Low‐Coordination Single Au Atoms on Ultrathin ZnIn₂S₄Nanosheets for Selective Photocatalytic CO₂Reduction towards CH₄

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(41)

Published: Aug. 22, 2022

Abstract Selective CO 2 photoreduction to hydrocarbon fuels such as CH 4 is promising and sustainable for carbon‐neutral future. However, lack of proper binding strengths with reaction intermediates makes it still a challenge photocatalytic methanation both high activity selectivity. Here, low‐coordination single Au atoms (Au 1 ‐S ) on ultrathin ZnIn S nanosheets was synthesized by complex‐exchange route, enabling exceptional reduction performance. Under visible light irradiation, /ZnIn catalyst exhibits yield 275 μmol g −1 h selectivity 77 %. As revealed detailed characterizations density functional theory calculations, structure not only display fast carrier transfer underpin its superior activity, but also greatly reduce the energy barrier protonation *CO stabilize *CH 3 intermediate, thereby leading selective generation from photoreduction.

Language: Английский

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Dislocated Bilayer MOF Enables High‐Selectivity Photocatalytic Reduction of CO₂ to CO

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(10)

Published: Jan. 2, 2023

The highly selective photoreduction of CO2 into valuable small-molecule chemical feedstocks such as CO is an effective strategy for addressing the energy crisis and environmental problems. However, it remains a challenge because complex process usually generates multiple possible products requires subsequent separation step. In this paper, 2D monolayer bilayer porphyrin-based metal-organic frameworks (MOFs) are successfully constructed by adjusting reaction temperature solvent polarity with 5,10,15,20-tetrakis(4-pyridyl)porphyrin light-harvesting ligand. MOF low-dimensional special structure in which upper lower layers arranged dislocation bridged halogen ions. This exhibits 100% ultra-high selectivity reduction to under simulated sunlight without any cocatalyst or photosensitizer can be recycled at least three times. intrinsic mechanism photocatalytic explored through experimental characterization density functional theory (DFT) calculations. work shows that rational design number structures tune stability these opens new avenue photocatalysts.

Language: Английский

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Precise regulation of built-in electric field over NH2-MIL-125-Ti/WO3-x S-scheme heterojunction for achieving simultaneous formation of CO and H2O2 from CO2 and H2O

Chemical Engineering Journal, Journal Year: 2023, Volume and Issue: 466, P. 143129 - 143129

Published: April 24, 2023

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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Facet‐specific Active Surface Regulation of Bi_xMO_y (M=Mo, V, W) Nanosheets for Boosted Photocatalytic CO₂ reduction

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(50)

Published: Oct. 19, 2022

Photocatalytic performance can be optimized via introduction of reactive sites. However, it is practically difficult to engineer these on specific photocatalyst surfaces, because limited understanding atomic-level structure-activity. Here we report a facile sonication-assisted chemical reduction for facets regulation oxygen deprivation Bi-based photocatalysts. The modified Bi2 MoO6 nanosheets exhibit 61.5 and 12.4 μmol g-1 CO CH4 production respectively, ≈3 times greater than pristine catalyst, together with excellent stability/reproducibility ≈20 h. By combining advanced characterizations simulation, confirm the reaction mechanism surface-regulated photocatalysts, namely, induced defects highly-active surface accelerate charge separation/transfer lower energy barrier CO2 adsorption/activation/reduction. Promisingly, this method appears generalizable wider range materials.

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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Photochromic single atom Ag/TiO₂ catalysts for selective CO₂ reduction to CH₄

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 17(2), P. 518 - 530

Published: Dec. 7, 2023

A new all-in-one design concept of constructing photochromic single atom photocatalysts is proposed to achieve both high activity and selectivity photocatalytic CO 2 -to-CH 4 conversion.

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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Integrating Enrichment, Reduction, and Oxidation Sites in One System for Artificial Photosynthetic Diluted CO₂ Reduction

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(40)

Published: June 26, 2023

Artificial photosynthetic diluted CO2 reduction directly driven by natural sunlight is a challenging, but promising way to realize carbon-resources recycling utilization. Herein, three-in-one photocatalytic system of enrichment, and H2 O oxidation sites designed for reduction. A Zn-Salen-based covalent organic framework (Zn-S-COF) with reductive synthesized; then, ionic liquids (ILs) are loaded into the pores. As result, [Emim]BF4 @Zn-S-COF shows visible-light-driven -to-CO conversion rate 105.88 µmol g-1 h-1 under (15%) atmosphere, even superior than most photocatalysts in high concentrations . Moreover, also reaches 126.51 5 h. Further experiments theoretical calculations reveal that triazine ring Zn-S-COF promotes activity sites, ILs provide an enriched realizing efficient

Language: Английский

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Homogeneity of Supported Single‐Atom Active Sites Boosting the Selective Catalytic Transformations

Advanced Science, Journal Year: 2022, Volume and Issue: 9(24)

Published: July 9, 2022

Selective conversion of specific functional groups to desired products is highly important but still challenging in industrial catalytic processes. The adsorption state surface species the key factor modulating groups, which correspondingly determined by uniformity active sites. However, non-identical number metal atoms, geometric shape, and morphology conventional nanometer-sized particles/clusters normally lead non-uniform sites with diverse configurations local coordination environments, causes distinct states species. Hence, it modulate homogeneity so that transformations can be better confined direction. In this review, construction strategies characterization techniques uniform are atomically dispersed on various supports examined. particular, their unique behavior boosting performance chemical discussed, including selective hydrogenation, oxidation, Suzuki coupling, other reactions. addition, dynamic evolution under reaction conditions utilization single-atom catalysts highlighted. Finally, current challenges frontiers identified, perspectives flourishing field provided.

Language: Английский

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