Toward Electrocatalytic Methanol Oxidation Reaction: Longstanding Debates and Emerging Catalysts

Advanced Materials, Год журнала: 2023, Номер 35(26)

Опубликована: Янв. 27, 2023

The study of direct methanol fuel cells (DMFCs) has lasted around 70 years, since the first investigation in early 1950s. Though enormous effort been devoted this field, it is still far from commercialization. oxidation reaction (MOR), as a semi-reaction DMFCs, bottleneck that restricts overall performance DMFCs. To date, there intense debate on complex six-electron reaction, but barely any reviews have systematically discussed topic. end, controversies and progress regarding electrocatalytic mechanisms, evaluations well design science toward MOR electrocatalysts are summarized. This review also provides comprehensive introduction recent development emerging with focus innovation alloy, core-shell structure, heterostructure, single-atom catalysts. Finally, perspectives future outlook mechanisms provided.

Язык: Английский

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High-entropy alloys in electrocatalysis: from fundamentals to applications

Chemical Society Reviews, Год журнала: 2023, Номер 52(23), С. 8319 - 8373

Опубликована: Янв. 1, 2023

In this review, we provide a comprehensive summary of recent advances in the synthesis strategies, design principles, and characterization technologies high entropy alloys, their applications various electrocatalytic conversion reactions.

Язык: Английский

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Review on Electrocatalytic Coreduction of Carbon Dioxide and Nitrogenous Species for Urea Synthesis

ACS Nano, Год журнала: 2023, Номер 17(4), С. 3209 - 3224

Опубликована: Фев. 14, 2023

The electrochemical coreduction of carbon dioxide (CO2) and nitrogenous species (such as NO3–, NO2–, N2, NO) for urea synthesis under ambient conditions provides a promising solution to realize carbon/nitrogen neutrality mitigate environmental pollution. Although an increasing number studies have made some breakthroughs in synthesis, the unsatisfactory Faradaic efficiency, low yield rate, ambiguous C–N coupling reaction mechanisms remain major obstacles its large-scale applications. In this review, we present recent progress on based CO2 aqueous solutions conditions, providing useful guidance discussion rational design metal nanocatalyst, understanding mechanism, existing challenges prospects synthesis. We hope that review can stimulate more insights inspiration toward development electrocatalytic technology.

Язык: Английский

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High‐Entropy Alloy Aerogels: A New Platform for Carbon Dioxide Reduction

Advanced Materials, Год журнала: 2022, Номер 35(2)

Опубликована: Ноя. 14, 2022

High-entropy alloy aerogels (HEAAs) combined with the advantages of high-entropy alloys and are prospective new platforms in catalytic reactions. However, due to differences reduction potentials miscibility behavior different metals, realization HEAAs a single phase is still great challenge. Herein, series fabricated via freeze-thaw method as highly active durable electrocatalysts for carbon dioxide reaction (CO2 RR). Especially, PdCuAuAgBiIn can achieve Faradaic efficiency (FE) C1 products almost 100% from -0.7 -1.1 V versus reversible hydrogen electrode (VRHE ), maximum FE formic acid (FEHCOOH ) 98.1% at VRHE , outperforming particles (HEAPs) Pd metallic (MAs). Specifically, current density FEHCOOH 200 mA cm-2 87% flow cell. The impressive CO2 RR performance attributed strong interactions between metals surface unsaturated sites, which regulate electronic structures allow optimal HCOO* intermediate adsorption desorption onto catalysts enhance HCOOH production. work not only provides facile synthetic strategy fabricate HEAAs, but also opens avenue development efficient beyond.

Язык: Английский

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Intermetallic Nanocrystals for Fuel-Cells-Based Electrocatalysis

Chemical Reviews, Год журнала: 2023, Номер 123(22), С. 12507 - 12593

Опубликована: Ноя. 1, 2023

Electrocatalysis underpins the renewable electrochemical conversions for sustainability, which further replies on metallic nanocrystals as vital electrocatalysts. Intermetallic have been known to show distinct properties compared their disordered counterparts, and long explored functional improvements. Tremendous progresses made in past few years, with notable trend of more precise engineering down an atomic level investigation transferring into practical membrane electrode assembly (MEA), motivates this timely review. After addressing basic thermodynamic kinetic fundamentals, we discuss classic latest synthetic strategies that enable not only formation intermetallic phase but also rational control other catalysis-determinant structural parameters, such size morphology. We demonstrate emerging nanomaterials potentially advancement energy electrocatalysis. Then, state-of-the-art characterizations representative electrocatalysts emphasis oxygen reduction reaction evaluated a MEA setup. summarize review by laying out existing challenges offering perspective future research directions toward practicing conversions.

