Insight into Selectivity Differences of Glycerol Electro-Oxidation on Pt(111) and Ag(111)
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Insight into Selectivity Differences of Glycerol Electro-Oxidation on Pt(111) and Ag(111). / Meng, Zhe; Tran, David; Hjelm, Johan; Kristoffersen, Henrik H.; Rossmeisl, Jan.
I: ACS Catalysis, Bind 14, Nr. 4, 2024, s. 2455-2462.Publikation: Bidrag til tidsskrift › Tidsskriftartikel › Forskning › fagfællebedømt
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TY - JOUR
T1 - Insight into Selectivity Differences of Glycerol Electro-Oxidation on Pt(111) and Ag(111)
AU - Meng, Zhe
AU - Tran, David
AU - Hjelm, Johan
AU - Kristoffersen, Henrik H.
AU - Rossmeisl, Jan
N1 - Funding Information: The authors gratefully acknowledge financial support from Independent Research Fund Denmark, through grant no 1127-00372B. Z.M., H.H.K., and J.R. also acknowledge the Danish National Research Foundation Center for High-Entropy Alloy Catalysis (CHEAC) DNRF149. Publisher Copyright: © 2024 American Chemical Society
PY - 2024
Y1 - 2024
N2 - Electro-oxidation is a way to utilize glycerol, a byproduct of biodiesel production, to produce fuels and feedstock chemicals for the chemical industry. A significant challenge is to get products with high selectivity, so it is desirable to understand the glycerol oxidation mechanisms in further detail. Using density functional theory calculations, we investigated possible glycerol oxidation intermediates on Pt(111) and Ag(111). We find that the different adsorption preferences of the intermediates on Pt (adsorption via carbon atoms) and Ag (adsorption via oxygen atoms) lead to different preferred reaction pathways, resulting in different products. The reaction pathways on both surfaces involve glyceraldehyde as a key intermediate; however, upon further oxidation, Pt(111) preferentially produces glyceric acid (CH2OH-CHOH-COOH), while on Ag(111) C-C bonds are broken, which leads to the production of glycolaldehyde and formic acid (CH2OH-CHO and HCOOH). These predictions agree well with the experimental outcome of the electro-oxidation of glycerol on Pt and Ag surfaces. Our study therefore provides useful insights for optimizing the selectivity of glycerol oxidation and improving the utilization of glycerol.
AB - Electro-oxidation is a way to utilize glycerol, a byproduct of biodiesel production, to produce fuels and feedstock chemicals for the chemical industry. A significant challenge is to get products with high selectivity, so it is desirable to understand the glycerol oxidation mechanisms in further detail. Using density functional theory calculations, we investigated possible glycerol oxidation intermediates on Pt(111) and Ag(111). We find that the different adsorption preferences of the intermediates on Pt (adsorption via carbon atoms) and Ag (adsorption via oxygen atoms) lead to different preferred reaction pathways, resulting in different products. The reaction pathways on both surfaces involve glyceraldehyde as a key intermediate; however, upon further oxidation, Pt(111) preferentially produces glyceric acid (CH2OH-CHOH-COOH), while on Ag(111) C-C bonds are broken, which leads to the production of glycolaldehyde and formic acid (CH2OH-CHO and HCOOH). These predictions agree well with the experimental outcome of the electro-oxidation of glycerol on Pt and Ag surfaces. Our study therefore provides useful insights for optimizing the selectivity of glycerol oxidation and improving the utilization of glycerol.
KW - DFT calculations
KW - electrocatalysis
KW - glycerol
KW - oxidation
KW - platinum
KW - selectivity
KW - silver
U2 - 10.1021/acscatal.3c05551
DO - 10.1021/acscatal.3c05551
M3 - Journal article
AN - SCOPUS:85184830678
VL - 14
SP - 2455
EP - 2462
JO - ACS Catalysis
JF - ACS Catalysis
SN - 2155-5435
IS - 4
ER -
ID: 383191763