Electrocatalytic Upcycling of Biomass and Plastic Wastes to Biodegradable Polymer Monomers and Hydrogen Fuel at High Current Densities

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(11), С. 6144 - 6155

Опубликована: Фев. 17, 2023

Transformation of biomass and plastic wastes to value-added chemicals fuels is considered an upcycling process that beneficial resource utilization. Electrocatalysis offers a sustainable approach; however, it remains huge challenge increase the current density deliver market-demanded with high selectivity. Herein, we demonstrate electrocatalytic strategy for glycerol (from biodiesel byproduct) lactic acid ethylene glycol polyethylene terephthalate waste) glycolic acid, both products being as valuable monomers biodegradable polymer production. By using nickel hydroxide-supported gold electrocatalyst (Au/Ni(OH)2), achieve selectivities (77 91%, respectively) densities at moderate potentials (317.7 mA/cm2 0.95 V vs RHE 326.2 1.15 RHE, respectively). We reveal can be enriched Au/Ni(OH)2 interface through their adjacent hydroxyl groups, substantially increasing local concentrations thus densities. As proof concept, employed membrane-free flow electrolyzer triglyceride PET bottles, attaining 11.2 g coupled 9.3 L H2 13.7 9.4 H2, respectively, revealing potential coproduction fuel from in fashion.

Язык: Английский

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Photoredox-Catalyzed Plastic Waste Conversion: Nonselective Degradation versus Selective Synthesis

ACS Catalysis, Год журнала: 2023, Номер 13(6), С. 3575 - 3590

Опубликована: Фев. 27, 2023

Plastic waste pollution is becoming one of the most pressing environmental crises due to large-scale production without satisfactory recycling schemes, especially with outbreak COVID-19 pandemic in recent years. Upcycling plastic into valuable chemicals powered by solar energy presents a substantially untapped opportunity turn treasure. In this review, fundamental principles from nonselective degradation selective synthesis are first clarified. Then, we aim outline representative advances photoredox-based catalytic conversion. Particular emphasis placed on valorization regarding versus synthesis. Finally, present challenges and individual insights for further exploration conversion domain. It anticipated that timely critical review would provide an instructive direction foresight plastics value-added chemical feedstocks, thus stimulating development circular sustainable economy coming decades.

Язык: Английский

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Electrocatalytic upcycling of polyethylene terephthalate plastic to formic acid coupled with energy-saving hydrogen production over hierarchical Pd-doped NiTe nanoarrays

Applied Catalysis B Environment and Energy, Год журнала: 2023, Номер 340, С. 123236 - 123236

Опубликована: Авг. 28, 2023

Язык: Английский

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Energy-saving and product-oriented hydrogen peroxide electrosynthesis enabled by electrochemistry pairing and product engineering

Nature Communications, Год журнала: 2023, Номер 14(1)

Опубликована: Окт. 7, 2023

Hydrogen peroxide (H

Язык: Английский

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Electrochemical Production of Glycolate Fuelled By Polyethylene Terephthalate Plastics with Improved Techno‐Economics

Small, Год журнала: 2023, Номер 19(39)

Опубликована: Май 25, 2023

Electrochemical valorization of polyethylene terephthalate (PET) waste streams into commodity chemicals offers a potentially sustainable route for creating circular plastic economy. However, PET wastes upcycling valuable C2 product remains huge challenge by the lack an electrocatalyst that can steer oxidation economically and selectively. Here, it is reported catalyst comprising Pt nanoparticles hybridized with γ-NiOOH nanosheets supported on Ni foam (Pt/γ-NiOOH/NF) favors electrochemical transformation real-word hydrolysate glycolate high Faradaic efficiency (> 90%) selectivity across wide reactant (ethylene glycol, EG) concentration ranges under marginal applied voltage 0.55 V, which be paired cathodic hydrogen production. Computational studies combined experimental characterizations elucidate Pt/γ-NiOOH interface substantial charge accumulation gives rise to optimized adsorption energy EG decreased barrier potential determining step. A techno-economic analysis demonstrates that, nearly same amount resource investment, electroreforming strategy towards production raise revenue up 2.2 times relative conventional chemical process. This work may thus serve as framework process net-zero carbon footprint economic viability.

