Continuous seawater electrolysis is efficient for green hydrogen production, but some key issues have been overlooked. For example, the accumulated to saturated NaCl in electrolyte is poison to cathode by covering its surface and available active sites. Herein we demonstrate Pt/NiFe Prussian blue analogue (Pt/NiFePBA) electrode can continuously catalyze hydrogen evolution effectively at −500 mA·cm−2 in a 6 M NaOH electrolyte containing saturated NaCl, without being impeded by the formation of NaCl crystals on the electrode surface, which is in distinct contrast to commercial electrodes. Experimental results indicate that Fe(CN)64− spontaneously released by Pt/NiFePBA blocks the traditionally preferred basal plane growth of NaCl along {100} facets, but favors its growth along {110} basal plane. This alteration leads to an increased crystallization difficulty of NaCl near the electrode, rendering it halophobic (anti-NaCl precipitation) property. This investigation should shed light on general salt involving process besides the practical implementation of seawater electrolysis.
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Active and durable electrocatalysts for methanol oxidation reaction are of critical importance to the commercial viability of direct methanol fuel cell, which has already attracted growing popularities. However, current methanol oxidation electrocatalysts fall far short of expectations and suffer from excessive use of noble metal, mediocre activity, and rapid decay. Here we report the Pt anchored on NiFe-LDHs surface hybrid for stable methanol oxidation in alkaline media. Based on the high intrinsic methanol oxidation activity of Pt nanoparticles, the substrates NiFe-LDHs further enhanced anti-poisoning ability and maintained unaffected stability after 200,000 s cycle test compared to commercial Pt/C catalyst. The use of NiFe-LDHs is believed to play the decisive role to evenly disperse Pt nanoparticles on their surface using single atomic dispersed Fe as anchoring sites, making full use of abundant OH groups and subsequent facilitating the oxidative removal of carbonaceous poison on neighboring Pt sites. This work highlights the specialty of NiFe-LDHs in improving the overall efficiency of methanol oxidation reaction.
Porous monolithic catalysts with high specific surface areas, which can not only facilitate heat/mass transfer, but also help to expose active sites, are highly desired in strongly exothermic or endothermic gas–solid phase reactions. In this work, hierarchical spinel monolithic catalysts with a porous woodpile architecture were fabricated via extrusion-based three-dimensional (3D) printing (direct ink writing, DIW in brief) of aluminate-intercalated layered double hydroxide (AI-LDH) followed by low temperature calcination. The intercalation of aluminate in LDH is found crucial to tailor the M2+/Al3+ ratio, integrate LDH nanosheets into monolithic catalyst, and enable the conversion of LDH to spinel at the temperature as low as 500 °C with high specific surface areas (> 350 m2/g). The rapid mass/heat transfer resulted from the versatile 3D network at macroscale and the highly dispersed and fully exposed active sites benefited from the porous structure at microscale endow the 3D-printed Pd loaded spinel MgAl-mixed metal oxide (3D-AI-Pd/MMO) catalyst with excellent catalytic performance in semi-hydrogenation of acetylene, achieving 100% conversion at 60 °C with more than 84% ethylene selectivity.