Ordering‐Dependent Hydrogen Evolution and Oxygen Reduction Electrocatalysis of High‐Entropy Intermetallic Pt₄FeCoCuNi

Advanced Materials, Год журнала: 2023, Номер 35(28)

Опубликована: Май 11, 2023

Abstract Disordered solid‐solution high‐entropy alloys have attracted wide research attention as robust electrocatalysts. In comparison, ordered intermetallics been hardly explored and the effects of degree chemical ordering on catalytic activity remain unknown. this study, a series multicomponent intermetallic Pt 4 FeCoCuNi nanoparticles with tunable degrees is fabricated. The transformation mechanism from disordered structure into revealed at single‐particle level, it agrees macroscopic analysis by selected‐area electron diffraction X‐ray diffraction. electrocatalytic performance correlates well their crystal electronic structure. It found that increasing promotes performance. highly achieves highest mass activities toward both acidic oxygen reduction reaction (ORR) alkaline hydrogen evolution (HER) which are 18.9‐fold 5.6‐fold higher than those commercial Pt/C, respectively. experiment also shows catalyst demonstrates better long‐term stability partially Pt/C when subject to HER ORR. This ordering‐dependent structure–property relationship provides insight rational design catalysts stimulates exploration many other alloys.

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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Defect Engineering of a High‐Entropy Metallic Glass Surface for High‐Performance Overall Water Splitting at Ampere‐Level Current Densities

Advanced Materials, Год журнала: 2023, Номер 35(38)

Опубликована: Июнь 7, 2023

Platinum-based electrocatalysts possess high water electrolysis activity and are essential components for hydrogen evolution reaction (HER). A major challenge, however, is how to break the cost-efficiency trade-off. Here, a novel defect engineering strategy presented construct nanoporous (FeCoNiB0.75 )97 Pt3 (atomic %) high-entropy metallic glass (HEMG) with nanocrystalline surface structure that contains large amounts of lattice distortion stacking faults achieve excellent electrocatalytic performance using only 3 at% Pt. The defect-rich HEMG achieves ultralow overpotentials at ampere-level current density 1000 mA cm-2 HER (104 mV) oxygen (301 under alkaline conditions, while retains long-term durability exceeding 200 h 100 . Moreover, it requires 81 122 mV drive densities acidic neutral respectively. Modelling results reveal fault defects help optimize atomic configuration modulate electronic interaction, architecture provides abundant active sites, thus synergistically contributing reduced energy barrier electrolysis. This approach combined design expected be widely applicable development high-performance alloy catalysts.

Язык: Английский

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Alleviating OH Blockage on the Catalyst Surface by the Puncture Effect of Single-Atom Sites to Boost Alkaline Water Electrolysis

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(7), С. 4883 - 4891

Опубликована: Фев. 7, 2024

Nonprecious transition metal catalysts have emerged as the preferred choice for industrial alkaline water electrolysis due to their cost-effectiveness. However, overstrong binding energy adsorbed OH often results in blockage of active sites, particularly cathodic hydrogen evolution reaction. Herein, we found that single-atom sites exhibit a puncture effect effectively alleviate blockades, thereby significantly enhancing reaction (HER) performance. Typically, after anchoring single Ru atoms onto tungsten carbides, overpotential at 10 mA·cm–2 is reduced by more than 130 mV (159 vs 21 mV). Also, mass activity increased 16-fold over commercial Pt/C (MA100 = 17.3 A·mgRu–1 1.1 A·mgPt–1, Pt/C). More importantly, such electrocatalyst-based anion-exchange membrane electrolyzers can an ultralow potential (1.79 Vcell) and high stability current density 1.0 A·cm–2. Density functional theory (DFT) calculations reveal isolated could weaken surrounding local energy, thus puncturing constructing bifunctional interfaces between support accelerate dissociation. Our findings generality other (such Mo) contribute advancement industrial-scale electrolysis.

Язык: Английский

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Delaminated MBene sheets beyond usual 2D transition metal materials for securing Pt single atoms to boost hydrogen evolution

Energy & Environmental Science, Год журнала: 2023, Номер 16(9), С. 4093 - 4104

Опубликована: Янв. 1, 2023

The use of a minimum amount active metal makes single-atom catalysts (SACs) an effective route to economically catalyze electrochemical reactions.

