Materials Design for Photocatalytic CO₂ Conversion to C₂₊ Products

Chemistry of Materials, Journal Year: 2024, Volume and Issue: 36(4), P. 1793 - 1809

Published: Feb. 6, 2024

Recently, there has been a burgeoning interest in photocatalytic CO2 conversion from the general public and scientific community. In theory, this technology can harness abundant solar energy to transform waste into valuable chemicals, holding potential replace certain conventional chemical engineering methods for industrial production sustainable eco-friendly manner. Despite these promising aspects, practical application of hampered by its limited activity selectivity. Numerous efforts have dedicated enhancing over past few decades, driving progress. However, noticeable shortage research focused on improving selectivity process, particularly concerning generation high-value C2+ products. Perspective, our primary objective is delve recent developments conversion, with specific emphasis Our discussion will commence elucidating fundamental principles mechanisms underlying C–C coupling reaction. Subsequently, we provide an overview current techniques available fine-tuning reactions toward formation Finally, conclude perspective offering insights prospects advancements field.

Language: Английский

---

Defect and interface engineering for promoting electrocatalytic N-integrated CO2 co-reduction

CHINESE JOURNAL OF CATALYSIS (CHINESE VERSION), Journal Year: 2024, Volume and Issue: 57, P. 1 - 17

Published: Feb. 1, 2024

Language: Английский

---

CO₂ Reduction by an Iron(I) Porphyrinate System: Effect of Hydrogen Bonding on the Second Coordination Sphere

Inorganic Chemistry, Journal Year: 2024, Volume and Issue: 63(10), P. 4474 - 4481

Published: Feb. 26, 2024

Transforming CO2 into valuable materials is an important reaction in catalysis, especially because concentrations the atmosphere have been growing steadily due to extensive fossil fuel usage. From environmental perspective, reduction of should be catalyzed by environmentally benign catalyst and avoid use heavy transition-metal ions. In this work, we present a computational study novel iron(I) porphyrin for reduction, namely, with tetraphenylporphyrin ligand analogues. particular, investigated one meso-phenyl groups substituted o-urea, p-urea, or o-2-amide groups. These substituents can provide hydrogen-bonding interactions second coordination sphere bound ligands assist proton relay. Furthermore, our studies bicarbonate phenol as stabilizers donors mechanism. Potential energy landscapes double protonation porphyrinate are reported. The work shows that bridges urea/amide iron center provides tight bonding pattern strong facilitates easy delivery CO2. Specifically, low-energy shuttle mechanism form CO water efficiently. o-urea group locks orientation helps ideal transfer, while there more mobility lesser stability o-amide position instead. Our calculations show leads proton-transfer barriers, line experimental observation. We then applied electric-field-effect estimate effects on two steps reaction. describe perturbations enhance driving forces used make predictions about how catalysts further engineered enhanced processes.

Language: Английский

---

The Pd/ZrO2 catalyst inversely loaded with various metal oxides for methanol synthesis from carbon dioxide

Journal of Catalysis, Journal Year: 2024, Volume and Issue: 434, P. 115527 - 115527

Published: May 1, 2024

Language: Английский

---

Double-Edged Sword Effect of Classical Strong Metal–Support Interaction in Catalysts for CO₂ Hydrogenation to CO, Methane, and Methanol

ACS Materials Letters, Journal Year: 2023, Volume and Issue: 5(10), P. 2629 - 2647

Published: Aug. 30, 2023

Interesting phenomena such as encapsulation, charge transfer, and bond formation, etc. induced by classical strong metal–support interaction (SMSI) during high-temperature reduction have received wide attention for their potential to determine the catalytic behavior of supported metal catalysts. However, a systematically scientific understanding about effects SMSI on CO2 hydrogenation performance is still insufficient primarily due diversities in catalysts reaction conditions. Here, we outline "double-edged sword effects" activity, stability, even selectivity C1 high-value compounds (CO, methane, methanol). Specifically, moderate could efficiently optimize structural electronic properties tune conversion key intermediates involved hydrogenation, thereby enhancing performance. Nevertheless, excessive fatal methanation methanol synthesis catalysts, because encapsulation active centers suppresses further reactive intermediates. Additionally, alter regulating dissociation H2 breakage C–O bonds. Subsequently, dependencies are emphasized with aim providing guidance developing an appropriate rational design. To conclude, highlighted perspectives deeper also presented.

