Engineering Symmetry-Breaking Centers and d-Orbital Modulation in Triatomic Catalysts for Zinc-Air Batteries DOI

Junjie Zhong,

Zhanhao Liang,

Ning Liu

et al.

ACS Nano, Journal Year: 2024, Volume and Issue: unknown

Published: Feb. 5, 2024

Unraveling the configuration–activity relationship and synergistic enhancement mechanism (such as real active center, electron spin-state, d-orbital energy level) for triatomic catalysts, well their intrinsically bifunctional oxygen electrocatalysis, is a great challenge. Here we present catalyst (TAC) with trinuclear structure that displays extraordinary electrocatalysis reduction reaction (ORR) evolution (OER), greatly outperforming counterpart of single-atom diatomic catalysts. The aqueous Zn-air battery (ZAB) equipped TAC-based cathode exhibits rechargeable stability ultrarobust cycling performance (1970 h/3940 cycles at 2 mA cm–2, 125 h/250 10 cm–2 negligible voltage decay), quasi-solid-state ZAB outstanding rechargeability low-temperature adaptability (300 h/1800 −60 °C), other state-of-the-art ZABs. experimental theoretical analyses reveal symmetry-breaking CoN4 configuration under incorporation neighboring metal atoms (Fe Cu), which leads to modulation, low-shift d band weakened binding strength intermediates, decreased barrier electrocatalysis. This rational tricoordination design an in-depth analysis indicate hetero-TACs can be promisingly applied in various applications.

Language: Английский

Zn-based batteries for sustainable energy storage: strategies and mechanisms DOI Creative Commons
Lei Tang,

Haojia Peng,

Jiarui Kang

et al.

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(10), P. 4877 - 4925

Published: Jan. 1, 2024

This review systematically summarizes various redox mechanisms in Zn-based batteries and design strategies to improve their electrochemical performance, which provides a reference for future development of high-performance batteries.

Language: Английский

Citations

109
Inter-site structural heterogeneity induction of single atom Fe catalysts for robust oxygen reduction DOI Creative Commons
Peng Zhang, Hsiao‐Chien Chen, Houyu Zhu

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: March 7, 2024

Abstract Metal-nitrogen-carbon catalysts with hierarchically dispersed porosity are deemed as efficient geometry for oxygen reduction reaction (ORR). However, catalytic performance determined by individual and interacting sites originating from structural heterogeneity is particularly elusive yet remains to be understood. Here, an porous Fe single atom catalyst (Fe SAs-HP) prepared atoms densely resided at micropores mesopores. SAs-HP exhibits robust ORR half-wave potential of 0.94 V turnover frequency 5.99 e −1 s site 0.80 V. Theoretical simulations unravel a induced optimization, where mesoporous Fe-N 4 acts real active centers result long-range electron regulation adjacent microporous sites, facilitating O 2 activation desorption key intermediate *OH. Multilevel operando characterization results identify undergo dynamic evolution basic 3 under working conditions. Our findings reveal the origin enhanced intrinsic activity sites.

Language: Английский

Citations

94
Ru/Ir‐Based Electrocatalysts for Oxygen Evolution Reaction in Acidic Conditions: From Mechanisms, Optimizations to Challenges DOI Creative Commons
Rong Qin, Guanzhen Chen,

Caihong Feng

et al.

Advanced Science, Journal Year: 2024, Volume and Issue: 11(21)

Published: March 19, 2024

Abstract The generation of green hydrogen by water splitting is identified as a key strategic energy technology, and proton exchange membrane electrolysis (PEMWE) one the desirable technologies for converting renewable sources into hydrogen. However, harsh anode environment PEMWE oxygen evolution reaction (OER) involving four‐electron transfer result in large overpotential, which limits overall efficiency production, thus efficient electrocatalysts are needed to overcome high overpotential slow kinetic process. In recent years, noble metal‐based (e.g., Ru/Ir‐based metal/oxide electrocatalysts) have received much attention due their unique catalytic properties, already become dominant acidic OER process applied commercial devices. these still face thorny problem conflicting performance cost. this review, first, metal briefly classified according forms existence, mechanisms outlined. Then, focus on summarizing improvement strategies with respect activity stability over years. Finally, challenges development prospects discussed.

Language: Английский

Citations

82
A Review of Rechargeable Zinc–Air Batteries: Recent Progress and Future Perspectives DOI Creative Commons

Ghazanfar Nazir,

Adeela Rehman, Jong‐Hoon Lee

et al.

