{"title":"碳载体上垂直排列的 CoFe-LDH 在氧进化反应中的孔径调节","authors":"Parul Aggarwal, Palak Mehra and Amit Paul*, ","doi":"10.1021/acsanm.4c01018","DOIUrl":null,"url":null,"abstract":"<p >Porous carbon-supported CoFe-layered double hydroxide (LDH)-based catalysts were synthesized and utilized as excellent oxygen evolution reaction catalysts in alkaline medium. High-resolution transmission electron microscopy images and N<sub>2</sub>-sorption experiments suggested vertical growth of LDH on the carbon support and a narrow mesoporous nature of the materials, respectively. We proposed that the surface oxygen functional groups of carbon materials provided the nucleation sites for the crystal growth of the LDH on the carbon support utilizing short-range electrostatic interactions, which led to vertical growth of LDH with a narrow mesoporous nature. Among the synthesized materials, CoFe-LDH/MMC showed a remarkable mass activity of 559.2 A g<sup>–1</sup>, a turnover frequency of 4.22 s<sup>–1</sup>, and a massive roughness factor value of 269. This excellent reactivity has been attributed to (a) the vertically aligned narrow mesoporous nature of the material that increased the electrolyte accessibility inside the material and thus improved active sites for catalysis, (b) the high electrical conductivity of the material that also enhanced accessibility, reduced resistance for charge transfer at the electrode/electrolyte interface, and reduced resistance for intermediate formation during water oxidation, and (c) the increased electron contribution to the 3d orbital of cobalt from carbon that weakened the Co–oxygen bond and thus further facilitated the formation of the O–O bond and O<sub>2</sub> desorption during water oxidation.</p>","PeriodicalId":6,"journal":{"name":"ACS Applied Nano Materials","volume":"7 8","pages":"9532–9541"},"PeriodicalIF":5.3000,"publicationDate":"2024-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Pore Size-Regulated Vertically Aligned CoFe-LDH on a Carbon Support for the Oxygen Evolution Reaction\",\"authors\":\"Parul Aggarwal, Palak Mehra and Amit Paul*, \",\"doi\":\"10.1021/acsanm.4c01018\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Porous carbon-supported CoFe-layered double hydroxide (LDH)-based catalysts were synthesized and utilized as excellent oxygen evolution reaction catalysts in alkaline medium. High-resolution transmission electron microscopy images and N<sub>2</sub>-sorption experiments suggested vertical growth of LDH on the carbon support and a narrow mesoporous nature of the materials, respectively. We proposed that the surface oxygen functional groups of carbon materials provided the nucleation sites for the crystal growth of the LDH on the carbon support utilizing short-range electrostatic interactions, which led to vertical growth of LDH with a narrow mesoporous nature. Among the synthesized materials, CoFe-LDH/MMC showed a remarkable mass activity of 559.2 A g<sup>–1</sup>, a turnover frequency of 4.22 s<sup>–1</sup>, and a massive roughness factor value of 269. 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引用次数: 0
摘要
合成了多孔碳支撑 CoFe 层状双氢氧化物(LDH)基催化剂,并将其用作碱性介质中优良的氧进化反应催化剂。高分辨率透射电子显微镜图像和 N2 吸附实验分别表明了 LDH 在碳支撑上的垂直生长和材料的窄介孔性质。我们认为,碳材料表面的氧官能团利用短程静电作用为 LDH 在碳载体上的晶体生长提供了成核位点,从而导致 LDH 垂直生长并具有窄介孔性质。在合成的材料中,CoFe-LDH/MMC 的质量活性高达 559.2 A g-1,周转频率为 4.22 s-1,大规模粗糙度因子值为 269。这种出色的反应活性归功于:(a)材料垂直排列的窄介孔性质提高了材料内部电解质的可及性,从而改善了催化的活性位点;(b)材料的高导电性也提高了可及性、(c) 增加了碳对钴 3d 轨道的电子贡献,削弱了 Co 氧键,从而进一步促进了 O-O 键的形成和水氧化过程中的 O2 解吸。
Pore Size-Regulated Vertically Aligned CoFe-LDH on a Carbon Support for the Oxygen Evolution Reaction
Porous carbon-supported CoFe-layered double hydroxide (LDH)-based catalysts were synthesized and utilized as excellent oxygen evolution reaction catalysts in alkaline medium. High-resolution transmission electron microscopy images and N2-sorption experiments suggested vertical growth of LDH on the carbon support and a narrow mesoporous nature of the materials, respectively. We proposed that the surface oxygen functional groups of carbon materials provided the nucleation sites for the crystal growth of the LDH on the carbon support utilizing short-range electrostatic interactions, which led to vertical growth of LDH with a narrow mesoporous nature. Among the synthesized materials, CoFe-LDH/MMC showed a remarkable mass activity of 559.2 A g–1, a turnover frequency of 4.22 s–1, and a massive roughness factor value of 269. This excellent reactivity has been attributed to (a) the vertically aligned narrow mesoporous nature of the material that increased the electrolyte accessibility inside the material and thus improved active sites for catalysis, (b) the high electrical conductivity of the material that also enhanced accessibility, reduced resistance for charge transfer at the electrode/electrolyte interface, and reduced resistance for intermediate formation during water oxidation, and (c) the increased electron contribution to the 3d orbital of cobalt from carbon that weakened the Co–oxygen bond and thus further facilitated the formation of the O–O bond and O2 desorption during water oxidation.
期刊介绍:
ACS Applied Nano Materials is an interdisciplinary journal publishing original research covering all aspects of engineering, chemistry, physics and biology relevant to applications of nanomaterials. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials, engineering, physics, bioscience, and chemistry into important applications of nanomaterials.