skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

This content will become publicly available on January 27, 2021

Title: Simultaneously Integrating Single Atomic Cobalt Sites and Co 9 S 8 Nanoparticles into Hollow Carbon Nanotubes as Trifunctional Electrocatalysts for Zn–Air Batteries to Drive Water Splitting

Abstract

The development of rechargeable metal–air batteries and water electrolyzers are highly constrained by electrocatalysts for the oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER). However, the construction of efficient trifunctional electrocatalysts for ORR/OER/HER are highly desirable yet challenging. Herein, hollow carbon nanotubes integrated single cobalt atoms with Co9S8 nanoparticles (CoSA + Co 9S 8/HCNT) are fabricated by a straightforward in situ self-sacrificing strategy. The structure of the CoSA + Co 9S 8/HCNT are verified by X-ray absorption spectroscopy and aberration-corrected scanning transmission electron microscopy. Theoretical calculations and experimental results embrace the synergistic effects between Co 9S 8 nanoparticles and single cobalt atoms through optimizing the electronic configuration of the CoN4 active sites to lower the reaction barrier and facilitating the ORR, OER, and HER simultaneously. Consequently, rechargeable liquid and all-solid-state flexible Zn–air batteries based on CoSA + Co 9S 8/HCNT exhibit remarkable stability and excellent power density of 177.33 and 51.85 mW cm -2, respectively, better than Pt/C + RuO 2 counterparts. Moreover, the as-fabricated Zn–air batteries can drive an overall water splitting device assembled with CoSA + Co 9S 8/HCNT and achieve a current density of 10 mA cm -2 at a low voltagemore » of 1.59 V, also superior to Pt/C + RuO 2. Therefore, this work presents a promising approach to an efficient trifunctional electrocatalyst toward practical applications.« less

Authors:
 [1];  [2];  [1];  [1];  [1];  [1];  [1]; ORCiD logo [3]
  1. College of Chemistry/Institute of Polymers and Energy ChemistryNanchang University 999 Xuefu Avenue Nanchang 330031 China
  2. Stanford Synchrotron Radiation Lightsource (SSRL)SLAC National Accelerator Laboratory Menlo Park CA 94025 USA
  3. College of Chemistry/Institute of Polymers and Energy ChemistryNanchang University 999 Xuefu Avenue Nanchang 330031 China; Institute of Advanced Scientific Research (iASR)Jiangxi Normal University 99 Ziyang Avenue Nanchang 330022 China
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1605181
Grant/Contract Number:  
[AC02-76SF00515; 21704038; 51763018; 51761135114; 20171ACB21009; 2018ACB21021; 20192BCB23001; BX201700112; 2018M632599]
Resource Type:
Accepted Manuscript
Journal Name:
Small
Additional Journal Information:
[ Journal Volume: 16; Journal Issue: 10]; Journal ID: ISSN 1613-6810
Publisher:
Wiley
Country of Publication:
United States
Language:
English

