Li, Z;
Tian, Z;
Cheng, H;
Wang, T;
Zhang, W;
Lu, Y;
Lai, Y;
(2023)
Engineering d-band center of FeN<inf>4</inf> moieties for efficient oxygen reduction reaction electrocatalysts.
Energy Storage Materials
, 59
, Article 102764. 10.1016/j.ensm.2023.04.003.
(In press).
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Abstract
Atomically-dispersed FeN4 moieties are emerging as low-cost electrocatalysts for oxygen reduction reaction (ORR), which can be applied in fuel cells and metal-air batteries. Whereas, the unsatisfactory position of the d-band center from the metal sites offered by FeN4 affects the adsorption-desorption behaviors of oxygenated intermediates, further impeding the improvement of their ORR performances. Herein, we report a well-designed diatomic Fe/Zn-CNHC catalyst on a microporous hollow support. This strategy drives the position of the d-band center of Fe upward, thus making FeN4 active sites more favorable and stable during the ORR kinetic processes. The material exhibits an excellent ORR activity with a half-wave potential of 0.91 V and excellent stability (insignificant attenuation after 5,000 cycles), surpassing commercial Pt/C and many other single-atom catalysts. DFT calculations further indicate that the tuning effect of Zn on the d-orbital electron distribution of Fe facilitates the stretching and cleavage of Fe-O, thus accelerating the rate-determining step. This work presents a simple strategy to fabricate well-defined diatomic coordination in single-atom ORR electrocatalysts and inspires future research on developing new syntheses to control the coordination of single-atom electrocatalysts.
| Type: | Article |
|---|---|
| Title: | Engineering d-band center of FeN<inf>4</inf> moieties for efficient oxygen reduction reaction electrocatalysts |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1016/j.ensm.2023.04.003 |
| Language: | English |
| Additional information: | © 2023 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/). |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering |
| URI: | https://discovery-pp.ucl.ac.uk/id/eprint/10168462 |
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