{"title":"La0.8Sr0.2CoO3纳米粒子在碱性电解中增强点阵氧氧化的超粒子组装。","authors":"Mohaned Hammad*, , , Blaž Toplak, , , Adil Amin, , , Mena-Alexander Kräenbring, , , Ahammed Suhail Odungat, , , Mohammed-Ali Sheikh, , , Adarsh Jain, , , Amin S. Amin, , , Ralf Meckenstock, , , Thai Binh Nguyen, , , Khuzaifa Yahuza Muhammad, , , Abdallah Hamdan, , , Steven Angel, , , Michael Farle, , , Ulf-Peter Apfel, , , Hartmut Wiggers, , and , Doris Segets*, ","doi":"10.1021/acsami.5c11289","DOIUrl":null,"url":null,"abstract":"<p >Developing effective non-noble metal electrocatalysts for the oxygen evolution reaction (OER) remains challenging due to limited active sites, poor electronic conductivity, and high overpotentials associated with the conventional adsorbate evolution mechanism (AEM). To address these limitations, a one-step spray drying method is employed to assemble high-surface-area La<sub>0.8</sub>Sr<sub>0.2</sub>CoO<sub>3</sub> nanoparticles (LSCO-NP) into hierarchical supraparticles with ≈65% porosity and interconnected meso-/macropore networks. This architecture not only accelerates ion diffusion and interparticle electron transfer but also induces a mechanistic switch from the AEM to the lattice oxygen oxidation mechanism (LOM). La<sub>0.8</sub>Sr<sub>0.2</sub>CoO<sub>3</sub> supraparticles (LSCO-SP) demonstrate significantly enhanced OER performance, requiring ∼300 mV lower overpotential at 100 mA cm<sup>–2</sup> after 1 h compared to LSCO-NP. Moreover, LSCO-SP exhibit faster catalytic kinetics, evidenced by a smaller Tafel slope of 76.2 mV dec<sup>–1</sup> versus 82.5 mV dec<sup>–1</sup> and lower charge transfer resistance of 1.11 Ω versus 1.31 Ω for LSCO-NP. Structural analyses confirmed that the LSCO-SP maintained their integrity under OER conditions. Furthermore, post-mortem X-ray photoelectron spectroscopy (XPS) and electron paramagnetic resonance (EPR) analyses reveal an increased formation of oxygen vacancies (O<sub>vac</sub>) in LSCO-SP, confirming that the supraparticle design tunes the lattice oxygen-mediated mechanism–oxygen vacancy site mechanism (LOM–OVSM), enhancing OER performance. The hierarchical structure of LSCO-SP highlights their potential as a novel building block for catalyst layers in renewable energy applications.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"17 38","pages":"53413–53426"},"PeriodicalIF":8.2000,"publicationDate":"2025-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Supraparticle Assembly of La0.8Sr0.2CoO3 Nanoparticles for Enhanced Lattice Oxygen Oxidation in Alkaline Electrolysis\",\"authors\":\"Mohaned Hammad*, , , Blaž Toplak, , , Adil Amin, , , Mena-Alexander Kräenbring, , , Ahammed Suhail Odungat, , , Mohammed-Ali Sheikh, , , Adarsh Jain, , , Amin S. Amin, , , Ralf Meckenstock, , , Thai Binh Nguyen, , , Khuzaifa Yahuza Muhammad, , , Abdallah Hamdan, , , Steven Angel, , , Michael Farle, , , Ulf-Peter Apfel, , , Hartmut Wiggers, , and , Doris Segets*, \",\"doi\":\"10.1021/acsami.5c11289\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Developing effective non-noble metal electrocatalysts for the oxygen evolution reaction (OER) remains challenging due to limited active sites, poor electronic conductivity, and high overpotentials associated with the conventional adsorbate evolution mechanism (AEM). To address these limitations, a one-step spray drying method is employed to assemble high-surface-area La<sub>0.8</sub>Sr<sub>0.2</sub>CoO<sub>3</sub> nanoparticles (LSCO-NP) into hierarchical supraparticles with ≈65% porosity and interconnected meso-/macropore networks. This architecture not only accelerates ion diffusion and interparticle electron transfer but also induces a mechanistic switch from the AEM to the lattice oxygen oxidation mechanism (LOM). La<sub>0.8</sub>Sr<sub>0.2</sub>CoO<sub>3</sub> supraparticles (LSCO-SP) demonstrate significantly enhanced OER performance, requiring ∼300 mV lower overpotential