Язык: Английский

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Catalytic Upcycling of Polyolefins

Chemical Reviews, Год журнала: 2024, Номер 124(16), С. 9457 - 9579

Опубликована: Авг. 16, 2024

The large production volumes of commodity polyolefins (specifically, polyethylene, polypropylene, polystyrene, and poly(vinyl chloride)), in conjunction with their low unit values multitude short-term uses, have resulted a significant pressing waste management challenge. Only small fraction these is currently mechanically recycled, the rest being incinerated, accumulating landfills, or leaking into natural environment. Since are energy-rich materials, there considerable interest recouping some chemical value while simultaneously motivating more responsible end-of-life management. An emerging strategy catalytic depolymerization, which portion C-C bonds polyolefin backbone broken assistance catalyst and, cases, additional molecule reagents. When products molecules materials higher own right, as feedstocks, process called upcycling. This review summarizes recent progress for four major upcycling strategies: hydrogenolysis, (hydro)cracking, tandem processes involving metathesis, selective oxidation. Key considerations include macromolecular reaction mechanisms relative to mechanisms, design transformations, effect conditions on product selectivity. Metrics describing critically evaluated, an outlook future advances described.

Язык: Английский

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Corrosion Engineering of Part‐Per‐Million Single Atom Pt₁/Ni(OH)₂ Electrocatalyst for PET Upcycling at Ampere‐Level Current Density

Advanced Materials, Год журнала: 2024, Номер 36(23)

Опубликована: Март 20, 2024

Abstract The plastic waste issue has posed a series of formidable challenges for the ecological environment and human health. While conventional recycling strategies often lead to down‐cycling, electrochemical strategy recovering valuable monomers enables an ideal, circular economy. Here corrosion synthesized single atom Pt 1 /Ni(OH) 2 electrocatalyst with part‐per‐million noble loading highly efficient selective upcycling polyethylene terephthalate (PET) into chemicals (potassium diformate terephthalic acid) green hydrogen is reported. Electro‐oxidation PET hydrolysate, ethylene glycol (EG), formate processed high Faraday efficiency (FE) selectivity (>90%) at current density close 1000 mA cm −2 (1.444 V vs RHE). in situ spectroscopy functional theory calculations provide insights mechanism understanding efficiency. Remarkably, electro‐oxidation EG ampere‐level also successfully illustrated by using membrane‐electrode assembly FEs integrated production 500 h continuous operation. This process allows chemical space‐time yield profitable (588–700 $ ton −1 PET), showing industrial perspective on single‐atom catalysis upcycling.

Язык: Английский

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Advancements and future directions in waste plastics recycling: From mechanical methods to innovative chemical processes

Chemical Engineering Journal, Год журнала: 2024, Номер 493, С. 152727 - 152727

Опубликована: Июнь 1, 2024

Язык: Английский

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Recent advances in oxidative degradation of plastics

Chemical Society Reviews, Год журнала: 2024, Номер 53(14), С. 7309 - 7327

Опубликована: Янв. 1, 2024

Oxidative degradation is a powerful method to degrade plastics into oligomers and small oxidized products. While thermal energy has been conventionally employed as an external stimulus, recent advances in photochemistry have enabled photocatalytic oxidative of polymers under mild conditions. This tutorial review presents overview degradation, from its earliest examples emerging strategies. briefly discusses the motivation development with focus on underlying mechanisms. Then, we will examine modern studies primarily relevant catalytic degradation. Lastly, highlight some unique using unconventional approaches for polymer such electrochemistry.

Язык: Английский

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Depolymerization mechanisms and closed-loop assessment in polyester waste recycling

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Июль 25, 2024

Alcoholysis of poly(ethylene terephthalate) (PET) waste to produce monomers, including methanolysis yield dimethyl terephthalate (DMT) and glycolysis generate bis-2-hydroxyethyl (BHET), is a promising strategy in PET management. Here, we introduce an efficient PET-alcoholysis approach utilizing oxygen-vacancy (V

Язык: Английский

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