Upcycling Spent Cathodes from Li–Ion Batteries into a High-Entropy Alloy Catalyst with Reverse Electron Transfer for Li–O2 Batteries DOI
Peng Wang, Shan Guo, Yongbin Xu

et al.

ACS Nano, Journal Year: 2025, Volume and Issue: unknown

Published: April 30, 2025

Traditional recovery of valuable metals from spent ternary lithium-ion batteries concentrates on complicated pyrometallurgy and hydrometallurgy routes. Direct reutilization these used to catalyze Li-O2 is highly appealing yet remains a significant challenge. Here, we report general synthesis ultrafine αNiCoMn (α = Pt, Ir, Ru) high-entropy alloy (HEA) nanoparticles anchored nitrogen-doped carbon (N-C) support through facile one-step Joule heating, which serves as high-efficiency catalyst for batteries. Solution alloying recycled NiCoMn with Pt group facilitates catalytic efficiency 3d-5d electronic interactions the assembly effect. Both experimental calculation results reveal that, driven by rapid, nonequilibrium thermal shock, electron transfer defies conventional expectations, where electrons are inclined higher electronegative surrounding atoms. This interesting reverse local charge redistribution orbital hybridization endow an elevated d-band center optimized structure. The induced coordination effects further generate active catalysis surfaces, favoring adsorption LiO2 intermediates facilitating rapid decomposition kinetics nanoscale Li2O2 products. These advantages HEA@N-C superior bifunctional activity, achieving ultralow polarization 0.27 V significantly enhanced cycling life 240 cycles. We anticipate that this work will provide insights into upcycling constructing efficient HEA electrocatalysts.

Language: Английский

A 3d‐4d‐5d High Entropy Alloy as a Bifunctional Oxygen Catalyst for Robust Aqueous Zinc–Air Batteries DOI
Ren He, Linlin Yang, Yu Zhang

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(46)

Published: July 24, 2023

High entropy alloys (HEAs) are highly suitable candidate catalysts for oxygen evolution and reduction reactions (OER/ORR) as they offer numerous parameters optimizing the electronic structure catalytic sites. Herein, FeCoNiMoW HEA nanoparticles synthesized using a solution-based low-temperature approach. Such show high properties, subtle lattice distortions, modulated structure, leading to superior OER performance with an overpotential of 233 mV at 10 mA cm-2 276 100 . Density functional theory calculations reveal structures active sites optimized d-band center position that enables adsorption OOH* intermediates reduces Gibbs free energy barrier in process. Aqueous zinc-air batteries (ZABs) based on this demonstrate open circuit potential 1.59 V, peak power density 116.9 mW , specific capacity 857 mAh gZn-1, excellent stability over 660 h continuous charge-discharge cycles. Flexible solid ZABs also assembled tested, displaying different bending angles. This work shows significance 4d/5d metal-modulated ability improve OER/ORR, ZABs, beyond.

Language: Английский

Citations

100
Why do Single‐Atom Alloys Catalysts Outperform both Single‐Atom Catalysts and Nanocatalysts on MXene? DOI Open Access

Shuyan Guan,

Zhenluo Yuan,

Zechao Zhuang

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 63(4)

Published: Dec. 1, 2023

Abstract Single‐atom alloys (SAAs), combining the advantages of single‐atom and nanoparticles (NPs), play an extremely significant role in field heterogeneous catalysis. Nevertheless, understanding catalytic mechanism SAAs catalysis reactions remains a challenge compared with single atoms NPs. Herein, ruthenium‐nickel (RuNi ) synthesized by embedding atomically dispersed Ru Ni NPs are anchored on two‐dimensional Ti 3 C 2 T x MXene. The RuNi SAA‐3 −Ti catalysts exhibit unprecedented activity for hydrogen evolution from ammonia borane (AB, NH BH hydrolysis mass‐specific (r mass value 333 L min −1 g . Theoretical calculations reveal that anchoring optimizes dissociation AB H O as well binding ability H* intermediates during due to d‐band structural modulation caused alloying effect metal‐supports interactions (MSI) This work provides useful design principles developing optimizing efficient hydrogen‐related demonstrates over energy

Language: Английский

Citations

77
Controllable synthesis of high-entropy alloys DOI
Jingjing Liang,

Guanghui Cao,

Mengqi Zeng

et al.

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(12), P. 6021 - 6041

Published: Jan. 1, 2024

This review provides a comprehensive overview of the recent advancements in controllable synthesis high-entropy alloys, ranging from approach and significance composition, morphology, structure, surface/interface engineering.

Language: Английский

Citations

21
High entropy energy storage materials: Synthesis and application DOI

Jianping Ma,

Chengde Huang

Journal of Energy Storage, Journal Year: 2023, Volume and Issue: 66, P. 107419 - 107419

Published: April 25, 2023

Language: Английский

Citations

41
Status and Prospects of MXene‐Based Lithium–Oxygen Batteries: Theoretical Prediction and Experimental Modulation DOI
Xingzi Zheng, Mengwei Yuan,

Yuelin Zhao

et al.

