Engineering CuZnOAl2O3 Catalyst for Enhancing CO2 Hydrogenation to Methanol DOI Creative Commons

Peixiang Shi,

Jiahao Han, Yuhao Tian

et al.

Molecules, Journal Year: 2025, Volume and Issue: 30(6), P. 1350 - 1350

Published: March 18, 2025

The CuZnOAl2O3 catalyst shows excellent activity and selectivity in the reaction of CO2 hydrogenation to methanol as a consequence its controllable physicochemical properties, which is expected offer an efficient route renewable energy. In this study, catalysts are engineered by special pretreatment, constructing carbonate structure on surface catalyst. Compared unmodified catalyst, optimized (CZA-H-C1) not only exhibits improved 62.5% (250 °C 3 MPa) but also retains minimal degree deactivation 9.57% over 100 h period. By characterizing with XRD, TEM, XPS situ DRIFTS spectroscopy, it was found that species Cu-based could significantly enhance shield active sites. This study offers theoretical insights practical strategies for rational design optimization high-performance heterogeneous catalysts.

Language: Английский

An overview on copper in industrial chemistry: From ancient pigment to modern catalysis DOI
Mohammad Soleiman‐Beigi, Masoud Mohammadi,

Homa Kohzadi

et al.

Coordination Chemistry Reviews, Journal Year: 2025, Volume and Issue: 529, P. 216438 - 216438

Published: Jan. 17, 2025

Language: Английский

Citations

8
Hydrogenation of CO 2 for sustainable fuel and chemical production DOI
Jingyun Ye, Nikolaos Dimitratos, Liane M. Rossi

et al.

Science, Journal Year: 2025, Volume and Issue: 387(6737)

Published: Feb. 27, 2025

Catalytic carbon dioxide (CO2) hydrogenation is a potential route for producing sustainable fuels and chemicals, but existing catalysts need improvement. In particular, identifying active sites understanding the interaction between components dynamic behavior of participant species remain unclear. This fundamental knowledge essential design more efficient stable catalysts. Because nature site (metal, oxide, carbide) main factor that determines catalytic activity catalysts, this Review focuses on various types heterogeneous have been recently reported in literature as CO2 conversion to C1 [carbon monoxide (CO), methanol (CH3OH), methane (CH4)], higher hydrocarbons. We focus establishing key connections active-site structures selectivity, regardless catalyst composition.

Language: Английский

Citations

5
Rules Describing CO2 Activation on Single-Atom Alloys from DFT-Meta-GGA Calculations and Artificial Intelligence DOI Creative Commons
Herzain I. Rivera-Arrieta, Lucas Foppa

ACS Catalysis, Journal Year: 2025, Volume and Issue: 15(4), P. 2916 - 2926

Published: Feb. 4, 2025

Single-atom alloys (SAAs) arise as a promising concept for the design of improved CO2 hydrogenation catalysts. However, from immense number possible SAA compositions and structures, only few might display properties required to be useful Thus, direct, high-throughput screening materials is inefficient. Here, we use artificial intelligence derive rules describing surface sites SAAs that provide an effective activation, crucial initial step convert molecule into valuable products. We start by modeling interaction with 780 flat stepped surfaces composed Cu, Zn, Pd hosts via high-quality DFT-mBEEF calculations. Then, apply subgroup discovery determine constraints on key physicochemical properties, out 24 offered candidate descriptive parameters, characterizing subgroups (SGs) where chemisorbed displays large elongations its C–O bonds. The identified parameters are free-atom elements constituting sites, such their electron affinity, electronegativity, radii d-orbitals. Additionally, generalized coordination selected geometrical parameter. SG applied identify space over 1500 ones in different single-atom dual-atom alloys. Some predicted were explicitly tested additional calculations confirmed significant activation.

Language: Английский

Citations

1
Low-Temperature Exsolution of Rh from Mixed ZnFeRh Oxides toward Stable and Selective Catalysts in Liquid-Phase Hydroformylation DOI Creative Commons
Daniel Delgado, Gregor Koch, Shan Jiang

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 10, 2025

The exsolution of metal nanoparticles offers a promising strategy to enhance catalyst stability and fine-tune metal–support interactions. Expanding the use exsolved in heterogeneous catalysis requires development low-temperature (T < 400 °C) processes. In this study, we report synthesis phase-pure ZnFe2–xRhxO4 oxide precursors with spinel-type crystal structure. isomorphic substitution Fe3+ host lattice by Rh3+ was confirmed X-ray diffraction Raman spectroscopy combined DFT calculations. hydrothermal method specifically chosen so that very small particles 10–20 nm were obtained, which enabled Rh particle size about 1 2 at temperatures below 200 °C hydrogen-containing atmosphere. Compared prepared conventional wet impregnation ZnFe2O4, catalysts obtained show superior properties terms selectivity toward aldehydes hydroformylation 1-hexene liquid phase. addition, there is no loss due leaching, main challenge for used phase reactions. exceptionally strong interaction imparts unique nanostructures electronic nanoparticles, as revealed electron energy (EELS) diffuse reflectance infrared Fourier transform (DRIFT) spectroscopy. specific adsorption sites on lead stronger metal–hydride weaker metal–carbonyl bonds surface, steering reaction pathway rather than olefin isomerization.

