Journal of CO2 Utilization最新文献_第3页

Machine learning integration in thermodynamics: Predicting CO2 mixture saturation properties for sustainable refrigeration applications

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-04-04 DOI: 10.1016/j.jcou.2025.103072

Carlos G. Albà , Ismail I.I. Alkhatib , Lourdes F. Vega , Fèlix Llovell

The need for sustainable alternatives in refrigeration has grown as Europe enforces mandates on avoiding high global warming potential (GWP) refrigerants. CO₂-based refrigerants have emerged as a promising choice in response, distinguished by its low GWP and reduced flammability, compared to formulated hydrofluoroolefins, thus offering a safer and sustainable solution in the context of next generation drop-in refrigerants. This study presents a machine-learning-based methodology to estimate the saturation properties of CO₂-based mixtures, allowing for the precise tuning of molecular-based models like the polar soft-SAFT, used for technical evaluation, without relying on experimental data, often unavailable for such systems. The approach departs from the thermodynamic characterization of several pure-components, including novel fluorine-based refrigerants. The parametrization allows an excellent description of the vapor pressure, saturated densities, and latent heat. Next, a constant, temperature-independent binary parameter is used to estimate the solubility profiles of CO₂-derived mixtures in selected refrigerants. The model effectively captures azeotropic and zeotropic behaviors, demonstrating its strength in fine-tuning solubility with minimal corrections. Subsequently, data from the molecular characterization via polar soft-SAFT is used as output targets to train a machine learning algorithm based on artificial neural networks, enabling the prediction of mixture saturation properties out of the training dataset's scope. Using COSMO σ-profiles, the developed ANN demonstrates high efficiency in predicting saturation bubble and dew temperatures, achieving R² > 0.9999, RMSE< 0.0959, AARD < 0.0220 %, and NMAD of 0.00044. Statistical analysis confirms minimal mean deviations, with outliers limited to 2.63 % for bubble and 2.44% for dew phase predictions, respectively.

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引用次数: 0

Photocatalytic and surface consequences of thermal treatments on Pt nanoparticles onto carbon nitrides during CO2-to-CO conversion 在二氧化碳转化为二氧化碳的过程中，对氮化碳上的铂纳米颗粒进行热处理的光催化效应和表面效应

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-03-29 DOI: 10.1016/j.jcou.2025.103068

S. Vaquero-Vílchez , P. Nimax , E. Valtierra-Martinez , I. Ayesta , I. Agirrezabal-Telleria

Photocatalysis is an emerging alternative to convert CO₂ into relevant products, but it faces technological challenges related to charge recombination and low efficiency. Thermally coupled gas phase photocatalysis can address these issues by lowering reaction temperatures and improving process efficiency. This work demonstrates that defect engineering, combined with Pt impregnation at various metal dispersion and sizes, can enhance photocatalytic properties in g-C₃N₄ materials. Structural changes in g-C₃N₄ and Pt oxidation state modification, significantly impact CO productivity from CO₂. This study investigates how thermal treatments in H₂ affect defect and thus vacancy formation in g-C₃N₄. Materials with 2 wt% Pt²⁺ species generate C–N₃ vacancies, while Pt⁰ species with the same content lead to both C–N₃ and N–C₃ vacancies– within g-C₃N₄. These differences exhibit distinct reaction trends under dark conditions or upon light irradiation. To further understand these effects, detailed XPS analyses clarify the impact of reaction conditions on the material after pretreatment and catalysis. The findings show that g-C₃N₄ materials can reform their C–Nbonds after electron excitation through light exposure, enhancing and stabilizing the reaction's productivity. As a result, CO productivities up to 1.1 mmol·g_cat⁻¹·h⁻¹ are achieved. This work is expected to contribute to understanding the effect of thermal treatment on carbon nitrides, particularly regarding defect engineering, and more broadly, the effects of temperature in photocatalysis.

