Carbon dioxide (CO2) methanation is an essential technology for addressing global challenges such as sustainable energy storage, space exploration, and the reduction of CO2 emission. This technology has attracted broad attention in recent years. To really implement the CO2 methanation process, it is crucial to design stable and highly effective catalysts. The activity and selectivity of heterogeneous catalysts can be efficiently tuned by controlling the metal-support interaction, and this strategy has been widely used in the catalyst design for CO2 methanation. In fact, the catalytic activity can be enhanced by up to ∼25 times in a CO2 methanation catalyst due to metal-support interaction. In this review, we summarize the recent progress on metal-support interaction in heterogeneous catalysts for CO2 methanation. At first, we will systemically discuss the effect of metal-support interaction in CO2 methanation catalysts, followed by a detailed introduction to its modulation strategy. Through quantitative analysis, we will point out changing chemical composition of catalyst support is the most efficient method to enhance the catalytic performance, and the primary goal of catalyst design is the modulation of electron transfer between metal particles and the support. We will also sketch the potential research direction of this promising field.
{"title":"Modulation strategy and effect of metal-support interaction over catalysts for carbon dioxide methanation","authors":"Shuaishuai Lyu , Dejian Zhao , Hao Zhang , Hongwei Li , Fuli Wen , Qiuming Zhou , Rongjun Zhang , Yu Wu , Chaopeng Hou , Guofu Xia , Run Xu , Xingang Li","doi":"10.1016/j.ccst.2025.100381","DOIUrl":"10.1016/j.ccst.2025.100381","url":null,"abstract":"<div><div>Carbon dioxide (CO<sub>2</sub>) methanation is an essential technology for addressing global challenges such as sustainable energy storage, space exploration, and the reduction of CO<sub>2</sub> emission. This technology has attracted broad attention in recent years. To really implement the CO<sub>2</sub> methanation process, it is crucial to design stable and highly effective catalysts. The activity and selectivity of heterogeneous catalysts can be efficiently tuned by controlling the metal-support interaction, and this strategy has been widely used in the catalyst design for CO<sub>2</sub> methanation. In fact, the catalytic activity can be enhanced by up to ∼25 times in a CO<sub>2</sub> methanation catalyst due to metal-support interaction. In this review, we summarize the recent progress on metal-support interaction in heterogeneous catalysts for CO<sub>2</sub> methanation. At first, we will systemically discuss the effect of metal-support interaction in CO<sub>2</sub> methanation catalysts, followed by a detailed introduction to its modulation strategy. Through quantitative analysis, we will point out changing chemical composition of catalyst support is the most efficient method to enhance the catalytic performance, and the primary goal of catalyst design is the modulation of electron transfer between metal particles and the support. We will also sketch the potential research direction of this promising field.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"14 ","pages":"Article 100381"},"PeriodicalIF":0.0,"publicationDate":"2025-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143156855","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-29DOI: 10.1016/j.ccst.2025.100382
Tian Heng Qin , Guozhao Ji , Boyu Qu , Alan J McCue , Shaoliang Guan , Jos Derksen , Ye Shui Zhang
The production of H2-rich syngas from pyrolysis-catalytic gasification of plastic waste bottles has been investigated. The hybrid-functional materials consisting of Ni as catalyst, CaO as CO2 sorbent and Ca2SiO4 as a polymorphic active spacer were synthesized. The different parameters (Ni loading, temperature, N2 flow rate and feedstock-to-catalyst ratio) have been investigated to optimise the H2 production. The catalysts were analysed by N2 physisorption, scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Temperature-programmed reduction (TPR) and in-situ Transmission Electron Microscopy (TEM). Temperature-programmed oxidation (TPO) was used to analyse the carbon formation on the used catalysts. The highest H2 production of 59.15 mmol g-1of plastic was obtained in the presence of a catalyst with 20 wt.% Ni loading, which amounts to H2 purity as high as 54.2 vol% in gas production. Furthermore, 90.63 mmol g-1of plastic of syngas was produced by increasing the feedstock-to-catalyst ratio to 4:1, yielding 84.4 vol.% of total gas product (53.1 vol.% of H2 and 31.3 vol.% of CO, respectively). The Ni-CaOCa2SiO4 hybrid-functional material is a very promising catalyst in the pyrolysis-catalytic gasification process by capturing CO2 as it is produced, therefore shifting the water gas shift (WGS) reaction to enhance H2 production from plastic waste. Detailed elucidation of the roles of each component at the microscale during the catalytic process was also provided through in-situ TEM analysis. The finding could guide the industry for future large-scale application to convert abundant plastic waste into H2-rich syngas, therefore contributing to the global ‘net zero’ ambition.
