17 research outputs found
Indium-decorated Pd nanocubes degrade nitrate anions rapidly
Indium-decorated palladium nanoparticles (In-on-PdNPs) are active for room-temperature catalytic reduction of aqueous nitrate, where the active sites are metallic In atoms on the Pd surface. The PdNPs are pseudo-spherical in shape, and it is unclear if their faceted nature plays a role in nitrate reduction. We synthesized different-sized, cube-shaped NPs with differing In coverages (sc%), and studied the resultant In-on-Pd-nanocubes (NCs) for nitrate reduction. The NCs exhibited volcano-shape activity dependence on In sc%, with peak activity around 65–75 sc%. When rate constants were normalized to undercoordinated atoms (at edge + corners), the NCs exhibited near-identical maximum activity (20×-higher than In-on-PdNPs) at ρIn/Pd edge+corner ∼0.5 (∼5 In atoms per 10 edge and corner atoms). NCs with a higher In edge + corner density (ρIn/Pd edge+corner ∼1.5) were less active but did not generate NH4+ at nitrate conversions tested up to 36 %. Edge-decorated cubes may be the structural basis of improved bimetallic catalytic denitrification of water
Integration of daytime radiative cooling and solar heating
Summary: In recent years, sustainable energy development has become a major theme of research. The combination of solar heating and daytime radiative cooling has the potential to build a competitive strategy to alleviate current environmental and energy problems. Several studies on the combination of daytime radiative cooling and solar heating have been reported to improve energy utilization efficiency. However, most integrations still have a low solar/mid-infrared spectrum regulation range, low heating/cooling performance, and poor stability. To promote this technology further for real-world applications, herein we summarize the latest progress, technical features, bottlenecks, and future opportunities for the current integration of daytime radiative cooling and solar heating through the switch mode (including electrical, thermal-responsive, and mechanical regulations) and collaborative mode
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Indium-decorated Pd nanocubes degrade nitrate anions rapidly
Indium-decorated palladium nanoparticles (In-on-PdNPs) are active for room-temperature catalytic reduction of aqueous nitrate, where the active sites are metallic In atoms on the Pd surface. The PdNPs are pseudo-spherical in shape, and it is unclear if their faceted nature plays a role in nitrate reduction. We synthesized different-sized, cube-shaped NPs with differing In coverages (sc%), and studied the resultant In-on-Pd-nanocubes (NCs) for nitrate reduction. The NCs exhibited volcano-shape activity dependence on In sc%, with peak activity around 65-75 sc%. When rate constants were normalized to undercoordinated atoms (at edge+corners), the NCs exhibited near-identical maximum activity (20×-higher than In-on-PdNPs) at ρIn/Pd edge+corner ~0.5 (~5 In atoms per 10 edge and corner atoms). NCs with a higher In edge+corner density (ρIn/Pd edge+corner ~1.5) were less active but did not generate NH4+ at nitrate conversions tested up to 36%. Edge-decorated cubes may be the structural basis of improved bimetallic catalytic denitrification of water
Insights into Nitrate Reduction over Indium-Decorated Palladium Nanoparticle Catalysts
Nitrate
(NO<sub>3</sub><sup>−</sup>) is an ubiquitous groundwater
contaminant and is detrimental to human health. Bimetallic palladium-based
catalysts have been found to be promising for treating nitrate (and
nitrite, NO<sub>2</sub><sup>−</sup>) contaminated waters. Those
containing indium (In) are unusually active, but the mechanistic explanation
for catalyst performance remains largely unproven. We report that
In deposited on Pd nanoparticles (NPs) (“In-on-Pd NPs”)
shows room-temperature nitrate catalytic reduction activity that varies
with volcano-shape dependence on In surface coverage. The most active
catalyst had an In surface coverage of 40%, with a pseudo-first order
normalized rate constant of <i>k</i><sub>cat</sub> ∼
7.6 L g<sub>surface-metal</sub><sup>−1</sup> min<sup>−1</sup>, whereas monometallic Pd NPs and In<sub>2</sub>O<sub>3</sub> have
nondetectible activity for nitrate reduction. X-ray absorption spectroscopy
(XAS) results indicated that In is in oxidized form in the as-synthesized
catalyst; it reduces to zerovalent metal in the presence of H<sub>2</sub> and reoxidizes following NO<sub>3</sub><sup>−</sup> contact. Selectivity in excess of 95% to nontoxic N<sub>2</sub> was
observed for all the catalysts. Density functional theory (DFT) simulations
suggest that submonolayer coverage amounts of metallic In provide
strong binding sites for nitrate adsorption and they lower the activation
barrier for the nitrate-to-nitrite reduction step. This improved understanding
of the In active site expands the prospects of improved denitrification
using metal-on-metal catalysts