c4446f9e140fd9decee0a094291b977f che_a2023m6v5n2p1395-1406.pdf fb600a54fcf46f6c10a59d802deaa6c911ae0cc4 che_a2023m6v5n2p1395-1406.pdf f1c1f73a2265ea408d7d991f924a7b1ca1e7fce8cf2cceaa501e10a84fcd628c che_a2023m6v5n2p1395-1406.pdf Title: Au Single Metal Atom for Carbon Dioxide Reduction Reaction Subject: CO2 is the gas that contributes the most to the greenhouse effect and, therefore, to global warming. One of the greatest challenges facing humanity is the reduction of the concentration of CO2 in the air. Here, we analyze the possible use of Au1@g-C3N4 electrocatalyst to transform CO2 into added-value products. We use density functional theory (DFT) to determine the reaction Gibbs energies for eight electron–proton transfer reaction paths of the electrochemical carbon dioxide reduction reaction (CO2RR) using a single Au atom supported on 2D carbon nitride support. Our simulations classify the Au1@g-C3N4 electrocatalysts as “beyond CO” since their formation is energetically favored, although their strong binding with a Au single atom does not allow the desorption process. DFT calculations revealed that the lowest energy pathway is CO2 (g) COOH* CO* HCO* HCOH* CH2OH* CH2* CH3* CH4 (g), where the first hydrogenation of CO to HCO is predicted as the rate-limiting step of the reaction with slightly lower potential than predicted for Cu electrodes, the most effective catalysts for CO2RR. Methane is predicted to be the main reaction product after eight proton–electron transfers (CO2 + 8 H+ + 8e- CH4 + 2H2O). The generation of formaldehyde is discarded due to the large formation energy of the adsorbed moiety and the production of methanol is slightly less favorable than methane formation. Our computational study helps to identify suitable electrocatalysts for CO2RR by reducing the amount of metal and using stable and low-cost supports. Keywords: electrocatalysis; carbon dioxide reduction; Au single metal atom; carbon nitride; computational hydrogen electrode; methane production Author: Anna Vidal-López, Sergio Posada-Pérez, Miquel Solà and Albert Poater Creator: LaTeX with hyperref Producer: pdfTeX-1.40.21 CreationDate: Wed Jun 7 07:48:05 2023 CEST ModDate: Wed Jun 7 07:52:09 2023 CEST Custom Metadata: no Metadata Stream: no Tagged: no UserProperties: no Suspects: no Form: none JavaScript: no Pages: 12 Encrypted: no Page size: 595.276 x 841.89 pts (A4) Page rot: 0 File size: 1935327 bytes Optimized: no PDF version: 1.7 name type encoding emb sub uni object ID ------------------------------------ ----------------- ---------------- --- --- --- --------- XDVTPV+URWPalladioL-Bold Type 1 Custom yes yes no 10 0 ITAEXQ+URWPalladioL-Roma Type 1 Custom yes yes no 15 0 JIPAMR+URWPalladioL-Ital Type 1 Custom yes yes no 19 0 NIWPOC+CMSY10 Type 1 Builtin yes yes no 23 0 IYDCBB+VnURWPalladioL Type 1 Custom yes yes no 27 0 PURWBA+VnURWPalladioL-Bold Type 1 Custom yes yes no 32 0 ELGHHL+PalatinoLinotype,Bold TrueType WinAnsi yes yes no 95 0 ELGHHM+PalatinoLinotype CID TrueType Identity-H yes yes yes 98 0 ELGHHN+PalatinoLinotype TrueType WinAnsi yes yes no 104 0 ELGHHP+PalatinoLinotype,Italic TrueType WinAnsi yes yes no 107 0 ELGINJ+PalatinoLinotype TrueType MacRoman yes yes no 110 0 ELGHHL+PalatinoLinotype,Bold TrueType WinAnsi yes yes no 124 0 ELGHHM+PalatinoLinotype CID TrueType Identity-H yes yes yes 127 0 ELGHHN+PalatinoLinotype TrueType WinAnsi yes yes no 133 0 