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(20)

Published: April 7, 2023

Abstract The consumption of fossil fuels has contributed to global warming and other problems. It is urgent exploit progressive, low‐cost, environmentally friendly energy storage devices with super high density. Rechargeable lithium oxygen batteries (LOBs) a theoretical density (≈11400 Wh kg −1 ) are one the most promising chemical power supplies. MXenes have recently emerged in conversion due their superior conductivity adjustable structural properties. Here, this paper summarizes latest research progress MXene‐based materials cathode, anode, separator electrolyte LOBs emphasizes significance surface functionalization strategies design experimental modulation, which promote electrode reaction kinetics increase cyclability LOBs. also prospects challenges proposes novel battery performance, inspiring future designing high‐performance

Language: Английский

Citations

40
Working Principles of High-Entropy Electrolytes in Rechargeable Batteries DOI
Ke‐feng Ren,

He Liu,

Jiaxin Guo

et al.

ACS Energy Letters, Journal Year: 2024, Volume and Issue: 9(6), P. 2960 - 2980

Published: May 28, 2024

Rechargeable batteries are considered to be one of the most feasible solutions energy crisis and environmental pollution. As a bridge between cathode anode battery, electrolytes play critical roles in improving battery performance. Recently, high-entropy (HEEs) with unique properties were proposed. Specifically, HEEs can accelerate ionic diffusion kinetics promote dissolution salts as well broaden operating temperature batteries. This Review provides comprehensive summary application working mechanisms rechargeable First, motivation, history, definitions introduced. Then, enhancing electrochemical performance liquid solid-state presented, especially conductivity achieving wide range. Finally, current issues possible future directions new perspective on design high-performance electrolytes.

Language: Английский

Citations

12
Tuning Dual Catalytic Active Sites of Pt Single Atoms Paired with High-Entropy Alloy Nanoparticles for Advanced Li-O2 Batteries DOI
Lei Li, Minghao Hua,

J. W. Li

et al.

ACS Nano, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 17, 2025

To achieve a long cycle life and high-capacity performance for Li-O2 batteries, it is critical to rationally modulate the formation decomposition pathway of discharge product Li2O2. Herein, we designed highly efficient catalyst containing dual catalytic active sites Pt single atoms (PtSAs) paired with high-entropy alloy (HEA) nanoparticles oxygen reduction reaction (ORR) in batteries. HEA moderate d-band center enhance surface adsorbed LiO2 intermediate (LiO2(ads)), while PtSAs exhibit weak adsorption energy promote soluble (LiO2(sol)). An optimal ratio between LiO2(ads) LiO2(sol) was realized via regulating etching conditions dealloying synthesis process obtaining high-performance The ORR kinetics are accelerated, parasitic reactions restrained As result, batteries based on HEA@Pt-PtSAs demonstrate an ultralow overpotential (0.3 V) ultralong cycling 470 cycles at 1000 mA g-1. insights into synthetic strategies importance balancing pathways will offer guidance devising multisite synergistic catalysts accelerate redox-reaction

Language: Английский

Citations

1
CNTs-supported noble metal-free high-entropy alloys heterostructure NiMoCoMnLa/CNTs@Ni for electrochemical hydrogen evolution reaction DOI
Sixuan Zhang, Jinzhao Huang, Jun Tang

et al.

Applied Surface Science, Journal Year: 2024, Volume and Issue: 667, P. 160417 - 160417

Published: May 29, 2024

Language: Английский

Citations

8
High Entropy Materials for Reversible Electrochemical Energy Storage Systems DOI Creative Commons
Jing Zhao, Shang Gao, Haoming Wei

et al.

ChemElectroChem, Journal Year: 2024, Volume and Issue: 11(7)

Published: Jan. 8, 2024

Abstract High entropy materials have garnered considerable attention recently as a class of with intricate stoichiometry, exhibiting high levels entropy. These hold great promise candidates for electrochemical energy storage devices due to their ideal regulation, good mechanical and physical properties attractive synergy effects multi‐elements. In this perspective, we provide an overview used anodes, cathodes, electrolytes in rechargeable batteries, insight into the materials’ structure‐property relationship influence on battery performance. Additionally, offer insights future perspectives materials, emphasizing crucial role next‐generation batteries.

Language: Английский

Citations

7
Constructing Built‐In Electric Field in NiCo2O4‐CeO2 Heterostructures to Regulate Li2O2 Formation Routes at High Current Densities DOI

Renshu Huang,

Zhixiang Zhai,

Xingfa Chen

et al.

Small, Journal Year: 2024, Volume and Issue: 20(30)

Published: Feb. 22, 2024

Abstract Developing catalysts with suitable adsorption energy for oxygen‐containing intermediates and elucidating their internal structure‐performance relationships are essential the commercialization of Li–O 2 batteries (LOBs), especially under high current densities. Herein, NiCo O 4 ‐CeO heterostructure a spontaneous built‐in electric field (BIEF) is designed utilized as cathode catalyst LOBs at density. The driving mechanism electron pumping/accumulation heterointerface studied via experiments density functional theory (DFT) calculations, growth discharge products. results show that BIEF induced by work function difference optimizes affinity LiO promotes formation nano‐flocculent Li , thus improving performance Specifically, exhibits large capacity (9546 mAh g −1 4000 mA ) stability (>430 cycles ), which better than majority previously reported metal‐based catalysts. This provides new method tuning nucleation decomposition inspires design ideal to operate

Language: Английский

Citations

7