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Dual-Doped Nickel Sulfide for Electro-Upgrading Polyethylene Terephthalate into Valuable Chemicals and Hydrogen Fuel.

ABSTRACT: Electro-upcycling of plastic waste into value-added chemicals/fuels is an attractive and sustainable way for plastic waste management. Recently, electrocatalytically converting polyethylene terephthalate (PET) into formate and hydrogen has aroused great interest, while developing low-cost catalysts with high efficiency and selectivity for the central ethylene glycol (PET monomer) oxidation reaction (EGOR) remains a challenge. Herein, a high-performance nickel sulfide catalyst for plastic waste electro-upcycling is designed by a cobalt and chloride co-doping strategy. Benefiting from the interconnected ultrathin nanosheet architecture, dual dopants induced up-shifting d band centre and facilitated in situ structural reconstruction, the Co and Cl co-doped Ni₃S₂ (Co, Cl-NiS) outperforms the single-doped and undoped analogues for EGOR. The self-evolved sulfide@oxyhydroxide heterostructure catalyzes EG-to-formate conversion with high Faradic efficiency (> 92%) and selectivity (> 91%) at high current densities (> 400 mA cm^-2). Besides producing formate, the bifunctional Co, Cl-NiS-assisted PET hydrolysate electrolyzer can achieve a high hydrogen production rate of 50.26 mmol h^-1 in 2 M KOH, at 1.7 V. This study not only demonstrates a dual-doping strategy to engineer cost-effective bifunctional catalysts for electrochemical conversion processes, but also provides a green and sustainable way for plastic waste upcycling and simultaneous energy-saving hydrogen production.

SUBMITTER: Chen Z

PROVIDER: S-EPMC10495299 | biostudies-literature | 2023 Sep

REPOSITORIES: biostudies-literature

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Dual-Doped Nickel Sulfide for Electro-Upgrading Polyethylene Terephthalate into Valuable Chemicals and Hydrogen Fuel.

Chen Zhijie Z Zheng Renji R Bao Teng T Ma Tianyi T Wei Wei W Shen Yansong Y Ni Bing-Jie BJ

Nano-micro letters 20230911 1

Electro-upcycling of plastic waste into value-added chemicals/fuels is an attractive and sustainable way for plastic waste management. Recently, electrocatalytically converting polyethylene terephthalate (PET) into formate and hydrogen has aroused great interest, while developing low-cost catalysts with high efficiency and selectivity for the central ethylene glycol (PET monomer) oxidation reaction (EGOR) remains a challenge. Herein, a high-performance nickel sulfide catalyst for plastic waste e ...[more]

PMID: 37695408

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Project description:Biodegradation of terephthalate (TPA) is a highly desired catabolic process for the bacterial utilization of this polyethylene terephthalate (PET) depolymerization product, but to date, the structure of terephthalate dioxygenase (TPDO), a Rieske oxygenase (RO) that catalyzes the dihydroxylation of TPA to a cis-diol, is unavailable. In this study, we characterized the steady-state kinetics and first crystal structure of TPDO from Comamonas testosteroni KF1 (TPDOKF1). TPDOKF1 exhibited substrate specificity for TPA (kcat/Km = 57 ± 9 mM-1 s-1). The TPDOKF1 structure harbors characteristic RO features as well as a unique catalytic domain that rationalizes the enzyme's function. The docking and mutagenesis studies reveal that its substrate specificity for TPA is mediated by the Arg309 and Arg390 residues, positioned on opposite faces of the active site. Additionally, residue Gln300 is also proven to be crucial for the activity, as its mutation to alanine decreases the activity (kcat) by 80%. This study delineates the structural features that dictate the substrate recognition and specificity of TPDO. IMPORTANCE Global plastic pollution has become the most pressing environmental issue. Recent studies on enzymes depolymerizing polyethylene terephthalate plastic into terephthalate (TPA) show some potential for tackling this. Microbial utilization of this released product, TPA, is an emerging and promising strategy for waste-to-value creation. Research in the last decade has identified terephthalate dioxygenase (TPDO) as being responsible for initiating the enzymatic degradation of TPA in a few Gram-negative and Gram-positive bacteria. Here, we determined the crystal structure of TPDO from Comamonas testosteroni KF1 and revealed that it possesses a unique catalytic domain featuring two basic residues in the active site to recognize TPA. Biochemical and mutagenesis studies demonstrated the crucial residues responsible for the substrate specificity of this enzyme.

Dataset Information

Dual-Doped Nickel Sulfide for Electro-Upgrading Polyethylene Terephthalate into Valuable Chemicals and Hydrogen Fuel.

Publications

Dual-Doped Nickel Sulfide for Electro-Upgrading Polyethylene Terephthalate into Valuable Chemicals and Hydrogen Fuel.

Similar Datasets

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