Язык: Английский

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Optimization strategies of high-entropy alloys for electrocatalytic applications

Chemical Science, Год журнала: 2023, Номер 14(45), С. 12850 - 12868

Опубликована: Янв. 1, 2023

This review summarizes the synthesis methods, characterization research progress and regulation strategies of HAEs in field electrocatalytic HER, HOR, OER, ORR, CO 2 RR, NRR AOR, providing deep understanding for future applications.

Язык: Английский

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Single-atom Mo-tailored high-entropy-alloy ultrathin nanosheets with intrinsic tensile strain enhance electrocatalysis

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

Опубликована: Март 13, 2024

Abstract The precise structural integration of single-atom and high-entropy-alloy features for energy electrocatalysis is highly appealing conversion, yet remains a grand challenge. Herein, we report class Mo-tailored PdPtNiCuZn nanosheets with dilute Pt-Pt ensembles intrinsic tensile strain (Mo 1 -PdPtNiCuZn) as efficient electrocatalysts enhancing the methanol oxidation reaction catalysis. as-made Mo -PdPtNiCuZn delivers an extraordinary mass activity 24.55 A mg Pt −1 11.62 Pd+Pt , along impressive long-term durability. planted oxophilic single atoms promoters modify electronic structure isolated sites in host, suppressing formation CO adsorbates steering towards formate pathway. Meanwhile, synergistically optimize adsorption behaviour intermediates to achieve more energetically favourable pathway minimize barrier. This work advances design atomically catalytic by creating new paradigm atom-tailored high-entropy alloys, opening encouraging CO-tolerance electrocatalysts.

Язык: Английский

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Coordination engineering in single-site catalysts: General principles, characterizations, and recent advances

Chem, Год журнала: 2023, Номер 10(1), С. 48 - 85

Опубликована: Сен. 21, 2023

Язык: Английский

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Metal Alloys‐Structured Electrocatalysts: Metal–Metal Interactions, Coordination Microenvironments, and Structural Property–Reactivity Relationships

Advanced Materials, Год журнала: 2023, Номер 35(51)

Опубликована: Апрель 24, 2023

Metal alloys-structured electrocatalysts (MAECs) have made essential contributions to accelerating the practical applications of electrocatalytic devices in renewable energy systems. However, due complex atomic structures, varied electronic states, and abundant supports, precisely decoding metal-metal interactions structure-activity relationships MAECs still confronts great challenges, which is critical direct future engineering optimization MAECs. Here, this timely review comprehensively summarizes latest advances creating MAECs, including interactions, coordination microenvironments, relationships. First, fundamental classification, design, characterization, structural reconstruction are outlined. Then, merits modulation strategies recent breakthroughs for noble non-noble metal-structured thoroughly discussed, such as solid solution alloys, intermetallic single-atom alloys. Particularly, unique insights into bond theoretical understanding, operando techniques mechanism disclosure given. Thereafter, current states diverse with a focus on property-reactivity relationships, reaction pathways, performance comparisons discussed. Finally, challenges perspectives systematically It believed that comprehensive can offer substantial impact stimulating widespread utilization metal materials electrocatalysis.

Язык: Английский

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Multisite Synergism‐Induced Electron Regulation of High‐Entropy Alloy Metallene for Boosting Alkaline Hydrogen Evolution Reaction

Advanced Functional Materials, Год журнала: 2023, Номер 33(42)

Опубликована: Июнь 14, 2023

Abstract Designing the high‐entropy alloys (HEAs) electrocatalysts with controllable nanostructures is of great significance for development efficient alkaline hydrogen evolution reaction (HER) electrocatalysts. In this study, an ultrathin HEA‐PdPtRhIrCu metallene abundant lattice distortions and defects prepared via a facile one‐step hydrothermal method. The synthesized exhibits superior HER performance in 1 m KOH solution, where required overpotential only 15 mV to reach current density −10 mA cm −2 while possessing low Tafel slope 37 dec −1 . Density functional theory calculations further prove that synergistic effect five elements can optimize electronic structure enhance activity catalysts. particular, strong coupling bonding arising from interaction between multi‐metal components facilitate electron transfer surface high electroactivity. Moreover, optimized Pt promotes optimal PtH binding at site, thus promoting performance.

Язык: Английский

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