Constructing Built‐in Electric Field in Heterogeneous Nanowire Arrays for Efficient Overall Water Electrolysis

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(26)

Опубликована: Апрель 13, 2023

Efficient bifunctional electrocatalysts for hydrogen and oxygen evolution reactions are key to water electrolysis. Herein, we report a built-in electric field (BEF) strategy fabricate heterogeneous nickel phosphide-cobalt nanowire arrays grown on carbon fiber paper (Ni2 P-CoCH/CFP) with large work function difference (ΔΦ) as overall splitting. Impressively, Ni2 P-CoCH/CFP exhibits remarkable catalytic activity obtain 10 mA cm-2 , respectively. Moreover, the assembled lab-scale electrolyzer driven by an AAA battery delivers excellent stability after 50 h electrocatalysis 100 % faradic efficiency. Computational calculations combining experiments reveal interface-induced effect facilitates asymmetrical charge distributions, thereby regulating adsorption/desorption of intermediates during reactions. This offers avenue rationally design high-performance electrocatalysts.

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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Tailoring Built‐In Electric Field in a Self‐Assembled Zeolitic Imidazolate Framework/MXene Nanocomposites for Microwave Absorption

Advanced Materials, Год журнала: 2024, Номер 36(19)

Опубликована: Янв. 30, 2024

Abstract Heterointerface engineering, which plays a pivotal role in developing advanced microwave‐absorbing materials, is employed to design zeolitic imidazolate framework (ZIF)–MXene nanocomposites. The ZIF–MXene composites are prepared by electrostatic self‐assembly of negatively charged titanium carbide MXene flakes and positively Co‐containing ZIF nanomaterials. This approach effectively creates abundant Mott–Schottky heterointerfaces exhibiting robust built‐in electric field (BIEF) effect, as evidenced experimental theoretical analyses, leading notable attenuation electromagnetic energy. Systematic manipulation the BIEF‐exhibiting heterointerface, achieved through topological modulation ZIF, proficiently alters charge separation, facilitates electron migration, ultimately enhances polarization relaxation loss, resulting exceptional wave absorption performance (reflection loss RL min = −47.35 dB effective bandwidth f E 6.32 GHz). present study demonstrates an innovative model system for elucidating interfacial mechanisms pioneers novel functional materials with characteristics spatial engineering.

Язык: Английский

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Directional and Ultrafast Charge Transfer in Oxygen‐Vacancy‐Rich ZnO@Single‐Atom Cobalt Core‐Shell Junction for Photo‐Fenton‐Like Reaction

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(30)

Опубликована: Май 31, 2023

In photosynthesis, solar energy is harvested by photosensitizers, and then, the excited electrons transfer via a Z-Scheme mode to enzymatic catalytic centers trigger redox reactions. Herein, we constructed core-shell Z-scheme heterojunction of semiconductor@single-atom catalysts (SACs). The oxygen-vacancy-rich ZnO core single-atom Co-N4 sites supported on nitrogen-rich carbon shell (SA-Co-CN) act as photosensitizer enzyme-mimicking active centers, respectively. Driven built-in electric field across heterojunction, photoexcited could rapidly (2 ps) from n-type p-type SA-Co-CN shell, finally boosting performance surface-exposed for peroxymonosulfate (PMS) activation under light irradiation. synergies between photocatalysis heterogeneous Fenton-like reaction lead phenomenally enhanced production various reactive oxygen species rapid degradation microcontaminants in water. Experimental theoretical results validate that interfacial coupling with greatly facilitates PMS adsorption reducing enhancing cascade electron processes photo-Fenton-like reaction.

Язык: Английский

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Constructing Built‐in Electric Field in Heterogeneous Nanowire Arrays for Efficient Overall Water Electrolysis

Angewandte Chemie, Год журнала: 2023, Номер 135(26)

Опубликована: Апрель 13, 2023

Abstract Efficient bifunctional electrocatalysts for hydrogen and oxygen evolution reactions are key to water electrolysis. Herein, we report a built‐in electric field (BEF) strategy fabricate heterogeneous nickel phosphide‐cobalt nanowire arrays grown on carbon fiber paper (Ni 2 P‐CoCH/CFP) with large work function difference (ΔΦ) as overall splitting. Impressively, Ni P‐CoCH/CFP exhibits remarkable catalytic activity obtain 10 mA cm −2 , respectively. Moreover, the assembled lab‐scale electrolyzer driven by an AAA battery delivers excellent stability after 50 h electrocatalysis 100 % faradic efficiency. Computational calculations combining experiments reveal interface‐induced effect facilitates asymmetrical charge distributions, thereby regulating adsorption/desorption of intermediates during reactions. This offers avenue rationally design high‐performance electrocatalysts.

Язык: Английский

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The Heterointerface between Fe₁/NC and Selenides Boosts Reversible Oxygen Electrocatalysis

Advanced Functional Materials, Год журнала: 2023, Номер 33(40)

Опубликована: Июнь 13, 2023

Abstract The rational design and construction of efficient inexpensive bifunctional oxygen electrocatalysts are highly desirable for the development rechargeable Zn–air batteries (ZABs). Although single‐atom Fe sites anchored on N‐doped carbon catalysts (Fe 1 /NC) ensure high reduction reaction activity, their unitary atomically dispersed active center faces difficult condition in catalyzing evolution simultaneously. Herein, a composite catalyst containing heterointerface between /NC selenides ((Fe,Co)Se 2 ) is constructed. obtained (Fe,Co)Se @Fe exhibits extremely narrow potential gap 0.616 V remarkable stability alkaline media, outperforming benchmark (Pt/C+RuO : 0.720 V). Experimental results density functional theory calculations reveal that accelerates electron transfer provides more moderate adsorption sites, which endow with catalytic activity. This study not only superior ZABs, but also enriches application multifunctional energy storage conversion devices.

