Robust enhanced hydrogen production at acidic conditions over molybdenum oxides-stabilized ultrafine palladium electroca

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Laboratory of Materials Physics, Centre for Environmental and Energy Nanomaterials, Anhui Key Laboratory of Nanomaterials and Nanotechnology, CAS Center for Excellence in Nanoscience Institute, Institute of Solid State Physics, Chinese Academy of Sciences, Hefei 230031, China 2 University of Science and Technology of China, Hefei 230026, China 3 Centre for Clean Environment and Energy, Griffith University, Gold Coast Campus, QLD 4222, Australia § Ji Sun and Xian Zhang contributed equally to this work. © Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2020 Received: 15 July 2020 / Revised: 27 July 2020 / Accepted: 31 August 2020

ABSTRACT Electrochemical water splitting is quite seductive for eco-friendly hydrogen fuel energy production, however, the attainment of highly efficient, durable, and cheap catalysts for the hydrogen evolution reaction (HER) remains challenging. In this study, molybdenum oxides stabilized palladium nanoparticle catalysts (MoOx-Pd) are in situ prepared on commercial carbon cloth (CC) by the facile two-step method of dip-coating and electrochemical reduction. As a self-supported Pd-based catalyst electrode, the MoOx-Pd/CC presents a competitive Tafel slope of 45.75 mV·dec−1, an ultralow overpotential of 25 mV, and extremely long cycling durability (one week) in 0.5 M H2SO4 electrolyte, superior to unmodified Pd catalysts and comparable to commercial Pt mesh electrode. On the one hand, the introduction of MoOx can inhibit the growth of Pd particles to obtain ultrafine Pd nanoparticles, thus exposing more available active sites. On the other hand, density functional theory (DFT) calculation revealed that MoOx on the surface of Pd metal can regulate the electronic structure of Pd metal and enhance its intrinsic catalytic activity of HER. This work suggests that transitional metal nanoparticles stabilized by molybdenum oxides are hopeful approaches for obtaining fruitful hydrogen-producing electrocatalysts.

KEYWORDS MoOx, Pd nanoparticles, electrocatalysts, hydrogen evolution reaction

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Introduction

The status quo of energy scarcity and environmental imbalance and unsustainability caused by tremendously consumed fossil fuels has been deteriorating at an alarming rate. So it is imminent and essential for us to replace traditional fuels with a green renewable energy source. Hydrogen, a clean-burning energy resource of high energy density, is acknowledged as the promising fuel due to its plenitude, renewability, and remarkable efficiency [1, 2]. Among lots of advisable approaches to attaining green fuel energy of hydrogen gas, electrochemical water splitting has drawn broad attention and has been researched and discussed extensively, owing to its proficient ability to utilize discontinuous energy by transforming regenerable electricity to hydrogen energy ecofriendly [3–5]. At present, the alkaline electrolyzer is the most universal facility to hydrogen [6]. However, the ability of such a device is constrained by the slow rate of hydrogen evolution kinetics of t