Sabatier Relations in Electrocatalysts Based on High‐entropy Alloys with Wide‐distributed d‐band Centers for Li‐O₂ Batteries

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(44)

Опубликована: Сен. 12, 2023

Li-O2 battery (LOB) is a promising "beyond Li-ion" technology with ultrahigh theoretical energy density (3457 Wh kg-1 ), while currently impeded by the sluggish cathodic kinetics of reversible gas-solid reaction between O2 and Li2 . Despite many catalysts are developed for accelerating conversion process, lack design guidance achieving high performance makes exploring aleatory. The Sabatier principle an acknowledged theory connecting scaling relationship heterogeneous catalytic activity, providing tradeoff strategy topmost performance. Herein, series wide-distributed d-band centers (i.e., wide range adsorption strength) elaborately constructed via high-entropy strategy, enabling in-depth study relations in electrocatalysts LOBs. A volcano-type correlation center activity emerges. Both experimental results indicate that moderate appropriate strength propels up to top. As demonstration concept, LOB using FeCoNiMnPtIr as catalyst provides exceptional efficiency over 80 %, works steadily 2000 h fixed specific capacity 4000 mAh g-1 This work certifies applicability designing advanced assembled

Язык: Английский

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Tailoring the d‐Band Center over Isomorphism Pyrite Catalyst for Optimized Intrinsic Affinity to Intermediates in Lithium–Oxygen Batteries

Advanced Energy Materials, Год журнала: 2023, Номер 13(15)

Опубликована: Фев. 15, 2023

Abstract Rechargeable lithium–oxygen batteries (LOBs) are regarded as one of the most promising candidates for next generation energy storage devices. Nevertheless, lack understanding relationships between structure, property, and performance catalysts limits rational development efficient cathode catalysts, therefore, hinders commercial application LOBs. Herein, a d‐band center regulation strategy is proposed to construct an isomorphism composite NiS 2 ‐CoS @nitrogen‐doped carbon (NiS @NC) advanced catalyst boosting electrocatalytic activities Density functional theory calculations reveal that introduction Ni atoms not only redistributes internal charges on structure but also modulates adsorption capacities intermediates by tuning center, thus promoting oxygen reduction reaction/oxygen evolution reaction kinetics reducing overpotentials. As expected, @NC catalyzed LOBs present superior electrochemical including large initial discharge/charge specific capacity 14 551/13 563 mAh g −1 , ultralong cycle life over 490 cycles at current density 500 mA excellent rate performance. The insight into tailoring its facilitates construction electrocatalysts other systems.

Язык: Английский

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Homologous Heterostructured NiS/NiS₂@C Hollow Ultrathin Microspheres with Interfacial Electron Redistribution for High‐Performance Sodium Storage

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

Опубликована: Июнь 15, 2023

Nickel sulfides with high theoretical capacity are considered as promising anode materials for sodium-ion batteries (SIBs); however, their intrinsic poor electric conductivity, large volume change during charging/discharging, and easy sulfur dissolution result in inferior electrochemical performance sodium storage. Herein, a hierarchical hollow microsphere is assembled from heterostructured NiS/NiS2 nanoparticles confined by situ carbon layer (H-NiS/NiS2 @C) via regulating the sulfidation temperature of precursor Ni-MOFs. The morphology ultrathin spherical shells confinement to active provide rich channels ion/electron transfer alleviate effects agglomeration material. Consequently, as-prepared H-NiS/NiS2 @C exhibit superb properties, satisfactory initial specific 953.0 mA h g-1 at 0.1 A , excellent rate capability 509.9 2 superior longtime cycling life 433.4 after 4500 cycles 10 . Density functional theory calculation shows that heterogenous interfaces electron redistribution lead charge NiS NiS2 thus favor interfacial transport reduce ion-diffusion barrier. This work provides an innovative idea synthesis homologous heterostructures high-efficiency SIB electrode materials.

Язык: Английский

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Electronic Spin Alignment within Homologous NiS₂/NiSe₂ Heterostructures to Promote Sulfur Redox Kinetics in Lithium‐Sulfur Batteries

Advanced Materials, Год журнала: 2024, Номер 36(25)

Опубликована: Апрель 3, 2024

Abstract The catalytic activation of the Li‐S reaction is fundamental to maximize capacity and stability batteries (LSBs). Current research on catalysts mainly focuses optimizing energy levels promote adsorption conversion, while frequently overlooking electronic spin state influence charge transfer orbital interactions. Here, hollow NiS 2 /NiSe heterostructures encapsulated in a nitrogen‐doped carbon matrix (NiS @NC) are synthesized used as additive sulfur cathodes. heterostructure promotes splitting 3d orbital, driving Ni 3+ transformation from low high spin. This configuration raises level activates state. accelerates optimizes energy, lowering barrier polysulfides conversion. Benefiting these characteristics, LSBs based @NC/S cathodes exhibit initial (1458 mAh·g⁻ 1 at 0.1C), excellent rate capability (572 5C), stable cycling with an average decay only 0.025% per cycle 1C during 500 cycles. Even loadings (6.2 mg·cm⁻ ), capacities 1173 (7.27 mAh·cm⁻ ) measured 0.1C, 1058 retained after 300