Язык: Английский

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Effect of Heterostructure‐Modified Separator in Lithium–Sulfur Batteries

Small, Год журнала: 2023, Номер 19(42)

Опубликована: Июнь 9, 2023

Lithium-sulfur (Li-S) batteries with high energy density and low cost are the most promising competitor in next generation of new reserve devices. However, there still many problems that hinder its commercialization, mainly including shuttle soluble polysulfides, slow reaction kinetics, growth Li dendrites. In order to solve above issues, various explorations have been carried out for configurations, such as electrodes, separators, electrolytes. Among them, separator contact both anode cathode is a particularly special position. Reasonable design-modified material can key problems. Heterostructure engineering modification method combine characteristics different materials generate synergistic effect at heterogeneous interface conducive Li-S electrochemical behavior. This review not only elaborates role heterostructure-modified separators dealing problems, but also analyzes improvement wettability thermal stability by heterostructure materials, systematically clarifies advantages, summarizes some related progress recent years. Finally, future development direction heterostructure-based given.

Язык: Английский

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Constructing Built-In Electric Fields with Semiconductor Junctions and Schottky Junctions Based on Mo–MXene/Mo–Metal Sulfides for Electromagnetic Response

Nano-Micro Letters, Год журнала: 2024, Номер 16(1)

Опубликована: Июнь 11, 2024

Abstract The exploration of novel multivariate heterostructures has emerged as a pivotal strategy for developing high-performance electromagnetic wave (EMW) absorption materials. However, the loss mechanism in traditional is relatively simple, guided by empirical observations, and not monotonous. In this work, we presented semiconductor–semiconductor–metal heterostructure system, Mo–MXene/Mo–metal sulfides (metal = Sn, Fe, Mn, Co, Ni, Zn, Cu), including semiconductor junctions Mott–Schottky junctions. By skillfully combining these distinct functional components (Mo–MXene, MoS 2 , metal sulfides), can engineer multiple heterogeneous interface with superior capabilities, broad effective bandwidths, ultrathin matching thickness. successful establishment gives rise to built-in electric field that intensifies electron transfer, confirmed density theory, which collaborates dielectric polarization mechanisms substantially amplify EMW absorption. We detailed synthesis series featuring both semiconductor–semiconductor semiconductor–metal interfaces. achievements were most pronounced Mo–MXene/Mo–Sn sulfide, achieved remarkable reflection values − 70.6 dB at thickness only 1.885 mm. Radar cross-section calculations indicate MXene/Mo–metal have tremendous potential practical military stealth technology. This work marks departure from conventional component design limitations presents pathway creation advanced MXene-based composites potent capabilities.

Язык: Английский

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Tunable Built‐In Electric Field in Ru Nanoclusters‐Based Electrocatalyst Boosts Water Splitting and Simulated Seawater Electrolysis

Advanced Functional Materials, Год журнала: 2023, Номер 34(7)

Опубликована: Окт. 31, 2023

Abstract The development of bifunctional electrocatalysts suitable for a wide pH range and seawater splitting under simulated industrial electrolysis conditions is expected to advance practical applications clean hydrogen energy. Here, the study reports built‐in electric field approach assemble heterogeneous Ru nanoclusters (Ru NCs) anchored in P,O co‐doped NiFe layered double hydroxide NCs/P,O‐NiFe LDH) overall water splitting. It revealed that BEF ensures electron enrichment via unidirectional transfer from P,O‐NiFe LDH due difference corresponding Fermi levels. optimized LDH/NF shows excellent electrocatalytic activity toward evolution reaction, oxygen range, as well industry‐relevant conditions. long‐term catalyst stability high currents process temperatures also demonstrated. Density functional theory calculations further confirm active sites at interface effectively reduce energy barrier electrolysis, thereby facilitating processes.

Язык: Английский

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Directional and Ultrafast Charge Transfer in Oxygen‐Vacancy‐Rich ZnO@Single‐Atom Cobalt Core‐Shell Junction for Photo‐Fenton‐Like Reaction

Angewandte Chemie, Год журнала: 2023, Номер 135(30)

Опубликована: Май 31, 2023

Abstract In photosynthesis, solar energy is harvested by photosensitizers, and then, the excited electrons transfer via a Z‐Scheme mode to enzymatic catalytic centers trigger redox reactions. Herein, we constructed core–shell Z‐scheme heterojunction of semiconductor@single‐atom catalysts (SACs). The oxygen‐vacancy‐rich ZnO core single‐atom Co−N 4 sites supported on nitrogen‐rich carbon shell (SA‐Co‐CN) act as photosensitizer enzyme‐mimicking active centers, respectively. Driven built‐in electric field across heterojunction, photoexcited could rapidly (2 ps) from n ‐type p SA‐Co‐CN shell, finally boosting performance surface‐exposed for peroxymonosulfate (PMS) activation under light irradiation. synergies between photocatalysis heterogeneous Fenton‐like reaction lead phenomenally enhanced production various reactive oxygen species rapid degradation microcontaminants in water. Experimental theoretical results validate that interfacial coupling with greatly facilitates PMS adsorption reducing enhancing cascade electron processes photo‐Fenton‐like reaction.

Язык: Английский

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