Defective nickel sulfide hierarchical structures for efficient electrochemical conversion of plastic waste to value-added chemicals and hydrogen fuel

Chen, Z; Wei, W; Shen, Y; Ni, BJ

Defective nickel sulfide hierarchical structures for efficient electrochemical conversion of plastic waste to value-added chemicals and hydrogen fuel

Chen, Z

Wei, W

Shen, Y Ni, BJ

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Publisher:: ROYAL SOC CHEMISTRY
Publication Type:: Journal Article
Citation:: Green Chemistry, 2023, 25, (15), pp. 5979-5988
Issue Date:: 2023-07-04

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Field	Value	Language
dc.contributor.author	Chen, Z https://orcid.org/0000-0003-0627-0856
dc.contributor.author	Wei, W https://orcid.org/0000-0001-5613-337X
dc.contributor.author	Shen, Y
dc.contributor.author	Ni, BJ
dc.date.accessioned	2024-04-12T08:34:56Z
dc.date.available	2024-04-12T08:34:56Z
dc.date.issued	2023-07-04
dc.identifier.citation	Green Chemistry, 2023, 25, (15), pp. 5979-5988
dc.identifier.issn	1463-9262
dc.identifier.issn	1463-9270
dc.identifier.uri	http://hdl.handle.net/10453/177850
dc.description.abstract	Valorizing plastic waste into value-added chemicals/fuels in a green manner (e.g., electrochemical reforming) is a sustainable way to address the global pressing problem of plastic pollution. For the electro-reforming of plastic waste (e.g., polyethylene terephthalate (PET)), the development of highly active and selective catalysts remains a challenge. Herein, we have designed a low-cost and highly defective nickel sulfide to selectively convert ethylene glycol (PET monomer) into formate, with the co-production of hydrogen fuel. The optimal B and Co co-doped Ni3S2 (B,Co-NiS) only takes 1.341 V compared to the reversible hydrogen electrode (RHE) at 100 mA cm−2 for ethylene glycol oxidation, and it can realize high faradaic efficiency (>93%) and selectivity (>92%) for EG-to-formate conversion over a wide potential range. Furthermore, the bifunctional B,Co-NiS assisted real PET waste hydrolysate electrolysis in a membrane-electrode assembly (MEA) can generate 15.24 mmol formate per hour and attain H2 production efficiency over 70 times compared to conventional water electrolysis. Mechanism analyses indicate that the excellent catalytic performance of B,Co-NiS stems from the hierarchical structure, rich S defective sites, regulated electronic properties, and the dopant-facilitated in situ formation of an active sulfide@oxyhydroxide phase. This work provides an integrated nanostructure controlled-composition regulation strategy to design cost-effective catalysts for plastic electro-upcycling and paves the way for low-carbon plastic waste management.
dc.language	English
dc.publisher	ROYAL SOC CHEMISTRY
dc.relation	http://purl.org/au-research/grants/arc/DP220101139
dc.relation	http://purl.org/au-research/grants/arc/DE220100530
dc.relation.ispartof	Green Chemistry
dc.relation.isbasedon	10.1039/d3gc01499a
dc.rights	info:eu-repo/semantics/closedAccess
dc.subject	03 Chemical Sciences
dc.subject.classification	Organic Chemistry
dc.subject.classification	34 Chemical sciences
dc.title	Defective nickel sulfide hierarchical structures for efficient electrochemical conversion of plastic waste to value-added chemicals and hydrogen fuel
dc.type	Journal Article
utslib.citation.volume	25
utslib.for	03 Chemical Sciences
pubs.organisational-group	University of Technology Sydney
pubs.organisational-group	University of Technology Sydney/Faculty of Engineering and Information Technology
pubs.organisational-group	University of Technology Sydney/Faculty of Engineering and Information Technology/School of Civil and Environmental Engineering
pubs.organisational-group	University of Technology Sydney/Strength - CTWW - Centre for Technology in Water and Wastewater Treatment
utslib.copyright.status	closed_access	*
dc.date.updated	2024-04-12T08:34:54Z
pubs.issue	15
pubs.publication-status	Published
pubs.volume	25
utslib.citation.issue	15

Abstract:

Valorizing plastic waste into value-added chemicals/fuels in a green manner (e.g., electrochemical reforming) is a sustainable way to address the global pressing problem of plastic pollution. For the electro-reforming of plastic waste (e.g., polyethylene terephthalate (PET)), the development of highly active and selective catalysts remains a challenge. Herein, we have designed a low-cost and highly defective nickel sulfide to selectively convert ethylene glycol (PET monomer) into formate, with the co-production of hydrogen fuel. The optimal B and Co co-doped Ni3S2 (B,Co-NiS) only takes 1.341 V compared to the reversible hydrogen electrode (RHE) at 100 mA cm−2 for ethylene glycol oxidation, and it can realize high faradaic efficiency (>93%) and selectivity (>92%) for EG-to-formate conversion over a wide potential range. Furthermore, the bifunctional B,Co-NiS assisted real PET waste hydrolysate electrolysis in a membrane-electrode assembly (MEA) can generate 15.24 mmol formate per hour and attain H2 production efficiency over 70 times compared to conventional water electrolysis. Mechanism analyses indicate that the excellent catalytic performance of B,Co-NiS stems from the hierarchical structure, rich S defective sites, regulated electronic properties, and the dopant-facilitated in situ formation of an active sulfide@oxyhydroxide phase. This work provides an integrated nanostructure controlled-composition regulation strategy to design cost-effective catalysts for plastic electro-upcycling and paves the way for low-carbon plastic waste management.

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http://hdl.handle.net/10453/177850