{"title":"Pyrolysis-catalytic gasification of plastic waste for hydrogen-rich syngas production with hybrid-functional Ni-CaOCa2SiO4 catalyst","authors":"Tian Heng Qin , Guozhao Ji , Boyu Qu , Alan J McCue , Shaoliang Guan , Jos Derksen , Ye Shui Zhang","doi":"10.1016/j.ccst.2025.100382","DOIUrl":"10.1016/j.ccst.2025.100382","url":null,"abstract":"<div><div>The production of H<sub>2</sub>-rich syngas from pyrolysis-catalytic gasification of plastic waste bottles has been investigated. The hybrid-functional materials consisting of Ni as catalyst, CaO as CO<sub>2</sub> sorbent and Ca<sub>2</sub>SiO<sub>4</sub> as a polymorphic active spacer were synthesized. The different parameters (Ni loading, temperature, N<sub>2</sub> flow rate and feedstock-to-catalyst ratio) have been investigated to optimise the H<sub>2</sub> production. The catalysts were analysed by N<sub>2</sub> physisorption, scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Temperature-programmed reduction (TPR) and <em>in-situ</em> Transmission Electron Microscopy (TEM). Temperature-programmed oxidation (TPO) was used to analyse the carbon formation on the used catalysts. The highest H<sub>2</sub> production of 59.15 mmol g<sup>-1</sup><sub>of plastic</sub> was obtained in the presence of a catalyst with 20 wt.% Ni loading, which amounts to H<sub>2</sub> purity as high as 54.2 vol% in gas production. Furthermore, 90.63 mmol g<sup>-1</sup><sub>of plastic</sub> of syngas was produced by increasing the feedstock-to-catalyst ratio to 4:1, yielding 84.4 vol.% of total gas product (53.1 vol.% of H<sub>2</sub> and 31.3 vol.% of CO, respectively). The Ni-CaO<img>Ca<sub>2</sub>SiO<sub>4</sub> hybrid-functional material is a very promising catalyst in the pyrolysis-catalytic gasification process by capturing CO<sub>2</sub> as it is produced, therefore shifting the water gas shift (WGS) reaction to enhance H<sub>2</sub> production from plastic waste. Detailed elucidation of the roles of each component at the microscale during the catalytic process was also provided through <em>in-situ</em> TEM analysis. The finding could guide the industry for future large-scale application to convert abundant plastic waste into H<sub>2</sub>-rich syngas, therefore contributing to the global ‘net zero’ ambition.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"14 ","pages":"Article 100382"},"PeriodicalIF":0.0,"publicationDate":"2025-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143156853","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-28DOI: 10.1016/j.ccst.2024.100358
Hengyu Wei , Min Lin , Juping Zhang , Di Gao , Yuhao Chen , Liang Zhang , Xing Zhu
Coupled calcium cycling and dry reforming of methane (CaL-DRM) process has garnered significant attention in recent years as a promising technique for the CO2 capture and in-situ conversion. However, traditional Ni-CaO catalysts with substantial CaL-DRM activity are susceptible to severe carbon deposition, which greatly hinders their industrial application. A combination of sol-gel and impregnation methods to include LaFeO3 into Ni-CaO to enhance CO2 capture and conversion is utilized. The characterization results indicate that the incorporation of LaFeO3 significantly improves the dispersion of Ni and CaO, increases the concentration of oxygen vacancies, effectively suppresses the sintering and carbon deposition, and improves the cycling stability of Ni-CaO. In addition, LaFeO3 promotes the outward diffusion of lattice oxygen, thereby facilitating CO2 capture and CH4 conversion to syngas. At 700 ℃, up to 86.5 % CO2 conversion, 87.6 % CO selectivity, and syngas yield close to the theoretical value of 1.0 were achieved over 5Ni-30CaO-LFO (30 wt% CaO). More importantly, the activity of catalyst remains almost unchanged after 30 cycles. This study introduces an innovative approach for CaL-DRM, showing significant potential for effective and stable CO2 capture and in-situ conversion.
