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

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(11)

Published: Jan. 19, 2023

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 EG glycolic acid (GA) with a high Faraday efficiency selectivity (>85 %) even at industry-level current density (600 mA cm-2 1.15 V vs. RHE) over Pd-Ni(OH)2 catalyst. Notably, stable electrolysis 200 h can be achieved, outperforming all available Pd-based catalysts. Combined experimental theoretical results reveal that 1) OH* generation promoted by Ni(OH)2 plays critical role in facilitating EG-to-GA oxidation removing poisonous carbonyl species, thereby achieving activity stability; 2) Pd downshifted d-band center oxophilic Ni synergistically facilitate rapid desorption transfer GA from active sites inactive sites, avoiding over-oxidation thus selectivity.

Language: Английский

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Engineering strategies and active site identification of MXene-based catalysts for electrochemical conversion reactions

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(9), P. 3215 - 3264

Published: Jan. 1, 2023

This review summarizes engineering strategies to modify MXene-based catalysts and their active site identification for applications in electrochemical conversion reactions.

Language: Английский

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Why do Single‐Atom Alloys Catalysts Outperform both Single‐Atom Catalysts and Nanocatalysts on MXene?

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 63(4)

Published: Dec. 1, 2023

Abstract Single‐atom alloys (SAAs), combining the advantages of single‐atom and nanoparticles (NPs), play an extremely significant role in field heterogeneous catalysis. Nevertheless, understanding catalytic mechanism SAAs catalysis reactions remains a challenge compared with single atoms NPs. Herein, ruthenium‐nickel (RuNi ) synthesized by embedding atomically dispersed Ru Ni NPs are anchored on two‐dimensional Ti 3 C 2 T x MXene. The RuNi SAA‐3 −Ti catalysts exhibit unprecedented activity for hydrogen evolution from ammonia borane (AB, NH BH hydrolysis mass‐specific (r mass value 333 L min −1 g . Theoretical calculations reveal that anchoring optimizes dissociation AB H O as well binding ability H* intermediates during due to d‐band structural modulation caused alloying effect metal‐supports interactions (MSI) This work provides useful design principles developing optimizing efficient hydrogen‐related demonstrates over energy

Language: Английский

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Advanced heterostructure of Pd nanosheets@Pt nanoparticles boosts methanol electrooxidation

Journal of Energy Chemistry, Journal Year: 2023, Volume and Issue: 85, P. 430 - 438

Published: July 7, 2023

Language: Английский

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Energy‐Saving Hydrogen Production by Seawater Splitting Coupled with PET Plastic Upcycling

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(17)

Published: Feb. 8, 2024

Abstract Direct seawater electrolysis presents a promising route for grid‐scale green hydrogen (H 2 ) production without reliance on scarce freshwater. However, it is severely hampered by high energy consumption (> 4.3–5.73 kWh m −3 H and harmful chlorine corrosion. Herein, an energy‐saving chlorine‐free system coupling splitting upcycling of polyethylene terephthalate (PET) waste into value‐added glycolic acid (GA) over Pd─CuCo O 4 catalyst reported. An ultra‐low potential 1.15 V versus RHE required to achieve industry‐level current density 600 mA cm −2 , which reduces electricity cost 2.45 . Notably, this maintains 1.6 A longer than 100 h, demonstrating excellent stability. Experimental theoretical results unveil that 1) the specific adsorption PET‐derived ethylene glycol (EG) Pd enhances catalytic performance, downshifted d‐band center accelerates desorption GA prevent over‐oxidation; 2) strong OH − CuCo synergistically promotes EG electrooxidation (EGOR) forms negative charge layer effectively repels Cl electrostatic repulsion, thus preventing This work may provide new opportunities from vast marine resources PET waste.

