Journal of CO2 Utilization最新文献_第3页

Coupling Ni-based anodes for textile industry process stream electrooxidation with electrocatalytic CO2 reduction to formate in gas phase

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-03-01 DOI: 10.1016/j.jcou.2025.103053

Jose Antonio Abarca , Ghazaleh Abdolhosseini , Juan Marcos Sanz , Jose Solla-Gullón , Felipe A. Garcés-Pineda , Guillermo Díaz-Sainz , Angel Irabien

Scaling up CO₂ electroreduction to formate faces several challenges, including using chemicals as electrolytes and high energy demands. To address these issues, this study uses an industrial stream—specifically a caustic soda stream from the textile industry—as anolytes for the oxygen evolution reaction (OER). Using this approach, formate concentrations of 226 g L⁻¹ and Faradaic efficiencies (FE) of 53 % are achieved at 200 mA cm⁻², demonstrating the competitiveness of industrial streams compared to synthetic anolyte solutions. Various anode materials are tested to optimize OER kinetics under industrial conditions and reduce energy consumption. Ni foam exhibited promising results, achieving FEs of 78 % and 58 % at 90 and 200 mA cm⁻², with energy consumption between 236 and 385 kWh kmol⁻¹ , making it one of the most efficient options among commercially available materials. In addition, alternative materials, such as NiFeOx and NiZnFeOx particulate anodes, are synthesized to provide viable substitutes for commercial anodes that rely on scarce elements. These alternatives demonstrated similar formate concentrations, with FEs up to 74 % and reduced energy requirements compared to commercial NiO. The synthesized NiFe foam anode excelled in performance, with energy consumption below 210 and 380 kWh kmol⁻¹ and an impressive formate production of 255 g L⁻¹ of formate achieving a 60 % FE at 200 mA cm⁻². Overall, this research demonstrates the feasibility of CO₂ electroreduction to formate using textile effluents under relevant conditions, representing a significant step toward making this process a competitive option for decarbonizing hard-to-abate industries.

{"title":"Coupling Ni-based anodes for textile industry process stream electrooxidation with electrocatalytic CO2 reduction to formate in gas phase","authors":"Jose Antonio Abarca , Ghazaleh Abdolhosseini , Juan Marcos Sanz , Jose Solla-Gullón , Felipe A. Garcés-Pineda , Guillermo Díaz-Sainz , Angel Irabien","doi":"10.1016/j.jcou.2025.103053","DOIUrl":"10.1016/j.jcou.2025.103053","url":null,"abstract":"<div><div>Scaling up CO<sub>2</sub> electroreduction to formate faces several challenges, including using chemicals as electrolytes and high energy demands. To address these issues, this study uses an industrial stream—specifically a caustic soda stream from the textile industry—as anolytes for the oxygen evolution reaction (OER). Using this approach, formate concentrations of 226 g L⁻¹ and Faradaic efficiencies (FE) of 53 % are achieved at 200 mA cm⁻², demonstrating the competitiveness of industrial streams compared to synthetic anolyte solutions. Various anode materials are tested to optimize OER kinetics under industrial conditions and reduce energy consumption. Ni foam exhibited promising results, achieving FEs of 78 % and 58 % at 90 and 200 mA cm⁻², with energy consumption between 236 and 385 kWh kmol⁻¹ , making it one of the most efficient options among commercially available materials. In addition, alternative materials, such as NiFeOx and NiZnFeOx particulate anodes, are synthesized to provide viable substitutes for commercial anodes that rely on scarce elements. These alternatives demonstrated similar formate concentrations, with FEs up to 74 % and reduced energy requirements compared to commercial NiO. The synthesized NiFe foam anode excelled in performance, with energy consumption below 210 and 380 kWh kmol⁻¹ and an impressive formate production of 255 g L<sup>−1</sup> of formate achieving a 60 % FE at 200 mA cm<sup>−2</sup>. Overall, this research demonstrates the feasibility of CO₂ electroreduction to formate using textile effluents under relevant conditions, representing a significant step toward making this process a competitive option for decarbonizing hard-to-abate industries.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"93 ","pages":"Article 103053"},"PeriodicalIF":7.2,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143520028","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

CO2 capture from air and its conversion to CH4 using dual functional materials supported on high surface area graphite

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-03-01 DOI: 10.1016/j.jcou.2025.103054

Jorge Moral-Pombo , Enrique García-Bordejé , Yuefeng Liu , Antonio Guerrero-Ruiz , Inmaculada Rodríguez-Ramos

Several cycles of CO₂ capture from synthetic air containing 400 ppm of CO₂ and subsequent conversion to CH₄ have been performed using dual functional materials consisting of 4 wt% Ru and 10 wt% Ba or Cs supported on a high surface area graphite. The effect of the presence of humidity and the regeneration conditions have been assessed. The presence of moisture in the air enhances CO₂ capture. The capture material is not properly regenerated in the absence of H₂-containing atmosphere or at temperatures below 300 ºC. The exhaustive characterization by XRD, XPS, TEM and temperature programmed reduction and reaction allowed to shed some light about the reasons of the different behavior of Ba and Cs based dual functional materials. Cs is more efficiently utilized than Ba, providing higher CO₂ capture capacities (0.44 mmol g⁻¹) and CH₄ productivity (0.41 mmol g⁻¹). The outperformance of Cs is attributed to the more homogeneous and better dispersed species which are regenerated at lower temperatures.

