A highly efficient atomically thin curved PdIr bimetallene electrocatalyst

Fan Lv; Bolong Huang; Jianrui Feng; Weiyu Zhang; Kai Wang; Na Li; Jinhui Zhou; Peng Zhou; Wenxiu Yang; Yaping Du; Dong Su; Shaojun Guo

doi:10.1093/nsr/nwab019

A highly efficient atomically thin curved PdIr bimetallene electrocatalyst

Natl Sci Rev. 2021 Feb 2;8(9):nwab019. doi: 10.1093/nsr/nwab019. eCollection 2021 Sep.

Authors

Fan Lv¹, Bolong Huang², Jianrui Feng¹, Weiyu Zhang¹, Kai Wang¹, Na Li³, Jinhui Zhou¹, Peng Zhou¹, Wenxiu Yang¹, Yaping Du⁴, Dong Su⁵, Shaojun Guo¹

Affiliations

¹ School of Materials Science and Engineering, Peking University, Beijing 100871, China.
² Department of Applied Biology and Chemical Technology, Hong Kong Polytechnic University, Hong Kong, China.
³ Frontier Institute of Science and Technology jointly with College of Science, Xi'an Jiaotong University, Xi'an 710054, China.
⁴ School of Materials Science and Engineering & National Institute for Advanced Materials, Nankai University, Tianjin 300350, China.
⁵ Center for Functional Nanomaterials Brookhaven National Laboratory, Upton, NY 11973, USA.

Abstract

The multi-metallene with an ultrahigh surface area has great potential in precise tuning of surface heterogeneous d-electronic correlation by surface strain effect for the distinctive surface electronic structure, which is a brand new class of promising 2D electrocatalyst for sustainable energy device application. However, achieving such an atomically thin multi-metallene still presents a great challenge. Herein, we present a new synthetic method for an atomic-level palladium-iridium (PdIr) bimetallene with an average thickness of only ∼1.0 nm for achieving superior catalysis in the hydrogen evolution reaction (HER) and the formic acid oxidation reaction (FAOR). The curved PdIr bimetallene presents a top-ranked high electrochemical active area of 127.5 ± 10.8 m² g_Pd+Ir ^-1 in the reported noble alloy materials, and exhibits a very low overpotential, ultrahigh activity and improved stability for HER and FAOR. DFT calculation reveals that the PdIr bimetallene herein has a unique lattice tangential strain, which can induce surface distortion while concurrently creating a variety of concave-convex featured micro-active regions formed by variously coordinated Pd sites agglomeration. Such a strong strain effect correlates the abnormal on-site active 4d¹⁰-t_2g-orbital Coulomb correlation potential and directly elevates orbital-electronegativity exposure within these active regions, resulting in a preeminent barrier-free energetic path for significant enhancement of FAOR and HER catalytic performance.

Keywords: PdIr alloy; atomically thin; electrocatalyst; metallene; strain.