Breaking the Pt Electron Symmetry and OH Spillover towards PtIr Active Center for Performance Modulation in Direct Ammonia Fuel Cell.

Autor: Barik S; Physical & Materials Chemistry Division, CSIR-National Chemical Laboratory, Pune, 411008, India.; Academy of Scientific and Innovative Research (AcSIR), Ghaziabad, 201002, India., Kharabe GP; Physical & Materials Chemistry Division, CSIR-National Chemical Laboratory, Pune, 411008, India.; Academy of Scientific and Innovative Research (AcSIR), Ghaziabad, 201002, India., Samal PP; Physical & Materials Chemistry Division, CSIR-National Chemical Laboratory, Pune, 411008, India.; Academy of Scientific and Innovative Research (AcSIR), Ghaziabad, 201002, India., Urkude RR; Beamline Development and Application Section, Bhabha Atomic Research Centre, Mumbai, 400085, India., Kumar S; Physical & Materials Chemistry Division, CSIR-National Chemical Laboratory, Pune, 411008, India.; Academy of Scientific and Innovative Research (AcSIR), Ghaziabad, 201002, India., Yoyakki A; Physical & Materials Chemistry Division, CSIR-National Chemical Laboratory, Pune, 411008, India.; Academy of Scientific and Innovative Research (AcSIR), Ghaziabad, 201002, India., Vinod CP; Academy of Scientific and Innovative Research (AcSIR), Ghaziabad, 201002, India.; Catalysis & Inorganic Chemistry Division, CSIR-National Chemical Laboratory, Pune, 411008, India., Krishnamurty S; Physical & Materials Chemistry Division, CSIR-National Chemical Laboratory, Pune, 411008, India.; Academy of Scientific and Innovative Research (AcSIR), Ghaziabad, 201002, India., Kurungot S; Physical & Materials Chemistry Division, CSIR-National Chemical Laboratory, Pune, 411008, India.; Academy of Scientific and Innovative Research (AcSIR), Ghaziabad, 201002, India.
Jazyk: angličtina
Zdroj: Small (Weinheim an der Bergstrasse, Germany) [Small] 2024 Dec; Vol. 20 (49), pp. e2406589. Date of Electronic Publication: 2024 Oct 04.
DOI: 10.1002/smll.202406589
Abstrakt: The growing interest in low-temperature direct ammonia fuel cells (DAFCs) arises from the utilization of a carbon-neutral ammonia source; however, DAFCs encounter significant electrode overpotentials due to the substantial energy barrier of the *NH 2 to *NH dehydrogenation, compounded by the facile deactivation by *N on the Pt surface. In this work, a unique catalyst, Pt 4 Ir@AlOOH/NGr i.e., Pt 4 Ir/ANGr, is introduced composed of PtIr alloy nanoparticles controllably decorated on the pseudo-boehmite phase of AlOOH-supported nitrogen-doped reduced graphene (AlOOH/NGr) composite, synthesized via the polyol reduction method. The detailed studies on the structural and electronic properties of the catalyst by XAS and VB-XPS reveal the possible electronic modulations. The optimized Pt 4 Ir/ANGr composition exhibits a significantly improved onset potential and mass activity for AOR. The DFT study confirms the OH ad species spillover by AlOOH and Pt 4 Ir (100) facilitates the conversion of the *NH 2 to *NH with minimal energy barriers. Finally, testing of DAFC at the system level using a membrane electrode assembly (MEA) with Pt 4 Ir/ANGr as the anode catalyst, demonstrating the suitability of the catalyst for its practical applications. This study thus uncovers the potential of the Pt 4 Ir catalyst in synergy with ANGr, largely addressing the challenges in hydrogen transportation, storage, and safety within DAFCs.
(© 2024 Wiley‐VCH GmbH.)
Databáze: MEDLINE
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