Regulating the Local Electronic Structure of Copper Single Atoms with Unsaturated B,O-Coordination for Selective ¹O₂ Generation

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(18), P. 12414 - 12424

Published: Sept. 7, 2023

Generating singlet oxygen (1O2) on single atom catalysts (SACs) in peroxymonosulfate (PMS)-based Fenton-like reactions exhibits great potential for selective degradation of contaminants complex wastewater. Clarifying the structure–activity relationship between electronic structure SACs and 1O2 generation selectivity is crucial precise design efficient catalysts, but it challenging. Herein, Cu with different structures (namely, Cu–O2X, where X = N, S, B, P, O) investigated by density functional theory calculations using adsorption terminal atoms PMS as an activity descriptor. Significantly, affected center which electron-depleted Cu-O2B site a higher atoms. Experimentally, moiety superior catalytic activation, showing nearly 100% ciprofloxacin rate 0.2250 min–1, outperforming those other counterparts. The high attributed to asymmetric accelerating faster electron transfer O–O bond stretching, lowering energy barrier key intermediates toward generation. This work provides broader perspective regulating sites at atomic level catalysts.

Language: Английский

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Rechargeable Metal-Sulfur Batteries: Key Materials to Mechanisms

Chemical Reviews, Journal Year: 2024, Volume and Issue: 124(8), P. 4935 - 5118

Published: April 10, 2024

Rechargeable metal-sulfur batteries are considered promising candidates for energy storage due to their high density along with natural abundance and low cost of raw materials. However, they could not yet be practically implemented several key challenges: (i) poor conductivity sulfur the discharge product metal sulfide, causing sluggish redox kinetics, (ii) polysulfide shuttling, (iii) parasitic side reactions between electrolyte anode. To overcome these obstacles, numerous strategies have been explored, including modifications cathode, anode, electrolyte, binder. In this review, fundamental principles challenges first discussed. Second, latest research on is presented discussed, covering material design, synthesis methods, electrochemical performances. Third, emerging advanced characterization techniques that reveal working mechanisms highlighted. Finally, possible future directions practical applications This comprehensive review aims provide experimental theoretical guidance designing understanding intricacies batteries; thus, it can illuminate pathways progressing high-energy-density battery systems.

Language: Английский

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Electrocatalytic nitrate-to-ammonia conversion on CoO/CuO nanoarrays using Zn–nitrate batteries

Nanoscale, Journal Year: 2023, Volume and Issue: 15(48), P. 19577 - 19585

Published: Jan. 1, 2023

Zn-NO3- batteries can generate electricity while producing NH3 in an environmentally friendly manner, making them a very promising device. However, the conversion of NO3- to involves proton-assisted 8-electron (8e-) transfer process with high kinetic barrier, requiring high-performance catalysts realize potential applications this technology. Herein, we propose heterostructured CoO/CuO nanoarray electrocatalyst prepared on copper foam (CoO/CuO-NA/CF) that electrocatalytically and efficiently convert at low achieves maximum yield 296.9 μmol h-1 cm-2 Faraday efficiency (FE) 92.9% -0.2 V vs. reversible hydrogen electrode (RHE). Impressively, battery based monolithic CoO/CuO-NA/CF delivers 60.3 cm-2, FENH3 82.0%, power density 4.3 mW cm-2. This study provides paradigm for catalyst preparation energy-efficient production simultaneously generating electrical energy.

Language: Английский

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Engineering d‐p Orbital Hybridization with P, S Co‐Coordination Asymmetric Configuration of Single Atoms Toward High‐Rate and Long‐Cycling Lithium–Sulfur Battery

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(38)

Published: Aug. 1, 2024

Abstract Single‐atom catalysts (SACs) have been increasingly explored in lithium–sulfur (Li–S) batteries to address the issues of severe polysulfide shuttle effects and sluggish redox kinetics. However, structure‐activity relationship between single‐atom coordination structures performance Li–S remain unclear. In this study, a P, S co‐coordination asymmetric configuration single atoms is designed enhance catalytic activity Co central promote d‐p orbital hybridization atoms, thereby limiting polysulfides accelerating bidirectional process sulfur. The well‐designed SACs enable demonstrate an ultralow capacity fading rate 0.027% per cycle after 2000 cycles at high 5 C. Furthermore, they display excellent with 619 mAh g −1 ultrahigh 10 C due efficient catalysis CoSA‐N 3 PS. Importantly, assembled pouch cell still retains discharge 660 100 0.2 provides areal 4.4 cm −2 even sulfur loading 6 mg . This work demonstrates that regulating environment great significance for achieving state‐of‐the‐art batteries.

