Localizing Tungsten Single Atoms around Tungsten Nitride Nanoparticles for Efficient Oxygen Reduction Electrocatalysis in Metal–Air Batteries

Abstract Combining isolated atomic active sites with those in nanoparticles for synergizing complex multistep catalysis is being actively pursued in the design of new electrocatalyst systems. However, these novel systems have been rarely studied due to the challenges with synthesis and analysis. Her...

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Main Authors: Yuanyuan Ma, Yong Yu, Junhui Wang, Jason Lipton, Hui Ning Tan, Lirong Zheng, Tong Yang, Zhaolin Liu, Xian Jun Loh, Stephen J. Pennycook, Lei Shen, Zongkui Kou, André D. Taylor, John Wang
Format: Article
Language:English
Published: Wiley 2022-10-01
Series:Advanced Science
Subjects:
Online Access:https://doi.org/10.1002/advs.202105192
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author Yuanyuan Ma
Yong Yu
Junhui Wang
Jason Lipton
Hui Ning Tan
Lirong Zheng
Tong Yang
Zhaolin Liu
Xian Jun Loh
Stephen J. Pennycook
Lei Shen
Zongkui Kou
André D. Taylor
John Wang
author_facet Yuanyuan Ma
Yong Yu
Junhui Wang
Jason Lipton
Hui Ning Tan
Lirong Zheng
Tong Yang
Zhaolin Liu
Xian Jun Loh
Stephen J. Pennycook
Lei Shen
Zongkui Kou
André D. Taylor
John Wang
author_sort Yuanyuan Ma
collection DOAJ
description Abstract Combining isolated atomic active sites with those in nanoparticles for synergizing complex multistep catalysis is being actively pursued in the design of new electrocatalyst systems. However, these novel systems have been rarely studied due to the challenges with synthesis and analysis. Herein, a synergistically catalytic performance is demonstrated with a 0.89 V (vs reversible hydrogen electrode) onset potential in the four‐step oxygen reduction reaction (ORR) by localizing tungsten single atoms around tungsten nitride nanoparticles confined into nitrogen‐doped carbon (W SAs/WNNC). Through density functional theory calculations, it is shown that each of the active centers in the synergistic entity feature a specific potential‐determining step in their respective reaction pathway that can be merged to optimize the intermediate steps involving scaling relations on individual active centers. Impressively, the W SAs/WNNC as the air cathode in all‐solid‐state Zn‐air and Al‐air batteries demonstrate competitive durability and reversibility, despite the acknowledged low activity of W‐based catalyst toward the ORR.
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spelling doaj.art-5af84d933b884090b0568d3b259ddc862022-12-22T03:37:17ZengWileyAdvanced Science2198-38442022-10-01928n/an/a10.1002/advs.202105192Localizing Tungsten Single Atoms around Tungsten Nitride Nanoparticles for Efficient Oxygen Reduction Electrocatalysis in Metal–Air BatteriesYuanyuan Ma0Yong Yu1Junhui Wang2Jason Lipton3Hui Ning Tan4Lirong Zheng5Tong Yang6Zhaolin Liu7Xian Jun Loh8Stephen J. Pennycook9Lei Shen10Zongkui Kou11André D. Taylor12John Wang13Department of Materials Science and Engineering Faculty of Engineering National University of Singapore Singapore 117574 SingaporeDepartment of Materials Science and Engineering Faculty of Engineering National University of Singapore Singapore 117574 SingaporeDepartment of Materials Science and Engineering Faculty of Engineering National University of Singapore Singapore 117574 SingaporeDepartment of Chemical and Biomolecular Engineering Tandon School of Engineering New York University Brooklyn NY 11201 USADepartment of Materials Science and Engineering Faculty of Engineering National University of Singapore Singapore 117574 SingaporeBeijing Synchrotron Radiation Facility Institute of High Energy Physics Chinese Academy of Sciences Beijing 100049 ChinaDepartment of Applied Physics The Hong Kong Polytechnic University Hung Hom Hong Kong 999077 P. R. ChinaInstitute of Materials Research and Engineering Agency for Science Technology and Research (A* STAR) 2 Fusionopolis Way Innovis 138634 SingaporeInstitute of Materials Research and Engineering Agency for Science Technology and Research (A* STAR) 2 Fusionopolis Way Innovis 138634 SingaporeDepartment of Materials Science and Engineering Faculty of Engineering National University of Singapore Singapore 117574 SingaporeDepartment of Mechanical Engineering National University of Singapore Singapore 117575 SingaporeState Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 P. R. ChinaDepartment of Chemical and Biomolecular Engineering Tandon School of Engineering New York University Brooklyn NY 11201 USADepartment of Materials Science and Engineering Faculty of Engineering National University of Singapore Singapore 117574 SingaporeAbstract Combining isolated atomic active sites with those in nanoparticles for synergizing complex multistep catalysis is being actively pursued in the design of new electrocatalyst systems. However, these novel systems have been rarely studied due to the challenges with synthesis and analysis. Herein, a synergistically catalytic performance is demonstrated with a 0.89 V (vs reversible hydrogen electrode) onset potential in the four‐step oxygen reduction reaction (ORR) by localizing tungsten single atoms around tungsten nitride nanoparticles confined into nitrogen‐doped carbon (W SAs/WNNC). Through density functional theory calculations, it is shown that each of the active centers in the synergistic entity feature a specific potential‐determining step in their respective reaction pathway that can be merged to optimize the intermediate steps involving scaling relations on individual active centers. Impressively, the W SAs/WNNC as the air cathode in all‐solid‐state Zn‐air and Al‐air batteries demonstrate competitive durability and reversibility, despite the acknowledged low activity of W‐based catalyst toward the ORR.https://doi.org/10.1002/advs.202105192metal–air batteriesoxygen reduction reactionsingle atom catalystssynergistic effecttungsten nitrides
spellingShingle Yuanyuan Ma
Yong Yu
Junhui Wang
Jason Lipton
Hui Ning Tan
Lirong Zheng
Tong Yang
Zhaolin Liu
Xian Jun Loh
Stephen J. Pennycook
Lei Shen
Zongkui Kou
André D. Taylor
John Wang
Localizing Tungsten Single Atoms around Tungsten Nitride Nanoparticles for Efficient Oxygen Reduction Electrocatalysis in Metal–Air Batteries
Advanced Science
metal–air batteries
oxygen reduction reaction
single atom catalysts
synergistic effect
tungsten nitrides
title Localizing Tungsten Single Atoms around Tungsten Nitride Nanoparticles for Efficient Oxygen Reduction Electrocatalysis in Metal–Air Batteries
title_full Localizing Tungsten Single Atoms around Tungsten Nitride Nanoparticles for Efficient Oxygen Reduction Electrocatalysis in Metal–Air Batteries
title_fullStr Localizing Tungsten Single Atoms around Tungsten Nitride Nanoparticles for Efficient Oxygen Reduction Electrocatalysis in Metal–Air Batteries
title_full_unstemmed Localizing Tungsten Single Atoms around Tungsten Nitride Nanoparticles for Efficient Oxygen Reduction Electrocatalysis in Metal–Air Batteries
title_short Localizing Tungsten Single Atoms around Tungsten Nitride Nanoparticles for Efficient Oxygen Reduction Electrocatalysis in Metal–Air Batteries
title_sort localizing tungsten single atoms around tungsten nitride nanoparticles for efficient oxygen reduction electrocatalysis in metal air batteries
topic metal–air batteries
oxygen reduction reaction
single atom catalysts
synergistic effect
tungsten nitrides
url https://doi.org/10.1002/advs.202105192
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