Mohd Afshan, Subhabrata Das, Daya Rani, Soumyadip Sharangi, Harini E. M, Mansi Pahuja, Shumile Ahmed Siddiqui, Seema Rani, Nikita Chaudhary, Jyoti and Kaushik Ghosh*,
{"title":"双金属硒化物的协同表面重建和界面工程：推进可再生能源存储和析氧","authors":"Mohd Afshan, Subhabrata Das, Daya Rani, Soumyadip Sharangi, Harini E. M, Mansi Pahuja, Shumile Ahmed Siddiqui, Seema Rani, Nikita Chaudhary, Jyoti and Kaushik Ghosh*, ","doi":"10.1021/acsami.4c2264810.1021/acsami.4c22648","DOIUrl":null,"url":null,"abstract":"<p >Designing a bimetallic selenide-based heterostructure that possesses high catalytic efficiency, high capacity, and rate capability remains challenging due to constraints imposed by slow reaction kinetics, inadequate electrode utilization, and significant volume deformation. In this study, we successfully engineer a heterostructure comprising carbon nanotubes intertwined with sea urchin-like Bi<sub>2</sub>Se<sub>3</sub>@NiSe<sub>2</sub> nanostructures having high electronic conductivity, high specific capacity, sufficiently exposed active sites, and favorable charge carrier migration. The interface engineering of the multilevel Bi<sub>2</sub>Se<sub>3</sub>@NiSe<sub>2</sub> nanostructure on the carbon nanotube (CNT) framework synergistically reduces energetic barriers and accelerates oxygen evolution kinetics as well as promotes faster Faradaic reactions to enhance charge storage. As a consequence, the as-designed flexible supercapacitor device (Bi<sub>2</sub>Se<sub>3</sub>@NiSe<sub>2</sub>-CNT/CTs//AC-CNT/CTs) attains a peak energy density of 75.93 Wh kg<sup>–1</sup> and a maximum power density of 15.12 kW kg<sup>–1</sup>, demonstrating remarkable durability (94.35% capacitance retention) after 40k cycles. The higher density of states near the Fermi level in the Bi<sub>2</sub>Se<sub>3</sub>@NiSe<sub>2</sub> hybrid enhances electronic conductivity and charge carrier mobility, coupled with efficient OH<sup>–</sup> adsorption (Δ<i>E</i><sub>a</sub> = −4.352 eV@Bi site, Δ<i>E</i><sub>a</sub> = −4.932 eV@Ni site), thereby trapping more electrolyte ions and promoting faster redox reactions. Additionally, the induced electronic interactions between core selenides and surface-generated thin layers of hydroxide/oxide synergistically accelerate the reaction kinetics in terms of a lower overpotential (199 mV@20 mA cm<sup>–2</sup>), a lower Tafel slope (59.2 mV dec<sup>–1</sup>), and a higher electrochemical surface area (1460.0 cm<sup>2</sup>) toward oxygen evolution. The proposed study on the construction of dual redox-active site heterostructures is expected to create avenues for advancing renewable energy systems.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"17 16","pages":"23892–23910 23892–23910"},"PeriodicalIF":8.2000,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Synergistic Surface Reconstruction and Interface Engineering in Bimetallic Selenides: Advancing Renewable Energy Storage and Oxygen Evolution\",\"authors\":\"Mohd Afshan, Subhabrata Das, Daya Rani, Soumyadip Sharangi, Harini E. M, Mansi Pahuja, Shumile Ahmed Siddiqui, Seema Rani, Nikita Chaudhary, Jyoti and Kaushik Ghosh*, \",\"doi\":\"10.1021/acsami.4c2264810.1021/acsami.4c22648\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Designing a bimetallic selenide-based heterostructure that possesses high catalytic efficiency, high capacity, and rate capability remains challenging due to constraints imposed by slow reaction kinetics, inadequate electrode utilization, and significant volume deformation. In this study, we successfully engineer a heterostructure comprising carbon nanotubes intertwined with sea urchin-like Bi<sub>2</sub>Se<sub>3</sub>@NiSe<sub>2</sub> nanostructures having high electronic