{"title":"Carbon-resistant bifunctional catalyst composed of LaFeO3 enhanced Ni-CaO for integrated CO2 capture and conversion","authors":"Hengyu Wei , Min Lin , Juping Zhang , Di Gao , Yuhao Chen , Liang Zhang , Xing Zhu","doi":"10.1016/j.ccst.2024.100358","DOIUrl":"10.1016/j.ccst.2024.100358","url":null,"abstract":"<div><div>Coupled calcium cycling and dry reforming of methane (CaL-DRM) process has garnered significant attention in recent years as a promising technique for the CO<sub>2</sub> capture and <em>in-situ</em> conversion. However, traditional Ni-CaO catalysts with substantial CaL-DRM activity are susceptible to severe carbon deposition, which greatly hinders their industrial application. A combination of sol-gel and impregnation methods to include LaFeO<sub>3</sub> into Ni-CaO to enhance CO<sub>2</sub> capture and conversion is utilized. The characterization results indicate that the incorporation of LaFeO<sub>3</sub> significantly improves the dispersion of Ni and CaO, increases the concentration of oxygen vacancies, effectively suppresses the sintering and carbon deposition, and improves the cycling stability of Ni-CaO. In addition, LaFeO<sub>3</sub> promotes the outward diffusion of lattice oxygen, thereby facilitating CO<sub>2</sub> capture and CH<sub>4</sub> conversion to syngas. At 700 ℃, up to 86.5 % CO<sub>2</sub> conversion, 87.6 % CO selectivity, and syngas yield close to the theoretical value of 1.0 were achieved over 5Ni-30CaO-LFO (30 wt% CaO). More importantly, the activity of catalyst remains almost unchanged after 30 cycles. This study introduces an innovative approach for CaL-DRM, showing significant potential for effective and stable CO<sub>2</sub> capture and <em>in-situ</em> conversion.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"14 ","pages":"Article 100358"},"PeriodicalIF":0.0,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143157456","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-27DOI: 10.1016/j.ccst.2025.100375
Feras Rowaihy , Ali Hamieh , Naser Odeh , Mohamad Hejazi , Mohammed Al-Juaied , Abdulkader M. Afifi , Hussein Hoteit
The global drive for net-zero emissions has highlighted carbon capture, utilization, and storage (CCUS) as a critical tool to reduce CO₂ emissions from energy and industrial sectors. Achieving climate goals necessitates a comprehensive understanding of regional CO₂ emission profiles and capture costs to inform effective decarbonization strategies. As one of the largest CO₂ emitters globally, Saudi Arabia has committed to achieving net-zero emissions by 2060. However, the economic implications of deploying CCUS within the Kingdom remain insufficiently explored. This work provides updated estimates of CO₂ emissions across key sectors in Saudi Arabia, including electricity, petrochemicals, refineries, cement, steel, ammonia production, and desalination, based on 2022 data. The CO2 capture costs are estimated by incorporating stationary emission plant data with reference cases from analogous industrial sectors, including capital expenditure (CAPEX) and operating expenditure (OPEX). The total capture cost per ton of CO2 is determined by combining these cost components using an established economic model and a custom-developed tool. The study constructs a comprehensive CO₂ capture cost curve for Saudi Arabia, highlighting the variability of capture costs across regions and industries. Our analysis indicates an average CO₂ capture cost of $69/tCO₂, with substantial variability across industries. Ammonia production emerges as the most cost-efficient at $11/tCO₂, driven by its high CO₂ concentration, whereas smaller-scale operations can incur costs up to $189/tCO₂. Results show that economies of scale and CO₂ concentration play pivotal roles in determining capture feasibility, with low-cost opportunities identified in ammonia production and high-emission industrial clusters, particularly in the Eastern and Western regions. The Eastern region, with its planned CCS hub in Jubail, emerges as the most promising for near-term deployment. In contrast, the Western region requires additional focus on storage alternatives such as mineralization. Benchmarking against global capture costs reveals that Saudi Arabia's industrial landscape, characterized by large-scale emitters, is well-positioned for cost-effective CCUS implementation. The study highlights the need to prioritize low-cost capture opportunities and develop strategies tailored to regional and sector-specific conditions, offering a roadmap for the Kingdom's significant contribution to global net-zero ambitions.
{"title":"Decarbonizing Saudi Arabia energy and industrial sectors: Assessment of carbon capture cost","authors":"Feras Rowaihy , Ali Hamieh , Naser Odeh , Mohamad Hejazi , Mohammed Al-Juaied , Abdulkader M. Afifi , Hussein Hoteit","doi":"10.1016/j.ccst.2025.100375","DOIUrl":"10.1016/j.ccst.2025.100375","url":null,"abstract":"<div><div>The global drive for net-zero emissions has highlighted carbon capture, utilization, and storage (CCUS) as a critical tool to reduce CO₂ emissions from energy and industrial sectors. Achieving climate goals necessitates a comprehensive understanding of regional CO₂ emission profiles and capture costs to inform effective decarbonization strategies. As one of the largest CO₂ emitters globally, Saudi Arabia has committed to achieving net-zero emissions by 2060. However, the economic implications of deploying CCUS within the Kingdom remain insufficiently explored. This work provides updated estimates of CO₂ emissions across key sectors in Saudi Arabia, including electricity, petrochemicals, refineries, cement, steel, ammonia production, and desalination, based on 2022 data. The CO<sub>2</sub> capture costs are estimated by incorporating stationary emission plant data with reference