A Janus dual-atom catalyst for electrocatalytic oxygen reduction and evolution

Nature Synthesis, Год журнала: 2024, Номер 3(7), С. 878 - 890

Опубликована: Июнь 3, 2024

Язык: Английский

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Unlocking Bimetallic Active Centers via Heterostructure Engineering for Exceptional Phosphate Electrosorption: Internal Electric Field-Induced Electronic Structure Reconstruction

Environmental Science & Technology, Год журнала: 2023, Номер 58(4), С. 2112 - 2122

Опубликована: Дек. 26, 2023

Development of electrode materials exhibiting exceptional phosphate removal performance represents a promising strategy to mitigate eutrophication and meet ever-stricter stringent emission standards. Herein, we precisely designed novel LaCeOx heterostructure-decorated hierarchical carbon composite (L8C2PC) for high-efficiency electrosorption. This approach establishes an internal electric field within the heterostructure, where electrons transfer from Ce atoms neighboring La through superexchange interactions in La–O–Ce coordination units. The modulatory heterostructure endows positive shift d band sites increase electron density at Fermi level, promoting stronger orbital overlap binding interactions. introduction oxygen vacancies during situ nucleation process reduces kinetic barrier phosphate-ion migration supplies additional active centers. Moreover, framework ensures electrical double-layer capacitance storage interconnected ion channels. Such synergistically multiple centers grant L8C2PC with record As expected, demonstrates highest capability among reported saturation capacity 401.31 mg P g–1 dynamic 91.83 1.2 V. electrochemical system also performs well dephosphorization natural water samples low concentration that enable effluent first-class discharge standard China (0.5 L–1). study advances efficient techniques new level offers deep understanding regulates metal orbitals densities engineering.

Язык: Английский

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Salt Effect Engineering Single Fe‐N₂P₂‐Cl Sites on Interlinked Porous Carbon Nanosheets for Superior Oxygen Reduction Reaction and Zn‐Air Batteries

Advanced Science, Год журнала: 2024, Номер 11(12)

Опубликована: Янв. 15, 2024

Abstract Developing efficient metal‐nitrogen‐carbon (M‐N‐C) single‐atom catalysts for oxygen reduction reaction (ORR) is significant the widespread implementation of Zn‐air batteries, while synergic design matrix microstructure and coordination environment metal centers remains challenges. Herein, a novel salt effect‐induced strategy proposed to engineer N P coordinated atomically dispersed Fe atoms with extra‐axial Cl on interlinked porous carbon nanosheets, achieving superior catalyst (denoted as Fe‐NP‐Cl‐C) ORR batteries. The hierarchical nanosheet architecture can provide rapid mass/electron transfer channels facilitate exposure active sites. Experiments density functional theory (DFT) calculations reveal distinctive Fe‐N 2 ‐Cl sites afford significantly reduced energy barriers promoted kinetics ORR. Consequently, Fe‐NP‐Cl‐C exhibits distinguished performance half‐wave potential (E 1/2 ) 0.92 V excellent stability. Remarkably, assembled battery based delivers an extremely high peak power 260 mW cm −2 large specific capacity 812 mA h g −1 , outperforming commercial Pt/C most reported congeneric catalysts. This study offers new perspective structural optimization engineering electrocatalysis conversion devices.

Язык: Английский

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Current Status and Perspectives of Dual-Atom Catalysts Towards Sustainable Energy Utilization

Nano-Micro Letters, Год журнала: 2024, Номер 16(1)

Опубликована: Фев. 29, 2024

Abstract The exploration of sustainable energy utilization requires the implementation advanced electrochemical devices for efficient conversion and storage, which are enabled by usage cost-effective, high-performance electrocatalysts. Currently, heterogeneous atomically dispersed catalysts considered as potential candidates a wide range applications. Compared to conventional catalysts, metal atoms in carbon-based have more unsaturated coordination sites, quantum size effect, strong metal–support interactions, resulting exceptional catalytic activity. Of these, dual-atomic (DACs) attracted extensive attention due additional synergistic effect between two adjacent atoms. DACs advantages full active site exposure, high selectivity, theoretical 100% atom utilization, ability break scaling relationship adsorption free on sites. In this review, we summarize recent research advancement DACs, includes (1) comprehensive understanding synergy atomic pairs; (2) synthesis DACs; (3) characterization methods, especially aberration-corrected scanning transmission electron microscopy synchrotron spectroscopy; (4) energy-related last part focuses great catalysis small molecules, such oxygen reduction reaction, CO 2 hydrogen evolution N reaction. future challenges opportunities also raised prospective section.