{"title":"CO2 capture from air and its conversion to CH4 using dual functional materials supported on high surface area graphite","authors":"Jorge Moral-Pombo , Enrique García-Bordejé , Yuefeng Liu , Antonio Guerrero-Ruiz , Inmaculada Rodríguez-Ramos","doi":"10.1016/j.jcou.2025.103054","DOIUrl":"10.1016/j.jcou.2025.103054","url":null,"abstract":"<div><div>Several cycles of CO<sub>2</sub> capture from synthetic air containing 400 ppm of CO<sub>2</sub> and subsequent conversion to CH<sub>4</sub> have been performed using dual functional materials consisting of 4 wt% Ru and 10 wt% Ba or Cs supported on a high surface area graphite. The effect of the presence of humidity and the regeneration conditions have been assessed. The presence of moisture in the air enhances CO<sub>2</sub> capture. The capture material is not properly regenerated in the absence of H<sub>2</sub>-containing atmosphere or at temperatures below 300 ºC. The exhaustive characterization by XRD, XPS, TEM and temperature programmed reduction and reaction allowed to shed some light about the reasons of the different behavior of Ba and Cs based dual functional materials. Cs is more efficiently utilized than Ba, providing higher CO<sub>2</sub> capture capacities (0.44 mmol g<sup>−1</sup>) and CH<sub>4</sub> productivity (0.41 mmol g<sup>−1</sup>). The outperformance of Cs is attributed to the more homogeneous and better dispersed species which are regenerated at lower temperatures.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"93 ","pages":"Article 103054"},"PeriodicalIF":7.2,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143547859","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

Light-driven eosin Y-Ralstonia eutropha biohybrid for CO2 conversion to acetoin via specific photo-induced electron transfer and metabolic engineering

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-03-01 DOI: 10.1016/j.jcou.2025.103051

Yao Tian , Zhiqi Guo , Jiaping He , Dake Xu , Wen-Wei Li , Shaoan Cheng , Hao Song

Whole-cell photosynthetic biohybrid systems offer a promising route for CO₂ conversion into value-added chemicals. However, many existing systems suffer from inefficient electron transfer to intracellular catalytic CO₂ center, which arises from non-specific charge transfer between photosensitizer and microbe. Herein, we developed an efficient eosin Y-Ralstonia eutropha biohybrid system that achieved targeted electron transfer for powering CO₂ reduction into acetoin, a valuable platform chemical with broad applications. By spontaneously attaching eosin Y to the membrane-bound hydrogenase (MBH) of R. eutropha, we enabled direct and specific electron flow. The biohybrid system demonstrated sustainable and efficient light-energized CO₂ conversion to acetoin, even surpassing the yields from H₂-supplied autotrophic fermentation, which is considered the optimal source of reducing equivalents and energy for CO₂ fixation by R. eutropha. Mechanistic investigations indicated that the photo-induced electrons from eosin Y were transferred to MBH, resulting in the formation of H₂ intermediate in periplasm, which was subsequently oxidized by cytosolic soluble hydrogenase to generate NADH for energizing CO₂ fixation. To further enhance efficiency, metabolic engineering was applied to boost ATP synthesis by introducing a non-oxygen-dependent proton pump (Gloeobacter rhodopsin), while blocking L-lactate and acetate biosynthesis pathways to divert carbon flux toward acetoin production. The engineered eosin Y-R. eutropha biohybrid system achieved an acetoin yield of 1.41 ± 0.06 mM, representing 2.07 times greater than that of H₂-supplied autotrophic fermentation. This system exemplifies a sustainable, light-driven CO₂ conversion process, contributing significantly to the advancement of sustainable biocatalytic processes in the realms of green chemistry and CO₂ management.

