Gallium-Mediated Switch in Product Selectivity for Co2 Hydrogenation Over Ni/Ceo2 Catalysts DOI

Changxuan Zhang,

Zhourong Xiao, Hui Zhang

et al.

Published: Jan. 1, 2024

Achieving high activities and selectivity for the reverse water-gas shift (RWGS) reaction at low-temperatures continues to pose a significant challenge. Ni-based catalysts have been widely employed in CO2 hydrogenation due their strong capacity dissociate H2, but they exhibit low CO. Herein, we successfully altered product via controlling distribution of Ga species on Ni/CeO2 catalysts. When was combined with Ni form spinel NiGa2O4 (NiGa2O4/CeO2), main While, doped into CeO2 support (Ni/Ga4-CeO2), CH4. The supported exhibited excellent performance RWGS reaction, CO over 99%, production rate as 74.5 mmol/gcat·h 450 oC 24000 mL/gcat·h, without any loss activity after 72 h. Ni/Ga4-CeO2, containing metallic abundant oxygen vacancies, enhanced methanation process, conversion 81.38%, CH4 136 mmol/gcat·h. CO-TPD analysis revealed that NiGa2O4/CeO2 catalyst weak adsorption CO*, which played key role enhancing towards Subsequent in-situ DRIFTS further confirmed differences obtained from NiGa4/CeO2 Ni/Ga4-CeO2 were formation different intermediate surface, leading change products. This study provides new idea switch reduction by species.

Language: Английский

Recent Advances in Hydrogenation of CO2 to CO with Heterogeneous Catalysts Through the RWGS Reaction DOI
Wenting Zhang, Jiashu Sun, Hongli Wang

et al.

Chemistry - An Asian Journal, Journal Year: 2024, Volume and Issue: 19(4)

Published: Jan. 27, 2024

Abstract With the continuous increase in CO 2 emissions, primarily from combustion of coal and oil, ecosystem faces a significant threat. Therefore, as an effective method to minimize issue, Reverse Water Gas Shift (RWGS) reaction which converts towards attracts much attention, is environmentally‐friendly mitigate climate change lessen dependence on fossil fuels. Nevertheless, inherent thermodynamic stability kinetic inertness big challenge under mild conditions. In addition, it remains another fundamental RWGS owing selectivity issue caused by further hydrogenation CH 4 . Up till now, series catalysis systems have been developed for reduction produce CO. Herein, research progress well‐performed heterogeneous catalysts were summarized, including catalyst design, catalytic performance mechanism. This review will provide insights into efficient utilization promote development reaction.

Language: Английский

Citations

16

Designing Ni-in intermetallic alloy compounds for high activity and selectivity in low-temperature RWGS reaction DOI
Zhourong Xiao,

Changxuan Zhang,

Jianmin Gu

et al.

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 160529 - 160529

Published: Feb. 1, 2025

Language: Английский

Citations

2

Understanding and Tuning the Effects of H2O on Catalytic CO and CO2 Hydrogenation DOI
Mingrui Wang, Guanghui Zhang, Hao Wang

et al.

Chemical Reviews, Journal Year: 2024, Volume and Issue: 124(21), P. 12006 - 12085

Published: Oct. 31, 2024

Catalytic COx (CO and CO2) hydrogenation to valued chemicals is one of the promising approaches address challenges in energy, environment, climate change. H2O an inevitable side product these reactions, where its existence effect are often ignored. In fact, significantly influences catalytic active centers, reaction mechanism, performance, preventing us from a definitive deep understanding on structure-performance relationship authentic catalysts. It necessary, although challenging, clarify provide practical strategies tune concentration distribution optimize influence. this review, we focus how induces structural evolution catalysts assists processes, as well efforts understand underlying mechanism. We summarize discuss some representative tuning for realizing rapid removal or local enrichment around catalysts, along with brief techno-economic analysis life cycle assessment. These fundamental understandings further extended reactions CO CO2 reduction under external field (light, electricity, plasma). also present suggestions prospects deciphering controlling applications.

Language: Английский

Citations

11

Size‐Controlled Ni Nanoparticles Confined into Amino‐Modified Mesoporous Silica for Efficient Hydrodeoxygenation of Bio‐Derived Aromatic Aldehyde DOI Open Access

Zidan Zou,

Yue Shen, Chun Chen

et al.

