Electrocatalytic Ethylene Glycol to Long-Chain C<sub>3+</sub> α-Hydroxycarboxylic Acids via Cross-Coupling with Primary Alcohols

Electrocatalytic conversion of ethylene glycol (EG) into α-hydroxycarboxylic acids (α-HCAs) holds great importance for advancing sustainable chemical development since EG is widely accessible in polyethylene terephthalate (PET) plastic and biomass. Herein, we report the direct electrocatalytic cross-coupling of EG and primary C<sub>1</sub>-C<sub>4</sub> alcohol, producing carbon-chain-propagated C<sub>3</sub>-C<sub>6</sub> α-HCAs over a gold (Au) catalyst. Taking EG and methanol (MeOH) cross-coupling to lactic acid (LA) as an example, experimental evidence shows that stabilization of the aldehyde intermediates (glycolaldehyde and formaldehyde from EG and MeOH, respectively) without overoxidation is important for the following cross-coupling via aldol condensation and thus LA formation. Based on this understanding, we systematically modulate the catalyst and reaction conditions, achieving a high LA productivity of 268.1 μmol cm<sup>-2</sup> h<sup>-1</sup> with a Faradaic efficiency of 28.7% at a constant current of 100 mA cm<sup>-2</sup>. The carbon-chain propagation strategy shows generality for EG cross-coupling with C<sub>1</sub>-C<sub>4</sub> primary alcohols, successfully producing C<sub>3</sub>-C<sub>6</sub> α-HCAs. As a proof of concept, a postconsumer PET bottle is converted to LA with a good productivity of 224.5 μmol cm<sup>-2</sup> in a 2 h electrolysis. This work demonstrates the possibility of the electrocatalytic strategy to convert EG into long-chain compounds via C-C bond cross-coupling, representing a crucial step toward building a sustainable society.

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Journal
Journal of the American Chemical Society
Published
2025-04-08
DOI
https://doi.org/10.1021/jacs.5c04034
Citations
23
Primary Topic
Asymmetric Hydrogenation and Catalysis
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article
Field-Weighted Citation Impact
12.36
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article

Electrocatalytic Ethylene Glycol to Long-Chain C3+ α-Hydroxycarboxylic Acids via Cross-Coupling with Primary Alcohols

Haohong Duan, Qiujin Shi, Ruo-Pu Li, Xiang Liu et al.
23 citations
Journal of the American Chemical Society
Asymmetric Hydrogenation and Catalysis
12.36
article

Electrocatalytic Ethylene Glycol to Long-Chain C3+ α-Hydroxycarboxylic Acids via Cross-Coupling with Primary Alcohols

Haohong Duan, Qiujin Shi, Ruo-Pu Li, Xiang Liu, Xi Wang, Bo‐Jun Yuan, Yuquan Zhu, Wengio Tang
article en
23 citations

Abstract

Electrocatalytic conversion of ethylene glycol (EG) into α-hydroxycarboxylic acids (α-HCAs) holds great importance for advancing sustainable chemical development since EG is widely accessible in polyethylene terephthalate (PET) plastic and biomass. Herein, we report the direct electrocatalytic cross-coupling of EG and primary C<sub>1</sub>-C<sub>4</sub> alcohol, producing carbon-chain-propagated C<sub>3</sub>-C<sub>6</sub> α-HCAs over a gold (Au) catalyst. Taking EG and methanol (MeOH) cross-coupling to lactic acid (LA) as an example, experimental evidence shows that stabilization of the aldehyde intermediates (glycolaldehyde and formaldehyde from EG and MeOH, respectively) without overoxidation is important for the following cross-coupling via aldol condensation and thus LA formation. Based on this understanding, we systematically modulate the catalyst and reaction conditions, achieving a high LA productivity of 268.1 μmol cm<sup>-2</sup> h<sup>-1</sup> with a Faradaic efficiency of 28.7% at a constant current of 100 mA cm<sup>-2</sup>. The carbon-chain propagation strategy shows generality for EG cross-coupling with C<sub>1</sub>-C<sub>4</sub> primary alcohols, successfully producing C<sub>3</sub>-C<sub>6</sub> α-HCAs. As a proof of concept, a postconsumer PET bottle is converted to LA with a good productivity of 224.5 μmol cm<sup>-2</sup> in a 2 h electrolysis. This work demonstrates the possibility of the electrocatalytic strategy to convert EG into long-chain compounds via C-C bond cross-coupling, representing a crucial step toward building a sustainable society.

Journal of the American Chemical SocietyVol. 147(16)
CAS Key Laboratory of Urban Pollutant Conversion (CN), Unité Matériaux et Transformations (FR), Hubei Normal University (CN), Tsinghua University (CN)
Clean water and sanitation
Openalex Percentile: Top 1%
Asymmetric Hydrogenation and Catalysis
12.36
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