{"title":"Light-driven eosin Y-Ralstonia eutropha biohybrid for CO2 conversion to acetoin via specific photo-induced electron transfer and metabolic engineering","authors":"Yao Tian , Zhiqi Guo , Jiaping He , Dake Xu , Wen-Wei Li , Shaoan Cheng , Hao Song","doi":"10.1016/j.jcou.2025.103051","DOIUrl":"10.1016/j.jcou.2025.103051","url":null,"abstract":"<div><div>Whole-cell photosynthetic biohybrid systems offer a promising route for CO<sub>2</sub> conversion into value-added chemicals. However, many existing systems suffer from inefficient electron transfer to intracellular catalytic CO<sub>2</sub> center, which arises from non-specific charge transfer between photosensitizer and microbe. Herein, we developed an efficient eosin Y-<em>Ralstonia eutropha</em> biohybrid system that achieved targeted electron transfer for powering CO<sub>2</sub> reduction into acetoin, a valuable platform chemical with broad applications. By spontaneously attaching eosin Y to the membrane-bound hydrogenase (MBH) of <em>R. eutropha</em>, we enabled direct and specific electron flow. The biohybrid system demonstrated sustainable and efficient light-energized CO<sub>2</sub> conversion to acetoin, even surpassing the yields from H<sub>2</sub>-supplied autotrophic fermentation, which is considered the optimal source of reducing equivalents and energy for CO<sub>2</sub> fixation by <em>R. eutropha</em>. Mechanistic investigations indicated that the photo-induced electrons from eosin Y were transferred to MBH, resulting in the formation of H<sub>2</sub> intermediate in periplasm, which was subsequently oxidized by cytosolic soluble hydrogenase to generate NADH for energizing CO<sub>2</sub> fixation. To further enhance efficiency, metabolic engineering was applied to boost ATP synthesis by introducing a non-oxygen-dependent proton pump (<em>Gloeobacter</em> rhodopsin), while blocking L-lactate and acetate biosynthesis pathways to divert carbon flux toward acetoin production. The engineered eosin Y-<em>R. eutropha</em> biohybrid system achieved an acetoin yield of 1.41 ± 0.06 mM, representing 2.07 times greater than that of H<sub>2</sub>-supplied autotrophic fermentation. This system exemplifies a sustainable, light-driven CO<sub>2</sub> conversion process, contributing significantly to the advancement of sustainable biocatalytic processes in the realms of green chemistry and CO<sub>2</sub> management.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"93 ","pages":"Article 103051"},"PeriodicalIF":7.2,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143510743","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

Analysis of CO2 solubility in ionic liquids as promising absorbents using response surface methodology and machine learning

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-03-01 DOI: 10.1016/j.jcou.2025.103043

Alireza Rahimi, Fatemeh Bahmanzadegan, Ahad Ghaemi

This study explored CO₂ solubility in ionic liquids using Response Surface Methodology (RSM) and Artificial Neural Networks (ANNs), specifically Multilayer Perceptron (MLP) and Radial Basis Function (RBF) networks, to model and optimize absorption processes. In our study, we analyzed several ionic liquids (ILs), including [bmim][PF6], [P(5) mpyrr][Tf2N], [mp(3)pip][FSI], [mp(3)pyrr][FSI], [N1223][FSI], [bmmim][Tf2N], and [P4441][Tf2N], chosen for their unique properties such as high thermal stability and ionic conductivity. Experimental data analysis identified mass, viscosity, pressure, molar concentration, and surface tension as key influencing parameters. RSM demonstrated excellent fit with an R² of 0.9999, while ANNs exhibited superior predictive accuracy, with R² values approaching unity. The MLP network, employing a two-layer training activation function, achieved a minimum Mean Squared Error (MSE) of 0.001082 for test data. The RBF network with 26 neurons and a spread of 2 reached a minimum MSE of 0.0011252. 3D response surface analyses of MLP, RBF, and RSM revealed intricate parameter interdependencies. Increased ionic liquid mass enhances CO₂ absorption by expanding the interaction space and providing more binding sites. Elevated pressure significantly increases solubility by compressing the gas phase and driving more CO₂ molecules into the liquid. Higher viscosity impedes CO₂ movement within the liquid, while lower viscosity facilitates faster diffusion. A higher molar concentration of CO₂ in the gas phase increases the driving force for absorption, leading to a greater influx of CO₂ into the ionic liquid. While RSM surfaces exhibited rigid, polynomial-based trends, the smoother MLP plots effectively captured complex nonlinearities, highlighting ANNs' superior predictive capabilities for optimizing CO₂ capture systems in ionic liquids.