Язык: Английский

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Ultrathin two-dimensional materials: New opportunities and challenges in ultra-sensitive gas sensing

Coordination Chemistry Reviews, Год журнала: 2024, Номер 505, С. 215691 - 215691

Опубликована: Янв. 31, 2024

Язык: Английский

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Lattice-dependent activation of highly efficient SnTe cathode catalyst for Li–air batteries

Energy storage materials, Год журнала: 2024, Номер 69, С. 103392 - 103392

Опубликована: Апрель 8, 2024

Язык: Английский

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Multilevel Heterogeneous Interfaces Enhanced Polarization Loss of 3D-Printed Graphene/NiCoO₂/Selenides Aerogels for Boosting Electromagnetic Energy Dissipation

ACS Nano, Год журнала: 2024, Номер 18(14), С. 10184 - 10195

Опубликована: Март 26, 2024

Heterointerface engineering is an attractive approach to modulating electromagnetic (EM) parameters and EM wave absorption performance. However, the weak interfacial interactions poor impedance matching would lead unsatisfactory performance due limitation of construction materials design strategies. Herein, multilevel heterointerface proposed by in situ growing nanosheet-like NiCoO2 selenides with abundant interface structures on 3D-printed graphene aerogel (GA) skeletons, which strengthens effect improves dielectric polarization loss. Benefiting from features substantially enhanced loss optimized matching, graphene/S-NiCoO2/selenides (G/S-NCO/Se) have achieved brilliant a strong reflection (RL) value −60.7 dB broad effective bandwidth (EAB) 8 GHz, about six times greater than that (−9.8 dB). Moreover, it further confirmed charge density differences off-axis electron holography large amount polarized accumulates at interface, leading significant relaxation behaviors. This work provides deep understanding heterogeneous loss, injects fresh infinite vitality for designing high-efficiency absorbers.

Язык: Английский

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Tunable Interfacial Electric Field‐Mediated Cobalt‐Doped FeSe/Fe₃Se₄ Heterostructure for High‐Efficiency Potassium Storage

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(28)

Опубликована: Апрель 25, 2024

Abstract The interfacial electric field (IEF) in the heterostructure can accelerate electron transport and ion migration, thereby enhancing electrochemical performance of potassium‐ion batteries (PIBs). Nevertheless, quantification modulation IEF for high‐efficiency PIB anodes currently remains a blank slate. Herein, we achieve first time tuning via amorphous carbon‐coated undifferentiated cobalt‐doped FeSe/Fe 3 Se 4 (denoted UN‐CoFe 5 /C) efficient potassium storage. Co doping increase , improving transport, promoting adsorption capacity, lowering diffusion barrier. As expected, magnitude /C is experimentally quantified as 62.84 mV, which 3.65 times larger than that (Fe /C). Benefiting from strong IEF, anode exhibits superior rate capability (145.8 mAh g −1 at 10.0 A ) long cycle lifespan (capacity retention 95.1 % over 3000 cycles 1.0 ). Furthermore, this strategy universally regulate CoSe 2 /Co 9 8 FeS /Fe 7 S heterostructures. This work provide fundamental insights into design advanced electrodes.

Язык: Английский

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Modulation of Charge Redistribution in Heterogeneous NiO‐Ni₃Se₄ Nanosheet Arrays for Advanced Water Electrolysis

Advanced Functional Materials, Год журнала: 2023, Номер 34(4)

Опубликована: Окт. 24, 2023

Abstract Developing highly effective electrocatalysts capable of bifunctionally facilitating hydrogen evolution reaction (HER) and oxygen (OER) is paramount for advancing water electrolysis. Herein, the authors report heterogeneous NiO‐Ni 3 Se 4 nanosheet arrays grown on Ti C 2 T x MXene (NiO‐Ni /MXene) with asymmetrical charge distribution as bifunctional to enhance electrocatalytic performance overall splitting. Impressively, meticulously engineered /MXene exhibits remarkable catalytic activities HER OER low overpotentials 50 mV 260 at 10 mA cm −2 , respectively. Moreover, electrolyzer equipped both cathode anode demonstrates outstanding performance, reaching a cell voltage 1.54 V maintaining exceptional long‐term durability over h. The combination theoretical calculations experiments unveils transfer induced heterointerfaces in heterogeneous, leading distributions, which modulate adsorption/desorption intermediates kinetics. This study presents promising approach rationalizing performance.

Язык: Английский

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Spatial separation strategy to construct N/S co-doped carbon nanobox embedded with asymmetrically coupled Fe-Co pair-site for boosted reversible oxygen electrocatalysis

Journal of Colloid and Interface Science, Год журнала: 2023, Номер 653, С. 1577 - 1587

Опубликована: Сен. 22, 2023

Язык: Английский

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