{"title":"电聚合PAA作为高效水氧化CeO2-NiO杂化电催化剂的功能基质。","authors":"Mrunal Bhosale, Pritam J Morankar, Yeonsu Lee, Hajin Seo, Chan-Wook Jeon","doi":"10.3390/polym17192631","DOIUrl":null,"url":null,"abstract":"<p><p>Electrochemical water splitting has emerged as a pivotal strategy for advancing sustainable and renewable energy technologies. However, its practical deployment is often hampered by sluggish reaction kinetics, large overpotentials, and the high cost of efficient electrocatalysts. To overcome these critical challenges, a novel bifunctional electrocatalyst based on electropolymerized CeO<sub>2</sub>-NiO with polyacrylic acid (Ce-Ni-PAA) has been rationally engineered for overall water splitting. The strategic incorporation of conductive polymer framework enables effective modulation of the local electronic structure, enhances charge transport pathways, and maximizes the density of electrochemically accessible active sites, thereby substantially boosting catalytic performance. When evaluated in a 1 M KOH alkaline medium, the optimized Ce-Ni-PAA<sub>0.5</sub>/NF hybrid demonstrates remarkable catalytic activity with 366.5 mV overpotential at 50 mA cm<sup>-2</sup>, coupled with lower Tafel slope of 93.5 mV dec<sup>-1</sup>. Additionally, the Ce-Ni-PAA<sub>0.5</sub>/NF electrocatalyst exhibits exceptional ECSA of 1092.3 cm<sup>2</sup>, which confirms the presence of a significantly larger number of electrochemically active sites. The electrocatalyst retains its performance even after 5000 continuous cycles of operation. The superior performance is attributed to the synergistic effects arising from the enriched composition, efficient electron transport channels, and abundant catalytic centers. Collectively, this study not only highlights the significance of rational structural and compositional design but also offers valuable insights toward the development of next-generation, cost-effective bifunctional electrocatalysts with strong potential for scalable water splitting and clean energy applications.</p>","PeriodicalId":20416,"journal":{"name":"Polymers","volume":"17 19","pages":""},"PeriodicalIF":4.9000,"publicationDate":"2025-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12526815/pdf/","citationCount":"0","resultStr":"{\"title\":\"Electropolymerized PAA as a Functional Matrix for CeO<sub>2</sub>-NiO Hybrid Electrocatalysts for Efficient Water Oxidation.\",\"authors\":\"Mrunal Bhosale, Pritam J Morankar, Yeonsu Lee, Hajin Seo, Chan-Wook Jeon\",\"doi\":\"10.3390/polym17192631\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>Electrochemical water splitting has emerged as a pivotal strategy for advancing sustainable and renewable energy technologies. However, its practical deployment is often hampered by sluggish reaction kinetics, large overpotentials, and the high cost of efficient electrocatalysts. To overcome these critical challenges, a novel bifunctional electrocatalyst based on electropolymerized CeO<sub>2</sub>-NiO with polyacrylic acid (Ce-Ni-PAA) has been rationally engineered for overall water splitting. The strategic incorporation of conductive polymer framework enables effective modulation of the local electronic structure, enhances charge transport pathways, and maximizes the density of electrochemically accessible active sites, thereby substantially boosting catalytic performance. When evaluated in a 1 M KOH alkaline medium, the optimized Ce-Ni-PAA<sub>0.5</sub>/NF hybrid demonstrates remarkable catalytic activity with 366.5 mV overpotential at 50 mA cm<sup>-2</sup>, coupled with lower Tafel slope of 93.5 mV dec<sup>-1</sup>. Additionally, the Ce-Ni-PAA<sub>0.5</sub>/NF electrocatalyst exhibits exceptional ECSA of 1092.3 cm<sup>2</sup>, which confirms the presence of a significantly larger number of electrochemically active sites. The electrocatalyst retains its performance even after 5000 continuous cycles of operation. The superior performance is attributed to the synergistic effects arising from the enriched composition, efficient electron transport channels, and abundant catalytic centers. 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引用次数: 0
摘要
电化学水分解已成为推进可持续和可再生能源技术的关键战略。然而,它的实际应用往往受到反应动力学缓慢、过电位大和高效电催化剂成本高的阻碍。为了克服这些关键的挑战,一种基于CeO2-NiO与聚丙烯酸(Ce-Ni-PAA)电聚合的新型双功能电催化剂被合理地设计用于整体水分解。导电聚合物框架的战略性结合能够有效调制局部电子结构,增强电荷传输途径,并最大化电化学可达活性位点的密度,从而大大提高催化性能。在1 M KOH碱性介质中,优化后的Ce-Ni-PAA0.5/NF复合物在50 mA cm-2下的过电位为366.5 mV, Tafel斜率为93.5 mV / dec1,具有显著的催化活性。此外,Ce-Ni-PAA0.5/NF电催化剂表现出1092.3 cm2的ECSA,这证实了存在大量的电化学活性位点。这种电催化剂在连续运行5000次后仍保持其性能。这种优异的性能是由于其丰富的成分、高效的电子传递通道和丰富的催化中心所产生的协同效应。总的来说,这项研究不仅强调了合理的结构和组成设计的重要性,而且为开发具有成本效益的下一代双功能电催化剂提供了有价值的见解,这些电催化剂具有可扩展的水分解和清洁能源应用的强大潜力。
Electropolymerized PAA as a Functional Matrix for CeO2-NiO Hybrid Electrocatalysts for Efficient Water Oxidation.
Electrochemical water splitting has emerged as a pivotal strategy for advancing sustainable and renewable energy technologies. However, its practical deployment is often hampered by sluggish reaction kinetics, large overpotentials, and the high cost of efficient electrocatalysts. To overcome these critical challenges, a novel bifunctional electrocatalyst based on electropolymerized CeO2-NiO with polyacrylic acid (Ce-Ni-PAA) has been rationally engineered for overall water splitting. The strategic incorporation of conductive polymer framework enables effective modulation of the local electronic structure, enhances charge transport pathways, and maximizes the density of electrochemically accessible active sites, thereby substantially boosting catalytic performance. When evaluated in a 1 M KOH alkaline medium, the optimized Ce-Ni-PAA0.5/NF hybrid demonstrates remarkable catalytic activity with 366.5 mV overpotential at 50 mA cm-2, coupled with lower Tafel slope of 93.5 mV dec-1. Additionally, the Ce-Ni-PAA0.5/NF electrocatalyst exhibits exceptional ECSA of 1092.3 cm2, which confirms the presence of a significantly larger number of electrochemically active sites. The electrocatalyst retains its performance even after 5000 continuous cycles of operation. The superior performance is attributed to the synergistic effects arising from the enriched composition, efficient electron transport channels, and abundant catalytic centers. Collectively, this study not only highlights the significance of rational structural and compositional design but also offers valuable insights toward the development of next-generation, cost-effective bifunctional electrocatalysts with strong potential for scalable water splitting and clean energy applications.
期刊介绍:
Polymers (ISSN 2073-4360) is an international, open access journal of polymer science. It publishes research papers, short communications and review papers. Our aim is to encourage scientists to publish their experimental and theoretical results in as much detail as possible. Therefore, there is no restriction on the length of the papers. The full experimental details must be provided so that the results can be reproduced. Polymers provides an interdisciplinary forum for publishing papers which advance the fields of (i) polymerization methods, (ii) theory, simulation, and modeling, (iii) understanding of new physical phenomena, (iv) advances in characterization techniques, and (v) harnessing of self-assembly and biological strategies for producing complex multifunctional structures.