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
{"title":"In Situ Reconstructing NiFe Oxalate Toward Overall Water Splitting.","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","doi":"10.1002/advs.202408754","DOIUrl":null,"url":null,"abstract":"<p><p>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 (Ni<sub>x</sub>Fe<sub>1-</sub> <sub>x</sub>C<sub>2</sub>O<sub>4</sub>, x = 1, 0.9, 0.7, 0.6, 0.5, and 0) are synthesized for overall water splitting electrocatalysis. Whilst Ni<sub>x</sub>Fe<sub>1-x</sub>C<sub>2</sub>O<sub>4</sub> shows great hydrogen evolution reaction (HER) activity, the in situ reconstructed Ni<sub>x</sub>Fe<sub>1-x</sub>OOH 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 Ni<sub>x</sub>Fe<sub>1-x</sub>C<sub>2</sub>O<sub>4</sub> into defective Ni<sub>x</sub>Fe<sub>1-x</sub>OOH and finally amorphous Ni<sub>x</sub>Fe<sub>1-x</sub>OOH active species (R-Ni<sub>x</sub>Fe<sub>1-x</sub>OOH) are confirmed upon cyclic voltammetry processes. Specifically, the fully reconstructed R-Ni<sub>0.6</sub>Fe<sub>0.4</sub>OOH demonstrates the best OER activity (179 mV to reach 10 mA cm<sup>-2</sup>), originating from its abundant real active sites and optimal d-band center. Benefiting from the reconstruction, an alkaline electrolyzer composed of a Ni<sub>0.6</sub>Fe<sub>0.4</sub>C<sub>2</sub>O<sub>4</sub> cathode and an in situ reconstructed R-Ni<sub>0.6</sub>Fe<sub>0.4</sub>OOH anode achieves a superb overall water splitting performance (1.52 V@10 mA cm<sup>-2</sup>). This work provides an in-depth structure-property relationship understanding on the reconstruction of catalysts and offers a new pathway to designing novel catalyst.</p>","PeriodicalId":117,"journal":{"name":"Advanced Science","volume":null,"pages":null},"PeriodicalIF":14.3000,"publicationDate":"2024-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Science","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1002/advs.202408754","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
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.
期刊介绍:
Advanced Science is a prestigious open access journal that focuses on interdisciplinary research in materials science, physics, chemistry, medical and life sciences, and engineering. The journal aims to promote cutting-edge research by employing a rigorous and impartial review process. It is committed to presenting research articles with the highest quality production standards, ensuring maximum accessibility of top scientific findings. With its vibrant and innovative publication platform, Advanced Science seeks to revolutionize the dissemination and organization of scientific knowledge.