Defect-Rich PdIr Bimetallene Nanoribbons with Interatomic Charge Localization for Isopropanol-Assisted Seawater Splitting.

ABSTRACT

Metallene with outstanding physicochemical properties is an efficient two-dimensional electrocatalysts for sustainable hydrogen (H2 ) production applications. However, the controllable fabrication of extended atomically thin metallene nanoribbons remains a formidable challenge. Herein, this work proposes a controllable preparation strategy for atomically thin defect-rich PdIr bimetallene nanoribbons (PdIr BNRs) with a thickness of only 1.5 nm for the efficient and stable isopropanol-assisted seawater electrolytic H2 production. When using PdIr BNRs as catalyst to build an isopropanol-assisted seawater electrolysis system, a voltage of only 0.38 V is required at @10 mA cm-2 to achieve energy-saving H2 production, while producing high value-added acetone at the anode. The aberration-corrected high-resolution transmission electron microscopy (HRTEM) clearly reveals that the PdIr BNRs possess abundant structural defects, which can additionally serve as highly catalytically active sites. Density functional theory (DFT) calculations combined with X-ray absorption spectroscopy studies reveal that the introduction of Ir atoms can induce the formation of a localized charge region and shift the d-band center of Pd down, thereby reducing the adsorption energy on the catalyst in favor of the rapid desorption of H2 . This work opens the way for the controllable design and construction of defect-rich atomically thin metallene nanoribbons for efficient electrocatalytic applications.