{"title":"Analysis of CO2 solubility in ionic liquids as promising absorbents using response surface methodology and machine learning","authors":"Alireza Rahimi, Fatemeh Bahmanzadegan, Ahad Ghaemi","doi":"10.1016/j.jcou.2025.103043","DOIUrl":"10.1016/j.jcou.2025.103043","url":null,"abstract":"<div><div>This study explored CO<sub>2</sub> solubility in ionic liquids using Response Surface Methodology (RSM) and Artificial Neural Networks (ANNs), specifically Multilayer Perceptron (MLP) and Radial Basis Function (RBF) networks, to model and optimize absorption processes. In our study, we analyzed several ionic liquids (ILs), including [bmim][PF6], [P(5) mpyrr][Tf2N], [mp(3)pip][FSI], [mp(3)pyrr][FSI], [N1223][FSI], [bmmim][Tf2N], and [P4441][Tf2N], chosen for their unique properties such as high thermal stability and ionic conductivity. Experimental data analysis identified mass, viscosity, pressure, molar concentration, and surface tension as key influencing parameters. RSM demonstrated excellent fit with an R² of 0.9999, while ANNs exhibited superior predictive accuracy, with R² values approaching unity. The MLP network, employing a two-layer training activation function, achieved a minimum Mean Squared Error (MSE) of 0.001082 for test data. The RBF network with 26 neurons and a spread of 2 reached a minimum MSE of 0.0011252. 3D response surface analyses of MLP, RBF, and RSM revealed intricate parameter interdependencies. Increased ionic liquid mass enhances CO<sub>2</sub> absorption by expanding the interaction space and providing more binding sites. Elevated pressure significantly increases solubility by compressing the gas phase and driving more CO<sub>2</sub> molecules into the liquid. Higher viscosity impedes CO<sub>2</sub> movement within the liquid, while lower viscosity facilitates faster diffusion. A higher molar concentration of CO<sub>2</sub> in the gas phase increases the driving force for absorption, leading to a greater influx of CO<sub>2</sub> into the ionic liquid. While RSM surfaces exhibited rigid, polynomial-based trends, the smoother MLP plots effectively captured complex nonlinearities, highlighting ANNs' superior predictive capabilities for optimizing CO<sub>2</sub> capture systems in ionic liquids.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"93 ","pages":"Article 103043"},"PeriodicalIF":7.2,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143520034","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

Techno-economic analysis of integrating an on-board CCS system and a PtG technology in a heavy vehicle fleet

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-03-01 DOI: 10.1016/j.jcou.2025.103046

Alexander García Mariaca , Jorge Perpiñán , Uriel Fernando Carreño Sayago

Decarbonising the heavy-duty transport sector requires switching internal combustion engine (ICE) fuel from fossil to synthetic fuels. In this context, on-board carbon capture and storage (OCCS) in ICEs could provide the CO₂ needed by Power-to-gas (PtG) technologies to produce synthetic natural gas (SNG), which is then consumed again by the vehicle fleet, closing in this way the carbon loop. This study presents a techno-economic analysis of a heavy-duty vehicle fleet integrating an OCCS system with a PtG plant. The OCCS system operates by temperature swing adsorption where two sorbents, PPN-6-CH₂-DETA and zeolite 13X, are evaluated at carbon capture rates (CCR) of 70 % and 100 %. A fifth scenario examined the effect of varying the H₂:CO₂ ratio in the methanation plant at 100 % CCR using PPN-6-CH₂-DETA. Both systems were simulated using Aspen Plus and AVL Boost softwares. Moreover, a sensitivity analysis was conducted considering three key performance indicators: the CO₂ tax, natural gas (NG), and electricity prices. The results indicate that the carbon abatement cost reaches a break-even point at 150 €/tCO₂ for a fleet size of 400 vehicles. However, the capital expenditures do not achieve payback within 20 years due to the high operational expenditures and low incomes in the evaluated scenarios. The sensitivity analyses show that the CO₂ tax and the NG price must be higher than 400 €/tCO₂ and 160 €/MWh, respectively, to compensate for the current electricity price and allow the proposed systems to be techno-economic feasible.

{"title":"Techno-economic analysis of integrating an on-board CCS system and a PtG technology in a heavy vehicle fleet","authors":"Alexander García Mariaca , Jorge Perpiñán , Uriel Fernando Carreño Sayago","doi":"10.1016/j.jcou.2025.103046","DOIUrl":"10.1016/j.jcou.2025.103046","url":null,"abstract":"<div><div>Decarbonising the heavy-duty transport sector requires switching internal combustion engine (ICE) fuel from fossil to synthetic fuels. In this context, on-board carbon capture and storage (OCCS) in ICEs could provide the CO<sub>2</sub> needed by Power-to-gas (PtG) technologies to produce synthetic natural gas (SNG), which is then consumed again by the vehicle fleet, closing in this way the carbon loop. This study presents a techno-economic analysis of a heavy-duty vehicle fleet integrating an OCCS system with a PtG plant. The OCCS system operates by temperature swing adsorption where two sorbents, PPN-6-CH<sub>2</sub>-DETA and zeolite 13X, are evaluated at carbon capture rates (CCR) of 70 % and 100 %. A fifth scenario examined the effect of varying the H<sub>2</sub>:CO<sub>2</sub> ratio in the methanation plant at 100 % CCR using PPN-6-CH<sub>2</sub>-DETA. Both systems were simulated using Aspen Plus and AVL Boost softwares. Moreover, a sensitivity analysis was conducted considering three key performance indicators: the CO<sub>2</sub> tax, natural gas (NG), and electricity prices. The results indicate that the carbon abatement cost reaches a break-even point at 150 €/tCO₂ for a fleet size of 400 vehicles. However, the capital expenditures do not achieve payback within 20 years due to the high operational expenditures and low incomes in the evaluated scenarios. The sensitivity analyses show that the CO<sub>2</sub> tax and the NG price must be higher than 400 €/tCO₂ and 160 €/MWh, respectively, to compensate for the current electricity price and allow the proposed systems to be techno-economic feasible.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"93 ","pages":"Article 103046"},"PeriodicalIF":7.2,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143520035","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

