Engineering Dual Single‐Atom Sites on 2D Ultrathin N‐doped Carbon Nanosheets Attaining Ultra‐Low‐Temperature Zinc‐Air Battery

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(12)

Published: Jan. 7, 2022

Herein, a novel dual single-atom catalyst comprising adjacent Fe-N4 and Mn-N4 sites on 2D ultrathin N-doped carbon nanosheets with porous structure (FeMn-DSAC) was constructed as the cathode for flexible low-temperature Zn-air battery (ZAB). FeMn-DSAC exhibits remarkable bifunctional activities oxygen reduction reaction (ORR) evolution (OER). Control experiments density functional theory calculations reveal that catalytic activity arises from cooperative effect of Fe/Mn dual-sites aiding *OOH dissociation well nanosheet promoting active sits exposure mass transfer during process. The excellent enables ZAB to operate efficiently at ultra-low temperature -40 °C, delivering 30 mW cm-2 peak power retaining up 86 % specific capacity room counterpart.

Language: Английский

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Design concept for electrocatalysts

Nano Research, Journal Year: 2021, Volume and Issue: 15(3), P. 1730 - 1752

Published: Sept. 4, 2021

Language: Английский

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Understanding the structure-performance relationship of active sites at atomic scale

Nano Research, Journal Year: 2022, Volume and Issue: 15(8), P. 6888 - 6923

Published: June 14, 2022

Language: Английский

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Theory-oriented screening and discovery of advanced energy transformation materials in electrocatalysis

Advanced Powder Materials, Journal Year: 2021, Volume and Issue: 1(1), P. 100013 - 100013

Published: Nov. 15, 2021

Various metal-based electrocatalysts from nanocrystals, to clusters and single-atoms, have been well-discovered towards high-efficient power devices electrocatalytic conversion. To accelerate energy transformation materials discovery, developing high-throughput DFT calculations machine-learning techniques is of great necessity. This review comprehensively outlines the latest progress theory-guided design advanced materials. Especially, we focus on study single atoms in various devices, such as fuel cell (oxygen reduction reaction, ORR; acid oxidation reaction; alcohol reaction), other reactions for energy-related conversion small molecules, H2O2 evolution (2e− ORR), water splitting (H2 reaction/O2 HER/OER), N2 reaction (NRR), CO2 (CO2RR). Firstly, electronic structure, interaction mechanism, activation path are discussed provide an overall blueprint electrocatalysis batteries mentioned above. Thereafter, experimental synthesis strategies, structural recognition, performance figured out. Finally, some viewpoints into current issues future concept provided.

Language: Английский

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Superiority of Dual‐Atom Catalysts in Electrocatalysis: One Step Further Than Single‐Atom Catalysts

Advanced Energy Materials, Journal Year: 2022, Volume and Issue: 12(9)

Published: Jan. 18, 2022

Abstract In recent years, dual‐atom catalysts (DACs) have attracted extensive attention, as an extension of single‐atom (SACs). Compared with SACs, DACs higher metal loading and more complex flexible active sites, thus achieving better catalytic performance providing opportunities for electrocatalysis. This review introduces the research progress in years on how to design new enhance Firstly, advantages increasing are introduced. Then, role changing adsorption condition reactant molecules atoms is discussed. Moreover, ways which can reduce reaction energy barrier key steps change path explored. Catalytic applications different electrocatalytic reactions, including carbon dioxide reduction reaction, oxygen evolution hydrogen nitrogen followed. Finally, a brief summary made challenges prospects

Language: Английский

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Iron atom–cluster interactions increase activity and improve durability in Fe–N–C fuel cells

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: May 26, 2022

Simultaneously increasing the activity and stability of single-atom active sites M-N-C catalysts is critical but remains a great challenge. Here, we report an Fe-N-C catalyst with nitrogen-coordinated iron clusters closely surrounding Fe-N4 for oxygen reduction reaction in acidic fuel cells. A strong electronic interaction built between satellite due to unblocked electron transfer pathways very short interacting distances. The optimize adsorption strength intermediates on also shorten bond amplitude incoherent vibrations. As result, both are increased by about 60% terms turnover frequency demetalation resistance. This work shows potential interactions multiphase metal species improvements catalysts.

Language: Английский

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Regulations of active moiety in single atom catalysts for electrochemical hydrogen evolution reaction

Nano Research, Journal Year: 2022, Volume and Issue: 15(7), P. 5792 - 5815

Published: May 4, 2022

Language: Английский

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Single‐Atom Fe Catalysts for Fenton‐Like Reactions: Roles of Different N Species

Advanced Materials, Journal Year: 2022, Volume and Issue: 34(17)

Published: March 8, 2022

Recognizing and controlling the structure-activity relationships of single-atom catalysts (SACs) is vital for manipulating their catalytic properties various practical applications. Herein, Fe SACs supported on nitrogen-doped carbon (SA-Fe/CN) are reported, which show high reactivity (97% degradation bisphenol A in only 5 min), stability (80% maintained after five runs), wide pH suitability (working range 3-11) toward Fenton-like reactions. The roles different N species these reactions further explored, both experimentally theoretically. It discovered that graphitic an adsorptive site target molecule, pyrrolic coordinates with Fe(III) plays a dominant role reaction, pyridinic N, coordinated Fe(II), minor contributor to SA-Fe/CN. Density functional theory (DFT) calculations reveal lower d-band center location pyrrolic-type sites leads easy generation Fe-oxo intermediates, thus, excellent properties.

Language: Английский

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Emerging low-nuclearity supported metal catalysts with atomic level precision for efficient heterogeneous catalysis

Nano Research, Journal Year: 2022, Volume and Issue: 15(9), P. 7806 - 7839

Published: June 2, 2022

Language: Английский

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Quasi-solid-state Zn-air batteries with an atomically dispersed cobalt electrocatalyst and organohydrogel electrolyte

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: June 27, 2022

Abstract Quasi-solid-state Zn-air batteries are usually limited to relatively low-rate ability (<10 mA cm −2 ), which is caused in part by sluggish oxygen electrocatalysis and unstable electrochemical interfaces. Here we present a high-rate robust quasi-solid-state battery enabled atomically dispersed cobalt sites anchored on wrinkled nitrogen doped graphene as the air cathode polyacrylamide organohydrogel electrolyte with its hydrogen-bond network modified addition of dimethyl sulfoxide. This design enables cycling current density 100 over 50 h at 25 °C. A low-temperature stability 300 (at 0.5 ) 90% capacity retention −60 °C broad temperature adaptability (−60 60 °C) also demonstrated.

Language: Английский

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