Carbon Nitride Supported High‐Loading Fe Single‐Atom Catalyst for Activation of Peroxymonosulfate to Generate ¹O₂ with 100 % Selectivity

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(40), P. 21751 - 21755

Published: Aug. 4, 2021

Abstract Singlet oxygen ( 1 O 2 ) is an excellent active species for the selective degradation of organic pollutions. However, it difficult to achieve high efficiency and selectivity generation . In this work, we develop a graphitic carbon nitride supported Fe single‐atoms catalyst (Fe /CN) containing highly uniform Fe‐N 4 sites with loading 11.2 wt %. The /CN achieves 100 % by activating peroxymonosulfate (PMS), which shows ultrahigh p‐chlorophenol efficiency. Density functional theory calculations results demonstrate that in contrast Co Ni single‐atom sites, adsorb terminal PMS, can facilitate oxidization PMS form SO 5 .− , thereafter efficiently generate selectivity. addition, exhibits strong resistance inorganic ions, natural matter, pH value during pollutants presence PMS. This work develops novel production efficient pollutants.

Language: Английский

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Single-atom catalysts for photocatalytic energy conversion

Joule, Journal Year: 2022, Volume and Issue: 6(1), P. 92 - 133

Published: Jan. 1, 2022

Artificial photocatalytic energy conversion represents a highly intriguing strategy for solving the crisis and environmental problems by directly harvesting solar energy. The development of efficient photocatalysts is central task pushing real-world application reactions. Due to maximum atomic utilization efficiency distinct advantages outstanding catalytic activity, single-atom catalysts (SACs) have emerged as promising candidates photocatalysts. In current review, recent progresses challenges on SACs systems are presented. Fundamental principles focusing charge separation/transfer molecular adsorption/activation photocatalysis systemically explored. We outline how isolated reactive sites facilitate photogenerated electron–hole transfer promote construction photoactivation cycles. widespread adoption in diverse reactions also comprehensively introduced. By presenting these advances addressing some future with potential solutions related integral over SACs, we expect shed light forthcoming research conversion.

Language: Английский

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Rational Design of Single‐Atom Site Electrocatalysts: From Theoretical Understandings to Practical Applications

Advanced Materials, Journal Year: 2021, Volume and Issue: 33(34)

Published: July 8, 2021

Atomically dispersed metal-based electrocatalysts have attracted increasing attention due to their nearly 100% atomic utilization and excellent catalytic performance. However, current fundamental comprehension summaries reveal the underlying relationship between single-atom site (SACs) corresponding application are rarely reported. Herein, understandings intrinsic mechanisms SACs electrocatalytic applications systemically summarized. Different preparation strategies presented synthetic with engineering well-defined on basis of theoretical principle (size effect, metal-support interactions, electronic structure coordination environment effect). Then, an overview is presented, including oxygen reduction reaction, hydrogen evolution oxidation small organic molecules, carbon dioxide nitrogen reaction. The structure-performance reactions also discussed in depth expound enhancement mechanisms. Finally, a summary provided perspective supplied demonstrate challenges opportunities for rational designing, synthesizing, modulating advanced toward reactions.

Language: Английский

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Defective g-C3N4/covalent organic framework van der Waals heterojunction toward highly efficient S-scheme CO2 photoreduction

Applied Catalysis B Environment and Energy, Journal Year: 2021, Volume and Issue: 301, P. 120814 - 120814

Published: Oct. 14, 2021

Language: Английский

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Selective photocatalytic CO2 reduction in aerobic environment by microporous Pd-porphyrin-based polymers coated hollow TiO2

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

Published: March 17, 2022

Abstract Direct photocatalytic CO 2 reduction from primary sources, such as flue gas and air, into fuels, is highly desired, but the thermodynamically favored O almost completely impedes this process. Herein, we report on efficacy of a composite photocatalyst prepared by hyper-crosslinking porphyrin-based polymers hollow TiO surface subsequent coordinating with Pd(II). Such exhibits high resistance against inhibition, leading to 12% conversion yield air after 2-h UV-visible light irradiation. In contrast, over Pd/TiO without polymer severely inhibited presence ( ≥ 0.2 %). This study presents feasible strategy, building Pd(II) sites -adsorptive surface, for realizing H in an aerobic environment /O adsorption selectivity efficient charge separation oxidation , respectively.