A co-feeding strategy of formate and H2 for methanogens – Enhancing growth parameters and methane production

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-03-01 DOI: 10.1016/j.jcou.2025.103049

Björn Sabel-Becker , Nicolas Patrick Jost , Anne-Kristin Kaster , Dirk Holtmann

Carbon dioxide emissions could be reduced by developing alternative production processes based on a renewable C1 building block. Formate could link the electrical and chemical sectors as its production can be realized through the electrochemical reduction of CO₂. Its function could be either a long-term energy storage medium or a starting material in a bioprocess. In this study, formate served as an energy and carbon source for methane production with a formatotrophic mixed culture. It was successfully shown that the theoretical maximum of 0.25 methane per formate can be overcome by co-feeding formate with H₂. The production yield doubled to 0.555 ± 0.021 in a CO₂-free buffer and 0.591 ± 0.032 in a bicarbonate buffer. With excess CO₂ in the bicarbonate buffered culture, it was shown that the H₂ transfer rate was the limiting factor for this process. Otherwise, the bicarbonate buffered culture outperformed other buffered cultures in terms of start-up time, formate consumption, and methane production rate. The additional CO₂ in the gas phase might have enhanced the growth of methanogens in an early stage of cultivation. 16S sequencing revealed the composition of the cultures. With nearly 25 %, the genus Methanofollis was one of the most dominant strains and the only detectable methanogen in the mixed culture, making it an interesting candidate for formatotrophic methane production. In summary, the co-feeding strategy might be an approach to utilizing formate as feedstock for the bioproduction of methane if hurdles like the H₂ transfer rates can be overcome.

{"title":"A co-feeding strategy of formate and H2 for methanogens – Enhancing growth parameters and methane production","authors":"Björn Sabel-Becker , Nicolas Patrick Jost , Anne-Kristin Kaster , Dirk Holtmann","doi":"10.1016/j.jcou.2025.103049","DOIUrl":"10.1016/j.jcou.2025.103049","url":null,"abstract":"<div><div>Carbon dioxide emissions could be reduced by developing alternative production processes based on a renewable C1 building block. Formate could link the electrical and chemical sectors as its production can be realized through the electrochemical reduction of CO<sub>2</sub>. Its function could be either a long-term energy storage medium or a starting material in a bioprocess. In this study, formate served as an energy and carbon source for methane production with a formatotrophic mixed culture. It was successfully shown that the theoretical maximum of 0.25 methane per formate can be overcome by co-feeding formate with H<sub>2</sub>. The production yield doubled to 0.555 ± 0.021 in a CO<sub>2</sub>-free buffer and 0.591 ± 0.032 in a bicarbonate buffer. With excess CO<sub>2</sub> in the bicarbonate buffered culture, it was shown that the H<sub>2</sub> transfer rate was the limiting factor for this process. Otherwise, the bicarbonate buffered culture outperformed other buffered cultures in terms of start-up time, formate consumption, and methane production rate. The additional CO<sub>2</sub> in the gas phase might have enhanced the growth of methanogens in an early stage of cultivation. 16S sequencing revealed the composition of the cultures. With nearly 25 %, the genus <em>Methanofollis</em> was one of the most dominant strains and the only detectable methanogen in the mixed culture, making it an interesting candidate for formatotrophic methane production. In summary, the co-feeding strategy might be an approach to utilizing formate as feedstock for the bioproduction of methane if hurdles like the H<sub>2</sub> transfer rates can be overcome.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"93 ","pages":"Article 103049"},"PeriodicalIF":7.2,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143547858","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

Black-box and white-box machine learning tools to estimate the frost formation condition during cryogenic CO2 capture from natural gas blends

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-02-26 DOI: 10.1016/j.jcou.2025.103052

Farag M.A. Altalbawy , Fadhel F. Sead , Dharmesh Sur , Anupam Yadav , José Gerardo León Chimbolema , Suhas Ballal , Abhayveer Singh , Anita Devi , Kamal Kant Joshi , Nizomiddin Juraev , Hossein Mahabadi Asl

