Boosting Oxygen Reduction of Single Iron Active Sites via Geometric and Electronic Engineering: Nitrogen and Phosphorus Dual Coordination
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- 5 January 2020
- journal article
- research article
- Published by American Chemical Society (ACS) in Journal of the American Chemical Society
- Vol. 142 (5), 2404-2412
- https://doi.org/10.1021/jacs.9b11852
Abstract
Atomically dispersed transition metal active sites have emerged as one of the most important fields of study because they display promising performance in catalysis and have potential to serve as ideal models for fundamental understanding. How-ever, both the preparation and determination of such active sites remain a challenge. The structural engineering of carbon and nitrogen coordinated metal sites (M-N-C, M=Fe, Co, Ni, Mn, Cu, etc.) via employing new heteroatoms, e.g. P and S, remains challenging. In this study, carbon nanosheets embedded with nitrogen and phosphorus dual-coordinated iron active sites (denoted as Fe-N/P-C) were developed and determined using cutting edge techniques. Both experimental and theoretical results suggested that the N and P dual-coordinated iron sites were favorable for oxygen intermediate adsorption/desorption, resulting in accelerated reaction kinetics and promising catalytic oxygen reduction activity. This work not only provides effi-cient way to prepare well-defined single atom active sites to boost catalytic performance but also paves the way to identify the dual-coordinated single metal atom sites.Funding Information
- China Postdoctoral Science Foundation (2018M632599)
- Shanghai Municipal Human Resources and Social Security Bureau (18PJ1406100, 19JC412600)
- Central China Normal University (CCNU18TS045)
- Ministry of Human Resources and Social Security (BX201700112)
- National Natural Science Foundation of China (2018CFB531, 21704038, 21720102002, 5171101862, 51722304, 51761135114, 51811530013, 51973114)
- Natural Science Foundation of Jiangxi Province (20171ACB21009, 2018ACB21021, 20192BCB23001)
- National Key Research and Development Program of China (2017YFE9134000)
This publication has 55 references indexed in Scilit:
- Identification of active sites for acidic oxygen reduction on carbon catalysts with and without nitrogen dopingNature Catalysis, 2019
- Fe–N–C electrocatalyst with dense active sites and efficient mass transport for high-performance proton exchange membrane fuel cellsNature Catalysis, 2019
- Tunable intrinsic strain in two-dimensional transition metal electrocatalystsScience, 2019
- Ultralow-loading platinum-cobalt fuel cell catalysts derived from imidazolate frameworksScience, 2018
- In situ Raman spectroscopic evidence for oxygen reduction reaction intermediates at platinum single-crystal surfacesNature Energy, 2018
- Atomically dispersed manganese catalysts for oxygen reduction in proton-exchange membrane fuel cellsNature Catalysis, 2018
- Direct transformation of bulk copper into copper single sites via emitting and trapping of atomsNature Catalysis, 2018
- Nonprecious Metal Catalysts for Oxygen Reduction in Heterogeneous Aqueous SystemsChemical Reviews, 2018
- Design of N-Coordinated Dual-Metal Sites: A Stable and Active Pt-Free Catalyst for Acidic Oxygen Reduction ReactionJournal of the American Chemical Society, 2017
- Direct atomic-level insight into the active sites of a high-performance PGM-free ORR catalystScience, 2017