Well-defined diatomic catalysis for photosynthesis of C2H4 from CO2

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: March 18, 2024

Abstract Owing to the specific electronic-redistribution and spatial proximity, diatomic catalysts (DACs) have been identified as principal interest for efficient photoconversion of CO 2 into C H 4 . However, predominant bottom-up strategy DACs synthesis has critically constrained development highly ordered due random distribution heteronuclear atoms, which hinders optimization catalytic performance exploration actual reaction mechanism. Here, an up-bottom ion-cutting architecture is proposed fabricate well-defined DACs, superior proximity CuAu diatomics (DAs) decorated TiO (CuAu-DAs-TiO ) successfully constructed compact heteroatomic spacing (2-3 Å). profoundly low C-C coupling energy barrier CuAu-DAs-TiO , a considerable production with sustainability achieved. Our discovery inspires novel fabrication motivate distinct deduction heteroatom synergistically

Language: Английский

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Superlative Porous Organic Polymers for Photochemical and Electrochemical CO₂ Reduction Applications: From Synthesis to Functionality

Langmuir, Journal Year: 2024, Volume and Issue: 40(20), P. 10414 - 10432

Published: May 10, 2024

To mimic the carbon cycle at a kinetically rapid pace, sustainable conversion of omnipresent CO

Language: Английский

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3D-Printed photocatalysts for revolutionizing catalytic conversion of solar to chemical energy

Progress in Materials Science, Journal Year: 2025, Volume and Issue: 151, P. 101427 - 101427

Published: Jan. 7, 2025

Language: Английский

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Copper Nanoparticles Anchored on the Metal–Organic Framework as Recyclable Catalyst for CO₂ Fixation to High-Value Compounds

ACS Applied Nano Materials, Journal Year: 2024, Volume and Issue: 7(13), P. 15488 - 15497

Published: July 2, 2024

Language: Английский

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COF‐Topological Quantum Material Nano‐heterostructure for CO₂ to Syngas Production under Visible Light

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(16)

Published: Feb. 24, 2024

Abstract Efficient solar‐driven syngas production (CO+H 2 mixture) from CO and H O with a suitable photocatalyst fundamental understanding of the reaction mechanism are desired approach towards carbon recycling process. Herein, we report design development an unique COF‐topological quantum material nano‐heterostructure, COF@TI newly synthesized donor‐acceptor based COF two dimensional (2D) nanosheets strong topological insulator ( TI ), PbBi Te 4 . The intrinsic robust metallic surfaces act as electron reservoir, minimising fast electron‐hole recombination process, presence 6s lone pairs in Pb 2+ Bi 3+ helps for efficient binding, which responsible boosting overall catalytic activity. In variable ratio acetonitrile‐water (MeCN : O) solvent mixture produces different ratios nano‐heterostructure enables to produce higher amount more controllable compared pristine transfer route was realized Kelvin probe force microscopy (KPFM) analysis, charge density difference calculation, excited state lifetime photoelectrochemical measurements. Finally, probable mechanistic pathway has been established after identifying sites intermediates by situ DRIFTS study DFT calculation.

Language: Английский

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Polyoxometalates Embedded into Covalent Triazine Frameworks Regulating Charge Transfer for Visible-Light-Driven Synthesis of Functionalized Sulfoxides and Detoxification of Mustard Gas Simulants

ACS Sustainable Chemistry & Engineering, Journal Year: 2024, Volume and Issue: 12(4), P. 1655 - 1665

