All-organic Z-scheme photoreduction of CO2 with water as the donor of electrons and protons

Mazzanti, Stefano; Cao, Shaowen; Brummelhuis, Katharina ten; Völkel, Antje; Khamrai, Jagadish; Sharapa, Dmitry I.; Youk, Sol; Heil, Tobias; Tarakina, Nadezda V.; Strauß, Volker; Ghosh, Indrajit; König, Burkhard; Oschatz, Martin; Antonietti, Markus; Savateev, Aleksandr

doi:10.1016/j.apcatb.2020.119773

Cited by 27 publications

(13 citation statements)

References 64 publications

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“…In the last decade, CN as a material in general has been studied in water splitting, production of hydrogen, conversion of CO 2 into valuable products, and synthesis of fine chemicals. − Due to the exciting properties of CN, the scope of applications for this material spans beyond photocatalysis, for example, to optoelectronics, , energy and membrane separation, among others. , …”

Section: Introductionmentioning

confidence: 99%

Carbon Nitride Thin Films as All-In-One Technology for Photocatalysis

et al. 2021

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Organic π-conjugated polymers are promising heterogeneous photocatalysts that involve photoredox or energy transfer processes. In such settings, the materials are usually applied in the form of dispersion in liquid medium, which is bound to certain technological limits of applicability. Herein, we present an innovative approach using carbon nitride thin films prepared via chemical vapor deposition at different vessel walls and using them as batch and microfluidic photoreactors. This approach allows us not only to fabricate technologically relevant and reusable devices but also to improve photophysical properties of carbon nitride, such as the singlet−triplet energy gap and lifetime of triplet excited states, when the material is assembled in thin films. These morphological changes are employed to maximize the performance of the materials in photocatalytic reactions, in which the carbon nitride thin films show at least 1 order of magnitude higher activity per area unit compared to photocatalysis using suspended particles.

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Section: Introductionmentioning

confidence: 99%

Carbon Nitride Thin Films as All-In-One Technology for Photocatalysis

et al. 2021

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“…Similar to CNs, flavin has been also regarded as a metal‐free and photoactive material. Savateev and co‐workers reported a biomimetic core−shell structure composed of micrometer‐sized flavins with potassium poly(heptazine imide), [ 164 ] which successfully converted CO 2 molecule into CO, CH 4 , MeOH, and EtOH in the water vapor atmosphere. The Z‐scheme heterojunction possessed an overall wide bandgap, which significantly extended its excited states lifetimes, thus facilitating the photoredox processes and suppressing the interface charge recombination.…”

Section: Photocatalysismentioning

confidence: 99%

Recent Progress in Materials Exploration for Thermocatalytic, Photocatalytic, and Integrated Photothermocatalytic CO₂‐to‐Fuel Conversion

Zhang

Pérez‐Ramírez

et al. 2021

Adv Energy and Sustain Res

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The excess depletion of carbon‐rich fossil fuels and agroforest biomass resources has aggravated the energy crisis and environmental pollution, causing increased CO2 emissions. Accordingly, the goal of “peak CO2 emissions and carbon neutrality” is proposed to alleviate global warming. CO2‐to‐fuel conversion is considered as a preferable move for reducing the atmospheric CO2 concentration and further upgrading to chemical feedstocks. However, the highly efficient CO2 conversion remains challenging due to the thermodynamic limits and kinetic barriers, which require high energy input through conventional thermocatalysis. Inspired by “artificial photosynthesis,” photocatalytic CO2 transformation has received tremendous attention and makes remarkable progress over the past decades, although it is still far from practical application. Recently, the integrated photothermocatalysis has emerged as an intelligent strategy to utilize solar energy to induce local heating and energetic hot carriers, which synergistically promote CO2‐to‐fuel conversion. The key to the success of CO2 upgradation is catalysts’ development with improved activity, selectivity, and stability. This review highlights the recent advancements in materials designing for practical CO2 conversion through thermocatalysis, photocatalysis, and photothermocatalysis during the past five years, emphasizing the reaction pathways and mechanism on the CO bond activation and intermediates formation. Finally, the current challenges and future opportunities are described.

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“…Visible light photocatalysis is seen as one of the prominent alternatives to conventional chemistry, which through harvesting solar light and followed by photoinduced electron transfer enables many important chemical transformations, including H 2 production, − CO 2 conversion, − pollutant degradation, , and also organic synthesis. , Previously, the photocatalytic alternative to the Meerwein method was proposed by Jacobi von Wangelin et al in 2017 . To enable this reaction, the authors used a transition-metal-based catalyst tris(2,2′-bipyridine)ruthenium(II)dichloride [Ru(bpy) 3 ]Cl 2 .…”

Section: Introductionmentioning

confidence: 99%

Synthesis of Sulfonyl Chlorides from Aryldiazonium Salts Mediated by a Heterogeneous Potassium Poly(heptazine imide) Photocatalyst

2021

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Visible light photocatalysis is a tool in synthetic chemistry that allows us to utilize the energy of photons via photoinduced electron transfer to promote diverse organic reactions. Herein, a heterogeneous transition metal-free material, a type of carbon nitride photocatalyst, potassium poly(heptazine imide), is employed to produce sulfonyl chlorides from arenediazonium salts under mild conditions (visible light irradiation, room temperature) with 50−95% yields. The method is suitable for the synthesis of both electron rich and electron deficient compounds, and it shows high tolerance toward different functional groups (halides, ester, nitro, cyano groups). Thus, a sustainable photocatalytic alternative to the Meerwein chlorosulfonylation reaction is offered.

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All-organic Z-scheme photoreduction of CO2 with water as the donor of electrons and protons

Cited by 27 publications

References 64 publications

Carbon Nitride Thin Films as All-In-One Technology for Photocatalysis

Carbon Nitride Thin Films as All-In-One Technology for Photocatalysis

Recent Progress in Materials Exploration for Thermocatalytic, Photocatalytic, and Integrated Photothermocatalytic CO₂‐to‐Fuel Conversion

Synthesis of Sulfonyl Chlorides from Aryldiazonium Salts Mediated by a Heterogeneous Potassium Poly(heptazine imide) Photocatalyst

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All-organic Z-scheme photoreduction of CO2 with water as the donor of electrons and protons

Cited by 27 publications

References 64 publications

Carbon Nitride Thin Films as All-In-One Technology for Photocatalysis

Carbon Nitride Thin Films as All-In-One Technology for Photocatalysis

Recent Progress in Materials Exploration for Thermocatalytic, Photocatalytic, and Integrated Photothermocatalytic CO2‐to‐Fuel Conversion

Synthesis of Sulfonyl Chlorides from Aryldiazonium Salts Mediated by a Heterogeneous Potassium Poly(heptazine imide) Photocatalyst

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Product

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Recent Progress in Materials Exploration for Thermocatalytic, Photocatalytic, and Integrated Photothermocatalytic CO₂‐to‐Fuel Conversion