries. Herein, we report a homo-triatomic molybdenum cluster catalyst with Mo<sub>3</sub>-O<sub>3</sub>N<sub>3</sub> motifs embedded within a carbon matrix (Mo<sub>3</sub>/ONC) that addresses this challenge. The Mo<sub>3</sub>-O<sub>3</sub>N<sub>3</sub> motifs with a triangular configuration feature multi-active sites and interatomic synergies, which can flexibly adjust the corresponding Mo─S pathway according to different intermediate sulfur species, thereby making the adsorption strength of all species favorable. Meanwhile, the optimized Mo─S interactions can induce more electrons to transfer from the intermediate sulfur species to the Mo<sub>3</sub>-O<sub>3</sub>N<sub>3</sub> catalytic sites, thus weakening the S─S bond and remarkably reducing the energy barriers for the sulfur conversion. Besides, the electrochemical and in situ spectroscopic experiments disclose that the sulfur redox kinetics on Mo<sub>3</sub>/ONC is significantly improved compared to the Mo-single-atom catalyst (Mo<sub>1</sub>/ONC) counterpart. As thus, the as-designed Mo<sub>3</sub>/ONC catalyst renders the Li-S battery with a large rate capability of 661.2 mAh g<sup>-1</sup> and a capacity decay as low as 0.027% per cycle at 10 C for 1200 cycles. This work provides a new perspective on the fundamental design principles of triatomic catalysts for improving the Li-S performance.