Pub Date : 2024-11-20DOI: 10.1016/j.jcou.2024.102977
Marcelo Echeverri , Eva M. Maya , Dulce M. Muñoz
Two families of heterogeneous porous catalysts based on iron or cobalt poly(azomethine) (PAM) networks were reported to synthesize cyclic carbonates from bio-based aliphatic oxides epoxides and carbon dioxide (CO2). The different PAM supports were prepared by reacting 2,6-pyridine dicarboxaldehyde with 1,3,5 tris(4 aminophenyl)benzene (PAM-1) or with melamine (PAM-2) by microwave activation. Both supports exhibited high thermal stability and similar CO2 uptake (1.3 mmol/g) but PAM-2 showed higher specific surface area (779 m2/g vs 401 m2/g), more crystallinity and less capacity for anchoring metals than PAM-1. The novel catalysts were used in the cycloaddition of CO2 to renewable feedstocks. Thus, using epoxidized methyl oleate (MOE) the corresponding cyclic carbonates were obtained with excellent yields (78–96 %) using a CO2 pressure of 7 bars, 120 ºC and 16 h of reaction. The best catalysts of the series, Fe@PAMs were also evaluated in the cycloaddition of CO2 to epoxidized soybean oil (ESBO) in the same condition reaction obtaining excellent performance, epoxide conversions and cyclic carbonate yields greater than 90 %.
{"title":"Formation of bio-based cyclic carbonates from CO2 and renewable feedstocks via porous poly(azomethine) -based heterogeneous catalysts approach","authors":"Marcelo Echeverri , Eva M. Maya , Dulce M. Muñoz","doi":"10.1016/j.jcou.2024.102977","DOIUrl":"10.1016/j.jcou.2024.102977","url":null,"abstract":"<div><div>Two families of heterogeneous porous catalysts based on iron or cobalt poly(azomethine) (PAM) networks were reported to synthesize cyclic carbonates from bio-based aliphatic oxides epoxides and carbon dioxide (CO<sub>2</sub>). The different PAM supports were prepared by reacting 2,6-pyridine dicarboxaldehyde with 1,3,5 tris(4 aminophenyl)benzene (PAM-1) or with melamine (PAM-2) by microwave activation. Both supports exhibited high thermal stability and similar CO<sub>2</sub> uptake (1.3 mmol/g) but PAM-2 showed higher specific surface area (779 m<sup>2</sup>/g vs 401 m<sup>2</sup>/g), more crystallinity and less capacity for anchoring metals than PAM-1. The novel catalysts were used in the cycloaddition of CO<sub>2</sub> to renewable feedstocks. Thus, using epoxidized methyl oleate (MOE) the corresponding cyclic carbonates were obtained with excellent yields (78–96 %) using a CO<sub>2</sub> pressure of 7 bars, 120 ºC and 16 h of reaction. The best catalysts of the series, Fe@PAMs were also evaluated in the cycloaddition of CO<sub>2</sub> to epoxidized soybean oil (ESBO) in the same condition reaction obtaining excellent performance, epoxide conversions and cyclic carbonate yields greater than 90 %.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"90 ","pages":"Article 102977"},"PeriodicalIF":7.2,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142706940","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}
Pub Date : 2024-11-19DOI: 10.1016/j.jcou.2024.102979
Xingyu Liu, Wei Yan
Electric arc furnace (EAF) steelmaking offers significant advantages in terms of low CO2 emissions, making it a promising avenue for achieving carbon peaking and carbon neutrality in the iron and steel industry. However, the conventional slag foaming practice through injection of fossil-based carbon (coal and coke) and oxygen still contributes most direct CO2 emissions to EAF steelmaking. Development of low-fossil carbon even fossil carbon-free slag foaming technology has presented a new opportunity to further decrease the CO2 emissions of EAFs. The present review systematically delves into the current advancements in EAF slag foaming processes to inspire and give valuable insights on near-zero CO2 emission slag foaming technology. The foaming slag theory and evaluation models were first summarized. And then the strengths and weaknesses of most of distinct slag foaming processes, namely the conventional carbon-oxygen injection slag foaming process, the slag foaming process utilizing waste plastics and rubber, biomass chars, carbonates and nitrates, and the exogenous gas injection slag foaming process, were reviewed and analyzed from perspectives of foamy mechanism and performance, reduction of CO2, industrial application and challenge. In general, the carbon-free exogenous gas injection or combined injection with biomass char exhibit the most promising potential among these slag foaming processes in terms of great CO2 reduction and even near-zero CO2 emission. Ultimately, the future prospects surrounding the development directions and industrial application challenge of low-CO2 and near-zero CO2 emission slag foaming technology were discussed and summarized.
