Three-dimensional Ni/Ni3Fe embedded boron-doped carbon nanotubes nanochain frameworks as highly efficient and durable electrocatalyst for oxygen evolution reaction
Graphical abstract
Introduction
It is of great significance to produce environment-friendly and green-sustainable energy resources by the electrolytic and photo-assisted splitting of water. Especially, electron-driven oxygen evolution reaction (OER) has been motivated as a hot research topic among the researchers to obtain ultra-clean energy carrier, which is another way to battle against the depletion of fossil fuel and generous anxieties on greenhouse emission, towards the crave for a clean living environment [[1], [2], [3]]. So far, many earth-abundant transition metals supported electrocatalysts are being reported as an analogue/replace the benchmark oxygen evolution electrocatalysts (Pt/C, RuO2 and IrO2) for the accessible water oxidation electrocatalysis due to the cost and limited resources of those noble electrocatalysts, which absolutely promotes their widespread applications [[4], [5], [6]]. Unfortunately, most of the water-alkali OER electrocatalysts are still far from an application and suffer from efficiency due to the sluggish electron transfer kinetics. Therefore, it requires the speedy construction of alternative highly efficient earth-abundant electrocatalysts that should lower the overpotential/Tafel of water oxidation.
In this regard, keen attention has been dedicated to constructing earth-abundant alternative electrocatalysts for viable and economical water oxidation systems. 3D block transition-metal-based electrocatalysts, such as oxides [7], alloys [8], phosphides [9], carbides [10], selenides [11], borates [12], hydroxides [13], and nitrides [14] are fabricated via several facile strategies for high-performance water splitting electrocatalysis [15,16]. Moreover, sluggish four-electron-transfer kinetics, surface fouling, and aggregation of electro-active sites are the key determinants for the understanding of electrolytic water splitting applications, thus resulting in lack of efficiency [17,18]. On the other hand, most recent fundamental scientific and technological research interests suggest that the encapsulation of electro-active sites in heteroatom doped carbon-based hybrid materials is an extensive route to access the innovative materials with unique properties [[19], [20], [21], [22], [23]]. Moreover, it is necessary to have a general method to construct nanoarchitecture with controlled size, porosity with desired structural and chemical composition.
Recently, nickel and iron-based materials have been discovered as potentially desirable electrocatalysts due to their adsorptive properties, flexible-redox properties, and surface defects [[24], [25], [26]]. In particular, Ni3Fe and its composite materials have considerable attention within the researchers, owing to their exceptional electron/ion transport environments due to its typical redox properties, ultra-high surface areas, synergetic effect and unique electronic structure [27,28]. Previously, Ni3Fe and Ni3Fe supported materials have been concluded as a commendable oxygen evolution catalyst with ~300–400 mV overpotential [[29], [30], [31], [32], [33]]. In this sense, we intended to explore and boost the oxygen evolution behaviours of Ni/Ni3Fe materials by encapsulating in the boron-doped conductive carbon framework (CNT). In this work, for the first time, we present a novel construction of robust electrocatalyst based on Ni/Ni3Fe embedded boron-doped carbon nanotubes (Ni/Ni3Fe/B-CNT) nanoarchitecture, via self-assembly amine/borohydride hydrolysis driven approach of Ni/Fe/C precursor followed by in-situ reduction reaction for sustainable electro-oxidation of water (oxygen evolution) in alkali medium. Moreover, rationally designed Ni/Ni3Fe/B-CNT electrocatalyst overcomes sluggish kinetic barriers by attaining the high surface areas, abundant active sites, less aggregated porous nanoarchitecture, and thus facilitates the ion/electron transfer and bubble release. In addition, B-doped CNT with high flexibility contributes barrier free-electron transports to Ni/Ni3Fe active sites and keep high structure stability during electrolysis.
Section snippets
Materials
Cobalt nitrate hexahydrate (Co(NO3)3).6H2O), carbon nanotube paste (6% CNT), ferric nitrate nonahydrate (Fe(NO3)3).9H2O), sodium borohydride (NaBH4), ethylene glycol (EG), were purchased from Aladdin, Ltd., sodium hydroxide (NaOH), triethylamine (0.729 g mL−1, C6H15N, 99%, TEA), and ethanol were purchased from KESHI, KL., Nafion and platy-like ruthenium oxide nanostructure (RuO2 electrocatalyst, 99.9%) were procured from shanghai Macklin Ltd. All the chemicals were used as received; double
Formation of 3D porous Ni/Ni3Fe/B-CNT nanoarchitecture
It is quite challenging to construct highly-efficient earth-abundant electrocatalysts for OER water splitting due to their sluggish kinetics. To address such issue, based on our detailed results as shown in Fig. 2, Fig. 3, Fig. 4, Fig. 5 and other research literature reviews [34,35], a plausible reaction mechanism is proposed for the construction of Ni/Ni3Fe/B-CNT nanoarchitectures as demonstrated in Fig. 1. In general, the construction of composites or hybrid materials comprise multistage
Conclusions
In this work, to construct the thermodynamically and kinetically stable Ni/Ni3Fe homogeneously encapsulated flexible, inexpensive B-CNT nanosheets as a robust water-alkali electrocatalyst, a facile self-assembly amine hydrolysis driven approach was followed. This obtained result paves path to ease of fabrication of potentially desirable high-performance Ni/Ni3Fe/B-CNT with 265 mV overpotential with a less Tafel slope of 62.9 mV dec1, only composed of earth-abundant non-precious elements, as an
Declaration of competing interest
The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
Acknowledgments
The research was supported by the National Natural Science Foundation of China (Grant No's. 21773024, 51372033).
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