Modulating Electronic Structures of Iron Clusters through Orbital Rehybridization by Adjacent Single Copper Sites for Efficient Oxygen Reduction DOI Open Access

Chunhong Qi,

Haoyu Yang, Ziqi Sun

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(39)

Published: July 24, 2023

The atom-cluster interaction has recently been exploited as an effective way to increase the performance of metal-nitrogen-carbon catalysts for oxygen reduction reaction (ORR). However, rational design such and understanding their structure-property correlations remain a great challenge. Herein, we demonstrate that introduction adjacent metal (M)-N4 single atoms (SAs) could significantly improve ORR well-screened Fe atomic cluster (AC) catalyst by combining density functional theory (DFT) calculations experimental analysis. DFT studies suggest Cu-N4 SAs act modulator assist O2 adsorption cleavage O-O bond on AC active center, well optimize release OH* intermediates accelerate whole kinetic. depositing with nitrogen doped mesoporous carbon nanosheet are then constructed through universal interfacial monomicelles assembly strategy. Consistent theoretical predictions, resultant exhibits outstanding half-wave potential 0.92 eV in alkali 0.80 acid, high power 214.8 mW cm-2 zinc air battery. This work provides novel strategy precisely tuning atomically dispersed poly-metallic centers electrocatalysis.

Language: Английский

Understanding the Catalytic Kinetics of Polysulfide Redox Reactions on Transition Metal Compounds in Li–S Batteries DOI
Jiao Wu, Tong Ye, Yuchao Wang

et al.

ACS Nano, Journal Year: 2022, Volume and Issue: 16(10), P. 15734 - 15759

Published: Oct. 12, 2022

Because of their high energy density, low cost, and environmental friendliness, lithium–sulfur (Li–S) batteries are one the potential candidates for next-generation energy-storage devices. However, they have been troubled by sluggish reaction kinetics insoluble Li2S product capacity degradation because severe shuttle effect polysulfides. These problems overcome introducing transition metal compounds (TMCs) as catalysts into interlayer modified separator or sulfur host. This review first introduces mechanism redox reactions. The methods studying TMC in Li–S provided. Then, recent advances TMCs (such oxides, sulfides, selenides, nitrides, phosphides, carbides, borides, heterostructures) some helpful design modulation strategies highlighted summarized. At last, future opportunities toward presented.

Language: Английский

Citations

235

Synergistic Fe−Se Atom Pairs as Bifunctional Oxygen Electrocatalysts Boost Low‐Temperature Rechargeable Zn‐Air Battery DOI
Yao Wang, Jiao Wu, Shuaihao Tang

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(15)

Published: Feb. 18, 2023

Herein, we successfully construct bifunctional electrocatalysts by synthesizing atomically dispersed Fe-Se atom pairs supported on N-doped carbon (Fe-Se/NC). The obtained Fe-Se/NC shows a noteworthy oxygen catalytic performance with low potential difference of 0.698 V, far superior to that reported Fe-based single-atom catalysts. theoretical calculations reveal p-d orbital hybridization around the leads remarkably asymmetrical polarized charge distributions. based solid-state rechargeable Zn-air batteries (ZABs-Fe-Se/NC) present stable charge/discharge 200 h (1090 cycles) at 20 mA cm-2 25 °C, which is 6.9 times ZABs-Pt/C+Ir/C. At extremely temperature -40 ZABs-Fe-Se/NC displays an ultra-robust cycling 741 (4041 1 , about 11.7 More importantly, could be operated for 133 (725 even 5 °C.

Language: Английский

Citations

206

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

190

Advanced polymer-based electrolytes in zinc–air batteries DOI Creative Commons
Qingqing Liu, Ruiting Liu, Chaohui He

et al.

eScience, Journal Year: 2022, Volume and Issue: 2(5), P. 453 - 466

Published: Sept. 1, 2022

Zinc–air batteries (ZABs) are expected to be some of the most promising power sources for wearable and portable electronic devices have received widespread research interest. As an ion conductor connecting anodes cathodes, electrolyte is critical overall performance ZABs (e.g., energy density, rechargeability, operating voltage). Compared with liquid electrolytes, polymer-based electrolytes superior characteristics ZABs, such as negligible leakage, three-phase interface stabilization, dendrite suppression. In this perspective, we focus on recent progress in ZABs. After a brief introduction emphasize development terms their intrinsic properties interfacial chemistry. Finally, challenges viable strategies proposed We hope that work will provide useful guidance spur high-performance based advanced electrolytes.

Language: Английский

Citations

154

Polyhydroxylated Organic Molecular Additives for Durable Aqueous Zinc Battery DOI Open Access
Huan Liu,

Zijun Xin,

Bin Cao

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 34(4)

Published: Sept. 27, 2023

Abstract The large‐scale deployment of aqueous Zn‐ion batteries is hindered by Zn anode instability including surface corrosion, hydrogen gas evolution, and irregular deposition. To tackle these challenges, a polyhydroxylated organic molecular additive, trehalose, incorporated to refine the solvation structure promote planar Within regions involving hydroxy groups participate in reconstruction bond networks, which increases overpotential for water decomposition reaction. Moreover, at metal–molecule interface, chemisorption trehalose onto zinc enhances corrosion resistance facilitates deposition manner. optimized electrolyte significantly improves striping/plating reversibility maintains stable potentials over 1600 h 5 mA cm −2 with cutoff capacity 1 symmetric cells. When combined MnO 2 cathode, assembled coin cell retains ≈89% its after 1000 cycles. This molecule emphasizing role molecules fine‐tuning structures anode/electrolyte interfaces, holds promise enhancing various metal batteries.

