{"title":"掺铁 Ni3S2 可诱导尿素辅助水电解增强的自重构。","authors":"Xinyu Yang, Yifeng Liu, Qianqiao Chen, Wanchin Yu, Qin Zhong","doi":"10.1021/acs.langmuir.4c03343","DOIUrl":null,"url":null,"abstract":"<p><p>Urea oxidation reaction (UOR) is an attractive alternative anodic reaction to oxygen evolution reaction (OER) for its low thermodynamic potential (0.37 V vs RHE). A major challenge that prohibits its practical application is the six-electron transfer process during UOR, demanding enhancements in the catalytic activity. Herein, a Fe-doped Ni<sub>3</sub>S<sub>2</sub> catalyst with a uniform flower-like structure is synthesized <i>in situ</i> on nickel foam via a simple one-step hydrothermal method. The electrochemical properties of Fe-Ni<sub>3</sub>S<sub>2</sub> are significantly improved since a current density of 10 mA cm<sup>-2</sup> only requires a 1.33 V potential and remains stable for 60 h. The structural characterization demonstrates a strong interaction between Fe and Ni<sub>3</sub>S<sub>2</sub>. After Fe doping, the active site increases, which promotes the formation of NiOOH on the catalyst surface, thus speeding up the UOR process. These changes are beneficial to charge transfer and optimize the adsorption energy of the intermediates. <i>In situ</i> EIS further confirms that Fe promotes electron transfer during the UOR process, reduces the interface resistance between the catalyst and the electrolyte, and lowers the driving voltage.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.7000,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Fe-Doped Ni<sub>3</sub>S<sub>2</sub> Induces Self-Reconstruction for Urea-Assisted Water Electrolysis Enhancement.\",\"authors\":\"Xinyu Yang, Yifeng Liu, Qianqiao Chen, Wanchin Yu, Qin Zhong\",\"doi\":\"10.1021/acs.langmuir.4c03343\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>Urea oxidation reaction (UOR) is an attractive alternative anodic reaction to oxygen evolution reaction (OER) for its low thermodynamic potential (0.37 V vs RHE). A major challenge that prohibits its practical application is the six-electron transfer process during UOR, demanding enhancements in the catalytic activity. Herein, a Fe-doped Ni<sub>3</sub>S<sub>2</sub> catalyst with a uniform flower-like structure is synthesized <i>in situ</i> on nickel foam via a simple one-step hydrothermal method. The electrochemical properties of Fe-Ni<sub>3</sub>S<sub>2</sub> are significantly improved since a current density of 10 mA cm<sup>-2</sup> only requires a 1.33 V potential and remains stable for 60 h. The structural characterization demonstrates a strong interaction between Fe and Ni<sub>3</sub>S<sub>2</sub>. After Fe doping, the active site increases, which promotes the formation of NiOOH on the catalyst surface, thus speeding up the UOR process. These changes are beneficial to charge transfer and optimize the adsorption energy of the intermediates. <i>In situ</i> EIS further confirms that Fe promotes electron transfer during the UOR process, reduces the interface resistance between the catalyst and the electrolyte, and lowers the driving voltage.</p>\",\"PeriodicalId\":50,\"journal\":{\"name\":\"Langmuir\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":3.7000,\"publicationDate\":\"2024-11-06\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Langmuir\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1021/acs.langmuir.4c03343\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Langmuir","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acs.langmuir.4c03343","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
摘要
尿素氧化反应(UOR)的热力学电位较低(0.37 V 对 RHE),是氧进化反应(OER)的一种有吸引力的替代阳极反应。阻碍其实际应用的一个主要挑战是 UOR 反应过程中的六电子转移过程,这就要求提高催化活性。本文通过简单的一步水热法,在泡沫镍上原位合成了具有均匀花状结构的掺铁 Ni3S2 催化剂。由于 10 mA cm-2 的电流密度只需要 1.33 V 的电位,且能保持稳定 60 小时,Fe-Ni3S2 的电化学性能得到了显著改善。掺入 Fe 后,活性位点增加,促进了催化剂表面 NiOOH 的形成,从而加快了 UOR 过程。这些变化有利于电荷转移,并优化了中间产物的吸附能。原位 EIS 进一步证实,铁在 UOR 过程中促进了电子转移,降低了催化剂与电解质之间的界面电阻,并降低了驱动电压。
Fe-Doped Ni3S2 Induces Self-Reconstruction for Urea-Assisted Water Electrolysis Enhancement.
Urea oxidation reaction (UOR) is an attractive alternative anodic reaction to oxygen evolution reaction (OER) for its low thermodynamic potential (0.37 V vs RHE). A major challenge that prohibits its practical application is the six-electron transfer process during UOR, demanding enhancements in the catalytic activity. Herein, a Fe-doped Ni3S2 catalyst with a uniform flower-like structure is synthesized in situ on nickel foam via a simple one-step hydrothermal method. The electrochemical properties of Fe-Ni3S2 are significantly improved since a current density of 10 mA cm-2 only requires a 1.33 V potential and remains stable for 60 h. The structural characterization demonstrates a strong interaction between Fe and Ni3S2. After Fe doping, the active site increases, which promotes the formation of NiOOH on the catalyst surface, thus speeding up the UOR process. These changes are beneficial to charge transfer and optimize the adsorption energy of the intermediates. In situ EIS further confirms that Fe promotes electron transfer during the UOR process, reduces the interface resistance between the catalyst and the electrolyte, and lowers the driving voltage.
期刊介绍:
Langmuir is an interdisciplinary journal publishing articles in the following subject categories:
Colloids: surfactants and self-assembly, dispersions, emulsions, foams
Interfaces: adsorption, reactions, films, forces
Biological Interfaces: biocolloids, biomolecular and biomimetic materials
Materials: nano- and mesostructured materials, polymers, gels, liquid crystals
Electrochemistry: interfacial charge transfer, charge transport, electrocatalysis, electrokinetic phenomena, bioelectrochemistry
Devices and Applications: sensors, fluidics, patterning, catalysis, photonic crystals
However, when high-impact, original work is submitted that does not fit within the above categories, decisions to accept or decline such papers will be based on one criteria: What Would Irving Do?
Langmuir ranks #2 in citations out of 136 journals in the category of Physical Chemistry with 113,157 total citations. The journal received an Impact Factor of 4.384*.
This journal is also indexed in the categories of Materials Science (ranked #1) and Multidisciplinary Chemistry (ranked #5).