ELGHHP+PalatinoLinotype,Italic TrueType WinAnsi yes yes no 136 0 ELGINJ+PalatinoLinotype TrueType MacRoman yes yes no 139 0 ELGHHL+PalatinoLinotype,Bold TrueType WinAnsi yes yes no 153 0 ELGHHM+PalatinoLinotype CID TrueType Identity-H yes yes yes 156 0 ELGHHN+PalatinoLinotype TrueType WinAnsi yes yes no 162 0 ELGHHP+PalatinoLinotype,Italic TrueType WinAnsi yes yes no 165 0 ELGINJ+PalatinoLinotype TrueType MacRoman yes yes no 168 0 ELGHHL+PalatinoLinotype,Bold TrueType WinAnsi yes yes no 182 0 ELGHHM+PalatinoLinotype CID TrueType Identity-H yes yes yes 185 0 ELGHHN+PalatinoLinotype TrueType WinAnsi yes yes no 191 0 ELGHHP+PalatinoLinotype,Italic TrueType WinAnsi yes yes no 194 0 ELGINI+TimesNewRoman CID TrueType Identity-H yes yes yes 197 0 ELGINJ+PalatinoLinotype TrueType MacRoman yes yes no 203 0 GIGFZE+CMR10 Type 1 Builtin yes yes no 210 0 MPUDFL+PazoMath Type 1 Builtin yes yes no 220 0 GMSXPV+EURM10 Type 1 Builtin yes yes no 227 0 Jhove (Rel. 1.28.0, 2023-05-18) Date: 2024-04-20 02:36:18 CEST RepresentationInformation: che_a2023m6v5n2p1395-1406.pdf ReportingModule: PDF-hul, Rel. 1.12.4 (2023-03-16) LastModified: 2024-04-19 17:33:41 CEST Size: 1935327 Format: PDF Version: 1.7 Status: Well-Formed and valid SignatureMatches: PDF-hul MIMEtype: application/pdf PDFMetadata: Objects: 421 FreeObjects: 1 IncrementalUpdates: 0 DocumentCatalog: PageLayout: SinglePage PageMode: UseNone Outlines: Item: Title: Introduction Destination: section.1 Item: Title: Results Destination: section.2 Item: Title: Conclusions Destination: section.3 Item: Title: Computational Details and Models Destination: section.4 Item: Title: References Destination: section.5 Info: Title: Au Single Metal Atom for Carbon Dioxide Reduction Reaction Author: Anna Vidal-López, Sergio Posada-Pérez, Miquel Solà and Albert Poater Subject: CO2 is the gas that contributes the most to the greenhouse effect and, therefore, to global warming. One of the greatest challenges facing humanity is the reduction of the concentration of CO2 in the air. Here, we analyze the possible use of Au1@g-C3N4 electrocatalyst to transform CO2 into added-value products. We use density functional theory (DFT) to determine the reaction Gibbs energies for eight electron proton transfer reaction paths of the electrochemical carbon dioxide reduction reaction (CO2RR) using a single Au atom supported on 2D carbon nitride support. Our simulations classify the Au1@g-C3N4 electrocatalysts as “beyond CO” since their formation is energetically favored, although their strong binding with a Au single atom does not allow the desorption process. DFT calculations revealed that the lowest energy pathway is CO2 (g) COOH* CO* HCO* HCOH* CH2OH* CH2* CH3* CH4 (g), where the first hydrogenation of CO to HCO is predicted as the rate-limiting step of the reaction with slightly lower potential than predicted for Cu electrodes, the most effective catalysts for CO2RR. Methane is predicted to be the main reaction product after eight proton electron transfers (CO2 + 8 H+ + 8e- CH4 + 2H2O). The generation of formaldehyde is discarded due to the large formation energy of the adsorbed moiety and the production of methanol is slightly less favorable than methane formation. Our computational study helps to identify suitable electrocatalysts for CO2RR by reducing the amount of metal and using stable and low-cost supports. 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