Liyue Zhang , Qiucheng Xu , Rukai Zhao , Yanjie Hu , Hao Jiang , Chunzhong Li
{"title":"掺铁富硫Ni3S2纳米线促进水氧化的动力学研究","authors":"Liyue Zhang , Qiucheng Xu , Rukai Zhao , Yanjie Hu , Hao Jiang , Chunzhong Li","doi":"10.1016/j.gce.2021.12.012","DOIUrl":null,"url":null,"abstract":"<div><p>Exploring cost-effective and highly-active oxygen evolution reaction (OER) electrocatalysts is a pressing task to propel water electrolysis for green hydrogen production. Herein, we constructed a class of Fe-doped and S-enriched Ni<sub>3</sub>S<sub>2</sub> nanowires electrocatalysts for optimizing the target intermediates adsorption to decrease the OER overpotentials at various current densities. The optimal Ni<sub>3</sub>S<sub>2</sub>-1.4%Fe electrocatalyst possesses the most active sites and exhibits an ultralow overpotential of 190 mV at 10 mA cm<sup>−2</sup> with an excellent stability of > 60 h, exceeding the majority of recently-reported Ni<sub>3</sub>S<sub>2</sub>-based electrocatalysts. The trivalence Fe-doping not only reduces the electron density of the Ni center, but also enables the sulfur enrichment on the Ni<sub>3</sub>S<sub>2</sub> surface, which greatly improves the intrinsic activity and the number of target intermediates (∗OOH). A novel methanol-assisted electrochemical evaluation further reveals that the Ni<sub>3</sub>S<sub>2</sub>-1.4%Fe electrocatalyst demonstrates a weaker binding ability to ∗OH with the rapid generation of ∗OOH species, and thus gives a lower apparent activation energy compared with the surface sulfur reduced ones. This work provides a new perspective for regulating the adsorption of intermediates through doping strategy.</p></div>","PeriodicalId":66474,"journal":{"name":"Green Chemical Engineering","volume":"3 4","pages":"Pages 367-373"},"PeriodicalIF":9.1000,"publicationDate":"2022-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2666952821001023/pdfft?md5=91e6dcb034b0fdcaabf68920c31edc93&pid=1-s2.0-S2666952821001023-main.pdf","citationCount":"12","resultStr":"{\"title\":\"Fe-doped and sulfur-enriched Ni3S2 nanowires with enhanced reaction kinetics for boosting water oxidation\",\"authors\":\"Liyue Zhang , Qiucheng Xu , Rukai Zhao , Yanjie Hu , Hao Jiang , Chunzhong Li\",\"doi\":\"10.1016/j.gce.2021.12.012\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Exploring cost-effective and highly-active oxygen evolution reaction (OER) electrocatalysts is a pressing task to propel water electrolysis for green hydrogen production. Herein, we constructed a class of Fe-doped and S-enriched Ni<sub>3</sub>S<sub>2</sub> nanowires electrocatalysts for optimizing the target intermediates adsorption to decrease the OER overpotentials at various current densities. The optimal Ni<sub>3</sub>S<sub>2</sub>-1.4%Fe electrocatalyst possesses the most active sites and exhibits an ultralow overpotential of 190 mV at 10 mA cm<sup>−2</sup> with an excellent stability of > 60 h, exceeding the majority of recently-reported Ni<sub>3</sub>S<sub>2</sub>-based electrocatalysts. The trivalence Fe-doping not only reduces the electron density of the Ni center, but also enables the sulfur enrichment on the Ni<sub>3</sub>S<sub>2</sub> surface, which greatly improves the intrinsic activity and the number of target intermediates (∗OOH). A novel methanol-assisted electrochemical evaluation further reveals that the Ni<sub>3</sub>S<sub>2</sub>-1.4%Fe electrocatalyst demonstrates a weaker binding ability to ∗OH with the rapid generation of ∗OOH species, and thus gives a lower apparent activation energy compared with the surface sulfur reduced ones. This work provides a new perspective for regulating the adsorption of intermediates through doping strategy.</p></div>\",\"PeriodicalId\":66474,\"journal\":{\"name\":\"Green Chemical Engineering\",\"volume\":\"3 4\",\"pages\":\"Pages 367-373\"},\"PeriodicalIF\":9.1000,\"publicationDate\":\"2022-12-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://www.sciencedirect.com/science/article/pii/S2666952821001023/pdfft?md5=91e6dcb034b0fdcaabf68920c31edc93&pid=1-s2.0-S2666952821001023-main.pdf\",\"citationCount\":\"12\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Green Chemical Engineering\",\"FirstCategoryId\":\"1089\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2666952821001023\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Green Chemical Engineering","FirstCategoryId":"1089","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2666952821001023","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
引用次数: 12
摘要
探索高性价比、高活性的析氧反应(OER)电催化剂是推进水电解绿色制氢的紧迫任务。在此,我们构建了一类掺铁富s的Ni3S2纳米线电催化剂,用于优化靶中间体的吸附,以降低不同电流密度下的OER过电位。优选的Ni3S2-1.4%Fe电催化剂具有最高的活性位点,在10 mA cm−2下具有190 mV的超低过电位,并具有优异的稳定性;60 h,超过了最近报道的大多数ni3s2基电催化剂。三价fe掺杂不仅降低了Ni中心的电子密度,而且使Ni3S2表面的硫富集,从而大大提高了Ni3S2的本特征活性和靶中间体(∗OOH)的数量。一种新的甲醇辅助电化学评价进一步表明,Ni3S2-1.4%Fe电催化剂对∗OH的结合能力较弱,与表面硫还原的催化剂相比,其表观活化能较低。本研究为通过掺杂策略调控中间体的吸附提供了新的视角。
Fe-doped and sulfur-enriched Ni3S2 nanowires with enhanced reaction kinetics for boosting water oxidation
Exploring cost-effective and highly-active oxygen evolution reaction (OER) electrocatalysts is a pressing task to propel water electrolysis for green hydrogen production. Herein, we constructed a class of Fe-doped and S-enriched Ni3S2 nanowires electrocatalysts for optimizing the target intermediates adsorption to decrease the OER overpotentials at various current densities. The optimal Ni3S2-1.4%Fe electrocatalyst possesses the most active sites and exhibits an ultralow overpotential of 190 mV at 10 mA cm−2 with an excellent stability of > 60 h, exceeding the majority of recently-reported Ni3S2-based electrocatalysts. The trivalence Fe-doping not only reduces the electron density of the Ni center, but also enables the sulfur enrichment on the Ni3S2 surface, which greatly improves the intrinsic activity and the number of target intermediates (∗OOH). A novel methanol-assisted electrochemical evaluation further reveals that the Ni3S2-1.4%Fe electrocatalyst demonstrates a weaker binding ability to ∗OH with the rapid generation of ∗OOH species, and thus gives a lower apparent activation energy compared with the surface sulfur reduced ones. This work provides a new perspective for regulating the adsorption of intermediates through doping strategy.