Title: A highly efficient atomically thin curved PdIr bimetallene electrocatalyst

Abstract

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 gPd+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-t2g-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 andmore » HER catalytic performance.« less

Authors:

Lv, Fan ^[1]; Huang, Bolong ^[2]; Feng, Jianrui ^[1]; Zhang, Weiyu ^[1]; Wang, Kai ^[1]; Li, Na ^[3]; Zhou, Jinhui ^[1]; Zhou, Peng ^[1]; Yang, Wenxiu ^[1]; Du, Yaping ^[4]; Su, Dong ^[5]; Guo, Shaojun ^[6]

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+ Show Author 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, Center for Functional Nanomaterials Brookhaven National Laboratory, Upton, NY 11973, USA
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
6. School of Materials Science and Engineering, Peking University, Beijing 100871, China, College of Engineering, Peking University, Beijing 100871, China

Publication Date:

Tue Feb 02 00:00:00 EST 2021

Sponsoring Org.:

USDOE

OSTI Identifier:

1819800

Alternate Identifier(s):

OSTI ID: 1775186

Grant/Contract Number:  

SC0012704

Resource Type:

Published Article

Journal Name:

National Science Review

Additional Journal Information:

Journal Name: National Science Review Journal Volume: 8 Journal Issue: 9; Journal ID: ISSN 2095-5138

Publisher:

Oxford University Press

Country of Publication:

China

Language:

English