Язык: Английский

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Electrocatalysts Design Guided by Active Intermediates of Hydrogen Evolution Reaction

Advanced Energy Materials, Год журнала: 2023, Номер 13(43)

Опубликована: Окт. 6, 2023

Abstract Hydrogen production from water electrolysis plays an important role for the development of hydrogen‐based energy sources. Developing efficient electrocatalysts is crucial accelerating reaction kinetics and achieving large‐scale electrolysis. Despite significant advancements in hydrogen evolution (HER) achieved over past few decades, there remains a lack comprehensive discussion on in‐depth mechanism enhanced activity, particularly with regard to active intermediates. Recently, state‐of‐the‐art characterization methods theoretical computation, optimizing interaction between intermediates corresponding sites has been demonstrated as effective strategy enhance intrinsic catalytic activity. Herein, recent advances design guided by HER are presented. Emphasis focused key that determine activity strategies tune Finally, outlook future challenges perspectives based given.

Язык: Английский

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Cation Vacancy Clusters in Ti₃C₂T_x MXene Induce Ultra‐Strong Interaction with Noble Metal Clusters for Efficient Electrocatalytic Hydrogen Evolution

Advanced Energy Materials, Год журнала: 2023, Номер 13(23)

Опубликована: Май 1, 2023

Abstract MXenes are promising substrates for supported noble metal electrocatalysts. Yet, it is a significant challenge to modulate the metal–support interaction (MSI) enhancing catalytic performance. Herein, employing facile HF etching method, cation vacancy structures in Ti 3 C 2 T x controllably tuned, producing nearly vacancy‐free (Ti ‐V 0 ), single atom S or cluster ) engineered MXenes. Ruthenium atomic clusters, as model catalyst, successfully anchor on all MXene substrates. Different from terminal O/F coordination groups routine surfaces, clusters create unique lattice carbon ligand environment toward Ru species, which induces ultra‐strong MSI. As result, compared and , modulated (Ru@Ti exhibit optimized balance of H O adsorption/dissociation OH/H desorption, thereby delivering superior electrocatalytic performance alkaline hydrogen evolution reaction (HER). Within wide range laboratory‐level (90 mA cm −2 industrial‐level (1.5 A current density, Ru@Ti outperforms commercial Pt/C terms overpotential mass activity. Moreover, universal substrate catalysts, can also Ir/Pt/Rh enable excellent HER This work expands scope MSI between catalysts.

Язык: Английский

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A high-efficiency electrochemical proton-conducting membrane reactor for ammonia production at intermediate temperatures

Joule, Год журнала: 2023, Номер 7(6), С. 1333 - 1346

Опубликована: Июнь 1, 2023

Язык: Английский

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Manipulating the Microenvironment of Single Atoms by Switching Support Crystallinity for Industrial Hydrogen Evolution

Angewandte Chemie International Edition, Год журнала: 2023, Номер 63(7)

Опубликована: Дек. 28, 2023

Abstract Modulating the microenvironment of single‐atom catalysts (SACs) is critical to optimizing catalytic activity. Herein, we innovatively propose a strategy improve local reaction environment Ru single atoms by precisely switching crystallinity support from high crystalline and low crystalline, which significantly improves hydrogen evolution (HER) The catalyst anchored on low‐crystalline nickel hydroxide (Ru−LC−Ni(OH) 2 ) reconstructs distribution balance interfacial ions due activation effect metal dangling bonds support. Single‐site with oxidation state induces aggregation hydronium (H 3 O + ), leading formation acidic in alkaline media, breaking pH‐dependent HER As comparison, high‐crystalline (Ru−HC−Ni(OH) exhibits sluggish Volmer step conventional environment. expected, Ru−LC−Ni(OH) requires overpotentials 9 136 mV at 10 1000 mA cm −2 conditions operates stably 500 for h an seawater anion exchange membrane (AEM) electrolyzer. This study provides new perspective constructing highly active electrocatalysts.

Язык: Английский

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Tailoring supports for enhancing the electrocatalytic hydrogen evolution performance of platinum species: a review

Journal of Materials Chemistry A, Год журнала: 2023, Номер 11(37), С. 19812 - 19844

Опубликована: Янв. 1, 2023

Recent advances and perspectives in utilizing various supports to maximize the HER performance of Pt species are reviewed, along with strategies for tailoring future challenges opportunities regulating supports.

Язык: Английский

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