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Water electrolysis is one promising and eco-friendly technique for energy storage, yet its overall efficiency is hindered by the sluggish kinetics of oxygen evolution reaction (OER). In response, developing strategies to boost OER catalyst performance is crucial. With the advances in characterization techniques, an extensive phenomenon of surface structure evolution into an active amorphous layer was uncovered. Surface reconstruction in a controlled fashion was then proposed as an emerging strategy to elevate water oxidation efficiency. In this work, Cr substitution induces the reconstruction of NiFexCr2-xO4 during cyclic voltammetry (CV) conditioning by Cr leaching, which leads to a superior OER performance. The best-performed NiFe0.25Cr1.75O4 shows a ~1500% current density promotion at overpotential η = 300 mV, which outperforms many advanced NiFe-based OER catalysts. It is also found that their OER activities are mainly determined by Ni:Fe ratio rather than Fe content in all metal elements. Meanwhile, the turnover frequency (TOF) values based on redox peak and total mass were obtained and analysed, and their possible limitations in the case of NiFexCr2-xO4 are discussed. Additionally, the high activity and durability were further verified in a membrane electrode assembly (MEA) cell, highlighting its potential for practical large-scale and sustainable hydrogen gas generation.
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Developing technologies based on the concept of methanol electrochemical refinery (e-refinery) is promising for carbon-neutral chemical manufacturing. However, a lack of mechanism understanding and material properties that control the methanol e-refinery catalytic performances hinders the discovery of efficient catalysts. Here, using 18O isotope-labeled catalysts, we find that the oxygen atoms in formate generated during the methanol e-refinery reaction can originate from the catalysts' lattice oxygen and the O-2p-band center levels can serve as an effective descriptor to predict the catalytic performance of the catalysts, namely, the formate production rates and Faradaic efficiencies. Moreover, the identified descriptor is consolidated by additional catalysts and theoretical mechanisms from density functional theory. This work provides direct experimental evidence of lattice oxygen participation and offers an efficient design principle for the methanol e-refinery reaction to formate, which may open up new research directions in understanding and designing electrified conversions of small molecules.
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Understanding and mastering the structural evolution of water oxidation electrocatalysts lays the foundation to finetune their catalytic activity. Herein, we demonstrate that surface reconstruction of spinel oxides originates from the metal-oxygen covalency polarity in the MT-O-MO backbone. A stronger MO-O covalency relative to MT-O covalency is found beneficial for a more thorough reconstruction towards oxyhydroxides. The structure-reconstruction relationship allows precise prediction of the reconstruction ability of spinel pre-catalysts, based on which the reconstruction degree towards the in situ generated oxyhydroxides can be controlled. The investigations of oxyhydroxides generated from spinel pre-catalysts with the same reconstruction ability provide guidelines to navigate the cation selection in spinel pre-catalysts design. This work reveals the fundamentals for manipulating the surface reconstruction of spinel pre-catalysts for water oxidation.
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Developing new strategies to advance the fundamental understanding of electrochemistry is crucial to mitigating multiple contemporary technological challenges. In this regard, magnetoelectrochemistry offers many strategic advantages in controlling and understanding electrochemical reactions that might be tricky to regulate in conventional electrochemical fields. However, the topic is highly interdisciplinary, combining concepts from electrochemistry, hydrodynamics, and magnetism with experimental outcomes that are sometimes unexpected. In this Review, we survey recent advances in using a magnetic field in different electrochemical applications organized by the effect of the generated forces on fundamental electrochemical principles and focus on how the magnetic field leads to the observed results. Finally, we discuss the challenges that remain to be addressed to establish robust applications capable of meeting present needs.
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Glycerol is a byproduct of biodiesel production and can be a low-cost source for some high-value C1-C3 chemicals. The conversion can be achieved by photo-, thermo-, and electro-catalysis methods. The electrocatalytic oxidation method is attractive due to its moderate reaction conditions and high electron to product efficiency. Most reported catalysts are based on noble metals, while metal oxides are rarely reported. Here, we investigated the electro-oxidation of glycerol on a series of ZnFexCo2-xO4 (x = 0, 0.4, 1.0, 1.4, and 2.0) spinel oxides. Seven types of value-added C1-C3 products including formate, glycolate, lactate, and glycerate can be obtained by this approach. The selectivity and Faraday efficiency toward these products can be tuned by adjusting the Fe/Co ratio and other experimental parameters, such as the applied potential, glycerol concentration, and electrolyte pH.
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THIS ARTICLE WAS WITHDRAWN BY THE PUBLISHER IN MARCH 2021