光催化是将二氧化碳转化为相关产品的一种新兴替代方法，但它面临着与电荷重组和低效率有关的技术挑战。热耦合气相光催化技术可以通过降低反应温度和提高工艺效率来解决这些问题。这项研究表明，缺陷工程与不同金属分散度和尺寸的铂浸渍相结合，可以增强 g-C3N4 材料的光催化性能。g-C3N4 的结构变化和铂氧化态的改变会显著影响二氧化碳的 CO 产率。本研究探讨了 H2 中的热处理如何影响 g-C3N4 中的缺陷和空位形成。含有 2 wt% Pt2+ 物种的材料会产生 C-N3 空位，而相同含量的 Pt0 物种则会在 g-C3N4 中产生 C-N3 和 N-C3 空位。这些差异在黑暗条件下或光照下表现出截然不同的反应趋势。为了进一步了解这些影响，详细的 XPS 分析阐明了预处理和催化后反应条件对材料的影响。研究结果表明，g-C3N4 材料在光照射下受到电子激发后，其 C-N 键可以发生重整，从而提高并稳定了反应的生产率。因此，一氧化碳的生产率可达 1.1 mmol-gcat-1-h-1。这项研究有望帮助人们了解热处理对碳氮化物的影响，特别是缺陷工程方面的影响，以及更广泛的光催化过程中温度的影响。

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引用次数: 0

Elucidating operational drivers of CO2 transfer and utilization efficiency in photosynthetic algae cultivation systems

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-03-29 DOI: 10.1016/j.jcou.2025.103069

Mauro Lua , Everett Eustance , Arnav Deshpande , John McGowen , Lieve M.L. Laurens

While photosynthetic algae-based systems have shown promise for reducing the carbon footprint associated with biofuel and biochemical production due higher yields than terrestrial crops, there are challenges associated with CO₂ delivery and utilization resulting from the chemical and physical environment experienced. Point-source CO₂ delivery is a critical component of intensive algal cultivation, but a significant fraction of the CO₂ sparged into the aqueous environment is lost. In this context, we review the theoretical considerations for deconvoluting carbon transfer efficiency (CTE) and carbon utilization efficiency (CUE), specifically in microalgal cultivation in response to changes in media formulation and alkalinity. We introduce an empirical and operational approach to increase the efficiency of CO₂ transfer and ultimately prime algal cultures for photosynthetic carbon assimilation. We define operational boundaries for improving CUE under a neutral pH regime, with conditions that maintain high algal biomass productivity. Our work supports both the implementation of strategies for increasing CUE as well as provides a framework for monitoring inorganic and organic carbon balances in controlled aqueous systems. The integration of water chemistry in media formulation with dissolved inorganic carbon (DIC) and alkalinity are primary drivers of the inorganic carbon flux from a concentrated CO₂ source towards an accessible carbon source for microalgae. We outline a systematic approach by leveraging control over carbon delivery, operational pH in the neutral pH regime, and alkalinity to match available DIC of the media with the demands of the algae to help optimize CTE and CUE. This control increases the feasibility of large-scale biotic CO₂ capture in aqueous systems.

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引用次数: 0

Impact of particle breakage on the carbonation of argon oxygen decarburization slag - limitations and energy assessment

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-03-28 DOI: 10.1016/j.jcou.2025.103073

Nina Miladinović , Luka Ceyssens , Giuseppe Granata , Tom Van Gerven

Disposing waste from the steel-making industry and the ongoing rise in global carbon dioxide emissions represent significant challenges to overcome. Carbonation of steel slags, the main waste material formed in steelmaking processes, is one of the possible solutions. In this research, three different kinds of mills are compared in order to most effectively approach the carbonation of argon oxygen decarburization (AOD) steel slag while simultaneously milled. Using breakage potential as a parameter for quantitative comparison, it is shown that the planetary ball mill is noticeably performing better than the vibratory mill and the McCrone mill – up to 39 % in terms of breakage of particles. The breakage potential correlates well with the carbonation rate at all three examined speeds (200 rpm, 500 rpm and 800 rpm) in the planetary ball mill. However, it is estimated that energy up to 120 kJ/g is used for the breakage of particles. Energy applied above this threshold contributes mainly to the agglomeration, but at different rates depending on the implemented speed. This difference is due to the varying contribution of two influencing parameters during simultaneous carbonation and milling - the presence of water and the number of collisions of the grinding balls with the AOD steel slag. The present work gives insights into the breakage of steel slag particles, their carbonation potential and limitations for achieving higher carbonation rates as well as predicted energy usage to obtain these processes.

