Recent Progress of Metal Sulfide Photocatalysts for Solar Energy Conversion

Advanced Materials, Год журнала: 2022, Номер 34(45)

Опубликована: Май 27, 2022

Artificial photosynthetic solar-to-chemical cycles enable an entire environment to operate in a more complex, yet effective, way perform natural photosynthesis. However, such artificial systems suffer from lack of well-established photocatalysts with the ability harvest solar spectrum and rich catalytic active-site density. Benefiting extensive experimental theoretical investigations, this bottleneck may be overcome by devising photocatalytic platform based on metal sulfides predominant electronic, physical, chemical properties. These tunable properties can endow them abundant active sites, favorable light utilization, expedited charge transportation for conversion. Here, it is described how some vital lessons extracted previous investigations are employed promote further development photosynthesis, including water splitting, CO2 reduction, N2 pollutant removal. Their functions, properties, synthetic strategies, emerging issues, design principles, intrinsic functional mechanisms redox reactions discussed detail. Finally, associated challenges prospects utilization highlighted future trends photocatalysis envisioned.

Язык: Английский

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A Bifunctional CdS/MoO₂/MoS₂ Catalyst Enhances Photocatalytic H₂ Evolution and Pyruvic Acid Synthesis

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(44)

Опубликована: Сен. 10, 2022

The best use of photogenerated electrons and holes is crucial to boosting photocatalytic activity. Herein, a bifunctional dual-cocatalyst-modified photocatalyst constructed based on CdS/MoO2 /MoS2 hollow spheres for hydrogen evolution coupled with selective pyruvic acid (PA) production from lactic (LA) oxidation. MoS2 MoO2 are simultaneously obtained the conversion CdMoO4 in one step. In process, function as reduction oxidation centers which accumulate used reaction (HER) PA synthesis, respectively. By monitoring intermediates, two-step single-electron route proposed, initiated by cleavage α-C(sp3 )-H bond LA. LA selectivity can reach ca. 29 % 95 after five-hour reaction,

Язык: Английский

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Solar utilization beyond photosynthesis

Nature Reviews Chemistry, Год журнала: 2022, Номер 7(2), С. 91 - 105

Опубликована: Дек. 19, 2022

Язык: Английский

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Trash to Treasure: Photoreforming of Plastic Waste into Commodity Chemicals and Hydrogen over MoS₂-Tipped CdS Nanorods

ACS Catalysis, Год журнала: 2022, Номер 12(20), С. 12823 - 12832

Опубликована: Окт. 7, 2022

Plastic valorization presents a significantly untapped opportunity to address environmental issues while creating the necessary economic push for circular carbon economy. Compared with conventional routes processing plastics (e.g., pyrolysis and gasification), photoreforming strategy, namely, photocatalytic plastic oxidation paired water splitting, aims achieve into commodity chemicals under mild conditions offering hydrogen fuels. Here, we implement MoS2-tipped CdS nanorod photocatalysts in an aqueous medium reform pretreated that range from polyesters polylactic acid (PLA) polyethylene terephthalate (PET)) polyolefins (PE)). The architecture of MoS2/CdS takes advantage anisotropic morphology rapid charge transfer features nanorods, by collecting electrons at MoS2 tip evolution utilizing entire sidewall nanorods rich holes toward oxidation. It is shown continuous H2 can be evolved PLA, PET (commercial granules real-world bottles), PE, these substrates are accordingly converted series valuable chemicals. This work provides effective way harness solar energy realize transformation trash (plastics) treasure (gaseous/liquid chemicals).

Язык: Английский

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Tailor‐Engineered 2D Cocatalysts: Harnessing Electron–Hole Redox Center of 2D g‐C₃N₄ Photocatalysts toward Solar‐to‐Chemical Conversion and Environmental Purification

Advanced Functional Materials, Год журнала: 2022, Номер 32(29)

Опубликована: Фев. 23, 2022

Abstract Sparked by natural photosynthesis, solar photocatalysis using metal‐free graphitic carbon nitride (g‐C 3 N 4 ) with appealing electronic structure has turned up as the most captivating technique to quest for sustainable energy generation and pollution‐free environment. Nonetheless, low‐dimensional g‐C is thwarted from sluggish kinetics rapid recombination of photogenerated carriers upon light irradiation. Among multifarious modification strategies, engineering 2D cocatalysts anticipated accelerate redox kinetics, augment active sites ameliorate electron–hole separation boosted activity thanks its face‐to‐face contact surface. It timely technological significance review 2D/2D interfaces state‐of‐the‐art cocatalysts, spanning carbon‐containing phosphorus‐containing, metal dichalcogenide, other cocatalysts. Fundamental principles each photocatalytic application will be introduced. Thereafter, recent advances cocatalyst‐mediated systems critically evaluated based on their interfacial engineering, emerging roles, impacts toward stability catalytic efficiency. Importantly, mechanistic insights into charge dynamics structure–performance relationship deciphered. Last, noteworthy research directions are prospected deliver insightful ideas future development . Overall, this serve a scaffold cornerstone in designing dimensionality‐dependent cocatalyst‐assisted renewable ecologically green