Language: Английский

---

Advancement and State-of-art of heterogeneous catalysis for selective CO2 hydrogenation to methanol

Coordination Chemistry Reviews, Journal Year: 2023, Volume and Issue: 497, P. 215409 - 215409

Published: Sept. 15, 2023

Language: Английский

---

Stable Cuδ+ species - Catalyzed CO₂ hydrogenation to methanol in silanol nests on Cu/S-1 catalyst

Applied Energy, Journal Year: 2024, Volume and Issue: 365, P. 123247 - 123247

Published: April 24, 2024

Language: Английский

---

Paired Electrosynthesis of Formaldehyde Derivatives from CO₂ Reduction and Methanol Oxidation

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 63(2)

Published: Nov. 29, 2023

Abstract Utilizing CO 2 ‐derived formaldehyde derivatives for fuel additive or polymer synthesis is a promising approach to reduce net carbon dioxide emissions. Existing methodologies involve converting methanol by thermal hydrogenation, followed electrochemical thermochemical oxidation produce formaldehyde. Adding the conventional pathway, we propose new simultaneously generate at both electrodes partial and direct reduction of . To achieve this, method directly cathode required. Still, it has been scarcely reported previously due acidity formic acid intermediate facile over‐reduction methanol. By enabling activation subsequent stabilization respectively in solvent, were able implement strategy where generated alongside anode. Further mechanism studies revealed that protons supplied from anodic reaction contribute product. Additionally, was found cathodic derivative Faradaic efficiency can be further increased through prolonged electrolysis time up 50 % along with maximum 90 %.

Language: Английский

---

Parametric analysis of CO2 hydrogenation via Fischer-Tropsch synthesis: A review based on machine learning for quantitative assessment

International Journal of Hydrogen Energy, Journal Year: 2024, Volume and Issue: 59, P. 1023 - 1041

Published: Feb. 14, 2024

This review focuses on the parametric impacts upon conversion and selectivity during CO2 hydrogenation via Fischer-Tropsch (FT) synthesis using iron-based catalyst to provide quantitative evaluation. Using all collected data from reported literatures as training dataset artificial neural networks (ANNs) in TensorFlow, three categorized parameters (namely: operational, informatic mass transfer) were deployed assess their conversions (CO2) selectivity. The lump kinetic power expressions among literature reports compared, best fit model is one that was proposed by this work without arbitrarily assuming values of individual partial pressure (CO H2). More than five sets binary systematically investigated find out corresponding evolving patterns Aided machine learning, tailoring product distributions based specific or for optimization purpose practically achievable deploying predictions generated ANNs work.

Language: Английский

---

Versatile stereoselective oxidative alkoxycarbonylation of styrenes at room-temperature

Journal of Catalysis, Journal Year: 2024, Volume and Issue: 432, P. 115397 - 115397

Published: March 1, 2024

Carbonylation reactions carried out at room temperature and atmospheric pressure of carbon monoxide are highly attractive extremely rare the same time. Here, oxidative alkoxycarbonylation styrenes to industrially relevant cinnamates has been developed under such a mild conditions (rt, 1 atm CO) in presence palladium(II) complex bearing bis(aryl)acenaphthenequinonediimine ligand, benzoquinone p-toluenesulfonic acid. Remarkably, variously substituted styrene derivatives have efficiently carbonylated using nearly stoichiometric amount alcohols, with dramatic reduction waste. Even reluctant internal alkenes shown be compatible these carbonylative conditions. In consideration experimental results DFT calculations mechanistic rationale proposed. Based on this study, found promote final palladium reoxidation, boost reaction unprecedent The present methodology successfully exploited for synthesis high value-added cinnamoyl glycerols cinnamic acid sugar esters, including 6-O-p-coumaroyl-D-glucose natural product.

Language: Английский

---