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引用次数: 0

Orientational-growth of Cu2O {111} or {110} facets induced by frustules for CO2-H2O specific photo(electro)chemical conversion into methanol/ethanol under visible-light

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-03-27 DOI: 10.1016/j.jcou.2025.103071

Michele Aresta , Tomasz Baran , Domenico Caringella , Shambel G. Wasse , Yusuf I. Abubakar , Alessandra Petrucciani , Alessandra Norici , Ernesto Mesto , Elvira De Giglio , Roberto Comparelli , Angela Dibenedetto

p-Type-semiconductor Cu₂O facets {111} (octahedral) and {110} (rhombododecahedral) present a higher photo(electro)catalytic activity towards CO2RRs (CO₂ Reduction Reaction) than {100} (cubic). Two frustules (the siliceous skeleton of microalgae Diatoms) having a different morphology, namely: Navicula sp. (Nsp, elongated pore-shape) and Conticribra weissflogii (Cw, round pore-shape) have been used for the first time in this work as template for the orientational growth of Cu₂O facets. Frustules are calcinated at 700 °C to avoid residual organics that may give false positives during photo(electro)catalysis. Each of the frustules is found to induce a facet of Cu₂O preferentially. Nsp induces the {111} facet (Band-gap=2.26 eV), while Cw preferentially induces the {110} facet (Band-gap=1.96 eV). Under visible light irradiation, Nsp-grown Cu₂O converts CO₂ and H₂O into methanol, while Cw-grown Cu₂O produces ethanol. The different behaviour is related to the different Cu-Cu distance (the active catalytic centres) in the two facets.

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引用次数: 0

Mid-temperature CO2 deoxygenation to CO over Fe-CeO2 中温二氧化碳在 Fe-CeO2 上脱氧生成 CO

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-03-26 DOI: 10.1016/j.jcou.2025.103074

Jing-Ting Huang, Ruo-Yun Lin, Tzu-Hsun Tsai, Tzu-Peng Lin, Shawn D. Lin

CO₂ capture and utilization is a must for easing the global warming caused by the uses of fossil fuels. We examine M-CeO₂ (M = Cu, Co, and Fe @M/Ce = 2/8) prepared by coprecipitation and hard template synthesis. Fe-CeO₂ is the only one showing thermal CO₂ deoxygenation to CO at below 700 °C after reduction. XRD analyses of as prepared Fe-CeO₂ demonstrate the presence of segregated Fe₂O₃ and CeO₂ phases with partial mixing. Both Fe₂O₃ phase and CeO₂ phase show redox during sequential TPR (temperature-programmed reduction)-CO₂-TPRx (temperature-programmed reaction) up to 700 °C. The evolved Fe⁰ after TPR appears to be the main active phase for CO₂ deoxygenation which becomes oxidized back to Fe₂O₃ after CO₂-TPRx. The results indicate that the interface (interphase) between Fe-domain and CeO₂-domain is involved leading to the observed deoxygenation reactivity. That the stripped oxygen from CO₂ over Fe-domain can spillover to CeO₂ domain is considered as a possible explanation. We perform isothermal CO₂ deoxygenation test at 600 °C over TPR-treated Fe-CeO₂ using oxygen-conducting membrane reactor, and the CO₂ deoxygenation capacity is found significantly higher than that observed when in the absence of oxygen conducting membrane. This demonstrates not only the possible oxygen spillover but also the possibility of achieving a sustainable CO₂ deoxygenation process.

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引用次数: 0

Cu single atoms supported on crystalline graphdiyne porphyrin analogs with dual active sites for enhanced C2 product formation

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-03-25 DOI: 10.1016/j.jcou.2025.103067

Zubair Masaud , Kim R. Gustavsen , Hao Huang , Andy M. Booth , Lars Eric Roseng , Kaiying Wang

Developing advanced catalysts for efficient electrochemical CO₂ reduction has long been a sought-after objective, but designing catalysts with open porous structures, metal sites, high atom utilization, nanoporosity, and electrical conductivity, remains challenging. Downsizing metal sites to single atoms and supporting them on conductive Covalent Organic Frameworks (COFs) offers a strategic solution to these challenges. Herein, we report a novel catalyst with a combination of copper single-atom sites supported by a highly crystalline graphdiyne porphyrin analog (Cu-SGPA). Computational analysis reveals the presence of 2.34 nm open pores with conducting π-conjugated graphdiyne linkages. The joint action of the dual active sites of Cu single atoms and the adjacent carbon atoms facilitates carbon product formation through uniquely achieved intermediate species. Cu-SGPA demonstrates a remarkable faradaic efficiency (FE) of 70 % at optimized potentials of −1.0 V vs RHE, with over 45 % FE for C₂ products, surpassing FE for single-atom catalysts supported on COFs. This study introduces a promising catalyst design that will inspire future efforts in developing and optimizing similar single-atom catalysts supported on conductive COFs for enhanced CO₂ utilization.