Язык: Английский

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A new breakthrough in photocatalytic hydrogen evolution by amorphous and chalcogenide enriched cocatalysts

Chemical Engineering Journal, Год журнала: 2022, Номер 455, С. 140601 - 140601

Опубликована: Ноя. 26, 2022

Язык: Английский

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Stacking Engineering of Semiconductor Heterojunctions on Hollow Carbon Spheres for Boosting Photocatalytic CO₂ Reduction

ACS Catalysis, Год журнала: 2022, Номер 12(4), С. 2569 - 2580

Опубликована: Фев. 7, 2022

Fabrication of semiconductor heterojunctions into hollow nanostructures holds multiple intrinsic advantages in enhancing the photocatalytic performance but still faces lots challenges. To overcome obstacles, herein, we report an alternative stacking design on carbon spheres for significantly improved activity, selectivity, and stability CO2-to-CO conversion. In smart design, CdS nanoparticles are first deposited then selectively coated with ZnIn2S4 outer layers, producing a ternary C/CdS@ZnIn2S4 photocatalyst. The enhancements attributed to prominent features merits carbon: (i) light reflection scattering improving harvesting; (ii) electron collection behavior promoting charge separation; (iii) large surface area increasing CO2 adsorption; (iv) highly active selective sites targeted reduction reaction; (v) porous shell spatially separating oxidation half reactions; (vi) protective layer preserving from photocorrosion; (vii) ideal architecture deposition separated redox cocatalysts. It is expected that emerging would be extended other if only two semiconductors integrated core–shell nanostructure hole-accumulated electron-accumulated core.

Язык: Английский

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Unraveling Charge‐Separation Mechanisms in Photocatalyst Particles by Spatially Resolved Surface Photovoltage Techniques

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(16)

Опубликована: Янв. 31, 2022

Abstract The photocatalytic conversion of solar energy offers a potential route to renewable energy, and its efficiency relies on effective charge separation in nanostructured photocatalysts. Understanding the charge‐separation mechanism is key improving performance this has now been enabled by advances spatially resolved surface photovoltage (SRSPV) method. In Review we highlight progress made SRSPV mapping distributions at nanoscale determining driving forces heterogeneous photocatalyst particles. We discuss how arising from built‐in electric field, diffusion, trapping can be exploited optimized through design. also importance asymmetric engineering photocatalysts for separation. Finally, provide an outlook further opportunities that arise leveraging these insights guide rational design advance imaging technique expand knowledge

Язык: Английский

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Constructing interfacial active sites in Ru/g-C3N4−x photocatalyst for boosting H2 evolution coupled with selective benzyl-alcohol oxidation

Applied Catalysis B Environment and Energy, Год журнала: 2022, Номер 315, С. 121575 - 121575

Опубликована: Июнь 1, 2022

Язык: Английский

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Electron‐Rich Bi Nanosheets Promote CO₂⋅⁻ Formation for High‐Performance and pH‐Universal Electrocatalytic CO₂ Reduction

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(11)

Опубликована: Янв. 20, 2023

Electrochemical CO2 reduction reaction (CO2 RR) to chemical fuels such as formate offers a promising pathway carbon-neutral future, but its practical application is largely inhibited by the lack of effective activation molecules and pH-universal feasibility. Here, we report an electronic structure manipulation strategy electron-rich Bi nanosheets, where electrons transfer from Cu donor acceptor in bimetallic Cu-Bi, enabling RR towards with concurrent high activity, selectivity stability (acidic, neutral alkaline) electrolytes. Combined situ Raman spectra computational calculations unravel that promotes ⋅- formation activate molecules, enhance adsorption strength *OCHO intermediate up-shifted p-band center, thus leading superior activity formate. Further integration robust nanosheets into III-V-based photovoltaic solar cell results unassisted artificial leaf solar-to-formate (STF) efficiency 13.7 %.

Язык: Английский

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