A Unique Gas-Migration, Trapping, and Emitting Strategy for High-Loading Single Atomic Cd Sites for Carbon Dioxide Electroreduction.
basic_science · Level V
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- Record sourced from PubMed, PMID 33962514.
- Also identified by DOI 10.1021/acs.nanolett.1c00432.
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Abstract
Single-atom catalysts (SACs) exhibit great potential in heterogeneous catalysis. However, the achievement of obtaining high-loading SACs remains a bottleneck. Herein, we first demonstrate a unique gas-migration, trapping, and emitting strategy for building a kind of Cd-based SAC for CO<sub>2</sub> reduction (CO<sub>2</sub>RR). The gas-migration and trapping processes (≤750 °C) endows the material with an ultrahigh Cd loading amount of 30.3 wt %, while the emitting process can facilely modulate the loading amount from 30.3 to 1.4 wt %. For the CO<sub>2</sub>RR, the Cd-NC SACs with a loading amount of 18.4 wt % exhibits the maximum Faraday efficiency of 91.4% for CO at -0.728 V. The operando infrared spectroscopy studies prove the presence of main intermediates *COO<sup>-</sup>, *COOH, and *CO on Cd-NC-5M SACs during the catalytic process, indicating that the CO<sub>2</sub>RR follows the proton-decoupled electron-transfer mechanism. Density functional theory simulations reveal that the Cd-N<sub>4</sub> structure reduces the Gibbs free energy of the rate-determining step (the hydrogenation step of *COOH).