Methane Formation Induced via Face-to-Face Orientation of Cyclic Fe Porphyrin Dimer in Photocatalytic CO2 Reduction DOI Creative Commons
Yusuke Kuramochi,

Masaya Hashimoto,

Akiharu Satake

et al.

Molecules, Journal Year: 2024, Volume and Issue: 29(11), P. 2453 - 2453

Published: May 23, 2024

Iron porphyrins are known to provide CH4 as an eight-electron reduction product of CO2 in a photochemical reaction. However, there still some aspects the reaction mechanism that remain unclear. In this study, we synthesized iron porphyrin dimers and carried out reactions N,N-dimethylacetamide (DMA) containing photosensitizer presence 1,3-dimethyl-2-phenyl-2,3-dihydro-1H-benzo[d]imidazole (BIH) electron donor. We found that, despite low catalytic turnover number, was produced only when these were facing each other. The close proximity cyclic dimers, distinguishing them from linear Fe dimer monomers, induced multi-electron reduction, emphasizing unique role their structural arrangement formation.

Language: Английский

Metal‐Free Photocatalytic CO2 Reduction to CH4 and H2O2 under Non‐sacrificial Ambient Conditions DOI
W. Q. Zou,

Yingyi Cheng,

Yu‐Xin Ye

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(49)

Published: Oct. 19, 2023

Photocatalytic CO2 reduction to CH4 requires photosensitizers and sacrificial agents provide sufficient electrons protons through metal-based photocatalysts, the separation of from by-product O2 has poor applications. Herein, we successfully synthesize a metal-free photocatalyst novel electron-acceptor 4,5,9,10-pyrenetetrone (PT), our best knowledge, this is first time that catalyst achieves non-sacrificial photocatalytic easily separable H2 . This offers product 10.6 μmol ⋅ g-1 h-1 under ambient conditions (room temperature, only water), which two orders magnitude higher than reported photocatalysts. Comprehensive in situ characterizations calculations reveal multi-step reaction mechanism, long-lived oxygen-centered radical excited PT provides as site for activation, resulting stabilized cyclic carbonate intermediate with lower formation energy. key thermodynamically crucial subsequent electronic selectivity up 90 %. The work fresh insights on economic viability conditions.

Language: Английский

Citations

39
Halide Perovskites for Photoelectrochemical Water Splitting and CO2 Reduction: Challenges and Opportunities DOI Creative Commons
Krzysztof Bieńkowski, Renata Solarska, Linh Trinh

et al.

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(9), P. 6603 - 6622

Published: April 16, 2024

Photoelectrochemical water splitting and CO2 reduction provide an attractive route to produce solar fuels while reducing the level of emissions. Metal halide perovskites (MHPs) have been extensively studied for this purpose in recent years due their suitable optoelectronic properties. In review, we survey achievements field. After a brief introduction photoelectrochemical (PEC) processes, discussed properties, synthesis, application MHPs context. We also state-of-the-art findings regarding significant performance, developments addressing major challenges toxicity instability toward water. Efforts made replace toxic Pb with less materials like Sn, Ge, Sb, Bi. The stability has improved by using various methods such as compositional engineering, 2D/3D perovskite structures, surface passivation, use protective layers, encapsulation. last part, considering experience gained photovoltaic applications, provided our perspective future opportunities. place special emphasis on improvement challenge potential contribution machine learning identify most formulation desired

Language: Английский

Citations

13
High-efficiency CO2 conversion via mechano-driven dynamic strain engineering of ZnO nanostructures DOI
Jiangping Ma,

Xia Lü,

Di Wu

et al.

Nano Energy, Journal Year: 2024, Volume and Issue: 121, P. 109258 - 109258

Published: Jan. 4, 2024

Language: Английский

Citations

12
A Novel Non‐Fullerene D‐A Interface with Two Asymmetrical Electron Acceptors Facilitates Charge and Energy Transfer for Effective Carbon Dioxide Reduction DOI
Shiming Zhang, Yanping Hou, Libin Zhang

et al.

Small, Journal Year: 2024, Volume and Issue: 20(30)

Published: Feb. 23, 2024

Abstract Converting carbon dioxide (CO 2 ) into high‐value chemicals using solar energy remains a formidable challenge. In this study, the CSC@PM6:IDT6CN‐M:IDT8CN‐M non‐fullerene small‐molecule organic semiconductor is designed with highly efficient electron donor‐acceptor (D‐A) interface for photocatalytic reduction of CO . Atomic Force Microscope and Transmission Electron images confirmed formation an interpenetrating fibrillar network after combination donor acceptor. The yield from reached 1346 µmol g −1 h , surpassing those numerous reported inorganic photocatalysts. D‐A structure effectively facilitated charge separation to enable electrons transfer PM6 IDT6CN‐M:IDT8CN‐M. Meanwhile, attributing dipole moments strong intermolecular interactions between IDT6CN‐M IDT8CN‐M, forces are enhanced, laminar stacking π‐π strengthened, thereby reinforcing acceptor molecules significantly enhanced separation. Moreover, internal electric field in excited state lifetime PM6:IDT6CN‐M:IDT8CN‐M. situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) analysis demonstrated that carboxylate (COOH*) predominant intermediate during reduction, possible pathways deduced. This study presents novel approach designing materials achieve high activity.