{"title":"Cu single atoms supported on crystalline graphdiyne porphyrin analogs with dual active sites for enhanced C2 product formation","authors":"Zubair Masaud , Kim R. Gustavsen , Hao Huang , Andy M. Booth , Lars Eric Roseng , Kaiying Wang","doi":"10.1016/j.jcou.2025.103067","DOIUrl":"10.1016/j.jcou.2025.103067","url":null,"abstract":"<div><div>Developing advanced catalysts for efficient electrochemical CO2 reduction has long been a sought-after objective, but designing catalysts with open porous structures, metal sites, high atom utilization, nanoporosity, and electrical conductivity, remains challenging. Downsizing metal sites to single atoms and supporting them on conductive Covalent Organic Frameworks (COFs) offers a strategic solution to these challenges. Herein, we report a novel catalyst with a combination of copper single-atom sites supported by a highly crystalline graphdiyne porphyrin analog (Cu-SGPA). Computational analysis reveals the presence of 2.34 nm open pores with conducting π-conjugated graphdiyne linkages. The joint action of the dual active sites of Cu single atoms and the adjacent carbon atoms facilitates carbon product formation through uniquely achieved intermediate species. Cu-SGPA demonstrates a remarkable faradaic efficiency (FE) of 70 % at optimized potentials of −1.0 V vs RHE, with over 45 % FE for C2 products, surpassing FE for single-atom catalysts supported on COFs. This study introduces a promising catalyst design that will inspire future efforts in developing and optimizing similar single-atom catalysts supported on conductive COFs for enhanced CO2 utilization.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"95 ","pages":"Article 103067"},"PeriodicalIF":7.2,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143680475","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Advances in the development of innovative Bi-Sn-Sb-based Gas Diffusion Electrodes for continuous CO2 electroreduction to formate

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-03-25 DOI: 10.1016/j.jcou.2025.103070

Guillermo Díaz-Sainz , Kevin Fernández-Caso , Beatriz Ávila-Bolívar , Vicente Montiel , José Solla-Gullón , Manuel Alvarez-Guerra , Angel Irabien

The electrocatalytic reduction of CO₂ to formate or formic acid represents a promising approach to mitigating CO₂ emissions. Despite progress with Bi and Sn-based cathodes, there remains a demand for new electrocatalytic materials with enhanced activity for industrial-scale implementation. In a recent contribution, carbon-supported Bi-Sn-Sb nanoparticles with different atomic ratios were prepared and evaluated for the electrocatalytic reduction of CO₂ to formate, assessing their performance in terms of activity, selectivity, and stability under working conditions in an H-type cell. Under this electrochemical reactor configuration, the results clearly indicated that the incorporation of small amounts of Sb and Sn into Bi significantly enhanced stability without substantially affecting activity and selectivity, achieving promising results with Bi₈₀Sn₁₀Sb₁₀ electrocatalysts. Here, we report the use of Bi-Sn-Sb-based Gas Diffusion Electrodes (GDEs) in a flow electrochemical reactor for the electrocatalytic reduction of CO₂ to formate. The study also aims to rigorously compare the performance of Bi-Sn-Sb GDEs with that of analogous GDEs based solely on Bi or Sn. When compared to relevant references, the Bi-Sn-Sb catalyst demonstrates performance metrics that reflect comparable system efficiency to the Bi and Sn cathodes previously used by our research group, operating at current densities up to 200 mA·cm⁻² and achieving formate concentrations of approximately 15 g·L⁻¹. Furthermore, these materials exhibited technical feasibility, remaining stable throughout the 5-hour experiment with less than a 10 % decrease in concentration. This stability marks a vital first step toward the future implementation of this type of cathode in the electrochemical reduction of CO₂ to formate.

