Reactivity of quasi-free electrons toward N and its impact on H formation mechanism in water radiolysis.

Picosecond pulse radiolysis measurements were employed to assess the effectiveness of N in scavenging quasi-free electrons in aqueous solutions. The absorption spectra of hydrated electrons were recorded within a 100 ps timeframe across four distinct solutions with N concentrations of 0.5, 1, 2, and 5 M in water.

Direct time-resolved observation of surface-bound carbon dioxide radical anions on metallic nanocatalysts.

Time-resolved identification of surface-bound intermediates on metallic nanocatalysts is imperative to develop an accurate understanding of the elementary steps of CO reduction. Direct observation on initial electron transfer to CO to form surface-bound CO radicals is lacking due to the technical challenges. Here, we use picosecond pulse radiolysis to generate CO via aqueous electron attachment and observe the stabilization processes toward well-defined nanoscale metallic sites.

Selective CO reduction to CHOH over atomic dual-metal sites embedded in a metal-organic framework with high-energy radiation.

The efficient use of renewable X/γ-rays or accelerated electrons for chemical transformation of CO and water to fuels holds promise for a carbon-neutral economy; however, such processes are challenging to implement and require the assistance of catalysts capable of sensitizing secondary electron scattering and providing active metal sites to bind intermediates. Here we show atomic Cu-Ni dual-metal sites embedded in a metal-organic framework enable efficient and selective CHOH production (~98%) over multiple irradiated cycles. The usage of practical electron-beam irradiation (200 keV; 40 kGy min) with a cost-effective hydroxyl radical scavenger promotes CHOH production rate to 0.

Pulse radiolysis study on the reactivity of NO˙ radical toward uranous(iv), hydrazinium nitrate and hydroxyl ammonium nitrate at room temperature and at 45 °C.

Concentrated nitric acid solutions subjected to radiation produce radicals of extreme importance in the reprocessing of spent nuclear fuel. Knowledge of the different rate constants of the reactions involved in this chemistry is needed to improve the efficiency of the process and to define safe operating practices. Pulse radiolysis measurements are performed to find the rate constant of the reaction between NO3˙ radicals and U(iv) in highly concentrated nitrate solution.