Overcome the trade-off in electro-fenton chemistry for in situ H2O2 generation-activation by tandem CoFe bimetallic single-atom configuration DOI Creative Commons
Wenxin Sun, Yanan Zhou, Ming Liu

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 357, P. 124320 - 124320

Published: June 20, 2024

Dual-atomic catalysts (DACs) demonstrated remarkable potential in addressing key challenges electro-Fenton (EF) processes. In this study, we synthesized an EF DACs comprising both CoN4 and FeN4 sites, which was achieved a high H2O2 generation rate (1.68 mM−1h−1) 100 % bisphenol A degradation efficiency via successive two-electron oxygen reduction one-electron Fenton reactions (2e− ORR + 1e− Fenton). Our findings indicated that the single-atom nitrogen coordination of sites plays crucial roles regulating adsorption intermediates *OOH *H2O2. The bimetallic independently regulated binding energies on (pyrrole-type) for favorable its subsequent activation adjacent (pyridine-type). Thus, dual-site engineering addresses trade-off situ generation-activation chemistry, realizing electron utilization fast pollutant toward efficient sustainable water treatment.

Language: Английский

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

205
Geometric and Electronic Engineering of Atomically Dispersed Copper‐Cobalt Diatomic Sites for Synergistic Promotion of Bifunctional Oxygen Electrocatalysis in Zinc–Air Batteries DOI
Zhijun Li, Siqi Ji, Chun Wang

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(25)

Published: April 11, 2023

The development of rechargeable zinc-air batteries is heavily dependent on bifunctional oxygen electrocatalysts to offer exceptional reduction/evolution reaction (ORR/OER) activities. However, the design such with high activity and durability challenging. Herein, a strategy proposed create an electrocatalyst comprised copper-cobalt diatomic sites highly porous nitrogen-doped carbon matrix (Cu-Co/NC) abundantly accessible metal optimal geometric electronic structures. Experimental findings theoretical calculations demonstrate that synergistic effect Cu-Co dual-metal metal-N4 coordination induce asymmetric charge distributions moderate adsorption/desorption behavior intermediates. This exhibits extraordinary electrocatalytic activities in alkaline media, half-wave potential 0.92 V for ORR low overpotential 335 mV at 10 mA cm-2 OER. In addition, it demonstrates acidic (0.85 V) neutral (0.74 media. When applied battery, achieves operational performance outstanding (510 h), ranking as one most efficient reported date. work importance engineering isolated boosting electrochemical energy devices.

Language: Английский

Citations

152
A CrMnFeCoNi high entropy alloy boosting oxygen evolution/reduction reactions and zinc-air battery performance DOI
Ren He, Linlin Yang, Yu Zhang

et al.

Energy storage materials, Journal Year: 2023, Volume and Issue: 58, P. 287 - 298

Published: March 21, 2023

Language: Английский

Citations

88
Cooperation between Dual Metal Atoms and Nanoclusters Enhances Activity and Stability for Oxygen Reduction and Evolution DOI
Zhe Wang, Xiaoyan Jin,

Ruojie Xu

et al.

ACS Nano, Journal Year: 2023, Volume and Issue: 17(9), P. 8622 - 8633

Published: April 27, 2023

We have achieved the synthesis of dual-metal single atoms and atomic clusters that co-anchor on a highly graphitic carbon support. The catalyst comprises Ni4 (and Fe4) nanoclusters located adjacent to corresponding NiN4 FeN4) single-atom sites, which is verified by systematic X-ray absorption characterization density functional theory calculations. A distinct cooperation between Fe4 (Ni4) FeN4 (NiN4) sites optimizes adsorption energy reaction intermediates reduces barrier potential-determining steps. This exhibits enhanced oxygen reduction evolution activity long-cycle stability compared counterparts without commercial Pt/C. fabricated Zn-air batteries deliver high power long-term cyclability, demonstrating their prospects in storage device applications.

Language: Английский

Citations

84
Optimizing electronic synergy of atomically dispersed dual-metal Ni–N4 and Fe–N4 sites with adjacent Fe nanoclusters for high-efficiency oxygen electrocatalysis DOI
Haibing Meng, Bin Wu, Dantong Zhang

et al.

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 17(2), P. 704 - 716

Published: Dec. 7, 2023

The electronic synergy of Fe nanoclusters and Ni/Fe–N 4 single-atomic sites optimizes the adsorption/desorption oxygenated intermediates reduces energy barrier oxygen electrocatalysis, boosting Zn–air batteries performance.

