Electronic structure engineering to boost oxygen reduction activity by controlling the coordination of the central metal

Adjusting the electronic structure of the active center is a highly effective strategy for improving the performance of catalysts. Herein, we report an atomically dispersed catalyst (FeCl1N4/CNS), which realized for the first time a great improvement of the ORR by controlling the electronic structur...

Full description

Saved in:
Bibliographic Details
Main Authors: Han, Yunhu, Wang, Yanggang, Xu, Ruirui, Chen, Wenxing, Zheng, Lirong, Han, Aijuan, Zhu, Youqi, Zhang, Jian, Zhang, Huabin, Luo, Jun, Chen, Chen, Peng, Qing, Wang, Dingsheng, Li, Yadong
Other Authors: School of Chemical and Biomedical Engineering
Format: Article
Language:English
Published: 2020
Subjects:
Online Access:https://hdl.handle.net/10356/144573
Tags: Add Tag
No Tags, Be the first to tag this record!
Institution: Nanyang Technological University
Language: English
id sg-ntu-dr.10356-144573
record_format dspace
spelling sg-ntu-dr.10356-1445732020-11-13T02:23:39Z Electronic structure engineering to boost oxygen reduction activity by controlling the coordination of the central metal Han, Yunhu Wang, Yanggang Xu, Ruirui Chen, Wenxing Zheng, Lirong Han, Aijuan Zhu, Youqi Zhang, Jian Zhang, Huabin Luo, Jun Chen, Chen Peng, Qing Wang, Dingsheng Li, Yadong School of Chemical and Biomedical Engineering Engineering::Chemical engineering Chlorine Electrocatalysts Adjusting the electronic structure of the active center is a highly effective strategy for improving the performance of catalysts. Herein, we report an atomically dispersed catalyst (FeCl1N4/CNS), which realized for the first time a great improvement of the ORR by controlling the electronic structure of the central metal with a coordinated chlorine. The half-wave potential of FeCl1N4/CNS is E1/2 = 0.921 V, which is the highest among the reported values for non-precious metal electrocatalysts and far exceeds that of FeN4/CN and commercial Pt/C in alkaline solution. Besides an exceptionally high kinetic current density (Jk) of 41.11 mA cm−2 at 0.85 V, it also has a good methanol tolerance and outstanding stability. Experiments and DFT demonstrated that the near-range interaction with chlorine and the long-range interaction with sulfur of Fe modulated the electronic structure of the active site, thus resulting in a great improvement of the ORR in alkaline media. The present findings could open new avenues for the design of superior electrocatalysts. 2020-11-13T02:23:39Z 2020-11-13T02:23:39Z 2018 Journal Article Han, Y., Wang, Y., Xu, R., Chen, W., Zheng, L., Han, A., ... Li, Y. (2018). Electronic structure engineering to boost oxygen reduction activity by controlling the coordination of the central metal. Energy & Environmental Science, 11(9), 2348--2352. doi:10.1039/C8EE01481G 1754-5692 https://hdl.handle.net/10356/144573 10.1039/C8EE01481G 9 11 2348 2352 en Energy & Environmental Science © 2018 The Royal Society of Chemistry. All rights reserved.
institution Nanyang Technological University
building NTU Library
continent Asia
country Singapore
Singapore
content_provider NTU Library
collection DR-NTU
language English
topic Engineering::Chemical engineering
Chlorine
Electrocatalysts
spellingShingle Engineering::Chemical engineering
Chlorine
Electrocatalysts
Han, Yunhu
Wang, Yanggang
Xu, Ruirui
Chen, Wenxing
Zheng, Lirong
Han, Aijuan
Zhu, Youqi
Zhang, Jian
Zhang, Huabin
Luo, Jun
Chen, Chen
Peng, Qing
Wang, Dingsheng
Li, Yadong
Electronic structure engineering to boost oxygen reduction activity by controlling the coordination of the central metal
description Adjusting the electronic structure of the active center is a highly effective strategy for improving the performance of catalysts. Herein, we report an atomically dispersed catalyst (FeCl1N4/CNS), which realized for the first time a great improvement of the ORR by controlling the electronic structure of the central metal with a coordinated chlorine. The half-wave potential of FeCl1N4/CNS is E1/2 = 0.921 V, which is the highest among the reported values for non-precious metal electrocatalysts and far exceeds that of FeN4/CN and commercial Pt/C in alkaline solution. Besides an exceptionally high kinetic current density (Jk) of 41.11 mA cm−2 at 0.85 V, it also has a good methanol tolerance and outstanding stability. Experiments and DFT demonstrated that the near-range interaction with chlorine and the long-range interaction with sulfur of Fe modulated the electronic structure of the active site, thus resulting in a great improvement of the ORR in alkaline media. The present findings could open new avenues for the design of superior electrocatalysts.
author2 School of Chemical and Biomedical Engineering
author_facet School of Chemical and Biomedical Engineering
Han, Yunhu
Wang, Yanggang
Xu, Ruirui
Chen, Wenxing
Zheng, Lirong
Han, Aijuan
Zhu, Youqi
Zhang, Jian
Zhang, Huabin
Luo, Jun
Chen, Chen
Peng, Qing
Wang, Dingsheng
Li, Yadong
format Article
author Han, Yunhu
Wang, Yanggang
Xu, Ruirui
Chen, Wenxing
Zheng, Lirong
Han, Aijuan
Zhu, Youqi
Zhang, Jian
Zhang, Huabin
Luo, Jun
Chen, Chen
Peng, Qing
Wang, Dingsheng
Li, Yadong
author_sort Han, Yunhu
title Electronic structure engineering to boost oxygen reduction activity by controlling the coordination of the central metal
title_short Electronic structure engineering to boost oxygen reduction activity by controlling the coordination of the central metal
title_full Electronic structure engineering to boost oxygen reduction activity by controlling the coordination of the central metal
title_fullStr Electronic structure engineering to boost oxygen reduction activity by controlling the coordination of the central metal
title_full_unstemmed Electronic structure engineering to boost oxygen reduction activity by controlling the coordination of the central metal
title_sort electronic structure engineering to boost oxygen reduction activity by controlling the coordination of the central metal
publishDate 2020
url https://hdl.handle.net/10356/144573
_version_ 1688665270364667904