Designing a Built-In Electric Field for Efficient Energy Electrocatalysis

ACS Nano, Год журнала: 2022, Номер 16(12), С. 19959 - 19979

Опубликована: Дек. 15, 2022

To utilize intermittent renewable energy as well achieve the goals of peak carbon dioxide emissions and neutrality, various electrocatalytic devices have been developed. However, reactions, e.g., hydrogen evolution reaction/oxygen reaction in overall water splitting, polysulfide conversion lithium–sulfur batteries, formation/decomposition lithium peroxide lithium–oxygen nitrate reduction to degrade sewage, suffer from sluggish kinetics caused by multielectron transfer processes. Owing merits accelerated charge transport, optimized adsorption/desorption intermediates, raised conductivity, regulation microenvironment, ease combine with geometric characteristics, built-in electric field (BIEF) is expected overcome above problems. Here, we give a Review about very recent progress BIEF for efficient electrocatalysis. First, construction strategies characterization methods (qualitative quantitative analysis) are summarized. Then, up-to-date overviews engineering electrocatalysis, attention on electron structure optimization microenvironment modulation, analyzed discussed detail. In end, challenges perspectives proposed. This gives deep understanding design electrocatalysts next-generation storage devices.

Язык: Английский

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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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Engineering Multilevel Collaborative Catalytic Interfaces with Multifunctional Iron Sites Enabling High-Performance Real Seawater Splitting

ACS Nano, Год журнала: 2023, Номер 17(2), С. 1681 - 1692

Опубликована: Янв. 3, 2023

Given the abundant reserves of seawater and scarcity freshwater, real electrolysis is a more economically appealing technology for hydrogen production relative to orthodox freshwater electrolysis. However, this greatly precluded by undesirable chlorine oxidation reaction severe chloride corrosion at anode, further restricting catalytic efficiency overall splitting. Herein, feasible strategy engineering multifunctional collaborative interfaces reported develop porous metal nitride/phosphide heterostructure arrays anchoring on conductive Ni2P surfaces with affluent iron sites. Collaborative among phosphide, bimetallic nitride, supports play positive role in improving water adsorption/dissociation adsorption behaviors active Fe sites evidenced theoretical calculations evolution reactions, enhancing oxygenated species nitrate-rich passivating layers resistant oxygen reaction, thus cooperatively propelling high-performance bifunctional The resultant material Fe2P/Ni1.5Co1.5N/Ni2P performs excellently as self-standing catalyst alkaline It requires extremely low cell voltages 1.624 1.742 V afford current densities 100 500 mA/cm2 1 M KOH electrolytes, respectively, along superior long-term stability, outperforming nearly all ever-reported non-noble electrocatalysts benchmark Pt/IrO2 coupled electrodes freshwater/seawater This work presents an effective catalysts toward green from

Язык: Английский

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Multiscale Hierarchical Structured NiCoP Enabling Ampere‐Level Water Splitting for Multi‐Scenarios Green Energy‐to‐Hydrogen Systems

Advanced Energy Materials, Год журнала: 2023, Номер 13(22)

Опубликована: Апрель 28, 2023

Abstract Efficient and stable low‐cost catalysts are seriously lacking for industrial water electrolysis at large‐current‐density. To meet industrial‐scale hydrogen production, fully utilized active sites by a rational structure design is an attractive route. Herein, dynamic microstructure manipulation of bimetallic phosphide NiCoP conducted. Among different microstructures NiCoP, as‐obtained NiCoP‐120 hydrothermal temperature 120 °C, shows special multiscale hierarchical from 3D‐nickel foam substrates, 2D‐nanosheets to 1D‐nanoneedles, which conducive efficient utilization rapid gas release, thus manifesting outstanding electrocatalytic activities stability as required industry. reach current density 10 1000 mA cm −2 the evolution reaction (HER), requires ultra‐low overpotentials 56 247 mV, respectively. Particularly, bifunctional catalyst, it only needs 1.981 V drive 1 A overall splitting can maintain output 600 h, superior almost all reported non‐noble metal catalysts. Moreover, its application prospect in integrated green energy‐to‐hydrogen systems, including sunlight, wind, thermal, lithium cells, well demonstrated. This work provides guiding strategy establishment externally driven water‐splitting production system.

Язык: Английский

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Mo‐Modified ZnIn₂S₄@NiTiO₃ S‐Scheme Heterojunction with Enhanced Interfacial Electric Field for Efficient Visible‐Light‐Driven Hydrogen Evolution

Advanced Functional Materials, Год журнала: 2023, Номер 33(15)

Опубликована: Фев. 26, 2023

Abstract Designing and developing visible‐light‐responsive materials for solar to chemical energy is an efficient promising approach green sustainable carbon‐neutral systems. Herein, a facile in situ growth hydrothermal strategy using Mo‐modified ZnIn 2 S 4 (Mo‐ZIS) nanosheets coupled with NiTiO 3 (NTO) microrods synthesize multifunctional ZIS wrapped NTO (Mo‐ZIS@NTO) photocatalyst enhanced interfacial electric field (IEF) effect typical S‐scheme heterojunction reported. Mo‐ZIS@NTO catalyst possesses wide‐spectrum light absorption properties, excellent visible light‐to‐thermal effect, electron mobility, charges transfer, strong IEF exhibits solar‐to‐chemical conversion visible‐light‐driven photocatalytic hydrogen evolution. Notably, the engineered Mo 1.4 ‐ZIS@NTO superior performance H evolution rate of up 14.06 mmol g −1 h − 1 apparent quantum efficiency 44.1% at 420 nm. The scientific explorations provide in‐depth understanding microstructure, heterojunction, IEF, Mo‐dopant facilitation effect. Moreover, theoretical simulations verify critical role element promoting adsorption activation O molecules, modulating behavior on active sites, thus accelerating overall catalytic efficiency. mechanism via adjustable regulation over also demonstrated.

