Identification of Dynamic Active Sites Among Cu Species Derived from MOFs@CuPc for Electrocatalytic Nitrate Reduction Reaction to Ammonia

Nano-Micro Letters, Journal Year: 2023, Volume and Issue: 15(1)

Published: April 30, 2023

Direct electrochemical nitrate reduction reaction (NITRR) is a promising strategy to alleviate the unbalanced nitrogen cycle while achieving electrosynthesis of ammonia. However, restructuration high-activity Cu-based electrocatalysts in NITRR process has hindered identification dynamical active sites and in-depth investigation catalytic mechanism. Herein, Cu species (single-atom, clusters, nanoparticles) with tunable loading supported on N-doped TiO2/C are successfully manufactured MOFs@CuPc precursors via pre-anchor post-pyrolysis strategy. Restructuration behavior among co-dependent potential, as evidenced by advanced operando X-ray absorption spectroscopy, there exists an incompletely reversible transformation restructured structure initial state. Notably, CuN4&Cu4 deliver high NH3 yield 88.2 mmol h-1 gcata-1 FE (~ 94.3%) at - 0.75 V, resulting from optimal adsorption NO3- well rapid conversion *NH2OH *NH2 intermediates originated modulation charge distribution d-band center for site. This work not only uncovers have but also identifies dynamic that play critical role efficient electrocatalytic

Language: Английский

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Decade Milestone Advancement of Defect-Engineered g-C3N4 for Solar Catalytic Applications

Nano-Micro Letters, Journal Year: 2024, Volume and Issue: 16(1)

Published: Jan. 4, 2024

Over the past decade, graphitic carbon nitride (g-C

Language: Английский

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Noble‐Metal‐Free Single‐ and Dual‐Atom Catalysts for Artificial Photosynthesis

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(22)

Published: May 13, 2023

Abstract Artificial photosynthesis enables direct solar‐to‐chemical energy conversion aimed at mitigating environmental pollution and producing solar fuels chemicals in a green sustainable approach, efficient, robust, low‐cost photocatalysts are the heart of artificial systems. As an emerging new class cocatalytic materials, single‐atom catalysts (SACs) dual‐atom (DACs) have received great deal current attention due to their maximal atom utilization unique photocatalytic properties, whereas noble‐metal‐free ones impart abundance, availability, cost‐effectiveness allowing for scalable implementation. This review outlines fundamental principles synthetic methods SACs DACs summarizes most recent advances (Co, Fe, Cu, Ni, Bi, Al, Sn, Er, La, Ba, etc.) (CuNi, FeCo, InCu, KNa, CoCo, CuCu, based on non‐noble metals, confined arsenal organic or inorganic substrates (polymeric carbon nitride, metal oxides, sulfides, metal–organic frameworks, carbon, acting as versatile scaffolds solar‐light‐driven reactions, including hydrogen evolution, dioxide reduction, methane conversion, synthesis, nitrogen fixation, peroxide production, remediation. The concludes with challenges, opportunities, future prospects photosynthesis.

Language: Английский

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Improved Plasmonic Hot-Electron Capture in Au Nanoparticle/Polymeric Carbon Nitride by Pt Single Atoms for Broad-Spectrum Photocatalytic H2 Evolution

Nano-Micro Letters, Journal Year: 2023, Volume and Issue: 15(1)

Published: May 20, 2023

Rationally designing broad-spectrum photocatalysts to harvest whole visible-light region photons and enhance solar energy conversion is a "holy grail" for researchers, but still challenging issue. Herein, based on the common polymeric carbon nitride (PCN), hybrid co-catalysts system comprising plasmonic Au nanoparticles (NPs) atomically dispersed Pt single atoms (PtSAs) with different functions was constructed address this challenge. For dual decorated PCN (PtSAs-Au2.5/PCN), photoexcited generate electrons under UV short-wavelength visible light, synergetic NPs PtSAs not only accelerate charge separation transfer though Schottky junctions metal-support bond also act as H2 evolution. Furthermore, absorb long-wavelength light owing its localized surface plasmon resonance, adjacent trap hot-electrons evolution via direct electron effect. Consequently, PtSAs-Au2.5/PCN exhibits excellent photocatalytic activity rate of 8.8 mmol g-1 h-1 at 420 nm 264 μmol 550 nm, much higher than that Au2.5/PCN PtSAs-PCN, respectively. This work provides new strategy design reaction.