conductivity, high specific capacity, sufficiently exposed active sites, and favorable charge carrier migration. The interface engineering of the multilevel Bi<sub>2</sub>Se<sub>3</sub>@NiSe<sub>2</sub> nanostructure on the carbon nanotube (CNT) framework synergistically reduces energetic barriers and accelerates oxygen evolution kinetics as well as promotes faster Faradaic reactions to enhance charge storage. As a consequence, the as-designed flexible supercapacitor device (Bi<sub>2</sub>Se<sub>3</sub>@NiSe<sub>2</sub>-CNT/CTs//AC-CNT/CTs) attains a peak energy density of 75.93 Wh kg<sup>–1</sup> and a maximum power density of 15.12 kW kg<sup>–1</sup>, demonstrating remarkable durability (94.35% capacitance retention) after 40k cycles. The higher density of states near the Fermi level in the Bi<sub>2</sub>Se<sub>3</sub>@NiSe<sub>2</sub> hybrid enhances electronic conductivity and charge carrier mobility, coupled with efficient OH<sup>–</sup> adsorption (Δ<i>E</i><sub>a</sub> = −4.352 eV@Bi site, Δ<i>E</i><sub>a</sub> = −4.932 eV@Ni site), thereby trapping more electrolyte ions and promoting faster redox reactions. Additionally, the induced electronic interactions between core selenides and surface-generated thin layers of hydroxide/oxide synergistically accelerate the reaction kinetics in terms of a lower overpotential (199 mV@20 mA cm<sup>–2</sup>), a lower Tafel slope (59.2 mV dec<sup>–1</sup>), and a higher electrochemical surface area (1460.0 cm<sup>2</sup>) toward oxygen evolution. 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Synergistic Surface Reconstruction and Interface Engineering in Bimetallic Selenides: Advancing Renewable Energy Storage and Oxygen Evolution
Designing a bimetallic selenide-based heterostructure that possesses high catalytic efficiency, high capacity, and rate capability remains challenging due to constraints imposed by slow reaction kinetics, inadequate electrode utilization, and significant volume deformation. In this study, we successfully engineer a heterostructure comprising carbon nanotubes intertwined with sea urchin-like Bi2Se3@NiSe2 nanostructures having high electronic conductivity, high specific capacity, sufficiently exposed active sites, and favorable charge carrier migration. The interface engineering of the multilevel Bi2Se3@NiSe2 nanostructure on the carbon nanotube (CNT) framework synergistically reduces energetic barriers and accelerates oxygen evolution kinetics as well as promotes faster Faradaic reactions to enhance charge storage. As a consequence, the as-designed flexible supercapacitor device (Bi2Se3@NiSe2-CNT/CTs//AC-CNT/CTs) attains a peak energy density of 75.93 Wh kg–1 and a maximum power density of 15.12 kW kg–1, demonstrating remarkable durability (94.35% capacitance retention) after 40k cycles. The higher density of states near the Fermi level in the Bi2Se3@NiSe2 hybrid enhances electronic conductivity and charge carrier mobility, coupled with efficient OH– adsorption (ΔEa = −4.352 eV@Bi site, ΔEa = −4.932 eV@Ni site), thereby trapping more electrolyte ions and promoting faster redox reactions. Additionally, the induced electronic interactions between core selenides and surface-generated thin layers of hydroxide/oxide synergistically accelerate the reaction kinetics in terms of a lower overpotential (199 mV@20 mA cm–2), a lower Tafel slope (59.2 mV dec–1), and a higher electrochemical surface area (1460.0 cm2) toward oxygen evolution. The proposed study on the construction of dual redox-active site heterostructures is expected to create avenues for advancing renewable energy systems.
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.
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