Cryogenic carbon capture (CCC), a promising technology for the sequestration of CO₂ from natural gas streams, relies on the CO₂ frost formation at cryogenic temperatures. Precise estimation of the CO₂ frost formation temperature (FFT) is vital for optimizing CCC processes and maximizing efficiency. This study deals with the development of machine learning models for predicting the FFT of CO₂ in natural gas blends. A comprehensive dataset, including 430 experimental samples, was assembled from the literature. The foregoing dataset included the FFT data for binary and ternary natural gas blends across a wide range of pressures and component fractions. Three distinct black-box algorithms, including Regression Tree (RT), Radial Basis Function Neural Network (RBF-NN) and Support Vector Machine (SVM) were employed to model FFT. The performance of each model was rigorously explored through diverse statistical and graphical methods. While all developed models demonstrated high accuracy, the RBF-NN model was the superior predictive tool, achieving a mean absolute percentage error (MAPE) of 0.82 % and a standard deviation (SD) of 1.19 % during the validation phase. Also, an explicit correlation for FFT was proposed using the white-box machine learning technique of Gene Expression Programming (GEP), which achieved the MAPE of 0.59 % for all data. The models were also capable of predicting the FFT of CO₂ in both binary and ternary blends, and favorably captured the complicated physical variations of FFT under diverse operating conditions. To gain deeper insights into the most fundamental factors in controlling the FFT of CO₂, a sensitivity analysis was conducted. The findings of the current study, in turn, contribute to the understanding of FFT of CO₂ and the optimal design of the CCC processes in natural gas industries.

{"title":"Black-box and white-box machine learning tools to estimate the frost formation condition during cryogenic CO2 capture from natural gas blends","authors":"Farag M.A. Altalbawy , Fadhel F. Sead , Dharmesh Sur , Anupam Yadav , José Gerardo León Chimbolema , Suhas Ballal , Abhayveer Singh , Anita Devi , Kamal Kant Joshi , Nizomiddin Juraev , Hossein Mahabadi Asl","doi":"10.1016/j.jcou.2025.103052","DOIUrl":"10.1016/j.jcou.2025.103052","url":null,"abstract":"<div><div>Cryogenic carbon capture (CCC), a promising technology for the sequestration of CO<sub>2</sub> from natural gas streams, relies on the CO<sub>2</sub> frost formation at cryogenic temperatures. Precise estimation of the CO<sub>2</sub> frost formation temperature (FFT) is vital for optimizing CCC processes and maximizing efficiency. This study deals with the development of machine learning models for predicting the FFT of CO<sub>2</sub> in natural gas blends. A comprehensive dataset, including 430 experimental samples, was assembled from the literature. The foregoing dataset included the FFT data for binary and ternary natural gas blends across a wide range of pressures and component fractions. Three distinct black-box algorithms, including Regression Tree (RT), Radial Basis Function Neural Network (RBF-NN) and Support Vector Machine (SVM) were employed to model FFT. The performance of each model was rigorously explored through diverse statistical and graphical methods. While all developed models demonstrated high accuracy, the RBF-NN model was the superior predictive tool, achieving a mean absolute percentage error (MAPE) of 0.82 % and a standard deviation (SD) of 1.19 % during the validation phase. Also, an explicit correlation for FFT was proposed using the white-box machine learning technique of Gene Expression Programming (GEP), which achieved the MAPE of 0.59 % for all data. The models were also capable of predicting the FFT of CO<sub>2</sub> in both binary and ternary blends, and favorably captured the complicated physical variations of FFT under diverse operating conditions. To gain deeper insights into the most fundamental factors in controlling the FFT of CO<sub>2</sub>, a sensitivity analysis was conducted. The findings of the current study, in turn, contribute to the understanding of FFT of CO<sub>2</sub> and the optimal design of the CCC processes in natural gas industries.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"93 ","pages":"Article 103052"},"PeriodicalIF":7.2,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143487046","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

Direct biogas methanation at moderate pressure: Mechanism investigation over Ni-based catalysts

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-02-25 DOI: 10.1016/j.jcou.2025.103045

Ilenia Giarnieri , Sining Chen , Daniel Ballesteros-Plata , Juan P. Holgado , Francesco Maluta , Alfonso Caballero , Francesca Ospitali , Enrique Rodríguez-Castellón , Giuseppe Fornasari , Andrew M. Beale , Patricia Benito

