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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Surface decorated Ni sites for superior photocatalytic hydrogen production

SusMat, Journal Year: 2022, Volume and Issue: 2(4), P. 466 - 475

Published: July 30, 2022

Abstract Precise construction of isolated reactive centers on semiconductors with well‐controlled configurations affords a great opportunity to investigate the reaction mechanisms in photocatalytic process and realize targeted conversion solar energy steer charge kinetics for hydrogen evolution. In current research, we decorated Ni atoms surface CdS nanowires efficient production. X‐ray absorption fine structure investigations clearly demonstrate atomical dispersion sites nanowires. Experimental reveal that not only perform well as real but also greatly accelerate electron transfer via direct Ni–S coordination. Theoretical simulation further documents adsorption has been enhanced over semi‐coordinated through electronic coupling at atomic scale.

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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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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Highly Selective Photoconversion of CO₂ to CH₄ over SnO₂/Cs₃Bi₂Br₉ Heterojunctions Assisted by S-Scheme Charge Separation

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(19), P. 12623 - 12633

Published: Sept. 13, 2023

Exploring photocatalysts to promote the conversion of CO2 valuable chemical fuels is a highly promising approach for mitigating energy scarcity and environmental pollution. Lead-free perovskite Cs3Bi2Br9 quantum dots (QDs) have attracted considerable attention in photoreduction due robust reduction capability controllable product selectivity. Nevertheless, their potential has been impeded by rapid recombination charge carriers, leading unsatisfactory photocatalytic efficiency. Here, unique SnO2/Cs3Bi2Br9 S-scheme heterojunctions are constructed electrostatically self-assembling SnO2 nanofibers with QDs enhance performance. Density functional theory calculations, along experimental studies, reveal that electrons transfer from SnO2, creating directed interfacial electric field bending bands at interfaces. This facilitates transport photoelectrons Cs3Bi2Br9, forming enabling effective separation powerful photoexcited electron/hole pairs. Additionally, profiting enhanced light absorption contributed narrow-bandgap lower barrier CH4 production over surface, heterostructures unveil superior activities high selectivity 70%, without assistance any molecular catalyst or scavenger.

Language: Английский

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Ultra-thin Two-Dimensional Trimetallic Metal–Organic Framework for Photocatalytic Reduction of CO₂

ACS Catalysis, Journal Year: 2022, Volume and Issue: 12(5), P. 3238 - 3248

Published: Feb. 24, 2022

Photocatalytic reduction of carbon dioxide (CO2) into high-value chemicals is a very effective way to solve the greenhouse effect, improve utilization ratio resources, and cope with energy crisis. However, low catalytic activity poor product selectivity catalyst have been largely restricting its large-scale application. Herein, we successfully synthesized an ultra-thin two-dimensional trimetallic metal–organic framework (NiZrCu-BDC) nanosheet as photocatalyst for CO2 reduction, average thickness NiZrCu-BDC about 4 nm. The has ability reduce methanol (41.05 μmol h–1 g–1) ethanol (36.62 g–1), turnover frequency 34 times more than that NiZr-BDC. Zr Cu doping enables enrichment Ni surface charges promote chemisorption, structure can shorten electron transport path. Meanwhile, density catalytical sites in enhanced by facilitate COOH* CHO formation, which are deemed key species reactions liquid products. This work provides further insights photocatalytic based on multi-metal–organic framework.

