Understanding the activity of single atom catalysts for CO₂ reduction to C₂ products: A high throughput computational screening

Abstract

Tunable electronic structure of the central metal atoms in single-atom catalysts (SACs) helps to control the adsorption energy of reactants and different reaction intermediates involved in multistep chemical processes. Although...

Assessment of the Catalytic Performance of a Heterogeneous Fe2C Catalyst in the Formation of Multicarbon Products from Carbon Dioxide

“…54,55 This methodology has been employed to study CO 2 hydrogenation reactions on the surface of heterogeneous catalysts. 10,42,44,56 The combined experimental and computational investigation of the CO 2 to methanol on sulfur vacancyrich MoS 2 demonstrated by Deng and coworkers using a similar DFT method validates the reliability of the DFT methods employed in this study. 10 The surface of the orthorhombic model of Fe 2 C was built in a 2 × 2 × 2 supercell.…”

“…The periodic density functional calculations were performed using the Vienna Ab initio Simulation Package (VASP) , to get fundamental insight into the CO 2 hydrogenation pathway on the Fe 2 C catalyst surface. The projector augmented-wave pseudopotential method with the Perdew–Burke–Ernzerhof exchange-correlation functional and a plane-wave cutoff energy of 600 eV was adopted. , Grimme’s zero-damping DFT-D3 method was used to calculate the van der Waals correction. , This methodology has been employed to study CO 2 hydrogenation reactions on the surface of heterogeneous catalysts. ,,, The combined experimental and computational investigation of the CO 2 to methanol on sulfur vacancy-rich MoS 2 demonstrated by Deng and coworkers using a similar DFT method validates the reliability of the DFT methods employed in this study . The surface of the orthorhombic model of Fe 2 C was built in a 2 × 2 × 2 supercell.…”

Atomically dispersed Co2+ in a redox-active COF for electrochemical CO2 reduction to ethanol: unravelling mechanistic insight through operando studies

“…S33–S35, ESI‡). 14,16,20,22,69–71 In brief, the EXAFS study suggested a hexa-coordinated environment around Co 2+ , coordinated with two water molecules (axial positions), two chloride ions and two nitrogen atoms of the COF framework (Fig. 3(d)).…”

“…Interestingly, upon proton-coupled reduction of [Co II (η 2 -COF-N,N′)(CH 3 )(CO)Cl 2 ] ( OC*CH 3 ), a rapid C–C coupling is likely to be occurred to generate C 2 -intermediate [Co II (η 2 -COF-N,N′)(OCHCH 3 )Cl 2 ] ( *OCHCH 3 ) (Δ G = −1.48 eV). 69,70 In the next step, proton-coupled reduction of [Co II (η 2 -COF-N,N′)(OCHCH 3 )Cl 2 ] ( *OCHCH 3 ) would afford [Co II (η 2 -COF-N,N′)(OCH 2 CH 3 )Cl 2 ] ( *OCH 2 CH 3 ) (Δ G = +0.45 eV), which upon further proton-coupled reduction resulted in the formation of [Co II (η 2 -COF-N,N′)(HOCH 2 CH 3 )Cl 2 ] ( *HOCH 2 CH 3 ) (Δ G = −2.04 eV). Finally, the intermediate [Co II (η 2 -COF-N,N′)(HOCH 2 CH 3 )Cl 2 ] ( *HOCH 2 CH 3 ) expected to release ethanol (Δ G = +0.03 eV) and the initial catalyst [Co II (η 2 -COF-N,N′)(H 2 O) 2 Cl 2 ] ( H 2 O*OH 2 ) would be regenerated by retaking two water molecules, which would then re-enter into the catalytic cycle to continue the ethanol production (Fig.…”

Axial heteroatom (P, S and Cl)-decorated Fe single-atom catalyst for the oxygen reduction reaction: a DFT study

“…Other scholars came to similar results that were well-researched. 20,21 In addition, SACs exhibited good activity for electrochemical N 2 reduction, 22 CO 2 reduction, 23–25 lithium–sulfur batteries, 26 NO electroreduction 27,28 and CO detection. 29 Thus, the study on axial heteroatom-decorated Fe SAC for ORR is important, and this paper can shed light on the rational design of SAC catalysts with good performance.…”