In Situ Reconstructing NiFe Oxalate Toward Overall Water Splitting

Abstract Surface reconstruction plays an essential role in electrochemical catalysis. The structures, compositions, and functionalities of the real catalytic species and sites generated by reconstruction, however, are yet to be clearly understood, for the metastable or transit state of most reconstr...

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Main Authors: Zhen Zhang, Xiaoyu Ren, Wenyuan Dai, Hang Zhang, Zhengyin Sun, Zhuang Ye, Ying Hou, Peizhi Liu, Bingshe Xu, Lihua Qian, Ting Liao, Haixia Zhang, Junjie Guo, Ziqi Sun
Format: Article
Language:English
Published: Wiley 2024-11-01
Series:Advanced Science
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Online Access:https://doi.org/10.1002/advs.202408754
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author Zhen Zhang
Xiaoyu Ren
Wenyuan Dai
Hang Zhang
Zhengyin Sun
Zhuang Ye
Ying Hou
Peizhi Liu
Bingshe Xu
Lihua Qian
Ting Liao
Haixia Zhang
Junjie Guo
Ziqi Sun
author_facet Zhen Zhang
Xiaoyu Ren
Wenyuan Dai
Hang Zhang
Zhengyin Sun
Zhuang Ye
Ying Hou
Peizhi Liu
Bingshe Xu
Lihua Qian
Ting Liao
Haixia Zhang
Junjie Guo
Ziqi Sun
author_sort Zhen Zhang
collection DOAJ
description Abstract Surface reconstruction plays an essential role in electrochemical catalysis. The structures, compositions, and functionalities of the real catalytic species and sites generated by reconstruction, however, are yet to be clearly understood, for the metastable or transit state of most reconstructed structures. Herein, a series of NiFe oxalates (NixFe1‐xC2O4, x = 1, 0.9, 0.7, 0.6, 0.5, and 0) are synthesized for overall water splitting electrocatalysis. Whilst NixFe1‐xC2O4 shows great hydrogen evolution reaction (HER) activity, the in situ reconstructed NixFe1‐xOOH exhibits outstanding oxygen evolution reaction (OER) activity. As identified by the in situ Raman spectroscopy and quasi‐in situ X‐ray absorption spectroscopy (XAS) techniques, reconstructions from NixFe1‐xC2O4 into defective NixFe1‐xOOH and finally amorphous NixFe1‐xOOH active species (R‐NixFe1‐xOOH) are confirmed upon cyclic voltammetry processes. Specifically, the fully reconstructed R‐Ni0.6Fe0.4OOH demonstrates the best OER activity (179 mV to reach 10 mA cm−2), originating from its abundant real active sites and optimal d‐band center. Benefiting from the reconstruction, an alkaline electrolyzer composed of a Ni0.6Fe0.4C2O4 cathode and an in situ reconstructed R‐Ni0.6Fe0.4OOH anode achieves a superb overall water splitting performance (1.52 V@10 mA cm−2). This work provides an in‐depth structure‐property relationship understanding on the reconstruction of catalysts and offers a new pathway to designing novel catalyst.
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spelling doaj-art-db2c00d1d7474aec9d972669ad00618e2024-11-27T11:21:53ZengWileyAdvanced Science2198-38442024-11-011144n/an/a10.1002/advs.202408754In Situ Reconstructing NiFe Oxalate Toward Overall Water SplittingZhen Zhang0Xiaoyu Ren1Wenyuan Dai2Hang Zhang3Zhengyin Sun4Zhuang Ye5Ying Hou6Peizhi Liu7Bingshe Xu8Lihua Qian9Ting Liao10Haixia Zhang11Junjie Guo12Ziqi Sun13Key Laboratory of Interface Science and Engineering in Advanced Materials Ministry of Education College of Materials Science and Engineering Taiyuan University of Technology Taiyuan 030024 P. R. ChinaKey Laboratory of Interface Science and Engineering in Advanced Materials Ministry of Education College of Materials Science and Engineering Taiyuan University of Technology Taiyuan 030024 P. R. ChinaKey Laboratory of Interface Science and Engineering in Advanced Materials Ministry of Education College of Materials Science and Engineering Taiyuan University of Technology Taiyuan 030024 P. R. ChinaKey Laboratory of Interface Science and Engineering in Advanced Materials Ministry of Education College of Materials Science and Engineering Taiyuan University of Technology Taiyuan 030024 P. R. ChinaKey Laboratory of Interface Science and Engineering in Advanced Materials Ministry of Education College of Materials Science and Engineering Taiyuan University of Technology Taiyuan 030024 P. R. ChinaKey