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 8, 2025

Abstract For size‐sensitive catalytic reaction systems, precise control of geometric size heterogeneous transition metal catalysts, especially for non‐noble metals, is in desperate need and also a great challenge. Here, highly dispersed Ni nanoparticles (NPs) anchored within mesoporous silica (MS) fabricated through hybrid strategy amino‐modification vacuum‐impregnation. The NPs Ni/MS catalyst can be precisely regulated from 2.2 to 12.6 nm, causing variation the proportion low high coordination sites atoms. catalysts show volcanic trend between 2‐methoxy‐4‐methylphenol (MMP) yield geometry hydrodeoxygenation (HDO) bio‐derived vanillin, Ni/MS‐4.8 with middle (4.8 nm) shows optimal HDO performance highest MMP productivity 19.5 g −1 h . DFT calculation demonstrates that medium‐sized possesses abundant low/high coordinated atoms, wherein atoms facilitate adsorption H 2 promote dissociation activating C═O C─O bonds, thus displays superior reaction. This work paves way applicating catalysis.

Language: Английский

Citations

1

Oxide Support Inert in Its Interaction with Metal but Active in Its Interaction with Oxide and Vice Versa DOI

Cui Dong,

Rongtan Li, Zhenping Qu

et al.

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

Published: April 9, 2025

Supported metal or oxide nanostructures catalyze many industrial reactions, where the interaction of overlayer with its support can have a substantial influence on catalytic performance. In this work, we show that small Pt species be well stabilized CeO2 under both H2-containing and O2-containing atmospheres but sintering happens SiO2, indicating is active whereas SiO2 inert in Pt-support interaction. On other hand, Co (CoOx) supported maintain low-valence Co2+ state air during CO2 hydrogenation to CO, strong CoOx SiO2. However, has weak easily reduced metallic reaction producing CH4. Thus, active, for CoOx-support interaction, which counter common sense from Pt/oxide systems. Systematic studies stability behaviors nanocatalysts various oxides reducibility supports used describe catalyst-support Oxide high low metal-oxygen bond strength interact strongly metals, showing metalphilicity. Conversely, oxides, having oxidephilicity.

Language: Английский

Citations

1

Tuning Catalytic Activity of CO2 Hydrogenation to C1 Product via Metal Support Interaction Over Metal/Metal Oxide Supported Catalysts DOI
Weiwei Wang, Xiaoyu Zhang, S. WENG

et al.

ChemSusChem, Journal Year: 2024, Volume and Issue: 17(16)

Published: March 28, 2024

Abstract The metal supported catalysts are emerging that receiving a lot of attention in CO 2 hydrogenation to C1 products. Numerous experiments have demonstrated the support (usually an oxide) is crucial for catalytic performance. oxides used aid homogeneous dispersion particles, prevent agglomeration, and control morphology owing interaction (MSI). MSI can efficiently optimize structural electronic properties tune conversion key reaction intermediates involved hydrogenation, thereby enhancing There increasing being paid promotion effects process. However, systematically understanding about on products performance has not been fully studied yet due diversities conditions. Hence, characteristics modes elaborated detail our work.

Language: Английский

Citations

5

Constructing Co Cluster Sites for Selective CO<sub>2</sub> Hydrogenation via Phase Segregation from Co-Doped TiO<sub>2</sub> Nanocrystals DOI Creative Commons
Xiangru Wei, Yizhen Chen, Yulu Zhang

et al.

