Understanding Bridging Sites and Accelerating Quantum Efficiency for Photocatalytic CO_(2) Reduction

We report a novel double-shelled nanoboxes photocatalyst architecture with tailored interfaces that accelerate quantum efficiency for photocatalytic CO_(2) reduction reaction(CO_(2)RR)via Mo–S bridging bonds sites in S_(v)–In_(2)S_(3)@2H–MoTe_(2).The X-ray absorption near-edge structure shows that the formation of S_(v)–In_(2)S_(3)@2H–MoTe_(2) adjusts the coordination environment via interface engineering and forms Mo–S polarized sites at the interface.The interfacial dynamics and catalytic behavior are clearly revealed by ultrafast femtosecond transient absorption,time-resolved,and in situ diffuse reflectance–Infrared Fourier transform spectroscopy.A tunable electronic structure through steric interaction of Mo–S bridging bonds induces a 1.7-fold enhancement in S_(v)–In_(2)S_(3)@2H–MoTe_(2)(5)photogenerated carrier concentration relative to pristine S_(v)–In_(2)S_(3).Benefiting from lower carrier transport activation energy,an internal quantum efficiency of 94.01%at 380 nm was used for photocatalytic CO_(2)RR.This study proposes a new strategy to design photocatalyst through bridging sites to adjust the selectivity of photocatalytic CO_(2)RR.

Density Functional Theory Study on the Adsorption of Dioxygen on Small Pt-Pd Clusters

The electronic and physical properties of PtmPdn （m＋n≤5） metal clusters and their interactions with dioxygen have been studied by using hybrid density functional B3LYP method. The total energies, atomization energies, vibration frequencies, and charge distributions were reported. The Pt-Pt bridge site modified by Pd atoms was found to be the most active site for the dissociation of dioxygen, which was mainly due to the change of electronic structures of the Pt atoms in bimetallic Pt-Pd clusters.

Motivating Ru-bri site of RuO_(2)by boron doping toward high performance acidic and neutral oxygen evolution

The electrocatalysis of oxygen evolution reaction(OER)plays a key role in clean energy storage and transfer.Nonetheless,the sluggish kinetics and poor durability under acidic and neutral conditions severely hinder practical applications such as electrolyzer compatible with the powerful proton exchange membrane and biohybrid fuel production.Here,we report a borondoped ruthenium dioxide electrocatalyst(B-RuO_(2))fabricated by a facile boric acid assisted strategy which demonstrates excellent acidic and neutral OER performances.Density functional theory calculations and advanced characterizations reveal that the boron species form an anomalous B–O covalent bonding with the oxygen atoms of RuO_(2)and expose the fully coordinately bridge ruthenium site(Ru-bri site),which seems like a switch that turns on the inactive Ru-bri site into OER-active,resulting in more exposed active sites,modified electronic structure,and optimized binding energy of intermediates.Thus,the B-RuO_(2)exhibits an ultralow overpotential of 200 mV at 10 mA/cm^(2)and maintains excellent stability compared to commercial RuO_(2)in 0.5 M sulfuric acid.Moreover,the superior performance is as well displayed in neutral electrolyte,surpassing most previously reported catalysts.