Construction of Ultrathin S‐Scheme Heterojunctions of Single Ni Atom Immobilized Ti‐MOF and BiVO₄ for CO₂ Photoconversion of nearly 100% to CO by Pure Water

Advanced Materials, Journal Year: 2022, Volume and Issue: 34(41)

Published: Aug. 20, 2022

To rationally design single-atom metal-organic framework (MOF)-involving photocatalysts remains an ongoing challenge for efficient CO2 conversion. Here, cuppy microstructures, consisting of a Ti(IV)-oxo node and three linked carboxylic moieties, in the single-coordination-layer Ti2 (H2 dobdc)3 MOF (NTU-9) are exploited to immobilize abundant single Ni(II) sites (Ni@MOF). The coupling Ni@MOF with BiVO4 (BVO) nanosheets by H-bonding-induced assembly process obtains wide-spectrum 2D heterojunctions. optimal heterojunction exhibits competitive performance enables around 66-fold conversion that BVO nanoparticles pure water, nearly 100% CO selectivity. exceptional photoactivity is attributed favorable S-scheme charge transfer from then sites. Noteworthily, anchored vicinal moieties serving as unique local microenvironment (LME) found synergistically catalyze Specifically, hydroxyl groups can form H-bonds promote its adsorption on sites, also provide accessible protons facilitate H-assisted reduction. Moreover, desorption subsequent LME proved be thermodynamically favored, hence dominates high This work highlights significance modulating atoms realizing carbon neutralization.

Language: Английский

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Asymmetric Coupled Dual‐Atom Sites for Selective Photoreduction of Carbon Dioxide to Acetic Acid

Advanced Functional Materials, Journal Year: 2022, Volume and Issue: 32(41)

Published: Aug. 9, 2022

Abstract Photocatalytic reduction of CO 2 to value‐added liquid fuels is a promising approach alleviate the global energy and environmental problems. However, highly selective production C2+ products from reaction (CO RR) very difficult because sluggish CC coupling reaction. An asymmetric coupled heteronuclear photocatalyst designed overcome this limitation. The new catalyst contains single atoms nickel cobalt loaded on titanium dioxide. It exhibits an impressive 71% selectivity for acetic acid. experimental data theoretical calculations reveal that Ni Co atom sites not only significantly lower barrier electron transfer in photocatalysis but also efficiently promote toward CH 3 COOH. high activity such system will shed light future development effective materials RR.

Language: Английский

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Atomically Dispersed Cu Catalyst for Efficient Chemoselective Hydrogenation Reaction

Nano Letters, Journal Year: 2021, Volume and Issue: 21(24), P. 10284 - 10291

Published: Dec. 9, 2021

The Cu-based nanocatalysts have shown a high selectivity toward selective hydrogenation reaction, but the underlying catalytic mechanism is still murky. Herein, we report new gram-scale strategy for realizing single atom Cu site incorporated into melem ring of graphitic carbon nitride (Cu1/CN) understanding reaction. as-synthesized Cu1/CN exhibits unprecedented (100%), activity (TOF = 2.9 × 103 h-1), and outstanding stability 4-nitrostyrene. We reveal that presence hydroxymethyl from trimethylolmelamine beneficial to atomically disperse atoms in CN. X-ray absorption fine structure tests dominated by quaternary coordination way (Cu-N4) Density functional theory calculations confirm reactivity originate anchored sites creating optimal chemical environment highly efficient

Language: Английский

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Mechanistic Insight into the Synergy between Platinum Single Atom and Cluster Dual Active Sites Boosting Photocatalytic Hydrogen Evolution

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(25)

Published: March 28, 2023

In the energy transition context, design and synthesis of high-performance Pt-based photocatalysts with low Pt content ultrahigh atom-utilization efficiency for hydrogen production are essential. Herein, a facile approach decorating atomically dispersed cocatalysts having single-atom (SA) atomic cluster (C) dual active sites on CdS nanorods (PtSA+C /CdS) via layer deposition is reported. The size cocatalyst spatial intimacy precisely engineered at scale. PtSA+C /CdS show optimized photocatalytic evolution activity, achieving reaction rate 80.4 mmol h-1 g-1 , which 1.6- 7.3-fold higher than those PtSA PtNP photocatalysts, respectively. Thorough characterization theoretical calculations reveal that enhanced activity due to remarkable synergy between SAs clusters as sites, responsible water adsorption-dissociation desorption, A similar synergetic effect found in representative Pt/TiO2 system, indicating generality strategy. This study demonstrates significance enhancing efficiency, opening new avenue rational high efficiency.

