Reversible hydrogen spillover at the atomic interface for efficient alkaline hydrogen evolution

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(4), P. 1397 - 1406

Published: Jan. 1, 2024

Ru 1 –Mo 2 C, a novel dual-site synergistic catalyst, demonstrated exceptional performance for the alkaline hydrogen evolution reaction (HER) through reversible spillover mechanism.

Language: Английский

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

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(51)

Published: April 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.

Language: 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, Journal Year: 2023, Volume and Issue: 35(38)

Published: June 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.

Language: 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, Journal Year: 2023, Volume and Issue: 16(9), P. 4093 - 4104

Published: Jan. 1, 2023

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

Language: 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, Journal Year: 2024, Volume and Issue: 146(7), P. 4883 - 4891

Published: Feb. 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.

Language: Английский

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Electrocatalysts Design Guided by Active Intermediates of Hydrogen Evolution Reaction

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(43)

Published: Oct. 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.

Language: Английский

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Electronic Structure Engineering of Pt Species over Pt/WO₃ toward Highly Efficient Electrocatalytic Hydrogen Evolution

Small, Journal Year: 2023, Volume and Issue: 19(32)

Published: April 17, 2023

Abstract Pt‐based supported materials, a widely used electrocatalyst for hydrogen evolution reaction (HER), often experience unavoidable electron loss, resulting in mismatching of electronic structure and HER behavior. Here, Pt/WO 3 catalyst consisting Pt species strongly coupled with defective WO polycrystalline nanorods is rationally designed. The engineering sites on can be systematically regulated, so that the optimal electron‐rich ‐600 present an excellent activity only 8 mV overpotential at 10 mA cm −2 . Particularly, mass reaches 7015 mg −1 50 mV, up to 26‐fold higher than commercial Pt/C. combination experimental theoretical results demonstrates O vacancies effectively mitigate tendency transfer from , d‐band center could reach appropriate level relative Fermi level, endowing it suitable This work identifies influence catalytic activity.

Language: 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, Journal Year: 2023, Volume and Issue: 13(23)

Published: May 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.

Language: Английский

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Polyoxometalate‐Structured Materials: Molecular Fundamentals and Electrocatalytic Roles in Energy Conversion

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(15)

Published: Jan. 9, 2024

Polyoxometalates (POMs), a kind of molecular metal oxide cluster with unique physical-chemical properties, have made essential contributions to creating efficient and robust electrocatalysts in renewable energy systems. Due the fundamental advantages POMs, such as diversity structures large numbers redox active sites, numerous efforts been devoted extending their application areas. Up now, various strategies assembling POM molecules into superstructures, supporting POMs on heterogeneous substrates, POMs-derived compounds developed for synthesizing electrocatalysts. From multidisciplinary perspective, latest advances POM-structured materials focus fundamentals, electrocatalytic roles, recent breakthroughs POM-derived electrocatalysts, are systematically summarized. Notably, this paper focuses exposing current states, essences, mechanisms how influence activities discloses critical requirements future developments. The challenges, objectives, comparisons, perspectives also discussed. It is anticipated that review will offer substantial impact stimulating interdisciplinary prosperities widespread utilizations electrocatalysis.

Language: Английский

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Dual‐Type Ru Atomic Sites for Efficient Alkaline Overall Water Splitting

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(36)

Published: Feb. 14, 2024

Abstract Monotypic catalytic site for bifunctional hydrogen evolution reaction (HER) and oxygen (OER) at low overpotential is a grand challenge in alkaline water splitting. Herein, new strategy of dual‐type atomic site‐support interaction reported, which ruthenium heteroatoms are situ implanted into both the N‐C nanosheet matrix (Ru 1 ‐N‐C) supported Co 2 P nanoparticle lattice ‐P‐Co) boosting It found that Ru ‐N‐C ‐P‐Co can give rise to synergistic effect HER OER catalysis. Density functional theory calculations disclose HER, Ru‐functionalized sites assume task expediting H O adsorption‐dissociation, adjacent coordination unsaturated facilitate following desorption kinetic. The study spillover mechanism contributes an ultralow polarization 69 mV 10 mA cm −2 . While OER, due electronegativity discrepancies, doped within triggers electronic coupling, thereby efficiently tuning d ‐band center. This grants its characteristic preferred modulating rate‐determining step reduce corresponding energy barrier, leading superior activity work offers understandings catalyzing different reactions with multiple intermediate adsorptions by interplays.

Language: Английский

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