Engineering Co‐N‐Cr Cross‐Interfacial Electron Bridges to Break Activity‐Stability Trade‐Off for Superdurable Bifunctional Single Atom Oxygen Electrocatalysts DOI
Yunlong Zhang, Bo Liu, Yunkun Dai

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(15)

Published: Jan. 29, 2024

Abstract Atomically dispersed metal‐nitrogen‐carbon (M‐N‐C) catalysts have exhibited encouraging oxygen reduction reaction (ORR) activity. Nevertheless, the insufficient long‐term stability remains a widespread concern owing to inevitable 2‐electron byproducts, H 2 O . Here, we construct Co‐N‐Cr cross‐interfacial electron bridges (CIEBs) via interfacial electronic coupling between Cr 3 and Co‐N‐C, breaking activity‐stability trade‐off. The partially occupied 3d‐orbitals of CIEBs induce rearrangement CoN 4 sites, lowering Co‐OOH* antibonding orbital occupancy accelerating adsorption intermediates. Consequently, suppress two‐electron ORR process approach apex Sabatier volcano plot for four‐electron pathway simultaneously. As proof‐of‐concept, is synthesized by molten salt template method, exhibiting dominant 4‐electron selectively extremely low yield confirmed Damjanovic kinetic analysis. demonstrates impressive bifunctional catalytic activity (▵E=0.70 V) breakthrough durability including 100 % current retention after 10 h continuous operation cycling performance over 1500 Zn‐air battery. hybrid configuration understanding mechanism reported here could shed new light on design superdurable M‐N‐C catalysts.

Language: Английский

Sustainable zinc–air battery chemistry: advances, challenges and prospects DOI
Qichen Wang, Shubham Kaushik, Xin Xiao

et al.

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(17), P. 6139 - 6190

Published: Jan. 1, 2023

Sustainable zinc-air batteries (ZABs) are considered promising energy storage devices owing to their inherent safety, high density, wide operating temperature window, environmental friendliness, etc., showing great prospect for future large-scale applications. Thus, tremendous efforts have been devoted addressing the critical challenges associated with sustainable ZABs, aiming significantly improve efficiency and prolong operation lifespan. The growing interest in ZABs requires in-depth research on oxygen electrocatalysts, electrolytes, Zn anodes, which not systematically reviewed date. In this review, fundamentals of electrocatalysts air cathodes, physicochemical properties ZAB issues strategies stabilization anodes summarized from perspective fundamental characteristics design principles. Meanwhile, significant advances situ/operando characterization highlighted provide insights into reaction mechanism dynamic evolution electrolyte|electrode interface. Finally, several thoughts perspectives provided regarding opportunities ZABs. Therefore, review provides a thorough understanding advanced chemistry, hoping that timely comprehensive can shed light upcoming horizons prosperous area.

Language: Английский

Citations

184
Co-catalytic metal–support interactions in single-atom electrocatalysts DOI
Lucy Gloag, Samuel V. Somerville, J. Justin Gooding

et al.

Nature Reviews Materials, Journal Year: 2024, Volume and Issue: 9(3), P. 173 - 189

Published: Jan. 10, 2024

Language: Английский

Citations

110
Tailoring Oxygen Reduction Reaction Kinetics of Fe−N−C Catalyst via Spin Manipulation for Efficient Zinc–Air Batteries DOI
Huiwen Zhang, Hsiao‐Chien Chen,

Solmaz Feizpoor

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(25)

Published: April 9, 2024

The interaction between oxygen species and metal sites of various orbitals exhibits intimate correlation with the reduction reaction (ORR) kinetics. Herein, a new approach for boosting inherent ORR activity atomically dispersed Fe-N-C matrix is represented by implanting Fe atomic clusters nearby. as-prepared catalyst delivers excellent half-wave potentials 0.78 0.90 V in acidic alkaline solutions, respectively. decent can also be validated from high-performance rechargeable Zn-air battery. experiments density functional theory calculations reveal that electron spin-state monodispersed active transferred low spin (LS, t

Language: Английский

Citations

102
Bifunctional Single Atom Catalysts for Rechargeable Zinc–Air Batteries: From Dynamic Mechanism to Rational Design DOI

Peng Zhang,

Kuo Chen, Jiaye Li

et al.