Language: Английский

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Green synthesis and applications of MXene for lithium–sulfur batteries

Energy storage materials, Journal Year: 2024, Volume and Issue: 67, P. 103257 - 103257

Published: Feb. 11, 2024

Language: Английский

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Single Atom Catalysts Based on Earth-Abundant Metals for Energy-Related Applications

Chemical Reviews, Journal Year: 2024, Volume and Issue: 124(21), P. 11767 - 11847

Published: July 5, 2024

Anthropogenic activities related to population growth, economic development, technological advances, and changes in lifestyle climate patterns result a continuous increase energy consumption. At the same time, rare metal elements frequently deployed as catalysts processes are not only costly view of their low natural abundance, but availability is often further limited due geopolitical reasons. Thus, electrochemical storage conversion with earth-abundant metals, mainly form single-atom (SACs), highly relevant timely technologies. In this review application SACs electrocatalytic chemicals fuels or products high content discussed. The oxygen reduction reaction also appraised, which primarily harnessed fuel cell technologies metal-air batteries. coordination, active sites, mechanistic aspects transition analyzed for two-electron four-electron pathways. Further, water splitting toward green hydrogen discussed terms evolution reaction. Similarly, production ammonia clean via nitrogen portrayed, highlighting potential single species.

Language: Английский

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Three Birds with One Stone: Multifunctional TiN‐MXene‐Co@CNTs Network as Sulfur/Lithium Host for High‐Areal‐Capacity Lithium‐Sulfur Batteries

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(35)

Published: June 13, 2024

Abstract The inevitable shuttling and slow redox kinetics of lithium polysulfides (LiPSs) as well the uncontrolled growth Li dendrites have strongly limited practical applications lithium‐sulfur batteries (LSBs). To address these issues, we innovatively constructed carbon nanotubes (CNTs) encapsulated Co nanoparticles in situ grown on TiN‐MXene nanosheets, denoted TiN‐MXene‐Co@CNTs, which could serve simultaneously both sulfur/Li host to kill “three birds with one stone” (1) efficiently capture soluble LiPSs expedite their conversion, (2) accelerate nucleation/decomposition solid 2 S, (3) induce homogeneous deposition. Benefiting from synergistic effects, TiN‐MXene‐Co@CNTs/S cathode a sulfur loading 2.5 mg cm −2 show high reversible specific capacity 1129.1 mAh g −1 after 100 cycles at 0.1 C, ultralong cycle life over 1000 1.0 C. More importantly, it even achieves areal 6.3 50 under 8.9 low E/S ratio 5.0 μL . Besides, TiN‐MXene‐Co@CNTs deliver stable plating/striping behavior h.

Language: Английский

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Recent Progress and Challenge in Metal–Organic Frameworks for Lithium–Sulfur Battery Separators

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: June 4, 2024

Abstract The separators used in lithium‐sulfur (Li–S) batteries play a crucial role their cycling performance and safety. Current commercial lack the ability to efficiently regulate polysulfide shuttling are prone thermal runaway at high temperatures. Recent studies have shown that multifunctional can boost electrochemical safety of Li–S batteries. Metal–organic frameworks (MOFs) emerged as promising materials for modifying due large specific surface areas highly ordered tunable nanopores. Herein, this review focuses on advancements developing MOFs, derivatives, MOFs‐based composites separator coatings address shortcomings mechanisms behind these modified separators, designed inhibit lithium dendrite growth, discussed, emphasizing relationship between structure performance. impact battery is also explored, aiming design suitable composite films high‐safety Furthermore, future perspectives outlined guide practical applications overcome remaining challenges associated with MOFs‐modified separators.

Language: Английский

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Heteroatoms Modulate the Copper Single Atom Catalytic Host Materials for Promoting the Redox Reaction in Aqueous Zinc‐Selenium Batteries

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 18, 2024

Abstract Aqueous zinc‐selenium (Zn‐Se) batteries have garnered much attention due to their inherent safety and high specific capacity. Unfortunately, the problem of sluggish redox reaction represents a significant obstacle development aqueous Zn‐Se batteries. Here, nitrogen‐phosphorus asymmetrically coordinated copper single atom catalytic host material (CuN 3 P 1 @C) is synthesized for an battery. The CuN @C exhibits rich porous structure, high‐loading Cu atoms, unique asymmetric coordination environment, which significantly reduces energy barrier between Se Zn, enhancing electrochemical performance Consequently, Se/CuN cathode achieves capacity 756 mAh g −1 at 0.2 A cycling stability 4 000 cycles 5.0 (capacity decay 0.0044% per cycle). Meanwhile, conversion mechanism battery systematically explored via systematical characteristics density functional theory calculations. This work opens up novel approach boosting by modulating atom‐based materials heteroatoms.

Language: Английский

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Applications and Perspectives of Ti3C2Tx MXene in Electrochemical Energy Storage Systems

International Journal of Electrochemical Science, Journal Year: 2025, Volume and Issue: unknown, P. 100948 - 100948

Published: Jan. 1, 2025

Language: Английский

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