Laboratory of Interface Science and Engineering in Advanced Materials Ministry of Education College of Materials Science and Engineering Taiyuan University of Technology Taiyuan 030024 P. R. ChinaKey Laboratory of Interface Science and Engineering in Advanced Materials Ministry of Education College of Materials Science and Engineering Taiyuan University of Technology Taiyuan 030024 P. R. ChinaKey Laboratory of Interface Science and Engineering in Advanced Materials Ministry of Education College of Materials Science and Engineering Taiyuan University of Technology Taiyuan 030024 P. R. ChinaKey Laboratory of Interface Science and Engineering in Advanced Materials Ministry of Education College of Materials Science and Engineering Taiyuan University of Technology Taiyuan 030024 P. R. ChinaSchool of Physics Huazhong University of Science and Technology Wuhan 430074 P. R. ChinaSchool of Mechanical Medical and Process Engineering Queensland University of Technology George Street Brisbane QLD 4000 AustraliaKey Laboratory of Interface Science and Engineering in Advanced Materials Ministry of Education College of Materials Science and Engineering Taiyuan University of Technology Taiyuan 030024 P. R. ChinaKey Laboratory of Interface Science and Engineering in Advanced Materials Ministry of Education College of Materials Science and Engineering Taiyuan University of Technology Taiyuan 030024 P. R. ChinaCentre for Materials Science Queensland University of Technology 2 George Street Brisbane 4000 AustraliaAbstract Surface reconstruction plays an essential role in electrochemical catalysis. The structures, compositions, and functionalities of the real catalytic species and sites generated by reconstruction, however, are yet to be clearly understood, for the metastable or transit state of most reconstructed structures. Herein, a series of NiFe oxalates (NixFe1‐xC2O4, x = 1, 0.9, 0.7, 0.6, 0.5, and 0) are synthesized for overall water splitting electrocatalysis. Whilst NixFe1‐xC2O4 shows great hydrogen evolution reaction (HER) activity, the in situ reconstructed NixFe1‐xOOH exhibits outstanding oxygen evolution reaction (OER) activity. As identified by the in situ Raman spectroscopy and quasi‐in situ X‐ray absorption spectroscopy (XAS) techniques, reconstructions from NixFe1‐xC2O4 into defective NixFe1‐xOOH and finally amorphous NixFe1‐xOOH active species (R‐NixFe1‐xOOH) are confirmed upon cyclic voltammetry processes. Specifically, the fully reconstructed R‐Ni0.6Fe0.4OOH demonstrates the best OER activity (179 mV to reach 10 mA cm−2), originating from its abundant real active sites and optimal d‐band center. Benefiting from the reconstruction, an alkaline electrolyzer composed of a Ni0.6Fe0.4C2O4 cathode and an in situ reconstructed R‐Ni0.6Fe0.4OOH anode achieves a superb overall water splitting performance (1.52 V@10 mA cm−2). This work provides an in‐depth structure‐property relationship understanding on the reconstruction of catalysts and offers a new pathway to designing novel catalyst.https://doi.org/10.1002/advs.202408754amorphous catalystsdeep reconstructionin situ Ramanoverall water splittingoxalates
spellingShingle Zhen Zhang
Xiaoyu Ren
Wenyuan Dai
Hang Zhang
Zhengyin Sun
Zhuang Ye
Ying Hou
Peizhi Liu
Bingshe Xu
Lihua Qian
Ting Liao
Haixia Zhang
Junjie Guo
Ziqi Sun
In Situ Reconstructing NiFe Oxalate Toward Overall Water Splitting
Advanced Science
amorphous catalysts
deep reconstruction
in situ Raman
overall water splitting
oxalates
title In Situ Reconstructing NiFe Oxalate Toward Overall Water Splitting
title_full In Situ Reconstructing NiFe Oxalate Toward Overall Water Splitting
title_fullStr In Situ Reconstructing NiFe Oxalate Toward Overall Water Splitting
title_full_unstemmed In Situ Reconstructing NiFe Oxalate Toward Overall Water Splitting
title_short In Situ Reconstructing NiFe Oxalate Toward Overall Water Splitting
title_sort in situ reconstructing nife oxalate toward overall water splitting
topic amorphous catalysts
deep reconstruction
in situ Raman
overall water splitting
oxalates
url https://doi.org/10.1002/advs.202408754
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