Language: Английский

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Recent progress of metal single-atom catalysts for energy applications

Nano Energy, Journal Year: 2023, Volume and Issue: 111, P. 108404 - 108404

Published: April 5, 2023

Language: Английский

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Recent advances and future perspectives in MOF-derived single-atom catalysts and their application: a review

Journal of Materials Chemistry A, Journal Year: 2023, Volume and Issue: 11(7), P. 3315 - 3363

Published: Jan. 1, 2023

This article discusses the relationship between single-atom sites and catalytic mechanism of functional MOFs which is related to coordination environment metal ions, also summarizes research progress MOF-derived SACs in recent years.

Language: Английский

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Photothermal-enabled single-atom catalysts for high-efficiency hydrogen peroxide photosynthesis from natural seawater

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

Published: April 29, 2023

Hydrogen peroxide (H2O2) is a powerful industrial oxidant and potential carbon-neutral liquid energy carrier. Sunlight-driven synthesis of H2O2 from the most earth-abundant O2 seawater highly desirable. However, solar-to-chemical efficiency in particulate photocatalysis systems low. Here, we present cooperative sunlight-driven photothermal-photocatalytic system based on cobalt single-atom supported sulfur doped graphitic carbon nitride/reduced graphene oxide heterostructure (Co-CN@G) to boost photosynthesis natural seawater. By virtue photothermal effect synergy between Co single atoms heterostructure, Co-CN@G enables more than 0.7% under simulated sunlight irradiation. Theoretical calculations verify that combined with significantly promote charge separation, facilitate absorption reduce barriers for reduction water oxidation, eventually boosting photoproduction. The materials may provide possibility large-scale production inexhaustible sustainable way.

Language: Английский

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Single‐Atom Catalysts (SACs) for Photocatalytic CO₂ Reduction with H₂O: Activity, Product Selectivity, Stability, and Surface Chemistry

Small, Journal Year: 2022, Volume and Issue: 18(29)

Published: June 13, 2022

Abstract In recent years, single‐atom catalysts (SACs) have attracted the interest of researchers owing to their suitability for various catalytic applications. For instance, optoelectronic features, site‐specific activity, and cost‐effectiveness make SACs ideal photocatalytic CO 2 reduction. The product selectivity, photostability depend on factors such as nature metal/support material, interaction between metal atoms support, light‐harvesting ability, charge separation behavior, adsorption active sites, defects. Consequently, it is necessary investigate these in depth elucidate working principle(s) Herein, progress development reduction with H O reviewed. First, a brief overview photoreduction conversion provided. Several synthesis strategies useful techniques characterizing employed heterogeneous catalysis are then described. Next, challenges related optimization strategies, terms stability, explored. noble metal– transition metal–based dual‐SACs discussed. Finally, prospects considered.

Language: Английский

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Steering Unit Cell Dipole and Internal Electric Field by Highly Dispersed Er atoms Embedded into NiO for Efficient CO₂ Photoreduction

Advanced Functional Materials, Journal Year: 2022, Volume and Issue: 32(28)

Published: March 26, 2022

Abstract The weak internal electric field over antiferromagnetic materials makes it difficult to facilitate charge migration the surface, leading low performance for CO 2 photoreduction. asymmetry and polarization refinement structure can induce an intensive field. Herein, n‐type NiO is synthesized with highly dispersed erbium atoms doping (Er/NiO 1− x ) via a molten salt method accelerate separation transfer. of Er distort unit cell alter symmetry enhance field, in favor efficient charges. In addition, erbium‐doped largely boost adsorption activation , weaken energy barrier photoreduction reaction. Benefiting from unique features, optimal ratio (≈2%) achieves remarkable elevation carrier efficiency excellent yield 368 µmol g −1 h Ru(byp) 3 2+ /ethanolamine electron‐agent generating system, which 26.3‐fold 3.9‐fold relative traditional NiO, respectively. obtained Er/NiO photocatalyst dipole governing opens new window materials.

Language: Английский

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In situ growth strategy synthesis of single-atom nickel/sulfur co-doped g-C3N4 for efficient photocatalytic tetracycline degradation and CO2 reduction

Chemical Engineering Journal, Journal Year: 2022, Volume and Issue: 442, P. 136208 - 136208

Published: April 5, 2022

Language: Английский

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