{"title":"Advances in the development of innovative Bi-Sn-Sb-based Gas Diffusion Electrodes for continuous CO2 electroreduction to formate","authors":"Guillermo Díaz-Sainz , Kevin Fernández-Caso , Beatriz Ávila-Bolívar , Vicente Montiel , José Solla-Gullón , Manuel Alvarez-Guerra , Angel Irabien","doi":"10.1016/j.jcou.2025.103070","DOIUrl":"10.1016/j.jcou.2025.103070","url":null,"abstract":"<div><div>The electrocatalytic reduction of CO2 to formate or formic acid represents a promising approach to mitigating CO2 emissions. Despite progress with Bi and Sn-based cathodes, there remains a demand for new electrocatalytic materials with enhanced activity for industrial-scale implementation. In a recent contribution, carbon-supported Bi-Sn-Sb nanoparticles with different atomic ratios were prepared and evaluated for the electrocatalytic reduction of CO2 to formate, assessing their performance in terms of activity, selectivity, and stability under working conditions in an H-type cell. Under this electrochemical reactor configuration, the results clearly indicated that the incorporation of small amounts of Sb and Sn into Bi significantly enhanced stability without substantially affecting activity and selectivity, achieving promising results with Bi80Sn10Sb10 electrocatalysts. Here, we report the use of Bi-Sn-Sb-based Gas Diffusion Electrodes (GDEs) in a flow electrochemical reactor for the electrocatalytic reduction of CO2 to formate. The study also aims to rigorously compare the performance of Bi-Sn-Sb GDEs with that of analogous GDEs based solely on Bi or Sn. When compared to relevant references, the Bi-Sn-Sb catalyst demonstrates performance metrics that reflect comparable system efficiency to the Bi and Sn cathodes previously used by our research group, operating at current densities up to 200 mA·cm−2 and achieving formate concentrations of approximately 15 g·L−1. Furthermore, these materials exhibited technical feasibility, remaining stable throughout the 5-hour experiment with less than a 10 % decrease in concentration. This stability marks a vital first step toward the future implementation of this type of cathode in the electrochemical reduction of CO₂ to formate.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"95 ","pages":"Article 103070"},"PeriodicalIF":7.2,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143695976","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Effect of Ga doping on the catalytic performance of Zn-ZSM-5 for CO2-assisted oxidative dehydrogenation of C2H6

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-03-22 DOI: 10.1016/j.jcou.2025.103066

Haojue Wen , Xinru Han , Lina Zhang , Yongdong Chen , Wei Wei , Nannan Sun

Using a low silica-to-alumina ratio NaZSM-5 zeolite as the support, a bimetallic modified catalyst, Ga_xZnZ5, was prepared through ion-exchange method for CO₂-mediated oxidative dehydrogenation of C₂H₆ (CO₂-ODH). Based on systematic characterization and evaluation, it was found that Zn is the primary active component in the catalytic system for activating C₂H₆, but it is merely active towards CO₂, leading to rapid catalyst deactivation. Under the influence of Ga species, CO₂ can readily engage into the reaction network. During the initial stage of the reaction, the activated CO₂ primarily participants in dry reforming with C₂H_6-x species that rapidly formed on highly active Zn sites. However, the rapid cleavage of C-H bonds on these Zn sites leads to significant carbon deposition and subsequent deactivation. Following this rapid deactivation phase, CO₂ becomes involved in the reaction through the reverse water-gas shift (RWGS) reaction and carbon elimination reactions, thereby shifting the reaction equilibrium towards C₂H₄ formation while alleviating the accumulation of carbon deposition and thus enhancing stability. With the optimum catalyst (Ga_0.27ZnZ5), excellent and stable performance with 22.64 % C₂H₄ yield and nearly 100 % selectivity could be achieved after an induction period of ca. 100 minutes, these are among the highest values reported so far.

{"title":"Effect of Ga doping on the catalytic performance of Zn-ZSM-5 for CO2-assisted oxidative dehydrogenation of C2H6","authors":"Haojue Wen , Xinru Han , Lina Zhang , Yongdong Chen , Wei Wei , Nannan Sun","doi":"10.1016/j.jcou.2025.103066","DOIUrl":"10.1016/j.jcou.2025.103066","url":null,"abstract":"<div><div>Using a low silica-to-alumina ratio NaZSM-5 zeolite as the support, a bimetallic modified catalyst, GaxZnZ5, was prepared through ion-exchange method for CO2-mediated oxidative dehydrogenation of C2H6 (CO2-ODH). Based on systematic characterization and evaluation, it was found that Zn is the primary active component in the catalytic system for activating C2H6, but it is merely active towards CO2, leading to rapid catalyst deactivation. Under the influence of Ga species, CO2 can readily engage into the reaction network. During the initial stage of the reaction, the activated CO2 primarily participants in dry reforming with C2H6-x species that rapidly formed on highly active Zn sites. However, the rapid cleavage of C-H bonds on these Zn sites leads to significant carbon deposition and subsequent deactivation. Following this rapid deactivation phase, CO2 becomes involved in the reaction through the reverse water-gas shift (RWGS) reaction and carbon elimination reactions, thereby shifting the reaction equilibrium towards C2H4 formation while alleviating the accumulation of carbon deposition and thus enhancing stability. With the optimum catalyst (Ga0.27ZnZ5), excellent and stable performance with 22.64 % C2H4 yield and nearly 100 % selectivity could be achieved after an induction period of ca. 100 minutes, these are among the highest values reported so far.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"95 ","pages":"Article 103066"},"PeriodicalIF":7.2,"publicationDate":"2025-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143680412","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Effect of promoters on the syngas production in the microwave-enhanced methane dry reforming over Ni-x/AC (x = Mg, Ca, La, Ce) catalysts