Language: Английский

Citations

134

Construction of Catalytic Covalent Organic Frameworks with Redox‐Active Sites for the Oxygen Reduction and the Oxygen Evolution Reaction DOI
Minghao Liu, Sijia Liu, Cheng‐Xing Cui

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(49)

Published: Oct. 14, 2022

Construction of catalytic covalent organic frameworks (COFs) for oxygen reduction reaction (ORR) and evolution (OER) is significant but rarely demonstrated. In this work, we have first constructed bifunctional COFs towards ORR OER by integrating diarylamine derivatives into the Co-porphyrin based frameworks. Both new (CoTAPP-PATA-COF CoTAPP-BDTA-COF) good ordered structures, high surface areas, robust chemical stability. The units, as a typical electron donor redox-active cores, promote intramolecular transport along improve electrochemically active areas. Thus, showed higher activities than that COF without units. CoTAPP-PATA-COF had halfwave potential 0.80 V ORR, delieved an overpotential 420 mV in 0.1 M KOH. theoretical calculation revealed introducing unites improved electrocatalysis.

Language: Английский

Citations

126

N,O symmetric double coordination of an unsaturated Fe single-atom confined within a graphene framework for extraordinarily boosting oxygen reduction in Zn–air batteries DOI
Yuejiao Li, Yajun Ding, Bo Zhang

et al.

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(6), P. 2629 - 2636

Published: Jan. 1, 2023

A novel N,O symmetric double-coordinated configuration of unsaturated Fe single atoms confirmed within a graphene framework (Fe–N,O/G) is demonstrated experimentally and theoretically for highly active durable ORR catalyst in Zn-air batteries.

Language: Английский

Citations

109

Dual‐Sites Coordination Engineering of Single Atom Catalysts for Full‐Temperature Adaptive Flexible Ultralong‐Life Solid‐State Zn−Air Batteries DOI

Tengteng Gu,

Dantong Zhang,

Yan Yang

et al.

Advanced Functional Materials, Journal Year: 2022, Volume and Issue: 33(8)

Published: Dec. 14, 2022

Abstract High‐performance rechargeable Zn‐air batteries with long‐life stability are desirable for power applications in electric vehicles. The key component of the is bifunctional oxygen electrocatalyst, however, designing a electrocatalyst high intrinsic reversibility and durability challenge. Through density functional theory calculations, it found that catalytic activity originated from electronic geometric coordination structures synergistic effect Fe Co dual‐sites metal‐N 4 environment, assisting stronger hybridization orbitals between ( dxz, dz 2 ) OO* px, pz ), thus making O active ability site. These findings enable to development fancy dual single‐atom catalyst comprising adjacent FeN CoN sites on N‐doped carbon matrix (FeCo‐NC). FeCo‐NC exhibits extraordinary activities reduction evolution reaction (ORR/OER), which displays half‐wave potential (0.893 V) ORR, low overpotential (343 mV) at 10 mA cm −2 OER. assembled air‐electrode works well flexible solid‐state battery specific capacity 747.0 mAh g −1 , long‐time more than 400 h (30 °C), also superior performance extreme temperatures (−30 °C–60 °C).

Language: Английский

Citations

105

Altering the spin state of Fe-N-C through ligand field modulation of single-atom sites boosts the oxygen reduction reaction DOI

Dongping Xue,

Pengfei Yuan, Su Jiang

et al.

Nano Energy, Journal Year: 2022, Volume and Issue: 105, P. 108020 - 108020

Published: Nov. 21, 2022

Language: Английский

Citations

104

Dual‐Network Structured Hydrogel Electrolytes Engaged Solid‐State Rechargeable Zn‐Air/Iodide Hybrid Batteries DOI
Qingqing Liu,

Chenfeng Xia,

Chaohui He

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(44)

Published: Sept. 12, 2022

As a key component of batteries, the electrolyte determines ion transport and interface chemistry cathode anode. In this work, we develop dual-network structured hydrogel composed polyacrylamide (PAM), sodium alginate (SA) potassium iodide (KI) for solid-state zinc-air/iodide hybrid batteries. The assembled battery shows excellent renewability long cycling life 110 h with high energy efficiency 80 %. ion-crosslinked structure endows material improved mechanical strength increased ionic conductivity. More importantly, introduction iodine species not only offers more favorable cathodic kinetics iodide/iodate redox than oxygen electrocatalysis but also regulates solvation zinc ions to ensure better stability. This work provides significant concepts developing novel electrolytes realize high-performance devices technologies.

Language: Английский

Citations

96