cases from analogous industrial sectors, including capital expenditure (CAPEX) and operating expenditure (OPEX). The total capture cost per ton of CO<sub>2</sub> is determined by combining these cost components using an established economic model and a custom-developed tool. The study constructs a comprehensive CO₂ capture cost curve for Saudi Arabia, highlighting the variability of capture costs across regions and industries. Our analysis indicates an average CO₂ capture cost of $69/tCO₂, with substantial variability across industries. Ammonia production emerges as the most cost-efficient at $11/tCO₂, driven by its high CO₂ concentration, whereas smaller-scale operations can incur costs up to $189/tCO₂. Results show that economies of scale and CO₂ concentration play pivotal roles in determining capture feasibility, with low-cost opportunities identified in ammonia production and high-emission industrial clusters, particularly in the Eastern and Western regions. The Eastern region, with its planned CCS hub in Jubail, emerges as the most promising for near-term deployment. In contrast, the Western region requires additional focus on storage alternatives such as mineralization. Benchmarking against global capture costs reveals that Saudi Arabia's industrial landscape, characterized by large-scale emitters, is well-positioned for cost-effective CCUS implementation. The study highlights the need to prioritize low-cost capture opportunities and develop strategies tailored to regional and sector-specific conditions, offering a roadmap for the Kingdom's significant contribution to global net-zero ambitions.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"14 ","pages":"Article 100375"},"PeriodicalIF":0.0,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143157457","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-27DOI: 10.1016/j.ccst.2025.100379
Shervan Babamohammadi , Amy R Birss , Hamid Pouran , Jagroop Pandhal , Tohid N. Borhani
Diesel generators play a crucial role in providing electricity, particularly in less developed economies. As achieving Net Zero 2050 gains more traction, it is essential to address the environmental impacts and emission contributions of diesel generators. In this paper, we review the past decade of research into diesel generator emissions and discuss technologies available to mitigate their environmental effects. Starting with a description of the market importance and environmental problems caused by the release of chemicals like nitrogen oxides (NOX), sulphur oxides (SOX), carbon monoxide (CO), hydrocarbons (HC), and carbon dioxide (CO2) as well as particulate matter (soot), the paper categorises and evaluates advanced mitigation systems. These systems include After-treatment Technologies, Engine Modification Technologies, and Fuel Modification Strategies. After-treatment systems such as Diesel Particulate Filters (DPF), Diesel Oxidation Catalysts (DOC), Selective Catalytic Reduction (SCR) and Exhaust Gas Recirculation (EGR) and their recent advancement are reviewed, followed by Engine Modification technologies, including Fuel Injection Strategies, Miller Cycle and In-cylinder Combustion Control. Then, we summarise the Fuel Modification Strategies and recent developments such as Blending Biodiesel and Diesel, Nanofuel Additives to Diesel, Metal-based Additives to Diesel and blending of Alcohol and Diesel. Furthermore, the potential for retrofitting CO2 capture technologies to diesel generators is discussed as the topic that has received less attention compared to other areas mentioned above. CO2 abatement methods, including absorption, adsorption, algae bio-fixation, and oxy-combustion techniques and their potential to be retrofitted for diesel generators, are also discussed. The paper concludes by reflecting on the importance that these technology developments play in the United Nations Sustainable Development Goals (SDGs), specifically in promoting good health, sustainable energy, innovation, and climate action. The work aims to contribute to addressing the significant gap in the decarbonisation of diesel generators by cohesively and systematically reviewing the research topics mentioned earlier. This gap is particularly evident in the application of CO2 abatement technologies within the context of diesel generators, and this research strives to provide a foundation for further research in this critical area to meet Net Zero targets.
{"title":"Emission control and carbon capture from diesel generators and engines: A decade-long perspective","authors":"Shervan Babamohammadi , Amy R Birss , Hamid Pouran , Jagroop Pandhal , Tohid N. Borhani","doi":"10.1016/j.ccst.2025.100379","DOIUrl":"10.1016/j.ccst.2025.100379","url":null,"abstract":"<div><div>Diesel generators play a crucial role in providing electricity, particularly in less developed economies. As achieving Net Zero 2050 gains more traction, it is essential to address the environmental impacts and emission contributions of diesel generators. In this paper, we review the past decade of research into diesel generator emissions and discuss technologies available to mitigate their environmental effects. Starting with a description of the market importance and environmental problems caused by the release of chemicals like nitrogen oxides (NO<sub>X</sub>), sulphur oxides (SO<sub>X</sub>), carbon monoxide (CO), hydrocarbons (HC), and carbon dioxide (CO<sub>2</sub>) as well as particulate matter (soot), the paper categorises and evaluates advanced mitigation systems. These systems include After-treatment Technologies, Engine Modification Technologies, and Fuel Modification Strategies. After-treatment systems such as Diesel Particulate Filters (DPF), Diesel Oxidation Catalysts (DOC), Selective Catalytic Reduction (SCR) and Exhaust Gas Recirculation (EGR) and their recent advancement are reviewed, followed by Engine Modification technologies, including Fuel Injection Strategies, Miller Cycle and In-cylinder Combustion Control. Then, we summarise the Fuel Modification Strategies and recent developments such as Blending Biodiesel and Diesel, Nanofuel Additives to Diesel, Metal-based Additives to Diesel and blending of Alcohol and Diesel. Furthermore, the potential for retrofitting CO<sub>2</sub> capture technologies to diesel generators is discussed as the topic that has received less attention compared to other areas mentioned above. CO<sub>2</sub> abatement methods, including absorption, adsorption, algae bio-fixation, and oxy-combustion techniques and their potential to be retrofitted for diesel generators, are also discussed. The paper concludes by reflecting on the importance that these technology developments play in the United Nations Sustainable Development Goals (SDGs), specifically in promoting good health, sustainable energy, innovation, and climate action. The work aims to contribute to addressing the significant gap in the decarbonisation of diesel generators by cohesively and systematically reviewing the research topics mentioned earlier. This gap is particularly evident in the application of CO<sub>2</sub> abatement technologies within the context of diesel generators, and this research strives to provide a foundation for further research in this critical area to meet Net Zero targets.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"14 ","pages":"Article 100379"},"PeriodicalIF":0.0,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143157585","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-25DOI: 10.1016/j.ccst.2025.100378
Ziyi Li , Cong Wang , Jin Xiao , Xu Jiang , Ningqi Sun , Xiong Yang , Yingshu Liu
Adsorption has long been recognized as a vital and extensively utilized technology for CO2 capture, for which developing a cost-effective process is a long-sought goal. The structured adsorbent with faster heat and mass transfer, present new opportunities for advancing rotary adsorption process, however, lacks comprehensive evaluation and discussion on CO2 sorption. In this study, structured adsorbents were prepared by washcoating commercial NaY and 13X zeolites onto a fiberglass honeycomb support. A series of characterizations and breakthrough test demonstrated the advantages of structured adsorbents over conventional pellets. NaY zeolite emerged as the thermodynamically and kinetically preferred CO2 adsorbent, exhibiting an equilibrium adsorption capacity of 5.972 mmol·g-1 and an internal mass transfer coefficient of 5.12 × 10–3 s-1 (15 % CO2, 298 K, 1 bar). These values are 18.3 % and 164 % higher than those of its pellet counterpart and 12.3 % and 36.9 % higher than those of the 13X honeycomb. NaY's great adaptability across various applications was indicated by its breakthrough capacities at different temperatures and CO2 feed concentrations, as well as the minimal influence of feed gas flow rate on CO2 adsorption equilibrium and kinetics. By employing a recirculating thermal desorption strategy, CO2 can be enriched from 5 % to 61 %, 15 % to 79 %, and 55 % to 92 %, achieving a 90 % recovery under mild desorption conditions. A two-stage rotary adsorption process for low-concentration CO2 capture was proposed, enabling CO2 enriched from 5 % to 55 % in the first stage, and further to 90 % in the second stage. This work introduces a promising approaches for low-cost industrial carbon capture and even direct air carbon capture.
{"title":"Washcoated zeolite structured adsorbents for CO2 capture and recovery by rotary adsorption","authors":"Ziyi Li , Cong Wang , Jin Xiao , Xu Jiang , Ningqi Sun , Xiong Yang , Yingshu Liu","doi":"10.1016/j.ccst.2025.100378","DOIUrl":"10.1016/j.ccst.2025.100378","url":null,"abstract":"<div><div>Adsorption has long been recognized as a vital and extensively utilized technology for CO2 capture, for which developing a cost-effective process is a long-sought goal. The structured adsorbent with faster heat and mass transfer, present new opportunities for advancing rotary adsorption process, however, lacks comprehensive evaluation and discussion on CO<sub>2</sub> sorption. In this study, structured adsorbents were prepared by washcoating commercial NaY and 13X zeolites onto a fiberglass honeycomb support. A series of characterizations and breakthrough test demonstrated the advantages of structured adsorbents over conventional pellets. NaY zeolite emerged as the thermodynamically and kinetically preferred CO<sub>2</sub> adsorbent, exhibiting an equilibrium adsorption capacity of 5.972 mmol·g<sup>-1</sup> and an internal mass transfer coefficient of 5.12 × 10<sup>–3</sup> s<sup>-1</sup> (15 % CO<sub>2</sub>, 298 K, 1 bar). These values are 18.3 % and 164 % higher than those of its pellet counterpart and 12.3 % and 36.9 % higher than those of the 13X honeycomb. NaY's great adaptability across various applications was indicated by its breakthrough capacities at different temperatures and CO<sub>2</sub> feed concentrations, as well as the minimal influence of feed gas flow rate on CO<sub>2</sub> adsorption equilibrium and kinetics. By employing a recirculating thermal desorption strategy, CO<sub>2</sub> can be enriched from 5 % to 61 %, 15 % to 79 %, and 55 % to 92 %, achieving a 90 % recovery under mild desorption conditions. A two-stage rotary adsorption process for low-concentration CO<sub>2</sub> capture was proposed, enabling CO<sub>2</sub> enriched from 5 % to 55 % in the first stage, and further to 90 % in the second stage. This work introduces a promising approaches for low-cost industrial carbon capture and even direct air carbon capture.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"14 ","pages":"Article 100378"},"PeriodicalIF":0.0,"publicationDate":"2025-01-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143386562","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-25DOI: 10.1016/j.ccst.2025.100376