Citation Formats

Li, Yizhe, Cao, Rui, Li, Longbin, Tang, Xiannong, Chu, Tinglin, Huang, Bingyu, Yuan, Kai, and Chen, Yiwang. Simultaneously Integrating Single Atomic Cobalt Sites and Co9 S8 Nanoparticles into Hollow Carbon Nanotubes as Trifunctional Electrocatalysts for Zn–Air Batteries to Drive Water Splitting. United States: N. p., 2020. Web. doi:10.1002/smll.201906735.
Li, Yizhe, Cao, Rui, Li, Longbin, Tang, Xiannong, Chu, Tinglin, Huang, Bingyu, Yuan, Kai, & Chen, Yiwang. Simultaneously Integrating Single Atomic Cobalt Sites and Co9 S8 Nanoparticles into Hollow Carbon Nanotubes as Trifunctional Electrocatalysts for Zn–Air Batteries to Drive Water Splitting. United States. doi:10.1002/smll.201906735.
Li, Yizhe, Cao, Rui, Li, Longbin, Tang, Xiannong, Chu, Tinglin, Huang, Bingyu, Yuan, Kai, and Chen, Yiwang. Mon . "Simultaneously Integrating Single Atomic Cobalt Sites and Co9 S8 Nanoparticles into Hollow Carbon Nanotubes as Trifunctional Electrocatalysts for Zn–Air Batteries to Drive Water Splitting". United States. doi:10.1002/smll.201906735.
@article{osti_1605181,
title = {Simultaneously Integrating Single Atomic Cobalt Sites and Co9 S8 Nanoparticles into Hollow Carbon Nanotubes as Trifunctional Electrocatalysts for Zn–Air Batteries to Drive Water Splitting},
author = {Li, Yizhe and Cao, Rui and Li, Longbin and Tang, Xiannong and Chu, Tinglin and Huang, Bingyu and Yuan, Kai and Chen, Yiwang},
abstractNote = {The development of rechargeable metal–air batteries and water electrolyzers are highly constrained by electrocatalysts for the oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER). However, the construction of efficient trifunctional electrocatalysts for ORR/OER/HER are highly desirable yet challenging. Herein, hollow carbon nanotubes integrated single cobalt atoms with Co9S8 nanoparticles (CoSA + Co9S8/HCNT) are fabricated by a straightforward in situ self-sacrificing strategy. The structure of the CoSA + Co9S8/HCNT are verified by X-ray absorption spectroscopy and aberration-corrected scanning transmission electron microscopy. Theoretical calculations and experimental results embrace the synergistic effects between Co9S8 nanoparticles and single cobalt atoms through optimizing the electronic configuration of the CoN4 active sites to lower the reaction barrier and facilitating the ORR, OER, and HER simultaneously. Consequently, rechargeable liquid and all-solid-state flexible Zn–air batteries based on CoSA + Co9S8/HCNT exhibit remarkable stability and excellent power density of 177.33 and 51.85 mW cm-2, respectively, better than Pt/C + RuO2 counterparts. Moreover, the as-fabricated Zn–air batteries can drive an overall water splitting device assembled with CoSA + Co9S8/HCNT and achieve a current density of 10 mA cm-2 at a low voltage of 1.59 V, also superior to Pt/C + RuO2. Therefore, this work presents a promising approach to an efficient trifunctional electrocatalyst toward practical applications.},
doi = {10.1002/smll.201906735},
journal = {Small},
number = [10],
volume = [16],
place = {United States},
year = {2020},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on January 27, 2021
Publisher's Version of Record

Save / Share:

Works referenced in this record:

Novel MOF-Derived Co@N-C Bifunctional Catalysts for Highly Efficient Zn-Air Batteries and Water Splitting
journal, January 2018

  • Zhang, Mingdao; Dai, Quanbin; Zheng, Hegen
  • Advanced Materials, Vol. 30, Issue 10
  • DOI: 10.1002/adma.201705431

Defect-rich and ultrathin N doped carbon nanosheets as advanced trifunctional metal-free electrocatalysts for the ORR, OER and HER
journal, January 2019

  • Jiang, Hao; Gu, Jinxing; Zheng, Xusheng
  • Energy & Environmental Science, Vol. 12, Issue 1
  • DOI: 10.1039/C8EE03276A

Structural Design and Electronic Modulation of Transition-Metal-Carbide Electrocatalysts toward Efficient Hydrogen Evolution
journal, August 2018

  • Gao, Qingsheng; Zhang, Wenbiao; Shi, Zhangping
  • Advanced Materials, Vol. 31, Issue 2
  • DOI: 10.1002/adma.201802880

A Review of Precious-Metal-Free Bifunctional Oxygen Electrocatalysts: Rational Design and Applications in Zn−Air Batteries
journal, August 2018

  • Wang, Hao-Fan; Tang, Cheng; Zhang, Qiang
  • Advanced Functional Materials, Vol. 28, Issue 46
  • DOI: 10.1002/adfm.201803329

Atomic Fe‐Doped MOF‐Derived Carbon Polyhedrons with High Active‐Center Density and Ultra‐High Performance toward PEM Fuel Cells
journal, February 2019


Electronic structure and stability of the pentlandites Co 9 S 8 and ( F e , N i ) 9 S 8
journal, October 2002


The Hydrogen Evolution Reaction in Alkaline Solution: From Theory, Single Crystal Models, to Practical Electrocatalysts
journal, May 2018

  • Zheng, Yao; Jiao, Yan; Vasileff, Anthony
  • Angewandte Chemie International Edition, Vol. 57, Issue 26
  • DOI: 10.1002/anie.201710556

Atomic Fe Dispersed on N-Doped Carbon Hollow Nanospheres for High-Efficiency Electrocatalytic Oxygen Reduction
journal, December 2018


A universal principle for a rational design of single-atom electrocatalysts
journal, April 2018


In Situ Charge Exfoliated Soluble Covalent Organic Framework Directly Used for Zn–Air Flow Battery
journal, December 2018


Batteries and fuel cells for emerging electric vehicle markets
journal, April 2018


Wavelet analysis of extended x-ray absorption fine structure data
journal, March 2005


Achievements, challenges and perspectives on cathode catalysts in proton exchange membrane fuel cells for transportation
journal, July 2019