Nano-Micro Letters, Journal Year: 2024, Volume and Issue: 16(1)

Published: Feb. 29, 2024

Zinc-air batteries (ZABs) are gaining attention as an ideal option for various applications requiring high-capacity batteries, such portable electronics, electric vehicles, and renewable energy storage. ZABs offer advantages low environmental impact, enhanced safety compared to Li-ion cost-effectiveness due the abundance of zinc. However, early research faced challenges parasitic reactions at zinc anode slow oxygen redox kinetics. Recent advancements in restructuring anode, utilizing alternative electrolytes, developing bifunctional catalysts have significantly improved ZABs. Scientists achieved battery reversibility over thousands cycles, introduced new efficiency records surpassing 70%. Despite these achievements, there related lower power density, shorter lifespan, air electrode corrosion leading performance degradation. This review paper discusses different configurations, reaction mechanisms electrically mechanically rechargeable ZABs, proposes remedies enhance overall performance. The also explores recent advancements, applications, future prospects electrically/mechanically

Language: Английский

Citations

81
Microenvironment reconstitution of highly active Ni single atoms on oxygen-incorporated Mo2C for water splitting DOI Creative Commons

Mengyun Hou,

Lirong Zheng, Di Zhao

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Feb. 13, 2024

Abstract The rational design of efficient bifunctional single-atom electrocatalysts for industrial water splitting and the comprehensive understanding its complex catalytic mechanisms remain challenging. Here, we report a Ni single atoms supported on oxygen-incorporated Mo 2 C via Ni-O-Mo bridge bonds, that gives high oxygen evolution reaction (OER) hydrogen (HER) activity. By ex situ synchrotron X-ray absorption spectroscopy electron microscopy, found after HER, coordination number bond lengths Ni-O Ni-Mo (Ni-O-Mo) were all altered, yet species still atomically dispersed. In contrast, OER, dispersed agglomerated into very small clusters with new Ni-Ni (Ni-O-Ni) bonds appeared. Combining experimental results DFT calculations, infer oxidation degree configuration are both vital HER or OER. This study provides feasible strategy model to highly electrolysis.

Language: Английский

Citations

79
Vacancy Defects Inductive Effect of Asymmetrically Coordinated Single‐Atom Fe─N3S1 Active Sites for Robust Electrocatalytic Oxygen Reduction with High Turnover Frequency and Mass Activity DOI
Yilin Zhao, Hsiao‐Chien Chen, Xuelu Ma

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(11)

Published: Dec. 16, 2023

Abstract The development of facile, efficient synthesis method to construct low‐cost and high‐performance single‐atom catalysts (SACs) for oxygen reduction reaction (ORR) is extremely important, yet still challenging. Herein, an atomically dispersed N, S co‐doped carbon with abundant vacancy defects (NSC‐vd) anchored Fe single atoms (SAs) reported a inductive effect proposed promoting electrocatalytic ORR. optimized catalyst featured stable Fe─N 3 1 active sites exhibits excellent ORR activity high turnover frequency mass activity. In situ Raman, attenuated total reflectance surface enhanced infrared absorption spectroscopy reveal the exhibit different kinetic mechanisms in acidic alkaline solutions. Operando X‐ray spectra SAs/NSC‐vd electrolyte closely related coordination structure. Theoretical calculation reveals upshifted d band center facilitates adsorption O 2 accelerates kinetics process *OH reduction. around balance OOH* formation reduction, thus synergetically process.

Language: Английский

Citations

76
Structural engineering of atomic catalysts for electrocatalysis DOI Creative Commons

Tianmi Tang,

Xue Bai, Zhenlü Wang

et al.

Chemical Science, Journal Year: 2024, Volume and Issue: 15(14), P. 5082 - 5112

Published: Jan. 1, 2024

This review systematically introduces how to regulate the electronic structure and geometric configuration of atomic catalysts achieve high-efficiency electrocatalysis performances by analyzing detailed electrocatalytic applications mechanisms.

Language: Английский

Citations

66
Cobalt phosphide/nickel–cobalt phosphide heterostructured hollow nanoflowers for high-performance supercapacitor and overall water splitting DOI

Xiutao Fu,

Zhi Zhang, Yifan Zheng

et al.

Journal of Colloid and Interface Science, Journal Year: 2023, Volume and Issue: 653, P. 1272 - 1282

Published: Sept. 24, 2023

Language: Английский

Citations

54
Superstructure-Assisted Single-Atom Catalysis on Tungsten Carbides for Bifunctional Oxygen Reactions DOI
Hongguan Li,

Wu Wang,

Sikang Xue

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(13), P. 9124 - 9133

Published: March 22, 2024

Single-atom catalysis (SAC) attracts wide interest for zinc–air batteries that require high-performance bifunctional electrocatalysts oxygen reactions. However, catalyst design is still highly challenging because of the insufficient driving force promoting multiple-electron transfer kinetics. Herein, we report a superstructure-assisted SAC on tungsten carbides evolution and reduction In addition to usual single atomic sites, strikingly, reveal presence ordered Co superstructures in interfacial region with induce internal strain promote catalysis. Theoretical calculations show combined effects from atoms strongly reduce adsorption energy intermediates overpotential both The therefore presented impressive activity an ultralow potential gap 0.623 V delivered high power density 188.5 mW cm–2 assembled batteries. This work opens up new opportunities

Language: Английский

Citations

52
Advanced design strategies for Fe-based metal–organic framework-derived electrocatalysts toward high-performance Zn–air batteries DOI
Yafei Guo,

Shan Zhao,

Nan Zhang

et al.

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(5), P. 1725 - 1755

Published: Jan. 1, 2024

This article summarizes the regulation strategies of Fe-based MOFs-derived electrocatalysts for ZABs, and provides a prospect their future development.

Language: Английский

Citations

51