Xueyang Jiang , Xiaoshen Li , Shaohui Xiong , Wei Liu , Jiayan Yan , Xiang Duan , Song Song , Qingpeng Cheng , Ye Tian , Xingang Li
The hydrogenation of CO2 to methanol using H2 produced from renewable resources has been regarded as an effective way to mitigate CO2 emissions. Unfortunately, how to obtain both high activity and methanol selectivity is still a trade-off challenge for catalyst development. Herein, we synthesize Co-In-Zr ternary metal oxide precursors via a simple hydrothermal method for hydrogenation of CO2 to methanol. After reduction by H2, a part of Co and In cations could be reduced from the solid solution to generate CoIn alloy, simultaneously constructing oxygen vacancy rich environment on the catalyst surface. The increased concentration of surface oxygen vacancies can improve the adsorption and activation of CO2. Meanwhile, our findings show that the formed CoIn alloy significantly enhances the adsorption and dissociation of H2, thus accelerating successive hydroconversion of CO2 and intermediates to methanol. The synergy of CoIn alloy and oxygen vacancies significantly boosts both activity and methanol selectivity. Under the conditions of 300 °C and GHSV of 30,000 ml gcat-1 h-1, the catalyst with a Co: In: Zr molar ratio of 1: 2: 7 achieves the CO2 conversion of 10.2 %, the methanol selectivity of 81.5 %, and especially the methanol time-space yield up to 860 mg gcat-1 h-1, surpassing the majority of the state-of-the-art In-based catalysts. Moreover, the catalyst exhibits the excellent stability, maintaining the performance within 100 h. Our work provides insights into designing efficient none-noble-metal catalysts for CO2 hydrogenation reactions.
{"title":"Synergistical effect of CoIn alloy and oxygen vacancies over Co-In-Zr ternary catalysts boosting CO2 hydrogenation to methanol","authors":"Xueyang Jiang , Xiaoshen Li , Shaohui Xiong , Wei Liu , Jiayan Yan , Xiang Duan , Song Song , Qingpeng Cheng , Ye Tian , Xingang Li","doi":"10.1016/j.ccst.2025.100376","DOIUrl":"10.1016/j.ccst.2025.100376","url":null,"abstract":"<div><div>The hydrogenation of CO<sub>2</sub> to methanol using H<sub>2</sub> produced from renewable resources has been regarded as an effective way to mitigate CO<sub>2</sub> emissions. Unfortunately, how to obtain both high activity and methanol selectivity is still a trade-off challenge for catalyst development. Herein, we synthesize Co-In-Zr ternary metal oxide precursors via a simple hydrothermal method for hydrogenation of CO<sub>2</sub> to methanol. After reduction by H<sub>2</sub>, a part of Co and In cations could be reduced from the solid solution to generate CoIn alloy, simultaneously constructing oxygen vacancy rich environment on the catalyst surface. The increased concentration of surface oxygen vacancies can improve the adsorption and activation of CO<sub>2</sub>. Meanwhile, our findings show that the formed CoIn alloy significantly enhances the adsorption and dissociation of H<sub>2</sub>, thus accelerating successive hydroconversion of CO<sub>2</sub> and intermediates to methanol. The synergy of CoIn alloy and oxygen vacancies significantly boosts both activity and methanol selectivity. Under the conditions of 300 °C and GHSV of 30,000 ml g<sub>cat</sub><sup>-1</sup> h<sup>-1</sup>, the catalyst with a Co: In: Zr molar ratio of 1: 2: 7 achieves the CO<sub>2</sub> conversion of 10.2 %, the methanol selectivity of 81.5 %, and especially the methanol time-space yield up to 860 mg g<sub>cat</sub><sup>-1</sup> h<sup>-1</sup>, surpassing the majority of the state-of-the-art In-based catalysts. Moreover, the catalyst exhibits the excellent stability, maintaining the performance within 100 h. Our work provides insights into designing efficient none-noble-metal catalysts for CO<sub>2</sub> hydrogenation reactions.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"14 ","pages":"Article 100376"},"PeriodicalIF":0.0,"publicationDate":"2025-01-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143157581","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-21DOI: 10.1016/j.ccst.2025.100373
Hasan Can Gulbalkan , Alper Uzun , Seda Keskin
Given the vast number and diversity of metal-organic frameworks (MOFs) and ionic liquids (ILs), it is impractical to experimentally test the gas adsorption and separation potential of each one of the possible IL/MOF composites formed by the different combinations of these two components. In this study, we developed a comprehensive computational approach integrating Conductor-like Screening Model for Realistic Solvents (COSMO-RS) calculations, density functional theory (DFT) calculations, Grand Canonical Monte Carlo (GCMC) simulations, and machine learning (ML) algorithms to evaluate a wide variety of IL-incorporated ZIF-8 composites for CO2 separations. We examined 1322 different types of IL/ZIF-8 composites, covering the largest variety of ILs studied to date (8 cations and 35 anions) at various loadings, for flue gas separation and natural gas purification. We simulated CO2, CH4, and N2 adsorption properties of these composites and used this high-quality molecular simulation data to develop ML models that can predict gas uptakes of any IL/ZIF-8 composite when chemical and structural features of the IL are given. The accurate prediction power of these ML models was shown by comparing their estimates with the experimental and simulation data. Our approach significantly accelerates the assessment of a very large number of IL/ZIF-8 composites and reveals the key molecular features of ILs to make composites for achieving superior gas separation performance.