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

Published: June 7, 2023

Ever-growing demands for rechargeable zinc-air batteries (ZABs) call efficient bifunctional electrocatalysts. Among various electrocatalysts, single atom catalysts (SACs) have received increasing attention due to the merits of high utilization, structural tunability, and remarkable activity. Rational design SACs relies heavily on an in-depth understanding reaction mechanisms, especially dynamic evolution under electrochemical conditions. This requires a systematic study in mechanisms replace current trial error modes. Herein, fundamental oxygen reduction is first presented combining situ and/or operando characterizations theoretical calculations. By highlighting structure-performance relationships, rational regulation strategies are particularly proposed facilitate SACs. Furthermore, future perspectives challenges discussed. review provides thorough SACs, which expected pave avenue exploring optimum effective ZABs.

Language: Английский

Citations

101
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

82
A Janus dual-atom catalyst for electrocatalytic oxygen reduction and evolution DOI
Bing Tang, Yanan Zhou, Qianqian Ji

et al.

Nature Synthesis, Journal Year: 2024, Volume and Issue: 3(7), P. 878 - 890

Published: June 3, 2024

Language: Английский

Citations

78
Derived-2D Nb4C3Tx sheets with interfacial self-assembled Fe-N-C single-atom catalyst for electrocatalysis in water splitting and durable zinc-air battery DOI
Mahmood Ul Haq, Donghui Wu, Zeeshan Ajmal

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 344, P. 123632 - 123632

Published: Dec. 18, 2023

Language: Английский

Citations

75
Designing Oxide Catalysts for Oxygen Electrocatalysis: Insights from Mechanism to Application DOI Creative Commons
Ning Han, Wei Zhang, Wei Guo

et al.

Nano-Micro Letters, Journal Year: 2023, Volume and Issue: 15(1)

Published: July 29, 2023

Abstract The electrochemical oxygen reduction reaction (ORR) and evolution (OER) are fundamental processes in a range of energy conversion devices such as fuel cells metal–air batteries. ORR OER both have significant activation barriers, which severely limit the overall performance that utilize ORR/OER. Meanwhile, is another very important involving has been widely investigated. occurs aqueous solutions via two pathways: direct 4-electron or 2-electron pathways from O 2 to water (H O) hydrogen peroxide ). Noble metal electrocatalysts often used catalyze ORR, despite fact noble certain intrinsic limitations, low storage. Thus, it urgent develop more active stable low-cost electrocatalysts, especially for severe environments (e.g., acidic media). Theoretically, an ideal electrocatalyst should provide adequate binding species. Transition metals not belonging platinum group metal-based oxides substance could give d orbital species binding. As result, transition regarded substitute typical precious electrocatalysts. However, development oxide catalysts reactions still faces challenges, e.g., catalytic activity, stability, cost, mechanism. We discuss principles underlying design catalysts, including influence crystal structure, electronic structure on their performance. also challenges associated with developing potential strategies overcome these challenges.

Language: Английский

Citations

73
Coordination engineering in single-site catalysts: General principles, characterizations, and recent advances DOI Creative Commons
Haozhu Wang, Tao Yang, Jingyang Wang

et al.

Chem, Journal Year: 2023, Volume and Issue: 10(1), P. 48 - 85

Published: Sept. 21, 2023

Language: Английский

Citations

70
Self-carbon-thermal-reduction strategy for boosting the Fenton-like activity of single Fe-N4 sites by carbon-defect engineering DOI Creative Commons
Shengjie Wei,

Yibing Sun,

Yun-Ze Qiu

et al.

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: Nov. 20, 2023

Carbon-defect engineering in metal single-atom catalysts by simple and robust strategy, boosting their catalytic activity, revealing the carbon defect-catalytic activity relationship are meaningful but challenging. Herein, we report a facile self-carbon-thermal-reduction strategy for carbon-defect of single Fe-N4 sites ZnO-Carbon nano-reactor, as efficient catalyst Fenton-like reaction degradation phenol. The vacancies easily constructed adjacent to during synthesis, facilitating formation C-O bonding lowering energy barrier rate-determining-step Consequently, Fe-NCv-900 with exhibits much improved than Fe-NC-900 without abundant vacancies, 13.5 times improvement first-order rate constant phenol degradation. shows high (97% removal ratio only 5 min), good recyclability wide-ranging pH universality (pH range 3-9). This work not provides rational improving catalysts, also deepens fundamental understanding on how periphery environment affects property performance metal-N4 sites.

Language: Английский

Citations

70