An efficient cluster model to describe the oxygen reduction reaction activity of metal catalysts: a combined theoretical and experimental study

Abstract

An efficient model containing only 7 metal atoms was proposed to describe the ORR activity of metal catalysts by DFT calculation.

Utility of Silver Nanoparticles Embedded Covalent Organic Frameworks as Recyclable Catalysts for the Sustainable Synthesis of Cyclic Carbamates and 2-Oxazolidinones via Atmospheric Cyclizative CO2 Capture

“…While the chosen model is not an accurate representation of an Ag nanoparticle used in experiments, the simplistic Ag 6 /COF model has enabled us to include the influence of electronic interaction of the Ag nanoparticle and the COF support in the catalytic transformation of allyl carbamic acid to cyclic carbamate, while also keeping up with the computational time constraint. A similar model of small metal cluster embedded on catalyst supports has been used by Jia et al 69 and Cui et al 70 to study CO oxidation and oxygen reduction reaction trends over Ag/TiO 2 and Ag/CNT catalysts, respectively. Similarly, a 12 atom cluster model of transition metals has been successfully used by Howaltet al 71 to study the electrochemical production of ammonia over transition metal catalysts.…”

Atomically Dispersed Cu–N–C as a Promising Support for Low-Pt Loading Cathode Catalysts of Fuel Cells

“…Figures S1 and b show the schematic of relaxed structures of Pt/C and Pt/TM-SAC as well as the adsorption of ORR intermediates on the catalysts. During the ORR process, the adsorption of the intermediates, including HOO*, O*, and HO*, is crucial for the ORR activity. ,− The adsorption energy of O* on the catalysts (Δ E O ) is a good descriptor for the ORR activity of the catalysts . Pt is quite close to the top of the ORR volcano plots; however, the activity could be further improved if the adsorption of O* could be slightly weakened by ∼0.2 eV. , Figure c shows the Δ E O of Pt supported on various TM-SACs (TM = Fe, Co, Ni, Cu, Ag, or Au) in comparison to that of Pt/C by the DFT calculations.…”

“…A metal cluster with seven Pt atoms was used to represent Pt NPs according to our previous work. 43 The equation of free energy ΔG is obtained according to ref 44. The adsorption energy of O* (ΔE O ) is obtained as…”

“…All structures were fully relaxed until the convergence in energy and force reached 1.0 × 10 –4 eV and 1.0 × 10 –3 eV Å –1 , respectively. A metal cluster with seven Pt atoms was used to represent Pt NPs according to our previous work . The equation of free energy Δ G is obtained according to ref .…”

Nitrogénnel adalékolt grafén hordozós oxigénredukciós katalizátorok

“…Ugyanakkor az oxigénnel erősebb kötést alakít ki például a nikkel, molibdén, ruténium stb., így a reakció köztitermékeinek deszorpciója nehezebben megy végbe. Ez szintén az aktivitás csökkenését eredményezi[27,38]. ahol a nitrogén két szénatomhoz és egy oxigénatomhoz kapcsolódik[65].…”