Language: Английский

Citations

12
Recent developments and perspectives of Ti-based transition metal carbides/nitrides for photocatalytic applications: A critical review DOI
Jipeng Fan, Haitao Wang, Wei Sun

et al.

Materials Today, Journal Year: 2024, Volume and Issue: 76, P. 110 - 135

Published: June 11, 2024

Language: Английский

Citations

12
Cooperative Atomic Palladium Site and Island-Distributed S-Scheme Heterostructure for Photocatalytic C2H6 Production DOI
Yan Wu, Zhujie Li, Qingqing Chen

et al.

ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 3558 - 3569

Published: Feb. 12, 2025

Language: Английский

Citations

1
Photocatalytic product-selective reduction of CO2, CO, and carbonates DOI Creative Commons
Rohan Bhimpuria, Monika Tomar, Anders Thapper

et al.

Chem, Journal Year: 2025, Volume and Issue: unknown, P. 102450 - 102450

Published: Feb. 1, 2025

Language: Английский

Citations

1
Triarylamine-Substituted Benzimidazoliums as Electron Donor–Acceptor Dyad-Type Photocatalysts for Reductive Organic Transformations DOI

Ryo Miyajima,

Yuuki Ooe,

Tomoaki Miura

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(18), P. 10236 - 10248

Published: May 2, 2023

Triarylamine-substituted benzimidazoliums (BI+-PhNAr2), new electron donor-acceptor dyad molecules, were synthesized. Their photocatalytic properties for reductive organic transformations explored using absorption and fluorescence spectroscopy, redox potential determinations, density functional theory calculations, transient reduction reactions of selected substrates. The results show that irradiation BI+-PhNAr2 promotes photoinduced intramolecular transfer to form a long-lived (∼300 μs) charge shifted state (BI•-PhN•+Ar2). In the pathway photocatalysis substrates, BI•-PhN•+Ar2 is subsequently transformed neutral benzimidazolyl radical (BI•-PhNAr2) by single-electron from donor 1,3-dimethyl-2-phenylbenzimidazoline (BIH-Ph) serving as cooperative agent. Among explored, bromo-substituted analogue BI+-PhN(C6H4Br-p)2 in conjunction with BIH-Ph demonstrates most consistent catalytic performance.

Language: Английский

Citations

18
Isonitriles as Alkyl Radical Precursors in Visible Light Mediated Hydro‐ and Deuterodeamination Reactions** DOI Creative Commons
Irene Quirós, María Martín, Miguel Gomez‐Mendoza

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 63(7)

Published: Dec. 27, 2023

Herein, we report the use of isonitriles as alkyl radical precursors in light-mediated hydro- and deuterodeamination reactions. The reaction is scalable, shows broad functional group compatibility potential to be used late-stage functionalization. Importantly, method general for C

Language: Английский

Citations

18
Promoting Electrochemical CO2 Reduction to Formate via Sulfur‐Assisted Electrolysis DOI
Yuhang Liu, Zhiming Wei, Xiaozhi Su

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: May 16, 2024

Abstract Electrochemical CO 2 reduction reaction (CO RR) provides a renewable approach to transform produce chemicals and fuels. Unfortunately, it faces the challenges of sluggish activation slow water dissociation. This study reports modification Bi‐based electrocatalyst by S, which leads remarkable enhancement in activity selectivity during electrochemical formate. Based on comprehensive situ examinations kinetic evaluations, is observed that presence S species over Bi catalyst can significantly enhance its interaction with K + (H O) n , facilitating fast dissociation molecules generate protons. Further attenuated total reflectance surface‐enhanced infrared absorption spectroscopy (ATR‐SEIRAS) Raman measurements reveal able decrease oxidation state active site, effectively facilitate HCOO * intermediate formation while suppressing competing hydrogen evolution reaction. Consequently, S‐modified achieves impressive RR performance, reaching formate Faradaic efficiency (FE ) 91.2% at partial current density ≈135 mA cm −2 potential −0.8 V versus RHE an alkaline electrolyte.

Language: Английский

Citations

8