Language: Английский

Citations

1
Optimizing CO2 hydrogenation to methanol by enriching ZnOx/Cu interfacial sites in Zn-dispersed HKUST-1 derived catalysts DOI
Xiaohang Sun, Zong–Huai Liu, Yi Cheng

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2025, Volume and Issue: unknown, P. 125334 - 125334

Published: April 1, 2025

Language: Английский

Citations

1
Tandem Cu/ZnO/ZrO2-SAPO-34 System for Dimethyl Ether Synthesis from CO2 and H2: Catalyst Optimization, Techno-Economic, and Carbon-Footprint Analyses DOI Creative Commons
Jasan Robey Mangalindan, Fatima Mahnaz,

Jenna Vito

et al.

ACS Engineering Au, Journal Year: 2025, Volume and Issue: unknown

Published: April 8, 2025

Language: Английский

Citations

1
Design Principles of Catalytic Materials for CO2 Hydrogenation to Methanol DOI Creative Commons
Thaylan Pinheiro Araújo, Sharon Mitchell, Javier Pérez‐Ramírez

et al.

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

Published: Sept. 19, 2024

Abstract Heterogeneous catalysts are essential for thermocatalytic CO 2 hydrogenation to methanol, a key route sustainable production of this vital platform chemical and energy carrier. The primary catalyst families studied include copper‐based, indium oxide‐based, mixed zinc–zirconium oxides‐based materials. Despite significant progress in their design, research is often compartmentalized, lacking holistic overview needed surpass current performance limits. This perspective introduces generalized design principles catalytic materials ‐to‐methanol conversion, illustrating how complex architectures with improved functionality can be assembled from simple components (e.g., active phases, supports, promoters). After reviewing basic concepts ‐based methanol synthesis, engineering explored, building complexity single binary ternary systems. As nanostructures strongly depend on reaction environment, recent operando characterization techniques machine learning approaches examined. Finally, common rules centered around symbiotic interfaces integrating acid–base redox functions role optimization identified, pinpointing important future directions methanol.

Language: Английский

Citations

6
Synergistic Effects of Complex Cu Species in Cu–MgO Catalysts for the Water Gas Shift Reaction DOI
Mei‐Yao Wu, Shanqing Li, Wei-Wei Wang

et al.

ACS Catalysis, Journal Year: 2024, Volume and Issue: unknown, P. 13723 - 13735

Published: Aug. 30, 2024

Language: Английский

Citations

4
Experimental PSA reactor for methanol-enhanced production VIA CO2 hydrogenation DOI Creative Commons
Gonzalo Pascual-Muñoz, Rubén Calero-Berrocal, Marcos Larriba

et al.

Separation and Purification Technology, Journal Year: 2024, Volume and Issue: 351, P. 128030 - 128030

Published: May 20, 2024

Methanol synthesis via catalytic CO2 hydrogenation has emerged as one of the main ways to valorize CO2. The problem is that methanol reaction thermodynamically controlled, and there a parallel endothermic reaction, reverse water gas shift (RWGS), so low production ratios are achieved. In this scenario, process intensification, particularly multifunctional reactors where separation occur simultaneously, great interest. Sorption-enhanced processes (SERP) technologies widely used in equilibrium-controlled increase reagent conversion through selective product removal. Various authors have proposed SERP for methanol, but most them simulations studies it difficult find experimental data. aim work study selectivity based on four-step PSA reactor. been carried out with commercial Cu/ZnO/Al2O3 catalyst 3A zeolite adsorbent. Conversions beyond equilibrium achieved process, even complete at 50 bar, 250 °C, 300 °C. cyclic high conversions far from all range temperatures, 200–300 best results yield °C followed closely by 200 It worth mentioning methane detected transitory state bar. Also, purge step studied, concluding necessary adsorbent regeneration, improving steady state.

Language: Английский

Citations

3
Impact of quantum size effects to the band gap of catalytic materials: a computational perspective* DOI Creative Commons

Elisabetta Inico,

Clara Saetta,

Giovanni Di Liberto

et al.

Journal of Physics Condensed Matter, Journal Year: 2024, Volume and Issue: 36(36), P. 361501 - 361501

Published: June 3, 2024

Abstract The evolution of nanotechnology has facilitated the development catalytic materials with controllable composition and size, reaching sub-nanometer limit. Nowadays, a viable strategy for tailoring optimizing activity involves controlling size catalyst. This is underpinned by fact that properties reactivity objects dimensions on order nanometers can differ from those corresponding bulk material, due to emergence quantum effects. Quantum effects have deep influence band gap semiconducting materials. Computational studies are valuable predicting estimating impact perspective emphasizes crucial role modeling when simulating nanostructured It provides comprehensive overview fundamental principles governing physics confinement in various experimentally observable nanostructures. Furthermore, this work may serve as tutorial electronic simple nanostructures, highlighting working at nanoscale, finite material lead an increase because confinement. aspect sometimes overlooked computational chemistry focused surfaces

Language: Английский

Citations

3