期刊
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
卷 47, 期 63, 页码 27000-27011出版社
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.ijhydene.2022.06.055
关键词
Computational screening; Oxygen reduction reaction; Oxygen evolution reaction; Bifunctional ORR; OER catalyst; Density functional theory
资金
- National Science Foundation of China [51922113, 21703076]
- Natural Science Foundation of Jiangsu Province of China [BK20211609]
- Natural Science Research Program of Jiangsu Higher Education Institutions of China [18KJA140001]
- Natural Science Research Project of Huaian City of China [HABZ202117]
- HK PolyU Project [1-ZE8C]
- VILLUM FONDEN [9455]
This study systematically explores the potential of synthesized one-dimensional transition metal salen-type complexes (TM-SCs) as bi-functional electrocatalysts for ORR and OER through computational screening. Different macrocyclic ligands play a crucial role in governing the catalytic performances, with Co-SCs showing the highest bifunctional catalytic activities. The excellent electrocatalytic performance of Co salen-based chain is highlighted, showing promising implications for catalyst optimizations.
Developing high activities, stable, non-precious metal based bi-functional electrocatalysts oxygen evolution/reduction reactions (OER/ORR) in rechargeable metal-air batteries and regenerative fuel cell technologies is essential for future energy conversion and storage. In this work, the potential of utilizing the synthesized one-dimensional transition metal salen-type complexes (TM-SCs) as bi-functional electrocatalysts of ORR and OER is sys-tematically explored by computational screening approach. The results demonstrate that different types of macrocyclic ligands, including N2O2, N3O and N4 as donor groups around the active sites, govern the OER/ORR catalytic performances. Co-SCs with N2O2 ligands exhibit the highest bifunctional catalytic activities. In particular, low limiting over -potentials of 0.22 V for OER and 0.33 V for ORR can be observed on Co sites, which are even superior to those of noble metal catalysts. Analyzing the linear relationships between the adsorption strength of intermediates and the overpotentials shows that the origin of excellent electrocatalytic performance is the smaller slope (0.86) for OOH* vs OH* on TM-SCs compared to metal surfaces, resulting in strengthened binding of the OOH* interme-diate. Besides, the adsorption energies of the intermediates bound on Co-N2O2 are close to the ideal values, while too strong on the Co-N3O and Co-N4 catalysts. By applying external strains, the adsorption strengths of reaction intermediates can be further modulated due to the tunable d-band centers, and the resulting ORR/OER activities are further boosted. Considering that the Co salen-based chain has been synthesized experimentally, this work highlights the excellent electrocatalytic performances of this new material and devises novel strategy by straining for catalyst optimizations.(c) 2022 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
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