Understanding Catalytic Activity Trends in the Oxygen Reduction Reaction
journal, December 2017


Ambient Synthesis of Single‐Atom Catalysts from Bulk Metal via Trapping of Atoms by Surface Dangling Bonds
journal, September 2019


PdMo bimetallene for oxygen reduction catalysis
journal, September 2019


Cobalt Covalent Doping in MoS 2 to Induce Bifunctionality of Overall Water Splitting
journal, May 2018


Nitrogen-doped Carbon-CoO x Nanohybrids: A Precious Metal Free Cathode that Exceeds 1.0 W cm −2 Peak Power and 100 h Life in Anion-Exchange Membrane Fuel Cells
journal, November 2018

  • Peng, Xiong; Omasta, Travis J.; Magliocca, Emanuele
  • Angewandte Chemie International Edition, Vol. 58, Issue 4
  • DOI: 10.1002/anie.201811099

Novel Iron/Cobalt-Containing Polypyrrole Hydrogel-Derived Trifunctional Electrocatalyst for Self-Powered Overall Water Splitting
journal, March 2017


Highly uniform Ru nanoparticles over N-doped carbon: pH and temperature-universal hydrogen release from water reduction
journal, January 2018

  • Wang, Jing; Wei, Zhongzhe; Mao, Shanjun
  • Energy & Environmental Science, Vol. 11, Issue 4
  • DOI: 10.1039/C7EE03345A

Identifying the Key Role of Pyridinic-N-Co Bonding in Synergistic Electrocatalysis for Reversible ORR/OER
journal, April 2018


In situ nanoarchitecturing and active-site engineering toward highly efficient carbonaceous electrocatalysts
journal, May 2019


Trifunctional Self‐Supporting Cobalt‐Embedded Carbon Nanotube Films for ORR, OER, and HER Triggered by Solid Diffusion from Bulk Metal
journal, January 2019

  • Yang, Zhengkun; Zhao, Changming; Qu, Yunteng
  • Advanced Materials, Vol. 31, Issue 12
  • DOI: 10.1002/adma.201808043

Two-Dimensional Core-Shelled Porous Hybrids as Highly Efficient Catalysts for the Oxygen Reduction Reaction
journal, April 2016

  • Yuan, Kai; Zhuang, Xiaodong; Fu, Haiyan
  • Angewandte Chemie International Edition, Vol. 55, Issue 24
  • DOI: 10.1002/anie.201600850

Nonprecious Metal Catalysts for Oxygen Reduction in Heterogeneous Aqueous Systems
journal, December 2017


Nitrogen-Coordinated Single Cobalt Atom Catalysts for Oxygen Reduction in Proton Exchange Membrane Fuel Cells
journal, January 2018

  • Wang, Xiao Xia; Cullen, David A.; Pan, Yung-Tin
  • Advanced Materials, Vol. 30, Issue 11
  • DOI: 10.1002/adma.201706758

Insights into the role of active site density in the fuel cell performance of Co-N-C catalysts
journal, November 2019


A Cobalt–Iron Double-Atom Catalyst for the Oxygen Evolution Reaction
journal, August 2019

  • Bai, Lichen; Hsu, Chia-Shuo; Alexander, Duncan T. L.
  • Journal of the American Chemical Society, Vol. 141, Issue 36
  • DOI: 10.1021/jacs.9b05268

Single Cobalt Atom and N Codoped Carbon Nanofibers as Highly Durable Electrocatalyst for Oxygen Reduction Reaction
journal, September 2017


MOF-Derived Hollow CoS Decorated with CeO x Nanoparticles for Boosting Oxygen Evolution Reaction Electrocatalysis
journal, June 2018

  • Xu, Huajie; Cao, Jing; Shan, Changfu
  • Angewandte Chemie International Edition, Vol. 57, Issue 28
  • DOI: 10.1002/anie.201804673

Stereodefined Codoping of sp-N and S Atoms in Few-Layer Graphdiyne for Oxygen Evolution Reaction
journal, April 2019

  • Zhao, Yasong; Yang, Nailiang; Yao, Huiying
  • Journal of the American Chemical Society, Vol. 141, Issue 18
  • DOI: 10.1021/jacs.8b13695

Iron‐Free Cathode Catalysts for Proton‐Exchange‐Membrane Fuel Cells: Cobalt Catalysts and the Peroxide Mitigation Approach
journal, December 2018

  • Wang, Xiao Xia; Prabhakaran, Venkateshkumar; He, Yanghua
  • Advanced Materials, Vol. 31, Issue 31
  • DOI: 10.1002/adma.201805126