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Tailoring the high-density active sites via metal-coordinated ionic liquid encapsulated trimetallic core-shell MOF-derived catalysts for superior ORR in flexible Al-air batteries
Energy Storage Materials ( IF 20.4 ) Pub Date : 2024-05-03 , DOI: 10.1016/j.ensm.2024.103447
Muthukumar Perumalsamy , Arunprasath Sathyaseelan , Shanmugasundaram Kamalakannan , Vijayakumar Elumalai , Hyung Chul Ham , Sang-Jae Kim

The attainment of practicality in flexible Al-air batteries is impeded by the need for efficient air cathodes. To address this challenge, we systematically engineered the trimetallic (ZnCoFe)NC catalyst with a unique morphology of nitrogen-doped carbon nanotubes (NCNTs) on the 3D polyhedral structure (IL-ZnCoFe@CNT/NC) as an effective cathode. The augmented growth of NCNT facilitated by the metal-coordinated ionic liquid enhances both the specific surface area and the electrochemically active surface area (ECSA). As a result, IL-ZnCoFe@CNT/NC material exhibits a higher onset (1.0 V vs RHE) and half-wave potential (E = 0.89 V vs. RHE) as well as low Tafel slope (61 mV/dec) and surpassed the bare MOF-derived catalysts and Pt/C. E decreased by only 7 mV after the stability test describes the durability and fast reaction kinetics in the ORR. Upon testing on flexible Al-air with IL-ZnCoFe@CNT/NC cathode catalysts, it exhibited an OCV of 1.49 V and a peak power density of 34.7 mW cm with 1.3 times higher power performance than the commercial Pt/C along with 3 times longevity than bare catalysts. Additionally, the Density-functional theory (DFT) calculations provide rational evidence that the IL-ZnCoFe@CNT/NC catalyst has an upshifted d-band center, which, in turn, enhances the adsorption of reaction intermediates, making the catalyst highly promising towards ORR.

中文翻译:

通过金属配位离子液体封装的三金属核壳 MOF 衍生催化剂定制高密度活性位点,以在柔性铝空气电池中实现卓越的 ORR

对高效空气阴极的需求阻碍了柔性铝空气电池的实用化。为了应对这一挑战,我们系统地设计了三金属 (ZnCoFe)NC 催化剂,该催化剂在 3D 多面体结构 (IL-ZnCoFe@CNT/NC) 上具有独特的氮掺杂碳纳米管 (NCNT) 形态,作为有效的阴极。金属配位离子液体促进 NCNT 的增强生长,提高了比表面积和电化学活性表面积 (ECSA)。因此,IL-ZnCoFe@CNT/NC 材料表现出较高的起始电压(相对于 RHE 为 1.0 V)和半波电位(相对于 RHE,E = 0.89 V)以及较低的塔菲尔斜率 (61 mV/dec),并超过了裸露的 MOF 衍生催化剂和 Pt/C。稳定性测试后 E 仅下降 7 mV,描述了 ORR 的耐久性和快速反应动力学。在使用 IL-ZnCoFe@CNT/NC 阴极催化剂的柔性铝空气上进行测试时,其 OCV 为 1.49 V,峰值功率密度为 34.7 mW cm,功率性能比商用 Pt/C 高 1.3 倍,同时也是商用 Pt/C 的 3 倍。比裸催化剂寿命更长。此外,密度泛函理论(DFT)计算提供了合理的证据,表明IL-ZnCoFe@CNT/NC催化剂具有上移的d带中心,这反过来又增强了反应中间体的吸附,使该催化剂在ORR。
更新日期:2024-05-03
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