{"title":"Assessing CO2 separation performances of IL/ZIF-8 composites using molecular features of ILs","authors":"Hasan Can Gulbalkan , Alper Uzun , Seda Keskin","doi":"10.1016/j.ccst.2025.100373","DOIUrl":"10.1016/j.ccst.2025.100373","url":null,"abstract":"<div><div>Given the vast number and diversity of metal-organic frameworks (MOFs) and ionic liquids (ILs), it is impractical to experimentally test the gas adsorption and separation potential of each one of the possible IL/MOF composites formed by the different combinations of these two components. In this study, we developed a comprehensive computational approach integrating Conductor-like Screening Model for Realistic Solvents (COSMO-RS) calculations, density functional theory (DFT) calculations, Grand Canonical Monte Carlo (GCMC) simulations, and machine learning (ML) algorithms to evaluate a wide variety of IL-incorporated ZIF-8 composites for CO<sub>2</sub> separations. We examined 1322 different types of IL/ZIF-8 composites, covering the largest variety of ILs studied to date (8 cations and 35 anions) at various loadings, for flue gas separation and natural gas purification. We simulated CO<sub>2</sub>, CH<sub>4</sub>, and N<sub>2</sub> adsorption properties of these composites and used this high-quality molecular simulation data to develop ML models that can predict gas uptakes of any IL/ZIF-8 composite when chemical and structural features of the IL are given. The accurate prediction power of these ML models was shown by comparing their estimates with the experimental and simulation data. Our approach significantly accelerates the assessment of a very large number of IL/ZIF-8 composites and reveals the key molecular features of ILs to make composites for achieving superior gas separation performance.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"14 ","pages":"Article 100373"},"PeriodicalIF":0.0,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143157455","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-20DOI: 10.1016/j.ccst.2025.100368
Jie Chen, Zheming Zhang, Yizhe Shen, Hailong Li, Xiaoqing Lin, Xiaodong Li, Jianhua Yan
As a typical alkaline hazardous waste, municipal solid waste incineration fly ash is used for CO2 storage and cement supplementary material, contributing to carbon emission reduction and hazardous waste management. This study proposed a new idea of using ultrasonic accelerated carbonated fly ash (UFA) to modify CO2 mineralization cured cement, aimed at recycling FA while enhancing cement performance. Incorporating small amounts of UFA (5% and 10%) significantly improved the mechanical properties of cement paste, with the optimal inclusion of 10% UFA yielding a compressive strength of 50.23 MPa—higher than that of pure cement (41.04 MPa). The UFA contributed to pore filling and acts as a nucleation site for CO2 mineralization, forming stable flaky calcite and thus enhancing the microstructure. Conversely, higher UFA contents (20% and 50%) reduced performance due to a dilution effect that impaired the hydration product structure. Kinetic analysis via the Avrami-Erofeev model revealed that CO2 diffusion and crystal growth primarily control the mineralization reaction. The 50%UFA cement paste exhibited the greatest carbon fixation depth, with a carbon sequestration capacity of 186 g-CO2/kg-PC. This was attributed to its enhanced porosity and pore size, which facilitated CO2 diffusion. The 10%UFA cement paste, which had the highest compressive strength, also achieved a carbon sequestration capacity of 158 g-CO2/kg-PC, surpassing the 144 g-CO2/kg-PC of the pure cement paste. Moreover, the proposed UFA-modified CO2 mineralization cement displayed a low risk of heavy metal leaching under alkaline or acidic environment.