Published: Jan. 23, 2025

Article Constructing Co Cluster Sites for Selective CO2 Hydrogenation via Phase Segregation from Co-Doped TiO2 Nanocrystals Xiangru Wei 1, Yizhen Chen Yulu Zhang Liyue Lu Ma 2, Matthew M. Yung 3 and Sen 1,* 1 Department of Chemistry, University Virginia, Charlottesville, VA 22904, USA 2 National Synchrotron Light Source II, Brookhaven Laboratory, Upton, NY 11973, Bioenergy Science Technology Directorate, Renewable Energy Denver West Parkway, Golden, CO 80401, * Correspondence: [email protected] Received: 7 November 2024; Revised: January 2025; Accepted: Published: 23 2025 Abstract: This article presents a phase segregation strategy creating stable cluster catalytic sites on TiO2, enabling selective hydrogenation to CO. Through oxidative calcination, pre-synthesized Co-doped brookite nanorods transform into mixed phase, leading the species. The resulting clusters, stabilized by strong Co-TiO2 interactions during reductive hydrogenation, effectively suppress formation larger nanoparticles. undercoordinated these clusters promote high production rate with near-unit selectivity, contrasting nanoparticles, which favor CH4 under identical conditions. In-situ diffuse reflectance infrared Fourier spectroscopy (DRIFTS) analysis indicates that weakened adsorption is key their enhanced highlighting this method as promising approach efficient utilization.

Language: Английский

Citations

0

Minireview: Intensified Low-Temperature Fischer–Tropsch Reactors for Sustainable Fuel Production DOI Creative Commons
Yadolah Ganjkhanlou, Evert Boymans,

B.J. Vreugdenhil

et al.

Fuels, Journal Year: 2025, Volume and Issue: 6(2), P. 24 - 24

Published: April 1, 2025

Low-temperature Fischer–Tropsch (LTFT) synthesis converts syngas to diesel/wax at 200–250 °C. The LTFT reaction has recently received renewed interest, as it can be used for converting from renewable sources (biomass and waste) high-value fuels chemicals. Conventional reactors, such fixed-bed slurry are not entirely suitable bio-syngas conversion due their smaller scale compared fossil fuel-based processes. This review explores advancements in intensifying reactors conversion, enabling dynamic operation. Various strategies enhancing heat mass transfer discussed, including the use of microchannel structured other designs where either one or both intensified. These technologies offer improved performance economics small units by allowing flexible operation, with increased reduced risk overheating. Additionally, this presents our outlook perspectives on future intensification.

Language: Английский

Citations

0

Comparative Study of Supported Ni and Co Catalysts Prepared Using the All-in-One Method in the Hydrogenation of CO2: Effects of Using (Poly)Vinyl Alcohol (PVA) as an Additive DOI Open Access

Luisa F. Navarrete,

María Atienza‐Martínez, Inés Reyero

et al.

Catalysts, Journal Year: 2024, Volume and Issue: 14(1), P. 47 - 47

Published: Jan. 10, 2024

Two series of Ni and Co catalysts supported onto La-Al2O3 were prepared the CO2 hydrogenation reactions investigated. The catalytic performance was evaluated in terms evolution with reaction temperature conversion product (CH4 CO) yields, as well specific activities (TOF) apparent activation energies. CH4 favored over both metals while TOF for formation about three times higher than at 240–265 °C. Metallic particle size effects found, decreasing mean metallic decreased. In contrast, CO tended to increase a smallest sizes. energies very similar significantly decreased values 73–79 kJ/mol when dispersion increased. using all-in-one method, resulting (poly)vinyl alcohol (PVA) being key additive that allowed us enhance give effective catalysts. This comparative study joins few existing ones literature which based on these operated under strictly same conditions.

Language: Английский

Citations

3

Strong Metal‐Support Interactions: From Characterization, Manipulation to Application in Fischer‐Tropsch Synthesis and Atmospheric CO2 hydrogenation DOI
Wenzhe Zhang,

Heyun Lin,

Yunlei An

et al.

ChemCatChem, Journal Year: 2024, Volume and Issue: 16(15)

Published: Jan. 27, 2024

Abstract Strong metal‐support interactions (SMSI) featuring the formation of encapsulation overlayer around metal nanoparticles has drawn much attention in heterogeneous catalysis. Recent years, various novel SMSI phenomena have been observed and nature also revealed with improvement characterization techniques. Understanding effect could deepen insight into structure‐activity relationship metal‐supported catalysts, rationally guide design special metal‐interface sites to manipulate catalytic behavior chemical reaction. In this review, research progress its application CO x hydrogenation are briefly surveyed, emphasis on advanced characterization, manipulation strategy specific role Fischer‐Tropsch synthesis process, 2 methanation Reverse Water Gas Shift The current challenges perspectives for development discussed.

Language: Английский

Citations

3