Direct upgrading of biogas by CO₂ methanation aims to produce a gas to be injected into the grid. Operating at moderate pressures favors thermodynamics, but catalyst surface and reaction mechanism under realistic conditions are not well investigated. We study the role of basic and metallic sites on performance and mechanism of clean biogas methanation (CO₂/CH₄=1/1 v/v) at 1, 5 and 7 bar. Ni/Mg/La/Al hydrotalcite-derived catalysts, with different Ni and La contents, are investigated combining tests and physico-chemical characterization, including quasi-in situ XPS at 7 bar, with CO₂-adsorption and methanation DRIFTS at 1 and 7 bar, respectively. An optimized catalyst (6.5 wt% La, 35 wt% Ni) with 3–4 nm Ni⁰ and balanced basicity, achieves 96 L_CH4*gcat⁻¹* h⁻¹ (300°C, 7 bar). DRIFTS confirm catalysts activity experimental trend. Optimizing Ni and La results in higher consumption rates of formate intermediate and sufficient Ni⁰ sites for CO formation. Increasing pressure to 7 bar promotes CO and m-HCOO reactivity.

{"title":"Direct biogas methanation at moderate pressure: Mechanism investigation over Ni-based catalysts","authors":"Ilenia Giarnieri , Sining Chen , Daniel Ballesteros-Plata , Juan P. Holgado , Francesco Maluta , Alfonso Caballero , Francesca Ospitali , Enrique Rodríguez-Castellón , Giuseppe Fornasari , Andrew M. Beale , Patricia Benito","doi":"10.1016/j.jcou.2025.103045","DOIUrl":"10.1016/j.jcou.2025.103045","url":null,"abstract":"<div><div>Direct upgrading of biogas by CO<sub>2</sub> methanation aims to produce a gas to be injected into the grid. Operating at moderate pressures favors thermodynamics, but catalyst surface and reaction mechanism under realistic conditions are not well investigated. We study the role of basic and metallic sites on performance and mechanism of clean biogas methanation (CO<sub>2</sub>/CH<sub>4</sub>=1/1 v/v) at 1, 5 and 7 bar. Ni/Mg/La/Al hydrotalcite-derived catalysts, with different Ni and La contents, are investigated combining tests and physico-chemical characterization, including <em>quasi-in situ</em> XPS at 7 bar, with CO<sub>2</sub>-adsorption and methanation DRIFTS at 1 and 7 bar, respectively. An optimized catalyst (6.5 wt% La, 35 wt% Ni) with 3–4 nm Ni<sup>0</sup> and balanced basicity, achieves 96 L<sub>CH4</sub>*gcat<sup>−1</sup>* h<sup>−1</sup> (300°C, 7 bar). DRIFTS confirm catalysts activity experimental trend. Optimizing Ni and La results in higher consumption rates of formate intermediate and sufficient Ni<sup>0</sup> sites for CO formation. Increasing pressure to 7 bar promotes CO and m-HCOO reactivity.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"93 ","pages":"Article 103045"},"PeriodicalIF":7.2,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143487044","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 light-burned MgO on the microstructure and electrochemical corrosion behavior of carbonatable protective coatings

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-02-24 DOI: 10.1016/j.jcou.2025.103047

Zhaohua Xia , Chenxi Liu , Zhichao Liu , Fazhou Wang , Yunpeng Liu , Shuguang Hu

A novel γ-C₂S-MgO-based coatings were developed for steel protection by providing a carbonated layer on the surface of the steel. The effects of light-burned MgO on the coating's microstructure and electrochemical corrosion behavior were analyzed through XRD, FTIR, SEM, and electrochemical tests. The results showed that the incorporation of MgO inhibited the nucleation and growth of calcite, improved the cementation ability of carbonization products, and optimized the pore structure of the coating. Compared to the γ-C₂S group, the addition of MgO provides a two-stage densifying effect: it reacts with water and carbonate dioxide to generate magnesium carbonates at the first stage; then the partial crystalline transformation of magnesium carbonate occurs during the immersion process, provoking coating secondary compaction in the late period. The corrosion current density of the coating without film-forming components soaked in 3.5 wt% NaCl solution for 21 days maintained below 0.001 μA∙cm⁻². The impedance value of the EIS test reaches 10⁶ Ω·cm².

{"title":"Effect of light-burned MgO on the microstructure and electrochemical corrosion behavior of carbonatable protective coatings","authors":"Zhaohua Xia , Chenxi Liu , Zhichao Liu , Fazhou Wang , Yunpeng Liu , Shuguang Hu","doi":"10.1016/j.jcou.2025.103047","DOIUrl":"10.1016/j.jcou.2025.103047","url":null,"abstract":"<div><div>A novel γ-C<sub>2</sub>S-MgO-based coatings were developed for steel protection by providing a carbonated layer on the surface of the steel. The effects of light-burned MgO on the coating's microstructure and electrochemical corrosion behavior were analyzed through XRD, FTIR, SEM, and electrochemical tests. The results showed that the incorporation of MgO inhibited the nucleation and growth of calcite, improved the cementation ability of carbonization products, and optimized the pore structure of the coating. Compared to the γ-C<sub>2</sub>S group, the addition of MgO provides a two-stage densifying effect: it reacts with water and carbonate dioxide to generate magnesium carbonates at the first stage; then the partial crystalline transformation of magnesium carbonate occurs during the immersion process, provoking coating secondary compaction in the late period. The corrosion current density of the coating without film-forming components soaked in 3.5 wt% NaCl solution for 21 days maintained below 0.001 μA∙cm<sup>−2</sup>. The impedance value of the EIS test reaches 10<sup>6</sup> Ω·cm<sup>2</sup>.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"93 ","pages":"Article 103047"},"PeriodicalIF":7.2,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143479353","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