Language: Английский

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Single‐atom catalyst application in distributed renewable energy conversion and storage

SusMat, Journal Year: 2023, Volume and Issue: 3(2), P. 160 - 179

Published: March 2, 2023

Abstract In recent years, owing to the depletion of fossil energy and aggravation environmental pollution, conversion storage distributed renewable (such as solar energy, wind tidal energy) based on electrochemical technology have attracted extensive attention. Electrocatalytic processes with high efficiency selectivity play a key role in clean storage. With nearly 100% atomic utilization rate unique catalytic activity, single‐atom catalysts (SACs) been rapidly developed widely used field this review, we first introduce characteristics SACs. Then, focus application SACs conversion, including water electrolysis reaction, nitrogen reduction nitrate oxygen carbon dioxide reaction. terms storage, supercapacitors Li–S batteries. Further, enumerate some methods for synthesis metal loading or large scale. Finally, main challenges opportunities emerging future are discussed prospected.

Language: Английский

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Atomic-level coordination structures meet graphitic carbon nitride (g-C3N4) for photocatalysis: Energy conversion and environmental remediation

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: unknown, P. 123683 - 123683

Published: Jan. 1, 2024

Language: Английский

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Defect Engineering Simultaneously Regulating Exciton Dissociation in Carbon Nitride and Local Electron Density in Pt Single Atoms Toward Highly Efficient Photocatalytic Hydrogen Production

Small, Journal Year: 2024, Volume and Issue: 20(34)

Published: April 10, 2024

Abstract The high exciton binding energy ( E b ) and sluggish surface reaction kinetics have severely limited the photocatalytic hydrogen production activity of carbon nitride (CN). Herein, a hybrid system consisting nitrogen defects Pt single atoms is constructed through facile self‐assembly photodeposition strategy. Due to acceleration dissociation regulation local electron density along with introduction defects, optimized Pt‐MCT‐3 exhibits rate 172.0 µmol h −1 λ ≥ 420 nm), ≈41 times higher than pristine CN. apparent quantum yield for determined be 27.1% at nm. experimental characterizations theoretical calculations demonstrate that act as traps dissociation, resulting in decrease from 86.92 43.20 meV. Simultaneously, stronger interaction between neighboring directionally drives free electrons aggregate around atoms, tailors d ‐band Pt, forming moderate strength H* intermediates.

Language: Английский

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SiQDs-mediated highly efficient hole transfer for photocatalytic overall water splitting over Cu-doped ZnIn2S4

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 354, P. 124121 - 124121

Published: April 25, 2024

Language: Английский

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Bimetallic Single-Atom Catalysts for Water Splitting

Nano-Micro Letters, Journal Year: 2024, Volume and Issue: 17(1)

Published: Sept. 25, 2024

Abstract Green hydrogen from water splitting has emerged as a critical energy vector with the potential to spearhead global transition fossil fuel-independent society. The field of catalysis been revolutionized by single-atom catalysts (SACs), which exhibit unique and intricate interactions between atomically dispersed metal atoms their supports. Recently, bimetallic SACs (bimSACs) have garnered significant attention for leveraging synergistic functions two ions coordinated on appropriately designed BimSACs offer an avenue rich metal–metal metal–support cooperativity, potentially addressing current limitations in effectively furnishing transformations involve synchronous proton–electron exchanges, substrate activation reversible redox cycles, simultaneous multi-electron transfer, regulation spin states, tuning electronic properties, cyclic states low energies. This review aims encapsulate growing advancements bimSACs, emphasis pivotal role generation via splitting. We subsequently delve into advanced experimental methodologies elaborate characterization SACs, elucidate discuss local coordination environment. Overall, we present comprehensive discussion deployment bimSACs both evolution reaction oxygen reaction, half-reactions electrolysis process.

Language: Английский

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Exploring the Roles of Single Atom in Hydrogen Peroxide Photosynthesis

Nano-Micro Letters, Journal Year: 2023, Volume and Issue: 16(1)

Published: Nov. 20, 2023

This comprehensive review provides a deep exploration of the unique roles single atom catalysts (SACs) in photocatalytic hydrogen peroxide (H

Language: Английский

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