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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Engineering low-coordination atoms on RhPt bimetallene for 12-electron ethanol electrooxidation

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(6), P. 2219 - 2227

Published: Jan. 1, 2024

The three-dimensional perforated RhPt bimetallene achieves a high exposure ratio of low-coordinated diatomic sites, demonstrating excellent activity and remarkable selectivity for 12-electron ethanol oxidation to CO 2 .

Language: Английский

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RhCuBi Trimetallenes with Composition Segregation Coupled Crystalline‐Amorphous Heterostructure Toward Ethanol Electrooxidation

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(21)

Published: Feb. 19, 2024

Abstract The inefficiency of Pt and Pd benchmark catalysts in achieving complete ethanol oxidation, coupled with their inherent susceptibility to poisoning, poses a significant obstacle the advancement direct fuel cells. In this study, development self‐supported ultrathin RhCuBi trimetallenes, demonstrating exceptional performance electrooxidation through segregation interface engineering is presented. distinctive RhBi‐rich crystalline/RhCu‐rich amorphous heterostructure trimetallenes creates wealth highly active interfacial sites for oxidation reaction (EOR). This results an impressive 43.3% Faradaic efficiency C1 pathway peak mass activity 1.11 A mg Rh −1 at 0.68 V versus reversible hydrogen electrode. Moreover, retain 60% initial after 8.5 h constant potential electrolysis, outperforming commercial (<3%). In/ex situ infrared spectroscopy directly reveals generated products key CH 3 CO* intermediates EOR on trimetallenes. Theoretical calculations confirm that RhBi alloy, particularly lattice‐stretched crystalline/amorphous sites, facilitates adsorption/activation dehydrogenation toward EOR. breakthrough offers promising prospects enhancing stability cell applications.

Language: Английский

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Reducing Energy Costs during Hydrogen Production from Water Electrolysis by Coupling Small Molecule Oxidation: From Molecular Catalysis to Industrial Exploration

Precision Chemistry, Journal Year: 2024, Volume and Issue: 2(9), P. 447 - 470

Published: July 1, 2024

Hydrogen energy has garnered significant attention in recent years as a solution to address the global crisis and environmental pollution. While water electrolysis stands out most promising method produce green hydrogen, sluggish reaction kinetics of oxygen evolution (OER) on anode increases cost hydrogen production. One potential this challenge is replace OER with thermodynamically more favorable oxidation small molecules, which can efficiently reduce while simultaneously yielding high-value chemicals. Up now, various organic reactions have been reported couple evolution, including alcohol oxidation, biomass platform molecule upgrading, sacrificial reagents associated wastewater treatments. This review concentrates advancements mechanism, catalyst, reactor, process field, discussion its prospects for commercialization.

Language: Английский

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One-step growth of RuNi-MOF nanoarrays on carbon felt host as a high-performance binder-free electrode for dual application: Ethanol fuel cell and supercapacitor

Journal of Energy Storage, Journal Year: 2023, Volume and Issue: 79, P. 110146 - 110146

Published: Dec. 20, 2023

Language: Английский

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Tensile Strain and Interatomic Orbital Hybridization Effects Boost the Electrocatalytic Performance of Intermetallic Pd₃Pb Nanowires for Ethanol Electrooxidation^†

Chinese Journal of Chemistry, Journal Year: 2024, Volume and Issue: 42(21), P. 2633 - 2640

Published: July 10, 2024

Comprehensive Summary We present a strategy that effectively modulate the d‐band electronic structure of active center by strain effect and interatomic orbital hybridization. This efficiently promotes kinetic process ethanol oxidation reaction (EOR) in alkaline media. In intermetallic Pd 3 Pb nanowires, introduction not only causes lattice expansion but also achieves hybridization bonding with Pd. Such tensile can achieve co‐regulation Pd, which directly affects adsorption behavior intermediate on for EOR. Hence, nanowires demonstrate enhanced EOR activity anti‐poisoning ability against CO ads . Theoretical calculations show OH* low energy barrier oxidative dehydrogenation are keys to high stability nanowires.

Language: Английский

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Enhancing Ni oxidation reconstruction in Ni3Fe nanoalloy for efficient Electro-Oxidation of 5-Hydroxymethylfurfural

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: unknown, P. 156320 - 156320

Published: Oct. 1, 2024

Language: Английский

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Self-Powered Water Electrolysis with Sulfide Waste as Consumable

ACS Sustainable Chemistry & Engineering, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 11, 2025

Language: Английский

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Controlling rhodium-based nanomaterials for high-efficiency energy-related electrocatalysis

EnergyChem, Journal Year: 2025, Volume and Issue: unknown, P. 100148 - 100148

Published: Feb. 1, 2025

Language: Английский

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Cavities-Induced Compressive Strain in Unique Nanotubes Boosts the C1 Pathway of Ethanol Oxidation Electrocatalysis

ACS Nano, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 16, 2025

Engineering structural defects is beneficial for electrocatalytic performances. Herein, a class of acid-etched PtNiRh nanotubes with abundant around cavities were constructed. Modulated electronic and coordination structures closely associated boost the ethanol oxidation reaction (EOR) activity selectivity. The optimized PtNiRh-E-H exhibit an EOR mass specific 1.81 A mgPt–1 3.38 mA cm–2, respectively. high retention at 1.80 after chronoamperometric test 10000 s was achieved by nanotubes. Moreover, featuring compressive lattice strain lower-lying d band center display strong inclination C1 pathway, as evidenced higher linearly bonded CO intensity lower adsorbed acetate across applied potentials using attenuated total-reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS). Also, adsorption accelerated oxidative desorption OH species led to superior selectivity Differential spectrometry (DEMS) together ATR-SEIRAS provides explicit evidence catalytic pathway CH3CH2OH → CH3CH2OHads ··· CH3CHO CH3CO CH3 + 2CO2. work represents feasible strategy alcohol catalysis, wherein acid etching exposes significantly more brings about optimal structure strain.

Language: Английский

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