Efficient utilization of high CO2 landfill-gas for syngas generation: Ultra-rich combustion pathways study in porous media reactor via CFD simulation

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-02-20 DOI: 10.1016/j.jcou.2025.103044

Mohammadreza Mohammadpour , Amirreza Mohammadpour , Mehdi Ashjaee , Ehsan Houshfar

The current investigation explores the possibility of extracting syngas from low-calorific value landfill-gas rich-combustion with pure O₂, which contains a considerable amount of CO₂ in its composition as an effective strategy in CO₂ utilization. The results illustrate that enhancement in mixture velocity leads to a notable increment in syngas energy conversion efficiency from 36.9 % to 44.14 %. Furthermore, it was observed that the maximum rate of H₂ production occurs at an equivalence ratio of 2.2, followed by a subsequent decrease until the end of the studied interval. At a mixture velocity of 25 cm/s, CH₄ and CO₂ conversion ratios reach a maximum of 89.02 % and 42.85 %, respectively, alongside the highest syngas production efficiency. Moreover, with an equivalence ratio of 1.6 and a fuel mixture containing 70 % CH₄, the highest achievable syngas composition was found to be 0.3277 for CO, 0.2841 for H₂, 0.0676 for CH₄, and 0.2534 for CO₂, indicating useful conditions for syngas production. Eventually, reaction pathways analyses revealed that the hydrogen abstraction reactions of hydrocarbon species by H radical which majorly progress through direct CH₄ to H₂ conversion route, and hydrocarbon recombination routes have a key role in H₂ production from landfill gas. Moreover, for landfill gas with high CO₂ content, direct CO₂ to the CO reduction route is determinative. Conversely, when the CH₄ content of landfill gas is high, hydrocarbon recombination followed by ketenyl radical formation and decomposition to CO is the primary pathway in different mixture equivalence ratios.

{"title":"Efficient utilization of high CO2 landfill-gas for syngas generation: Ultra-rich combustion pathways study in porous media reactor via CFD simulation","authors":"Mohammadreza Mohammadpour , Amirreza Mohammadpour , Mehdi Ashjaee , Ehsan Houshfar","doi":"10.1016/j.jcou.2025.103044","DOIUrl":"10.1016/j.jcou.2025.103044","url":null,"abstract":"<div><div>The current investigation explores the possibility of extracting syngas from low-calorific value landfill-gas rich-combustion with pure O<sub>2</sub>, which contains a considerable amount of CO<sub>2</sub> in its composition as an effective strategy in CO<sub>2</sub> utilization. The results illustrate that enhancement in mixture velocity leads to a notable increment in syngas energy conversion efficiency from 36.9 % to 44.14 %. Furthermore, it was observed that the maximum rate of H<sub>2</sub> production occurs at an equivalence ratio of 2.2, followed by a subsequent decrease until the end of the studied interval. At a mixture velocity of 25 cm/s, CH<sub>4</sub> and CO<sub>2</sub> conversion ratios reach a maximum of 89.02 % and 42.85 %, respectively, alongside the highest syngas production efficiency. Moreover, with an equivalence ratio of 1.6 and a fuel mixture containing 70 % CH<sub>4</sub>, the highest achievable syngas composition was found to be 0.3277 for CO, 0.2841 for H<sub>2</sub>, 0.0676 for CH<sub>4</sub>, and 0.2534 for CO<sub>2</sub>, indicating useful conditions for syngas production. Eventually, reaction pathways analyses revealed that the hydrogen abstraction reactions of hydrocarbon species by H radical which majorly progress through direct CH<sub>4</sub> to H<sub>2</sub> conversion route, and hydrocarbon recombination routes have a key role in H<sub>2</sub> production from landfill gas. Moreover, for landfill gas with high CO<sub>2</sub> content, direct CO<sub>2</sub> to the CO reduction route is determinative. Conversely, when the CH<sub>4</sub> content of landfill gas is high, hydrocarbon recombination followed by ketenyl radical formation and decomposition to CO is the primary pathway in different mixture equivalence ratios.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"93 ","pages":"Article 103044"},"PeriodicalIF":7.2,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143444807","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