{"title":"A novel insight into CO2-cured cement modified by ultrasonic carbonated waste incineration fly ash: Mechanical properties, carbon sequestration, and heavy metals immobilization","authors":"Jie Chen, Zheming Zhang, Yizhe Shen, Hailong Li, Xiaoqing Lin, Xiaodong Li, Jianhua Yan","doi":"10.1016/j.ccst.2025.100368","DOIUrl":"10.1016/j.ccst.2025.100368","url":null,"abstract":"<div><div>As a typical alkaline hazardous waste, municipal solid waste incineration fly ash is used for CO<sub>2</sub> storage and cement supplementary material, contributing to carbon emission reduction and hazardous waste management. This study proposed a new idea of using ultrasonic accelerated carbonated fly ash (UFA) to modify CO<sub>2</sub> mineralization cured cement, aimed at recycling FA while enhancing cement performance. Incorporating small amounts of UFA (5% and 10%) significantly improved the mechanical properties of cement paste, with the optimal inclusion of 10% UFA yielding a compressive strength of 50.23 MPa—higher than that of pure cement (41.04 MPa). The UFA contributed to pore filling and acts as a nucleation site for CO<sub>2</sub> mineralization, forming stable flaky calcite and thus enhancing the microstructure. Conversely, higher UFA contents (20% and 50%) reduced performance due to a dilution effect that impaired the hydration product structure. Kinetic analysis via the Avrami-Erofeev model revealed that CO<sub>2</sub> diffusion and crystal growth primarily control the mineralization reaction. The 50%UFA cement paste exhibited the greatest carbon fixation depth, with a carbon sequestration capacity of 186 g-CO<sub>2</sub>/kg-PC. This was attributed to its enhanced porosity and pore size, which facilitated CO<sub>2</sub> diffusion. The 10%UFA cement paste, which had the highest compressive strength, also achieved a carbon sequestration capacity of 158 g-CO<sub>2</sub>/kg-PC, surpassing the 144 g-CO<sub>2</sub>/kg-PC of the pure cement paste. Moreover, the proposed UFA-modified CO<sub>2</sub> mineralization cement displayed a low risk of heavy metal leaching under alkaline or acidic environment.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"14 ","pages":"Article 100368"},"PeriodicalIF":0.0,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143100120","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-19DOI: 10.1016/j.ccst.2025.100370
Mohamed Essalhi , El-Hassan Mahmoud , Ali Tayeb , Rawan A. Al-Qahtani , Ahmad Salam Farooqi , Mahmoud Abdelnaby
Covalent organic frameworks (COFs) are an attractive subclass of porous solids due to their strong potential in various applications. The reticular chemistry behind COF design enables the achievement of desired functional properties. Additionally, the post-synthesis modification (PSM) of COFs is an effective method for tuning their skeleton architecture, chemical stability, and chemical interactions with guest molecules to enhance specific properties. However, the inherent challenges related to their chemical and thermal stability have limited their widespread use. Recently, various approaches for PSM on the pre-established covalent framework have been reported, providing an opportunity to tune the functional properties of COFs while maintaining and even strengthening their fundamental framework integrity and crystallinity. This review highlights recent advancements in synthesis strategies and PSM of COFs with enhanced stability and versatile functional properties. The discussion highlights different design approaches of COFs, such as the compatible reticular chemistry of their stronger covalent bonds and rigid building blocks and new innovative PSM techniques, including cross-linking and surface functionalization. Additionally, we explore the impact of these strategies on COF properties, such as porosity, chemical and thermal stability, and their surface chemistry, thereby expanding their practical applications. We provide a comprehensive overview of current advances in COF solids and performances in gas adsorption and separation applications, specifically for carbon capture and conversion, as well as in direct air capture (DAC) of CO2. This review aims to offer insights into the future directions of COF research, focusing on developing robust and functional COFs that meet real-world carbon capture and utilization requirements.
{"title":"Structural design of covalent organic frameworks and their recent advancements in carbon capture applications: A review","authors":"Mohamed Essalhi , El-Hassan Mahmoud , Ali Tayeb , Rawan A. Al-Qahtani , Ahmad Salam Farooqi , Mahmoud Abdelnaby","doi":"10.1016/j.ccst.2025.100370","DOIUrl":"10.1016/j.ccst.2025.100370","url":null,"abstract":"<div><div>Covalent organic frameworks (COFs) are an attractive subclass of porous solids due to their strong potential in various applications. The reticular chemistry behind COF design enables the achievement of desired functional properties. Additionally, the post-synthesis modification (PSM) of COFs is an effective method for tuning their skeleton architecture, chemical stability, and chemical interactions with guest molecules to enhance specific properties. However, the inherent challenges related to their chemical and thermal stability have limited their widespread use. Recently, various approaches for PSM on the pre-established covalent framework have been reported, providing an opportunity to tune the functional properties of COFs while maintaining and even strengthening their fundamental framework integrity and crystallinity. This review highlights recent advancements in synthesis strategies and PSM of COFs with enhanced stability and versatile functional properties. The discussion highlights different design approaches of COFs, such as the compatible reticular chemistry of their stronger covalent bonds and rigid building blocks and new innovative PSM techniques, including cross-linking and surface functionalization. Additionally, we explore the impact of these strategies on COF properties, such as porosity, chemical and thermal stability, and their surface chemistry, thereby expanding their practical applications. We provide a comprehensive overview of current advances in COF solids and performances in gas adsorption and separation applications, specifically for carbon capture and conversion, as well as in direct air capture (DAC) of CO<sub>2</sub>. This review aims to offer insights into the future directions of COF research, focusing on developing robust and functional COFs that meet real-world carbon capture and utilization requirements.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"14 ","pages":"Article 100370"},"PeriodicalIF":0.0,"publicationDate":"2025-01-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143157583","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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