Language: Английский

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Atomically Dispersed Indium‐Copper Dual‐Metal Active Sites Promoting C−C Coupling for CO₂ Photoreduction to Ethanol

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(40)

Published: Aug. 10, 2022

Photoreduction of CO2 to C2+ solar fuel is a promising carbon-neutral technology for renewable energy. This strategy challenged by its low productivity due efficiency in multielectron utilization and slow C-C coupling kinetics. work reports dual-metal photocatalyst consisting atomically dispersed indium copper anchored on polymeric carbon nitride (InCu/PCN), which the photoreduction delivered an excellent ethanol production rate 28.5 μmol g-1 h-1 with high selectivity 92 %. Coupled experimental investigation DFT calculations reveal following mechanisms underpinning performance this catalyst. Essentially, In-Cu interaction enhances charge separation accelerating transfer from PCN metal sites. Indium also transfers electrons neighboring via Cu-N-In bridges, increasing electron density active Furthermore, sites promote adsorption *CO intermediates lower energy barrier coupling.

Language: Английский

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Electronically and Geometrically Modified Single‐Atom Fe Sites by Adjacent Fe Nanoparticles for Enhanced Oxygen Reduction

Advanced Materials, Journal Year: 2021, Volume and Issue: 34(5)

Published: Nov. 19, 2021

Fe-N-C materials exhibit excellent activity and stability for oxygen reduction reaction (ORR), as one of the most promising candidates to replace commercial Pt/C catalysts. However, it is challenging unravel features superior ORR originating from materials. In this work, electronic geometric structures isolated sites their correlations with performance are investigated by varying secondary thermal activation temperature a rationally designed NC-supported Fe single-atom catalyst (SAC). The systematic analyses demonstrate significant role coordinated atoms SA metallic nanoparticles (NPs) in altering structure sites. Meanwhile, strong interaction between adjacent NPs can change Theoretical calculations reveal that optimal regulation co-existence narrows energy barriers rate-limiting steps ORR, resulting outstanding performance. This work not only provides fundamental understanding underlying structure-activity relationship, but also sheds light on designing efficient

Language: Английский

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Molecular-level insight into photocatalytic CO2 reduction with H2O over Au nanoparticles by interband transitions

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

Published: July 6, 2022

Achieving CO2 reduction with H2O on metal photocatalysts and understanding the corresponding mechanisms at molecular level are challenging. Herein, we report that quantum-sized Au nanoparticles can photocatalytically reduce to CO help of by electron-hole pairs mainly originating from interband transitions. Notably, photocatalyst shows a production rate 4.73 mmol g-1 h-1 (~100% selectivity), ~2.5 times during H2 under same experimental conditions, low-intensity irradiation 420 nm. Theoretical studies reveal increased activity is induced surface Au-O species formed decomposition, which synchronously optimizes rate-determining steps in oxidation reactions, lowers energy barriers for *CO desorption *OOH formation, facilitates O2 production. Our findings provide an in-depth mechanistic designing active efficient H2O.

Language: Английский

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Designing covalent organic frameworks with Co-O4 atomic sites for efficient CO2 photoreduction

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: Feb. 28, 2023

Abstract Cobalt coordinated covalent organic frameworks have attracted increasing interest in the field of CO 2 photoreduction to CO, owing their high electron affinity and predesigned structures. However, achieving conversion efficiency is challenging since most Co related coordination environments facilitate fast recombination photogenerated electron-hole pairs. Here, we design two kinds Co-COF catalysts with oxygen atoms find that after tuning environment, reported framework catalyst Co-O 4 sites exhibits a production rate 18000 µmol g −1 h selectivity as 95.7% under visible light irradiation. From in/ex-situ spectral characterizations theoretical calculations, it revealed significantly carrier migration matrixes inhibit pairs photocatalytic process. This work opens way for high-performance photoreduction.

Language: Английский

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Current Advances on the Single‐Atom Nanozyme and Its Bioapplications

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(10)

Published: Feb. 11, 2023

Nanozymes, a class of nanomaterials mimicking the function enzymes, have aroused much attention as candidate in diverse fields with arbitrarily tunable features owing to diversity crystalline nanostructures, composition, and surface configurations. However, uncertainty their active sites lower intrinsic deficiencies nanomaterial-initiated catalysis compared natural enzymes promote pursuing alternatives by imitating biological centers. Single-atom nanozymes (SAzymes) maximize atom utilization well-defined structure, providing an important bridge investigate mechanism relationship between structure catalytic activity. They risen new burgeoning alternative enzyme from vitro bioanalytical tool vivo therapy flexible atomic engineering structure. Here, focus is mainly on three parts. First, detailed overview single-atom catalyst synthesis strategies including bottom-up top-down approaches given. Then, according structural feature nanocatalysts, influence factors such central metal atom, coordination number, heteroatom doping, metal-support interaction are discussed representative applications (including antibacterial/antiviral performance, cancer therapy, biosensing) highlighted. In end, future perspective challenge facing demonstrated.

Language: Английский

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