Recent advancements and perspectives of the CO2 hydrogenation reaction

Green Carbon, Journal Year: 2023, Volume and Issue: 1(2), P. 133 - 145

Published: Oct. 23, 2023

Owing to excessive carbon dioxide (CO2) emissions, which cause severe environmental issues, the conversion and utilization of CO2 have received increasing attention. its high efficiency potential for industrial applications, converting into value-added chemicals via thermocatalytic hydrogenation is a highly effective route among electrocatalytic, photocatalytic, conversion. In past two decades, our group has developed novel technologies produce such as aliphatic hydrocarbons, methanol (MeOH), ethanol, aromatics (especially para-xylene, PX). this review, we summarize strategy rational design catalysts, including low-temperature MeOH synthesis capsule catalysts tandem catalysis. We also discuss challenges opportunities hydrogenation, capture, H2 prices, taxes. hope inspire new ideas through exploration reaction paths.

Language: Английский

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CO2 hydrogenation to methanol over the copper promoted In2O3 catalyst

Journal of Energy Chemistry, Journal Year: 2024, Volume and Issue: 93, P. 135 - 145

Published: Jan. 24, 2024

Language: Английский

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Nickel-modified In2O3 with inherent oxygen vacancies for CO2 hydrogenation to methanol

Science China Chemistry, Journal Year: 2024, Volume and Issue: 67(5), P. 1715 - 1728

Published: Jan. 23, 2024

Language: Английский

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Thermochemical CO₂ Reduction to Methanol over Metal-Based Single-Atom Catalysts (SACs): Outlook and Challenges for Developments

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(34), P. 23649 - 23662

Published: Aug. 20, 2024

The conversion of thermodynamically inert CO

Language: Английский

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Enhanced Surface Charge Localization Over Nitrogen-Doped In₂O₃ for CO₂ Hydrogenation to Methanol with Improved Stability

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(9), P. 6154 - 6168

Published: April 20, 2023

Indium oxide (In2O3) is active and promising for selective hydrogenation of CO2 to methanol. However, it suffers from over-reduction at elevated temperatures, causing deactivation. Herein, a nitrogen-doped In2O3 (N–In2O3) catalyst was prepared using plasma-intensified nitrogen-doping technology. It confirmed that nitrogen doping effective the stabilization In2O3. The doped enhances surface charge localization, which inhibits on limits generation excessive oxygen vacancies. also serves as site, synergistically with vacancy, leads an enhanced dissociation adsorbed CO* intermediates. electron-rich causes strong adsorption CO N–In2O3 formation free CO. A significantly improved methanol selectivity higher turnover frequency (TOF) thus achieved N–In2O3, compared un-doped For example, 21,000 cm3 h–1 gcat–1, 300 °C, 5 MPa, TOF reaches 37.0 75.1%, while only 16.0 62.3%. Different pristine In2O3, takes route This explains reason why possesses

Language: Английский

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Synergistic Catalysis at the Ni/ZrO_2–x Interface toward Low-Temperature CO₂ Methanation

ACS Applied Materials & Interfaces, Journal Year: 2023, Volume and Issue: 15(15), P. 19021 - 19031

Published: April 6, 2023

The CO2 methanation reaction, which achieves the carbon cycle and gains value-added chemicals, has attracted much attention, but design exploitation of highly active catalysts remain a big challenge. Herein, zirconium dioxide-supported Ni toward low-temperature are obtained via structural topological transformation NiZrAl-layered double hydroxide (LDH) precursors, have feature an interfacial structure (Ni-O-Zr3+-Vö) between nanoparticles ZrO2-x support (0 < x 1). optimized catalyst (Ni/ZrO2-x-S2) exhibits exceptional conversion (∼72%) at temperature as low 230 °C with ∼100% selectivity to CH4, without obvious deactivation within 110 h reaction high gas hourly space velocity 30,000 mL·g-1·h-1. Markedly, space-time yield CH4 reaches up ∼0.17 molCH4·gcat-1·h-1, is superior previously reported evaluated under similar conditions. Both in situ/operando investigations (diffuse reflectance infrared Fourier transform spectroscopy X-ray absorption fine structure) catalytic evaluations substantiate synergistic catalysis Ni/ZrO2-x interface: Zr3+-Vö facilitates activation adsorption CO2, while H2 molecule experiences dissociation metallic sites. This work demonstrates that metal-support interface effect plays key role improving behavior methanation, can be extended other high-performance heterogeneous structure-sensitive systems.

