Abstract

Material interfaces permit electron transfer that modulates the electronic structure and surface properties of catalysts, leading to radically enhanced rates for many important reactions. Unlike conventional thoughts, the nanoscale interfacial interactions have been recently envisioned to be able to affect the reactivity of catalysts far from the interface. However, demonstration of such unlocalized alterations in existing interfacial materials is rare, impeding the development of new catalysts. We report the observation of unprecedented long-range activation of polydymite Ni3S4 nanorods through the interfacial interaction created by PdSx nanodots (dot-on-rod structure) for high-performance water catalytic electroreduction. Experimental results show that this local interaction can activate Ni3S4 rods with length even up to 25 nanometers due to the tailored surface electronic structure. We anticipate that the long-range effect described here may be also applicable to other interfacial material systems, which will aid the development of newly advanced catalysts for modern energy devices.

Highlights

  • It has been almost 46 years since the proposition of the hydrogen economy concept, which depicted a clean, safe, and sustainable alternative to the current hydrocarbon economy [1]

  • We carefully examined the samples at different stages during the synthesis by Transmission electron microscopy (TEM) to probe the evolutionary process of PapdpSexa-Nreid3S4whheentertohneanmorixotdusre(FriegaucrheeSd102)5. 0R∘oCd, -lbikuet product without

  • Strong interfacial interaction that leads to enhanced catalytic properties was widely affirmed in metal-support heterogeneous catalysts [5,6,7,8,9,10,11,12,13,14]

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Summary

Introduction

It has been almost 46 years since the proposition of the hydrogen economy concept, which depicted a clean, safe, and sustainable alternative to the current hydrocarbon economy [1]. An intuitive and commonly used method towards better catalysts is to couple transition metal nanoparticles with oxide or carbon supports, which creates the so-called ‘strong metal-support interactions’ that modulate the electronic structure and surface properties of catalytic materials, leading to enhanced performances [5,6,7,8,9,10,11,12,13,14] This interaction-induced phenomena has been extensively studied since being discovered by Tauster et al in 1970s [14], which is understood to be due to the electron transfer across the formed interfaces [7]. Material interface engineering has led to substantial advances in Research

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