at 100 mA cm<sup>–2</sup> after 1 h compared to LSCO-NP. Moreover, LSCO-SP exhibit faster catalytic kinetics, evidenced by a smaller Tafel slope of 76.2 mV dec<sup>–1</sup> versus 82.5 mV dec<sup>–1</sup> and lower charge transfer resistance of 1.11 Ω versus 1.31 Ω for LSCO-NP. Structural analyses confirmed that the LSCO-SP maintained their integrity under OER conditions. Furthermore, post-mortem X-ray photoelectron spectroscopy (XPS) and electron paramagnetic resonance (EPR) analyses reveal an increased formation of oxygen vacancies (O<sub>vac</sub>) in LSCO-SP, confirming that the supraparticle design tunes the lattice oxygen-mediated mechanism–oxygen vacancy site mechanism (LOM–OVSM), enhancing OER performance. The hierarchical structure of LSCO-SP highlights their potential as a novel building block for catalyst layers in renewable energy applications.</p>\",\"PeriodicalId\":5,\"journal\":{\"name\":\"ACS Applied Materials & Interfaces\",\"volume\":\"17 38\",\"pages\":\"53413–53426\"},\"PeriodicalIF\":8.2000,\"publicationDate\":\"2025-09-11\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Applied Materials & Interfaces\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acsami.5c11289\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"MATERIALS SCIENCE, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Applied Materials & Interfaces","FirstCategoryId":"88","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acsami.5c11289","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
Supraparticle Assembly of La0.8Sr0.2CoO3 Nanoparticles for Enhanced Lattice Oxygen Oxidation in Alkaline Electrolysis
Developing effective non-noble metal electrocatalysts for the oxygen evolution reaction (OER) remains challenging due to limited active sites, poor electronic conductivity, and high overpotentials associated with the conventional adsorbate evolution mechanism (AEM). To address these limitations, a one-step spray drying method is employed to assemble high-surface-area La0.8Sr0.2CoO3 nanoparticles (LSCO-NP) into hierarchical supraparticles with ≈65% porosity and interconnected meso-/macropore networks. This architecture not only accelerates ion diffusion and interparticle electron transfer but also induces a mechanistic switch from the AEM to the lattice oxygen oxidation mechanism (LOM). La0.8Sr0.2CoO3 supraparticles (LSCO-SP) demonstrate significantly enhanced OER performance, requiring ∼300 mV lower overpotential at 100 mA cm–2 after 1 h compared to LSCO-NP. Moreover, LSCO-SP exhibit faster catalytic kinetics, evidenced by a smaller Tafel slope of 76.2 mV dec–1 versus 82.5 mV dec–1 and lower charge transfer resistance of 1.11 Ω versus 1.31 Ω for LSCO-NP. Structural analyses confirmed that the LSCO-SP maintained their integrity under OER conditions. Furthermore, post-mortem X-ray photoelectron spectroscopy (XPS) and electron paramagnetic resonance (EPR) analyses reveal an increased formation of oxygen vacancies (Ovac) in LSCO-SP, confirming that the supraparticle design tunes the lattice oxygen-mediated mechanism–oxygen vacancy site mechanism (LOM–OVSM), enhancing OER performance. The hierarchical structure of LSCO-SP highlights their potential as a novel building block for catalyst layers in renewable energy applications.
期刊介绍:
ACS Applied Materials & Interfaces is a leading interdisciplinary journal that brings together chemists, engineers, physicists, and biologists to explore the development and utilization of newly-discovered materials and interfacial processes for specific applications. Our journal has experienced remarkable growth since its establishment in 2009, both in terms of the number of articles published and the impact of the research showcased. We are proud to foster a truly global community, with the majority of published articles originating from outside the United States, reflecting the rapid growth of applied research worldwide.