Language: Английский

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Photo‐Induced Switching of CO₂ Hydrogenation Pathway towards CH₃OH Production over Pt@UiO‐66‐NH₂(Co)

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(9)

Published: Jan. 11, 2023

It is highly desired to achieve controllable product selectivity in CO2 hydrogenation. Herein, we report light-induced switching of reaction pathways hydrogenation towards CH3 OH production over actomically dispersed Co decorated Pt@UiO-66-NH2 . CO, being the main reverse water gas shift (RWGS) pathway under thermocatalysis condition, switched via formate with assistance light irradiation. Impressively, space-time yield photo-assisted (1916.3 μmol gcat-1 h-1 ) about 7.8 times higher than that without at 240 °C and 1.5 MPa. Mechanism investigation indicates upon irradiation, excited UiO-66-NH2 can transfer electrons Pt nanoparticles sites, which efficiently catalyze critical elementary steps (i.e., -to-*HCOO conversion), thus suppressing RWGS a high selectivity.

Language: Английский

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Mitigating the Poisoning Effect of Formate during CO₂ Hydrogenation to Methanol over Co-Containing Dual-Atom Oxide Catalysts

JACS Au, Journal Year: 2024, Volume and Issue: 4(3), P. 1048 - 1058

Published: Feb. 2, 2024

During the hydrogenation of CO2 to methanol over mixed-oxide catalysts, strong adsorption and formate poses a barrier for H2 dissociation, limiting selectivity productivity. Here we show that by using Co-containing dual-atom oxide poisoning effect can be countered separating site dissociation intermediates. We synthesized Co- In-doped ZrO2 catalyst (Co–In–ZrO2) containing atomically dispersed Co In species. Catalyst characterization showed atoms were in proximity each other owing random distribution. reaction, atom was responsible species, while nearby promoted adsorbed The cooperative increased 86% catalyst, productivity 2-fold comparison single-atom catalysts. This extended Co–Zn Co–Ga doped work presents different approach designing catalysts based on preferential substrates intermediates instead promoting mitigate poisonous effects

Language: Английский

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N-Heterocyclic Carbene Moiety in Highly Porous Organic Hollow Nanofibers for Efficient CO₂ Conversions: A Comparative Experimental and Theoretical Study

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(2), P. 718 - 727

Published: Jan. 2, 2024

Global warming and climate change are two severe environmental dangers brought on by the steady rise in carbon dioxide (CO2) concentration atmosphere. Thus, order to reduce this problem, it is essential find an efficient material for high CO2 capture that can simultaneously exhibit good catalytic activity utilization into useful chemicals. Herein, we report synthesis of N-heterocyclic carbene-based porous organic polymers (NHC-01 NHC-02) using Friedel–Crafts reaction with imidazolium salt bi-phenyl. Among polymers, NHC-01 exhibited outstanding stability, flexibility, BET surface area (1298 m2 g–1). displayed a uptake capacity 2.85 mmol g–1 under 1.0 bar pressure at 273 K. NHC-01/02 has been utilized as metal-free organocatalyst conversion due its area, absorption capacity, bears NHC moiety network. selectively reduced methanol via hydrosilylation complete silane atmospheric pressure. Furthermore, catalyst also shows toward N-formylation reductive cyclization reactions, which showed yields up least four cycles. The mechanisms studied theoretical simulation density functional theory (DFT), intermediates have appropriate free energy level promote low barrier.

Language: Английский

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Rational Control of Oxygen Vacancy Density in In₂O₃ to Boost Methanol Synthesis from CO₂ Hydrogenation

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(13), P. 9887 - 9900

Published: June 18, 2024

Oxygen vacancies (Ov) in reducible metal oxides are the vital active sites for methanol synthesis via a CO2 hydrogenation technology. However, relationship between density of Ov and performance is still ambiguous, it shows lack versatile strategy to precisely tailor number Ov. In this study, with In2O3 as representatively catalytic component, functional theory computation confirms that property, especially density, pivotal enhancing selectivity by suppressing undesirable reverse water–gas shift reaction CO formation, which attributed unique electronic atoms around To verify theoretical results, we report protocol optimize concentration on sequential carbonization oxidation (SCO) treatments In-based metal–organic frameworks, during consumption carbon species structural reconstruction crystal regulated particle size varying temperature. The In2O3-5 catalyst carbonized oxidized at 500 °C exhibits good (72.3%) conversion 9.9% under 330 °C, 3 MPa, high space velocity 12,000 L–1 kgcat–1 h–1. Multiple situ characterizations clarify proposed property regulating SCO convenient boost altering process HCOO* intermediate-dominated pathway. Our work provides design will shed light rational oxide-based catalysts controllable density.

Language: Английский

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