Язык: Английский

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Metal−support interaction in single-atom electrocatalysts: A perspective of metal oxide supports

eScience, Год журнала: 2024, Номер 4(5), С. 100269 - 100269

Опубликована: Апрель 15, 2024

The discovery of single-atom catalysts (SACs) represents a groundbreaking advancement in the field catalysis over past decades. With in-depth exploration relevant structure-activity relationships, metal-support interaction (MSI) is widely adopted to elucidate variations electronic structure and coordination configuration atomic active sites on various kinds supports. Herein, we briefly summarize metal oxide supports for SACs fabrication, including distinctive characteristics supports, enlightening advancements support-based (MO-SACs), feasible preparation methods MO-SACs effective regulation strategies MSI effect MO-SACs. In addition, present our viewpoints outlook this stimulate rational design construction novel applied diverse renewable energy devices, while some universal suggestions are sincerely given provoke thoughtful considerations during research process.

Язык: Английский

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Overcome the trade-off in electro-fenton chemistry for in situ H2O2 generation-activation by tandem CoFe bimetallic single-atom configuration

Applied Catalysis B Environment and Energy, Год журнала: 2024, Номер 357, С. 124320 - 124320

Опубликована: Июнь 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.

Язык: Английский

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Bioinspired Homonuclear Diatomic Iron Active Site Regulation for Efficient Antifouling Osmotic Energy Conversion

Advanced Materials, Год журнала: 2024, Номер unknown

Опубликована: Сен. 28, 2024

Abstract Membrane‐based reverse electrodialysis is globally recognized as a promising technology for harnessing osmotic energy. However, its practical application greatly restricted by the poor anti‐fouling ability of existing membrane materials. Inspired structural and functional models natural cytochrome c oxidases (C O), first use atomically precise homonuclear diatomic iron composites high‐performance energy conversion membranes with excellent demonstrated. Through rational tuning atomic configuration sites, oxidase‐like activity can be precisely tailored, leading to augmentation ion throughput capacity. Composite featuring direct Fe‐Fe motif configurations embedded within cellulose nanofibers (CNF/Fe‐DACs‐P) surpass state‐of‐the‐art CNF‐based power densities ca. 6.7 W m −2 44.5‐fold enhancement in antimicrobial performance. Combined, experimental characterization density theory simulations reveal that sites metal‐metal interactions achieve ideally balanced adsorption desorption intermediates, thus realizing superior activity, enhanced ionic flux, antibacterial activity.

Язык: Английский

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Integration of Single‐Atom Catalyst with Z‐Scheme Heterojunction for Cascade Charge Transfer Enabling Highly Efficient Piezo‐Photocatalysis

Advanced Science, Год журнала: 2023, Номер 10(28)

Опубликована: Авг. 6, 2023

Piezo-assisted photocatalysis (namely, piezo-photocatalysis), which utilizes mechanical energy to modulate spatial and distribution of photogenerated charge carriers, presents a promising strategy for molecule activation reactive oxygen species (ROS) generation toward applications such as environmental remediation. However, similarly photocatalysis, piezo-photocatalysis also suffers from inferior separation utilization efficiency. Herein, Z-scheme heterojunction composed single Ag atoms-anchored polymeric carbon nitride (Ag-PCN) SnO2-x is developed efficient carrier transfer/separation both within the catalyst between surface molecules (O2 ). As revealed by dynamics analysis theoretical simulations, synergy atoms initiates cascade electron transfer Ag-PCN then O2 adsorbed on Ag. With ultrasound irradiation, polarization field generated piezoelectric hybrid further accelerates regulates pathway. result, Ag-PCN/SnO2-x efficiently activates into ·O2- , ·OH, H2 under co-excitation visible light ultrasound, are consequently utilized trigger aerobic degradation refractory antibiotic pollutants. This work provides maneuver integrating single-atom catalysts (SACs) with heterojunction.

Язык: Английский

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Recent advances of ammonia synthesis under ambient conditions over metal-organic framework based electrocatalysts

Applied Catalysis B Environment and Energy, Год журнала: 2023, Номер 340, С. 123161 - 123161

Опубликована: Авг. 10, 2023

Язык: Английский

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Flash Nitrogen‐Doped Carbon Nanotubes for Energy Storage and Conversion

Small, Год журнала: 2023, Номер 20(3)

Опубликована: Сен. 13, 2023

Abstract In recent years, nitrogen‐doped carbons show great application potentials in the fields of electrochemical energy storage and conversion. Here, ultrafast green preparation carbon nanotubes (N‐CNTs) via an efficient flash Joule heating method is reported. The precursor 1D core–shell structure CNT@polyaniline first synthesized using situ polymerization then rapidly conversed into N‐CNTs at ≈1300 K within 1 s. Electrochemical tests reveal desirable capacitive property oxygen catalytic activity optimized N‐CNT material. It delivers improved area capacitance 101.7 mF cm −2 5 mV s −1 m KOH electrolyte, assembled symmetrical supercapacitor shows density 1.03 µWh excellent cycle stability over 10 000 cycles. addition, exhibit impressive performance toward reduction reaction with a half‐wave potential 0.8 V alkaline medium, comparable to sample prepared by conventional long‐time pyrolysis method. Zn–air battery presents superior charge–discharge ability long‐term durability relative commercial Pt/C catalyst. These remarkable performances validate superiorities preparing heteroatom‐doped materials for wide applications.

Язык: Английский

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