We report the discovery of a dramatically enhanced N electroreduction reaction (NRR) selectivity under ambient conditions via the Li incorporation into poly(N-ethyl-benzene-1,2,4,5-tetracarboxylic diimide) (PEBCD) as a catalyst. The detailed electrochemical evaluation and density functional theory calculations showed that Li association with the O atoms in the PEBCD matrix can retard the HER process and can facilitate the adsorption of N to afford a high potential scope for the NRR process to proceed in the "[O-Li]·N-H" alternating hydrogenation mode. This atomic-scale incorporation strategy provides new insight into the rational design of NRR catalysts with higher selectivity.
SignificanceThis work provides evidence that the protein tau induces changes in blood vessels distinct from the effects of amyloid beta on vasculature and indicates a previously unknown pathway by which pathological tau may accelerate cognitive decline in Alzheimer’s disease.
As the first example of a photocatalytic system for splitting water without additional cocatalysts and photosensitizers, the comparatively cost-effective Cu I -based MOF, Cu-I-bpy (bpy=4,4'-bipyridine) exhibited highly efficient photocatalytic hydrogen production (7.09 mmol g h ). Density functional theory (DFT) calculations established the electronic structures of Cu-I-bpy with a narrow band gap of 2.05 eV, indicating its semiconductive behavior, which is consistent with the experimental value of 2.00 eV. The proposed mechanism demonstrates that Cu I clusters of Cu-I-bpy serve as photoelectron generators to accelerate the copper(I) hydride interaction, providing redox reaction sites for hydrogen evolution. The highly stable cocatalyst-free and self-sensitized Cu-I-bpy provides new insights into the future design of cost-effective d -based MOFs for highly efficient and long-term solar fuels production.
A reduced graphene oxide (RGO)-ZnIn(2)S(4) nanosheet composite was successfully synthesized via an in situ controlled growth process. The as-obtained RGO-ZnIn(2)S(4) composite showed excellent visible light H(2) production activity in the absence of noble metal cocatalysts.
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