Published: Jan. 17, 2024

For environmentally friendly and sustainable development demands, visible-light-driven oxidation of sulfides has become one the most popular strategies to synthesize functionalized sulfoxides degrade mustard gas simulants. Herein, three novel polyoxometalate-based covalent triazine frameworks, SiW12-CTF (1), PW12-CTF (2) PMo12-CTF (3) (CTF = framework), were synthesized via hydrothermal reaction characterized by infrared spectroscopy, powder X-ray diffraction, XPS spectroscopy UV–vis DRS, etc. These compounds are excellent photocatalysts for selective synthesis various as well degradation 2-chloroethyl ethyl sulfide (CEES) illuminated a 10 W 425 nm LED in an O2 atmosphere. Oxygen-rich POMs with strong electronegativity modulate electronic structure create built-in electric field POM-CTFs, which promotes separation migration photogenerated carriers. Meanwhile, encapsulation POM guests into CTF induces different electron transfer behaviors, resulting photocatalytic activities. Specifically, PW12-CTF, visible-light-induced methyl phenyl sulfide, obtain sulfoxide yields 96% 88% within 2 h, respectively, is higher than (68%) SiW12 (5%). However, exhibits inferior properties, yield 35% under same conditions. The in-depth mechanism reveals that process dominated O2•– energy induced 1O2 exist system. In addition, can be used catalyze sulfur-containing maintains boosted structural stability catalytic activity after reaction.

Language: Английский

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Site-Selective Zn-Metalation in Poly-Triphenyl Amine-based Porous Organic Polymer for Solid–Gas Phase CO₂ Photoreduction

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(27), P. 34437 - 34449

Published: June 28, 2024

Harvesting solar energy to produce value-added chemicals from carbon dioxide (CO2) presents a promising route for addressing the complexities of sustainable systems and environmental issues. In this context, development metal-coordinated porous organic polymers (POPs) offers vital avenue improving photocatalytic performance motifs. The current study metal-integrated system (namely, Zn@BP-POP) developed via one-pot Friedel–Crafts (F.C.) acylation strategy, solid–gas phase photochemical CO2 reduction CO (CO2RR). postsynthetic incorporation metal (Zn) active sites on host polymeric backbone BP-POP significantly influences catalytic activity. Notably, Zn@BP-POP demonstrates good in absence any cocatalyst photosensitizer yielding while impeding competitive hydrogen evolution reaction (HER) water. experimental findings collectively propose that observed activity selectivity arise synergistic interplay between singular zinc centers light-harvesting capacity highly conjugated backbone. Further, X-ray absorption spectroscopy (XAS) analysis has highlighted prominent role played by ZnN2O4 single framework activating gaseous molecules. time-dependent density functional theory (DFT) also reveals thermodynamic feasibility CO2RR over HER under optimized conditions. This work cumulatively an effective strategy demonstrate importance metal-active effectively establish their structure-activity relationship during photocatalysis.

Language: Английский

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Modulating PCET Process via Optimizing Local Microenvironment of CdS@NiV-LDH Heterojunction for CO2 Reduction to Tunable Green Syngas Photosynthesis

Chemical Science, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

A novel CdS@NiV-LDH heterojunction with an optimized electric field microenvironment and reaction has been constructed for the photocatalytic reduction of CO 2 to tunable green syngas by rationally modulating PCET process.

Language: Английский

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Hydrogen-bond dominated phosphorus uptake by chitosan-calcium alginate coated melamine foam in ecological floating beds

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 494, P. 153303 - 153303

Published: June 18, 2024

Language: Английский

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Purification of Waste-Generated Biogas Mixtures Using Covalent Organic Framework’s High CO₂ Selectivity

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(17), P. 22066 - 22078

Published: April 17, 2024

Development of crystalline porous materials for selective CO2 adsorption and storage is in high demand to boost the carbon capture (CCS) technology. In this regard, we have developed a β-keto enamine-based covalent organic framework (VM-COF) via Schiff base polycondensation technique. The as-synthesized VM-COF exhibited excellent thermal chemical stability along with very surface area (1258 m2 g–1) capacity (3.58 mmol at room temperature (298 K). CO2/CH4 CO2/H2 selectivities by IAST method were calculated be 10.9 881.7, respectively, which further experimentally supported breakthrough analysis. Moreover, theoretical investigations revealed that carbonyl-rich sites polymeric backbone higher binding affinity energy (−39.44 KJ mol–1) compared other aromatic carbon-rich sites. Intrigued best selectivity, utilized biogas purification produced biofermentation municipal waste. Compared commercially available activated carbon, much better ability. This opens up new opportunity creation functionalized nanoporous large-scale waste-generated biogases address challenges associated environment.

Language: Английский

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