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-03-19 DOI: 10.1016/j.jcou.2025.103064

Miaomiao Zhang, Yibo Gao, Wenlong Wang, Zhanlong Song, Yanpeng Mao

Capitalizing on the targeted energy transfer, microwave-enhanced dry reforming of methane (MW-DRM) is an attractive CO₂ valorization technology. However, this process coupled with carbon-based catalysts may suffer from rapid deactivation due to severe carbon deposition/loss or active metal sintering. In this study, activated carbon (AC)-supported Ni catalysts modified with different promoters (Mg, Ca, La, Ce) were investigated for MW-DRM process. As proved by the experiment results, Ca-promoted catalyst exhibited the worst reforming activity and stability in the MW-DRM and conventional heating DRM (CH-DRM) processes due to the severe carbon gasification of AC support and the severe sintering of the active metal. Compared to Mg, Ca, and La promoters, Ni-Ce/AC catalyst was demonstrated the optimum catalyst for MW-DRM process, which showed the most excellent stability with good reforming activity over 96 % and 98 % for CH₄ and CO₂ conversion rates, respectively. By converting MW energy attenuation into heat and plasma, the locally-formed high-energy active sites composed of adjacent Ni, CeO₂ and AC support of the Ni-Ce/AC catalyst could contribute to achieving the effective and localized activation of CH₄ and CO₂ molecules, thus leading to the enhancement of the reforming activity and the reduction of the loss of AC support due to CO₂ gasification. Moreover, MW heating method could avoid the excessive consumption of the AC support in Ni-Ce/AC by increasing the graphitization degree of AC, thus prolonging the lifetime of the AC-based catalysts. Above all, these findings provide new insights for the synergistic effect of MW with AC-based catalysts for syngas production.

{"title":"Effect of promoters on the syngas production in the microwave-enhanced methane dry reforming over Ni-x/AC (x = Mg, Ca, La, Ce) catalysts","authors":"Miaomiao Zhang, Yibo Gao, Wenlong Wang, Zhanlong Song, Yanpeng Mao","doi":"10.1016/j.jcou.2025.103064","DOIUrl":"10.1016/j.jcou.2025.103064","url":null,"abstract":"<div><div>Capitalizing on the targeted energy transfer, microwave-enhanced dry reforming of methane (MW-DRM) is an attractive CO2 valorization technology. However, this process coupled with carbon-based catalysts may suffer from rapid deactivation due to severe carbon deposition/loss or active metal sintering. In this study, activated carbon (AC)-supported Ni catalysts modified with different promoters (Mg, Ca, La, Ce) were investigated for MW-DRM process. As proved by the experiment results, Ca-promoted catalyst exhibited the worst reforming activity and stability in the MW-DRM and conventional heating DRM (CH-DRM) processes due to the severe carbon gasification of AC support and the severe sintering of the active metal. Compared to Mg, Ca, and La promoters, Ni-Ce/AC catalyst was demonstrated the optimum catalyst for MW-DRM process, which showed the most excellent stability with good reforming activity over 96 % and 98 % for CH4 and CO2 conversion rates, respectively. By converting MW energy attenuation into heat and plasma, the locally-formed high-energy active sites composed of adjacent Ni, CeO2 and AC support of the Ni-Ce/AC catalyst could contribute to achieving the effective and localized activation of CH4 and CO2 molecules, thus leading to the enhancement of the reforming activity and the reduction of the loss of AC support due to CO2 gasification. Moreover, MW heating method could avoid the excessive consumption of the AC support in Ni-Ce/AC by increasing the graphitization degree of AC, thus prolonging the lifetime of the AC-based catalysts. Above all, these findings provide new insights for the synergistic effect of MW with AC-based catalysts for syngas production.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"95 ","pages":"Article 103064"},"PeriodicalIF":7.2,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143680487","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0