Language: Английский

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Shining light on ZnIn₂S₄ photocatalysts: Promotional effects of surface and heterostructure engineering toward artificial photosynthesis

EcoMat, Journal Year: 2022, Volume and Issue: 4(5)

Published: March 27, 2022

Abstract The gradual depletion of fossil fuel reserves that contribute to ~85% global energy production and release toxic effluents urges the transformation toward renewable fuels. Thus, sustainable utilization sunlight for water splitting CO 2 reduction with heterogeneous photocatalysts has come light. As a semiconductor photocatalyst, ZnIn S 4 hit limelight owing its narrow bandgap visible‐light‐responsive properties. However, limitations include limited active sites, fast charge‐carrier recombination, low photoconversion efficiency. Beginning from fundamental photocatalytic mechanism, this review then provides in‐depth insights into several modification strategies , extending defect engineering, facet cocatalyst loading junction enabling synergistic construction high‐performance ‐based systems. Subsequently, structure‐performance relation hydrogen evolution (HER), overall (OWS), applications in last years will be discussed concluded by future perspectives frontier. image

Language: Английский

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Solar‐powered chemistry: Engineering low‐dimensional carbon nitride‐based nanostructures for selective CO₂ conversion to C₁C₂ products

InfoMat, Journal Year: 2022, Volume and Issue: 4(1)

Published: Jan. 1, 2022

CO2 capture and conversion has been prospected as an auspicious technology to simultaneously tackle the rise in global emission produce value-added fuels with goal of accomplishing carbon neutrality. A sustainable route achieve this is via utilization solar energy, thereby harnessing abundant nonexhaustive resource shift our reliance away from rapidly depleting fossil fuels. Graphitic nitride (g-C3N4) its allotrope have earned rank a fascinating metal-free photocatalyst due superior stability, high surface-area-to-volume ratio, tunable surface engineering. By leveraging these properties, robust nitride-based nanostructures are engineered for photocatalytic energy-rich C1C2 product, which indispensable chemical industry. Thus, review presents latest panorama experimental computational research on tuning local electronic, coordination environment, charge dynamics optical properties low-dimensional allotropes toward highly selective efficient photoconversion. To name few, structural engineering, point-defect heterojunction construction, cocatalyst loading. advance frontier, critical insights elucidated establish structure-performance relationship unravel primary factors dictating selectivity molecules reduction. External-field assisted photocatalysis such electric (photoelectro-) heat (photothermal) discussed uncover synergistic contributions that drive development photochemistry. Last, future challenges prospects outlined potential application solar-driven conversion, along scale-up strategy economic viewpoint rational high-efficiency catalysts.

Language: Английский

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Ultrathin Nanosheet Assembled Multishelled Superstructures for Photocatalytic CO₂ Reduction

ACS Nano, Journal Year: 2022, Volume and Issue: 16(3), P. 4517 - 4527

Published: March 4, 2022

Solar-driven conversion of CO2 is considered an efficient way to tackle the energy and environmental crisis. However, photocatalytic performance severely restricted due insufficient accessible active sites inhibited electron transfer efficiency. This work demonstrates a general in situ topological transformation strategy for integration uniform Co-based species fabricate series multishelled superstructures (MSSs) conversion. Thorough characterizations reveal obtained MSSs feature ultrathin nanosheet assembled polyhedral structures with tunable shell numbers, inner cavity sizes, compositions. The increase spatial density while maintaining their high accessibility. Further, nanosheets also facilitate photogenerated electrons. As result, ZnCo bimetallic hydroxide featuring quadruple-shell hollow structure (ZnCo-OH QUNH) exhibits efficiency toward reduction CO evolution rate 134.2 μmol h-1 apparent quantum yield 6.76% at 450 nm. quasi spectra theoretical calculations disclose that Co ZnCo-OH QUNH act as highly centers stabilize COOH* intermediate, Zn play role adsorption [Ru(bpy)3]2+ molecules.

Language: Английский

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Graphitic carbon nitride (g-C₃N₄) based heterogeneous single atom catalysts: synthesis, characterisation and catalytic applications

Journal of Materials Chemistry A, Journal Year: 2023, Volume and Issue: 11(16), P. 8599 - 8646

Published: Jan. 1, 2023

The ease of anchoring single atoms on the g-C 3 N 4 matrix, through its abundant nitrogen sites, facilitates a variety atom catalysts for applications in multiple domains catalysis.

Language: Английский

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