Language: Английский

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Well-defined diatomic catalysis for photosynthesis of C2H4 from CO2

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: March 18, 2024

Abstract Owing to the specific electronic-redistribution and spatial proximity, diatomic catalysts (DACs) have been identified as principal interest for efficient photoconversion of CO 2 into C H 4 . However, predominant bottom-up strategy DACs synthesis has critically constrained development highly ordered due random distribution heteronuclear atoms, which hinders optimization catalytic performance exploration actual reaction mechanism. Here, an up-bottom ion-cutting architecture is proposed fabricate well-defined DACs, superior proximity CuAu diatomics (DAs) decorated TiO (CuAu-DAs-TiO ) successfully constructed compact heteroatomic spacing (2-3 Å). profoundly low C-C coupling energy barrier CuAu-DAs-TiO , a considerable production with sustainability achieved. Our discovery inspires novel fabrication motivate distinct deduction heteroatom synergistically

Language: Английский

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Electronegativity Induced d‐Band Center Offset for Pt‐Rh Dual Sites in High‐Entropy Alloy Boosts Liquid Fuels Electrooxidation

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(20)

Published: Feb. 19, 2024

Abstract Investigating the catalytic behavior of liquid fuels on well‐defined dual sites is crucial in understanding electrocatalytic reactions. Herein, concept holding bidirectional electronegativity dominant d ‐band center regulation Pt‐Rh proposed to tailor behaviors toward methanol oxidation reaction (MOR). The are engineered by introducing low‐electronegativity Ga/Ni and high‐electronegativity W elements PtRhGaNiW high‐entropy alloy (HEA), which can drive electron cloud redispersing over a wide orbit window. optimized HEA nanowire achieve high current density 5.61 mA cm −2 MOR, 3.38 9.75 times than that PtRh (1.66 ) Pt/C (0.57 ), as well remarkably stability CO ads poisonous resistance. theoretical calculations further disclose redistribution surface localized around promote direct ─OH, accelerate oxidation/removal. This work presents breakthrough designing advanced site electrocatalysts for complex

Language: Английский

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Advanced low-dimensional PdAg networked nanochains for the superior alcohol electrocatalysis

Applied Surface Science, Journal Year: 2024, Volume and Issue: 651, P. 159291 - 159291

Published: Jan. 2, 2024

Language: Английский

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Strong Component‐Interaction in N‐doped 2D Ti₃C₂T_x‐Supported Pt Electrocatalyst for Acidic Ethanol Oxidation Reaction

Advanced Sustainable Systems, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 5, 2025

Abstract Designing electrocatalysts with the selective C─C bond breaking in ethanol electro‐oxidation is of interest as an efficient strategy to accelerate large‐scale applications direct fuel cells (DEFCs).Pt nanoparticles (NPs) are herein on N‐doped 2D Ti 3 C 2 T x MXene via two‐step synthesis steps including NH ‐assisted hydrothermal and NaBH 4 ethylene glycol reduction routes. With breaking, as‐obtained 16 wt.% Pt/N‐Ti catalyst exhibits 435.35 mA mg Pt −1 mass activity 0.83 cm −2 specific activity, being 1.26‐ 1.77‐fold increase compared those commercially available 20 Pt/C (346.21 0.47 ). This originates from advantages unique structures strong interplay between NPs nitrogen‐doped . Also, shows superior CO‐poisoning resistance long‐term stability for acidic reaction (EOR). work demonstrates potential heteroatom‐doped MXenes 1 pathway selectivity catalytic performance Pt‐based DEFCs.

Language: Английский

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Functional MXenes: Progress and Perspectives on Synthetic Strategies and Structure–Property Interplay for Next‐Generation Technologies

Small, Journal Year: 2023, Volume and Issue: 20(4)

Published: Sept. 20, 2023

Abstract MXenes are a class of 2D materials that include layered transition metal carbides, nitrides, and carbonitrides. Since their inception in 2011, they have garnered significant attention due to diverse compositions, unique structures, extraordinary properties, such as high specific surface areas excellent electrical conductivity. This versatility has opened up immense potential various fields, catalyzing surge MXene research leading note worthy advancements. review offers an in‐depth overview the evolution over past 5 years, with emphasis on synthetic strategies, structure‐property relationships, technological prospects. A classification scheme for structures based entropy is presented updated summary elemental constituents family provided, documented recent literature. Delving into microscopic structure synthesis routes, intricate relationships explored at nano/micro level dictate macroscopic applications MXenes. Through extensive latest representative works, utilization energy, environmental, electronic, biomedical fields showcased, offering glimpse current bottlenecks, asstability, scalability, device integration. Moreover, pathways advancing toward next‐generation technologies highlighted.

Language: Английский

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