Language: Английский

Citations

74
Electronic modulation induced by decorating single-atomic Fe-Co pairs with Fe-Co alloy clusters toward enhanced ORR/OER activity DOI Open Access
Ping Li,

Fuqiang Qiang,

Xuehai Tan

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 340, P. 123231 - 123231

Published: Aug. 29, 2023

Language: Английский

Citations

63
Electrolyte Tuned Robust Interface toward Fast‐Charging Zn–Air Battery with Atomic Mo Site Catalyst DOI
Qichen Wang, Shuaihao Tang,

Zhiqiang Wang

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(47)

Published: Sept. 3, 2023

Abstract Stable operation of sustainable Zn–air batteries (ZABs) has attracted considerable attention, but it remains a huge challenge to achieve temperature‐adaptive and fast‐charging ZABs. The poor Zn | electrolyte interface the sluggish charging kinetic are major obstacles. Here, high‐performance ZABs constructed by designing polarized zincophilic solid‐state (SSE) with unique solvation interaction 2+ ethylene glycol (EG), atomic Mo site cathode catalyst. On one hand, modulation structure ions partial substitution H 2 O EG inhibits dendrite growth parasitic reactions, leading improvement interface. Moreover, terminal groups in SSE strongly coordinated Zn/H O, which exerts profound influence on stability low‐temperature properties. other incorporated α‐Co(OH) mesoporous nanosheets decrease overpotential oxygen evolution reaction via strong electronic interaction. Consequently, assembled aqueous exhibit ten‐time ability remarkable cycling stability. show unprecedented (1400 cycles at 5 mA cm −2 ) high energy efficiency −40 °C.

Language: Английский

Citations

55
D‐Orbital Manipulated Ru Nanoclusters for High‐Efficiency Overall Water Splitting at Industrial‐Level Current Densities DOI
Chenfei Zhao, Jing Wang, Ya Gao

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 34(7)

Published: Oct. 30, 2023

Abstract Owing to the Pt‐like electrocatalytic capability and moderate price, Ru‐based catalysts are considered as Pt alternatives for electrochemical water splitting. However, they demonstrate limited catalytic performance under industrial‐level current densities. Herein, a novel electrocatalyst with an extremely low amount (0.85 wt.%) of Ru nanoclusters anchored on Cr‐doped Fe‐metal–organic frameworks (Ru@Cr─FeMOF) through robust Cr─O─Ru bond is presented. The study unveils that such architecture facilitates fast electron transfer manipulates highest occupied d orbital d‐band centers sites, favoring both oxygen evolution reaction (OER) hydrogen (HER) catalysis. as‐prepared catalyst performs excellent activity 21 mV@10 mA cm −2 HER 230 mV@50 OER in alkaline solution, realizes water‐splitting at densities (1.72 V@1000 ), surpassing state‐of‐the‐art literatures.

Language: Английский

Citations

55
Advanced Architectures of Air Electrodes in Zinc–Air Batteries and Hydrogen Fuel Cells DOI Open Access

Longbin Li,

Xiannong Tang,

Bing Wu

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(13)

Published: Oct. 12, 2023

The air electrode is an essential component of air-demanding energy storage/conversion devices, such as zinc-air batteries (ZABs) and hydrogen fuel cells (HFCs), which determines the output power stability devices. Despite atom-level modulation in catalyst design being recently achieved, electrodes have received much less attention, causing a stagnation development equipment. Herein, evolution for ZABs HFCs from early stages to current requirements reviewed. In addition, operation mechanism corresponding electrocatalytic mechanisms are summarized. particular, by clarifying interfaces at different scales, several approaches improve rechargeable reviewed, including innovative structures bifunctional oxygen catalysts. Afterward, operating proton-exchange-membrane (PEMFCs) anion-exchange-membrane (AEMFCs) explained. Subsequently, strategies employed enhance efficiency membrane assembly (MEA) PEMFCs AEMFCs, respectively, highlighted discussed detail. Last, prospects considered discussing main challenges. aim this review facilitate industrialization HFCs.

Language: Английский

Citations

48
Highly Reversible Zinc‐Air Batteries at −40 °C Enabled by Anion‐Mediated Biomimetic Fat DOI Open Access

Danni Deng,

Jiao Wu, Qingguo Feng

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 34(2)

Published: Sept. 24, 2023

Abstract The wide application of portable electrical equipment, aerial vehicles, smart robotics, etc. has boosted the development advanced batteries with safety, high energy density, and environmental adaptability. Inspired by fat layer on animal bodies, biomimetic is constructed as electrolytes solid‐state zinc‐air to achieve excellent cycling performance at low temperatures. Via tailored anion‐H 2 O interaction, antifreezing gel electrolytes, multi‐performance interface compatibility, temperature adaptability, stable power supply simultaneously, build robust Zn|electrolyte interface, thus promoting uniform interfacial electric fields Zn deposition. Excellent long‐term cyclability 120 h a current density 50 mA cm −2 are exhibited 25 °C. Moreover, −40 °C, record‐long life 205 large 10 achieved.

Language: Английский

Citations

47