Transition metal on topological chiral semimetal PdGa with tailored hydrogen adsorption and reduction

Qun Yang,Yan Sun,Jiancun Rao,Claudia Felser,Jian Liu,Yudi Zhang,Thomas Heine,Guowei Li

doi:10.1038/s41524-021-00684-5

Abstract

The difficulties in designing high-performance hydrogen evolution reaction (HER) catalysts lie in the manipulation of adsorption behaviors of transition metals (TMs). Topological chiral semimetals with super-long Fermi arc surface states provide an ideal platform for engineering the catalytic performance of TMs through the metal-support interaction. We found the adsorption trends of TMs can be modified significantly when deposited at the surface of the PdGa chiral crystal. The electron transfer from the TMs to the surface states of the PdGa reshapes the d band structure of TMs and weakens the hydrogen intermediate bonding. Especially, W/PdGa is expected to be a good HER catalyst with close to zero Gibbs free energy. Experimentally, we found a Pt-like exchange current density and turnover frequency when depositing W atoms at the PdGa nanostructures surface. The findings provide a way to develop high-efficient electrocatalysts by the interplay between topological surface states and metal-support interaction.

Highlights

Topological materials have attracted extensive attention in the fields of chemistry and materials sciences owing to their robust topological surface states (TSSs) and high-mobility electrons
Supported metal catalysts are commonly used for many industrial chemical reactions as they can significantly boost the activities of supported metals.[11,12,13,14,15,16]
By combining the first-principles calculations and experimental measurements, we find that topological chiral semimetals, such as PdGa, could be a catalog of support that can greatly modify the adsorption behaviors of the supported metal catalysts of Mo, W, Ru, Rh, Pd, Pt, Ni, Co, and Fe via metal-support interaction (MSI)

Summary

INTRODUCTION

Topological materials have attracted extensive attention in the fields of chemistry and materials sciences owing to their robust topological surface states (TSSs) and high-mobility electrons. Benefited from the bulk symmetry-protected band structure and surface properties, topological materials are considered as a class of promising candidates for catalytic reactions such as hydrogen evolution, CO oxidation, and CO2 electroreduction.[1,2,3,4,5,6,7] Among them, topological chiral semimetal sharing the noncentrosymmetric cubic B20 structure is more attractive because of the experimentally confirmed super-long Fermi arcs that cross the entire Brillouin zone.[6,8,9,10] As HER catalysts, their topological surface states interact directly with hydrogen intermediates, exhibiting impressive high activities This class of topological chiral semimetals has large non-trivial energy windows up to 1 eV, and more importantly, 80% of the surface states are localized at the first atomic layer. The finding in this work reveals a valuable method to develop an efficient HER electrocatalyst by manipulating the MSI based on topological materials

RESULTS AND DISCUSSION

Computational methods

CODE AVAILABILITY