Computational screening of single-atom catalysts supported by VS₂ monolayers for electrocatalytic oxygen reduction/evolution reactions

Abstract

The development of highly-efficient bifunctional electrocatalysts to boost oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is highly desirable for energy conversion and storage devices. Herein, by means of...

Controlled synthesis of Ru-single-atoms on ordered mesoporous phosphine polymers for microwave-assisted conversion of biomass-derived sugars to artificial sweeteners

“…Over several years, supported single-atoms have been shown as a new frontier in solid catalysis owing to their large surface-tovolume ratio, high selectivity, and unique role compared to metals in the bulk or nano-state. [13][14][15][16] Nevertheless, metal single atoms containing isolated metals at the support are challenging as they are thermodynamically unstable and aggregated to nanoparticles and clusters. [17][18][19] For their stabilization, metal-organic frameworks (MOFs), carbon, graphene, metal hydroxides, and metal oxides have so far been used as supports; yet, their impact on activity and stability requires further attention due to inadequate metal-support interactions.…”

“…26,27 The microenvironment engineering of active sites by adjusting the neighboring steric effect of the organic ligand in the POP determines the adsorption of substrates, where phosphine and phosphates as ligand are utilized to tailor the selectivity of metal nanoparticles. 15,[27][28][29] Hence, phosphine exerts a unique "ligand effect" to adjust the neighboring environment of active metals. Thus, it would be encouraging to utilize the chemoselectivity of phosphinebased supports for hydrogenating C 5 and C 6 sugars, which is however extremely rare in the literature.…”

Rational Design of a Low-Dimensional and Metal-free Heterostructure for Efficient Water Oxidation: DFT and Experimental Studies

“…According to the difference of free energy of intermediates, it can be judged that the rate-determining step (RDS) is the third step (*O → *OOH) on both MWCNTs and (C 59 N) 2 / MWCNTs. 43 The (C 59 N) 2 /MWCNTs shows lower free energy of RDS (1.71 eV) than that of MWCNTs (2.10 eV) at a thermodynamic potential (U), U = 0 V. The uphill energy state of RDS decreased by the decoration of (C 59 N) 2 , confirming the superior electroactivity of (C 59 N) 2 /MWCNTs than that of MWCNTs alone. According to the Sabatier principle, too weak or too strong binding strength of intermediates goes against the adsorption and desorption on the catalyst surface.…”

“…As displayed in Figure e,f, a larger potential is needed for MWCNTs to drive the electrocatalytic OER than that of (C 59 N) 2 /MWCNTs. According to the difference of free energy of intermediates, it can be judged that the rate-determining step (RDS) is the third step (*O → *OOH) on both MWCNTs and (C 59 N) 2 /MWCNTs . The (C 59 N) 2 /MWCNTs shows lower free energy of RDS (1.71 eV) than that of MWCNTs (2.10 eV) at a thermodynamic potential ( U ), U = 0 V. The uphill energy state of RDS decreased by the decoration of (C 59 N) 2 , confirming the superior electroactivity of (C 59 N) 2 /MWCNTs than that of MWCNTs alone.…”

N-Doped CrS2 Monolayer as a Highly-Efficient Catalyst for Oxygen Reduction Reaction: A Computational Study

“…In recent years, single-layer transition metal dichalcogenides (TMDs) have become a hotspot of theoretical and experimental research owing to their large surface area, stability, and peculiar electronic structure [ 18 , 19 , 20 , 21 , 22 , 23 ]. Thus, TMD-based materials have been widely employed in nanoelectronics, nanophotonics, the absorber layer in solar cells, anode materials, field-effect transistors, and so on [ 24 , 25 , 26 , 27 , 28 ]. More interestingly, the heteroatom doped TMDs have attracted great interest because they have more active sites, low cost, high stability, and high efficiency as potential electrocatalytic catalysts [ 29 , 30 , 31 , 32 , 33 , 34 , 35 ].…”