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Title: Single Fe Atom on Hierarchically Porous S, N-Codoped Nanocarbon Derived from Porphyra Enable Boosted Oxygen Catalysis for Rechargeable Zn-Air Batteries

Abstract

Iron-nitrogen-carbon materials (Fe-N-C) are known for their excellent oxygen reduction reaction (ORR) performance. Unfortunately, they generally show a laggard oxygen evolution reaction (OER) activity, which results in a lethargic charging performance in rechargeable Zn-air batteries. Here porous S-doped Fe-N-C nanosheets are innovatively synthesized utilizing a scalable FeCl 3-encapsulated-porphyra precursor pyrolysis strategy. The obtained electrocatalyst exhibits ultrahigh ORR activity ( E 1/2 = 0.84 V vs reversible hydrogen electrode) and impressive OER performance ( Ej=10 = 1.64 V). The potential gap (Δ E = Ej=10 - E 1/2) is 0.80 V, outperforming that of most highly active bifunctional electrocatalysts reported to date. Furthermore, the key role of S involved in the atomically dispersed Fe-N x species on the enhanced ORR and OER activities is expounded for the first time by ultrasound-assisted extraction of the exclusive S source (taurine) from porphyra. Moreover, the assembled rechargeable Zn-air battery comprising this bifunctional electrocatalyst exhibits higher power density (225.1 mW cm -2) and lower charging-discharging overpotential (1.00 V, 100 mA cm -2 compared to Pt/C + RuO 2 catalyst). Here, the design strategy can expand the utilization of earth-abundant biomaterial-derived catalysts, and the mechanism investigations of S doping on the structure-activity relationship can inspire themore » progress of other functional electrocatalysts.« less

Authors:
 [1];  [1];  [2];  [1];  [1];  [3];  [3];  [1];  [1]; ORCiD logo [1]
  1. Central China Normal Univ., Wuhan (China)
  2. Central China Normal Univ., Wuhan (People's Republic of China)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1561217
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Small
Additional Journal Information:
Journal Volume: 15; Journal Issue: 24; Journal ID: ISSN 1613-6810
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; bifunctional catalysts; biomass; heteroatom doping; rechargeable Zn-air batteries; single-atom electrocatalysts

Citation Formats

Zhang, Jiting, Zhang, Meng, Zeng, Yan, Chen, Jisheng, Qiu, Lingxi, Zhou, Hua, Sun, Chengjun, Yu, Ying, Zhu, Chengzhou, and Zhu, Zhihong. Single Fe Atom on Hierarchically Porous S, N-Codoped Nanocarbon Derived from Porphyra Enable Boosted Oxygen Catalysis for Rechargeable Zn-Air Batteries. United States: N. p., 2019. Web. doi:10.1002/smll.201900307.
Zhang, Jiting, Zhang, Meng, Zeng, Yan, Chen, Jisheng, Qiu, Lingxi, Zhou, Hua, Sun, Chengjun, Yu, Ying, Zhu, Chengzhou, & Zhu, Zhihong. Single Fe Atom on Hierarchically Porous S, N-Codoped Nanocarbon Derived from Porphyra Enable Boosted Oxygen Catalysis for Rechargeable Zn-Air Batteries. United States. doi:10.1002/smll.201900307.
Zhang, Jiting, Zhang, Meng, Zeng, Yan, Chen, Jisheng, Qiu, Lingxi, Zhou, Hua, Sun, Chengjun, Yu, Ying, Zhu, Chengzhou, and Zhu, Zhihong. Mon . "Single Fe Atom on Hierarchically Porous S, N-Codoped Nanocarbon Derived from Porphyra Enable Boosted Oxygen Catalysis for Rechargeable Zn-Air Batteries". United States. doi:10.1002/smll.201900307.
@article{osti_1561217,
title = {Single Fe Atom on Hierarchically Porous S, N-Codoped Nanocarbon Derived from Porphyra Enable Boosted Oxygen Catalysis for Rechargeable Zn-Air Batteries},
author = {Zhang, Jiting and Zhang, Meng and Zeng, Yan and Chen, Jisheng and Qiu, Lingxi and Zhou, Hua and Sun, Chengjun and Yu, Ying and Zhu, Chengzhou and Zhu, Zhihong},
abstractNote = {Iron-nitrogen-carbon materials (Fe-N-C) are known for their excellent oxygen reduction reaction (ORR) performance. Unfortunately, they generally show a laggard oxygen evolution reaction (OER) activity, which results in a lethargic charging performance in rechargeable Zn-air batteries. Here porous S-doped Fe-N-C nanosheets are innovatively synthesized utilizing a scalable FeCl3-encapsulated-porphyra precursor pyrolysis strategy. The obtained electrocatalyst exhibits ultrahigh ORR activity (E1/2 = 0.84 V vs reversible hydrogen electrode) and impressive OER performance (Ej=10 = 1.64 V). The potential gap (ΔE = Ej=10 - E1/2) is 0.80 V, outperforming that of most highly active bifunctional electrocatalysts reported to date. Furthermore, the key role of S involved in the atomically dispersed Fe-Nx species on the enhanced ORR and OER activities is expounded for the first time by ultrasound-assisted extraction of the exclusive S source (taurine) from porphyra. Moreover, the assembled rechargeable Zn-air battery comprising this bifunctional electrocatalyst exhibits higher power density (225.1 mW cm-2) and lower charging-discharging overpotential (1.00 V, 100 mA cm-2 compared to Pt/C + RuO2 catalyst). Here, the design strategy can expand the utilization of earth-abundant biomaterial-derived catalysts, and the mechanism investigations of S doping on the structure-activity relationship can inspire the progress of other functional electrocatalysts.},
doi = {10.1002/smll.201900307},
journal = {Small},
number = 24,
volume = 15,
place = {United States},
year = {2019},
month = {5}
}

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