Nanoporous Palladium Hydride for Electrocatalytic N2 Reduction under Ambient Conditions. (24th January 2020)

• Record Type: Journal Article
• Authors: Xu, Wence; Fan, Guilan; Chen, Jialiang; Li, Jinhan; Zhang, Le; Zhu, Shengli; Su, Xuncheng; Cheng, Fangyi; Chen, Jun
• Is Part Of: Angewandte Chemie. Volume 132:Number 9(2020)
• Page Start: 3539
• Page End: 3544
• Publication Date: 2020-01-24
• Subjects: DFT-Rechnungen -- Hydride -- Nanoporöse Katalysatoren -- Stickstoffreduktionsreaktion -- Palladium; Chemistry -- Periodicals; 540
• DOI: 10.1002/ange.201914335
• Languages: English
• ISSNs: 0044-8249

Abstract

Abstract: The electrocatalytic nitrogen reduction reaction (NRR) is an alternative eco‐friendly strategy for sustainable N2 fixation with renewable energy. However, NRR suffers from sluggish kinetics owing to difficult N2 adsorption and N≡N cleavage. Now, nanoporous palladium hydride is reported as electrocatalyst for electrochemical N2 reduction under ambient conditions, achieving a high ammonia yield rate of 20.4 μg h −1 mg −1 with a Faradaic efficiency of 43.6 % at low overpotential of 150 mV. Isotopic hydrogen labeling studies suggest the involvement of lattice hydrogen atoms in the hydride as active hydrogen source. In situ Raman analysis and density functional theory (DFT) calculations further reveal the reduction of energy barrier for the rate‐limiting *N2 H formation step. The unique protonation mode of palladium hydride would provide a new insight on designing efficient and robust electrocatalysts for nitrogen fixation. Abstract : Nanoporöses Palladiumhydrid, das durch chemische Entlegierung und in‐situ‐Wasserstoffinjektion synthetisiert wurde, zeigt eine bemerkenswerte Aktivität in der elektrokatalytischen Stickstofffixierung. Die schnelle Aktivierungskinetik und effektive Umwandlung von N2 in das adsorbierte Zwischenprodukt *N2 H resultieren in einer hohen NH3 ‐Ausbeute (20.4 μg h −1 mg −1 ) und Faradayschem Wirkungsgrad (43.6 %).