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Article: Concerted and Selective Electrooxidation of Polyethylene‐Terephthalate‐Derived Alcohol to Glycolic Acid at an Industry‐Level Current Density over a Pd−Ni(OH)2 Catalyst

TitleConcerted and Selective Electrooxidation of Polyethylene‐Terephthalate‐Derived Alcohol to Glycolic Acid at an Industry‐Level Current Density over a Pd−Ni(OH)2 Catalyst
Authors
Keywords*OH adspecies
Alcohol Oxidation
d Band Center
Electrocatalysis
Plastic Upcycling
Issue Date2-Feb-2023
PublisherWiley
Citation
Angewandte Chemie International Edition, 2023, v. 62, n. 11 How to Cite?
Abstract

Electro-reforming of Polyethylene-terephthalate-derived (PET-derived) ethylene glycol (EG) into fine chemicals and H2 is an ideal solution to address severe plastic pollution. Here, we report the electrooxidation of EG to glycolic acid (GA) with a high Faraday efficiency and selectivity (>85 %) even at an industry-level current density (600 mA cm−2 at 1.15 V vs. RHE) over a Pd−Ni(OH)2 catalyst. Notably, stable electrolysis over 200 h can be achieved, outperforming all available Pd-based catalysts. Combined experimental and theoretical results reveal that 1) the OH* generation promoted by Ni(OH)2 plays a critical role in facilitating EG-to-GA oxidation and removing poisonous carbonyl species, thereby achieving high activity and stability; 2) Pd with a downshifted d-band center and the oxophilic Ni can synergistically facilitate the rapid desorption and transfer of GA from the active Pd sites to the inactive Ni sites, avoiding over-oxidation and thus achieving high selectivity.


Persistent Identifierhttp://hdl.handle.net/10722/331359
ISSN
2023 Impact Factor: 16.1
2023 SCImago Journal Rankings: 5.300
ISI Accession Number ID

 

DC FieldValueLanguage
dc.contributor.authorLiu, Fulai-
dc.contributor.authorGao, Xutao-
dc.contributor.authorShi, Rui-
dc.contributor.authorGuo, Zhengxiao-
dc.contributor.authorTse, Edmund C M-
dc.contributor.authorChen, Yong-
dc.date.accessioned2023-09-21T06:55:03Z-
dc.date.available2023-09-21T06:55:03Z-
dc.date.issued2023-02-02-
dc.identifier.citationAngewandte Chemie International Edition, 2023, v. 62, n. 11-
dc.identifier.issn1433-7851-
dc.identifier.urihttp://hdl.handle.net/10722/331359-
dc.description.abstract<p>Electro-reforming of Polyethylene-terephthalate-derived (PET-derived) ethylene glycol (EG) into fine chemicals and H<sub>2</sub> is an ideal solution to address severe plastic pollution. Here, we report the electrooxidation of EG to glycolic acid (GA) with a high Faraday efficiency and selectivity (>85 %) even at an industry-level current density (600 mA cm<sup>−2</sup> at 1.15 V vs. RHE) over a Pd−Ni(OH)<sub>2</sub> catalyst. Notably, stable electrolysis over 200 h can be achieved, outperforming all available Pd-based catalysts. Combined experimental and theoretical results reveal that 1) the OH* generation promoted by Ni(OH)<sub>2</sub> plays a critical role in facilitating EG-to-GA oxidation and removing poisonous carbonyl species, thereby achieving high activity and stability; 2) Pd with a downshifted d-band center and the oxophilic Ni can synergistically facilitate the rapid desorption and transfer of GA from the active Pd sites to the inactive Ni sites, avoiding over-oxidation and thus achieving high selectivity.<br></p>-
dc.languageeng-
dc.publisherWiley-
dc.relation.ispartofAngewandte Chemie International Edition-
dc.subject*OH adspecies-
dc.subjectAlcohol Oxidation-
dc.subjectd Band Center-
dc.subjectElectrocatalysis-
dc.subjectPlastic Upcycling-
dc.titleConcerted and Selective Electrooxidation of Polyethylene‐Terephthalate‐Derived Alcohol to Glycolic Acid at an Industry‐Level Current Density over a Pd−Ni(OH)2 Catalyst-
dc.typeArticle-
dc.identifier.doi10.1002/anie.202300094-
dc.identifier.scopuseid_2-s2.0-85147179593-
dc.identifier.volume62-
dc.identifier.issue11-
dc.identifier.eissn1521-3773-
dc.identifier.isiWOS:000924164300001-
dc.identifier.issnl1433-7851-

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