Язык: Английский

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Lattice Strain Engineering of Ni₂P Enables Efficient Catalytic Hydrazine Oxidation‐Assisted Hydrogen Production

Advanced Materials, Год журнала: 2023, Номер 35(42)

Опубликована: Июль 11, 2023

Hydrazine-assisted water electrolysis provides new opportunities to enable energy-saving hydrogen production while solving the issue of hydrazine pollution. Here, synthesis compressively strained Ni2 P as a bifunctional electrocatalyst for boosting both anodic oxidation reaction (HzOR) and cathodic evolution (HER) is reported. Different from multistep synthetic method that induces lattice strain by creating core-shell structures, facile strategy developed tune via dual-cation co-doping. The obtained with compressive -3.62% exhibits significantly enhanced activity HzOR HER than counterparts tensile without strain. Consequently, optimized delivers current densities 10 100 mA cm-2 at small cell voltages 0.16 0.39 V hydrazine-assisted electrolysis, respectively. Density functional theory (DFT) calculations reveal promotes dissociation concurrently tunes adsorption strength intermediates, thereby facilitating process on P. As HzOR, reduces energy barrier potential-determining step dehydrogenation *N2 H4 H3 . Clearly, this work paves pathway lattice-strained electrocatalysts

Язык: Английский

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Nanoreactors Encapsulating Built‐in Electric Field as a “Bridge” for Li–S Batteries: Directional Migration and Rapid Conversion of Polysulfides

Advanced Energy Materials, Год журнала: 2023, Номер 14(9)

Опубликована: Дек. 27, 2023

Abstract Lithium–sulfur batteries (Li–S) are recognized as the next generation of secondary due to their satisfactory theoretical specific capacity and energy density. However, a series problems such disordered migration behavior, sluggish redox kinetics, serious shuttle effect lithium polysulfides (LiPSs) greatly limit commercial application. Herein, nanoreactors encapsulate heterostructure guarantee sulfur conversion in hosts where consists FeP with moderate adsorption ability, excellent catalytic active low work function, Fe 3 O 4 strong ability high function. This rational configuration controls direction interface built‐in electric field (BIEF) between catalyst adsorbent, realizing successive “trapping‐directional migration‐conversion” reaction mechanism species. Thanks BIEF bridge connect trapping site site, /FeP@C─S cathode delivers an ultrahigh initial 1402 mAh g −1 at 0.1 C remains more than 450 5 after 350 cycles. Even loading 5.20 mg cm −2 , it displayed 970 . provided effective strategy design high‐performance electrocatalysts for Li–S batteries.

Язык: Английский

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Coupling NiSe₂ Nanoparticles with N-Doped Porous Carbon Enables Efficient and Durable Electrocatalytic Hydrogen Evolution Reaction at pH Values Ranging from 0 to 14

ACS Applied Nano Materials, Год журнала: 2023, Номер 7(1), С. 1138 - 1145

Опубликована: Дек. 20, 2023

Integrating metal-based species with a carbon matrix is promising approach for fabricating inexpensive, durable, and efficient electrocatalysts. Herein, NiSe2-decorated N-doped polyhedra (NC) are prepared as electrocatalysts hydrogen evolution reaction (HER) by template-assisted approach. The optimal NC-NiSe2 delivers extraordinary catalytic activities toward HER in wide pH range, overpotentials of 127 mV 0.5 M H2SO4, 226 1 PBS, 205 KOH to drive current density 10 mA cm–2. In addition, this catalyst undergoes fast kinetics via Volmer–Heyrovsky mechanism exhibits excelent long-term durability 48 h the full media. During electrocatalysis, when electrons pass through NC surface NiSe2 particles, water molecules at active sites reduced, then released. excellent activity mainly benefit from hierarchically porous architecture well synergistic interaction nanoparticles matrix, which not only significantly boost electronic conductivity generate plentiful but also guarantee chemical structural stabilities species. This work unravels deep insights into exploration carbon-supported metal chalcogenides highly full-pH values.

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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Manipulating Electron Redistribution in Ni₂P for Enhanced Alkaline Seawater Electrolysis

Advanced Materials, Год журнала: 2023, Номер 36(1)

Опубликована: Сен. 23, 2023

Abstract Developing bifunctional electrocatalyst for seawater splitting remains a persistent challenge. Herein, an approach is proposed through density functional theory (DFT) preanalysis to manipulate electron redistribution in Ni 2 P addressed by cation doping and vacancy engineering. The needle‐like Fe‐doped with (Fe‐Ni Pv) successfully synthesized on nickel foam, exhibiting superior hydrogen evolution reaction (HER) oxygen (OER) catalytic activity electrolysis alkaline condition. As result, Fe‐Ni Pv achieves the industrially required current densities of 1.0 3.0 A cm −2 at low voltages 1.68 1.73 V, respectively, 60 °C 6.0 m KOH circumstances. theoretical calculation experimental results collectively reveal reasons enhancement catalyst activity. Specifically, Fe vacancies can accelerate reconstruction OER active species optimize adsorption free energy (Δ G H* ) HER. In addition, sites are identified, where greatly improve electrical conductivity dominant centers, meanwhile atoms as centers study provides deep insight into exploration nickel‐based phosphide catalysts identification their real centers.

Язык: Английский

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