{"title":"Current advances in slag foaming processes toward reduced CO2 emission for electric arc furnace steelmaking","authors":"Xingyu Liu, Wei Yan","doi":"10.1016/j.jcou.2024.102979","DOIUrl":"10.1016/j.jcou.2024.102979","url":null,"abstract":"<div><div>Electric arc furnace (EAF) steelmaking offers significant advantages in terms of low CO<sub>2</sub> emissions, making it a promising avenue for achieving carbon peaking and carbon neutrality in the iron and steel industry. However, the conventional slag foaming practice through injection of fossil-based carbon (coal and coke) and oxygen still contributes most direct CO<sub>2</sub> emissions to EAF steelmaking. Development of low-fossil carbon even fossil carbon-free slag foaming technology has presented a new opportunity to further decrease the CO<sub>2</sub> emissions of EAFs. The present review systematically delves into the current advancements in EAF slag foaming processes to inspire and give valuable insights on near-zero CO<sub>2</sub> emission slag foaming technology. The foaming slag theory and evaluation models were first summarized. And then the strengths and weaknesses of most of distinct slag foaming processes, namely the conventional carbon-oxygen injection slag foaming process, the slag foaming process utilizing waste plastics and rubber, biomass chars, carbonates and nitrates, and the exogenous gas injection slag foaming process, were reviewed and analyzed from perspectives of foamy mechanism and performance, reduction of CO<sub>2</sub>, industrial application and challenge. In general, the carbon-free exogenous gas injection or combined injection with biomass char exhibit the most promising potential among these slag foaming processes in terms of great CO<sub>2</sub> reduction and even near-zero CO<sub>2</sub> emission. Ultimately, the future prospects surrounding the development directions and industrial application challenge of low-CO<sub>2</sub> and near-zero CO<sub>2</sub> emission slag foaming technology were discussed and summarized.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"90 ","pages":"Article 102979"},"PeriodicalIF":7.2,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142706939","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}
Pub Date : 2024-11-16DOI: 10.1016/j.jcou.2024.102976
Dongliang Wang , Yun Du , Zuwei Liao , Xiaodong Hong , Shilong Zhang
This paper focuses on a liquid-phase CO2 hydrogenation process for methanol synthesis to enhance CO2 conversion. The feasibility of a liquid-phase CO2 hydrogenation process is comprehensively evaluated through a techno-economic analysis. The solvent tetraethylene glycol dimethyl ether is identified as one of the most favorable options following an analysis of the solubility data pertaining to various solvents and their influence on the reaction equilibrium of the substances within the system. The influence of process parameters, including temperature, pressure, solvent amount, and gas hourly space velocity (GHSV), on the conversion of CO2 and the selectivity for methanol is examined and optimized in a liquid-phase CO2 hydrogenation to methanol process without a gas recycle (Process 1), optimal reaction conditions are determined and a CO2 conversion of 95.19 % and a CH3OH yield of 94.77 % with a purity of 99.9 % are achieved. A liquid-phase process with a gas recycle (Process 2) is implemented to enhance the utilization of feed gas, achieving a CO2 conversion rate of 95.23 % and a methanol yield of 99.69 %. The liquid-phase process is further optimized by incorporating reactive distillation technology (Process 3), to enhance reaction efficiency and reduce energy consumption. Following the techno-economic evaluation, the energy efficiency of Process 3 is 7.79 % and 4.99 % higher than that of Process 1 and Process 2, respectively. The product cost of Process 3 is reduced by 8.75 % compared to Process 1 and by 4.25 % compared to Process 2. This research offers insights into the challenges associated with the development of the liquid-phase method.
{"title":"Liquid-phase CO2 hydrogenation to methanol synthesis: Solvent screening, process design and techno-economic evaluation","authors":"Dongliang Wang , Yun Du , Zuwei Liao , Xiaodong Hong , Shilong Zhang","doi":"10.1016/j.jcou.2024.102976","DOIUrl":"10.1016/j.jcou.2024.102976","url":null,"abstract":"<div><div>This paper focuses on a liquid-phase CO<sub>2</sub> hydrogenation process for methanol synthesis to enhance CO<sub>2</sub> conversion. The feasibility of a liquid-phase CO<sub>2</sub> hydrogenation process is comprehensively evaluated through a techno-economic analysis. The solvent tetraethylene glycol dimethyl ether is identified as one of the most favorable options following an analysis of the solubility data pertaining to various solvents and their influence on the reaction equilibrium of the substances within the system. The influence of process parameters, including temperature, pressure, solvent amount, and gas hourly space velocity (GHSV), on the conversion of CO<sub>2</sub> and the selectivity for methanol is examined and optimized in a liquid-phase CO<sub>2</sub> hydrogenation to methanol process without a gas recycle (Process 1), optimal reaction conditions are determined and a CO<sub>2</sub> conversion of 95.19 % and a CH<sub>3</sub>OH yield of 94.77 % with a purity of 99.9 % are achieved. A liquid-phase process with a gas recycle (Process 2) is implemented to enhance the utilization of feed gas, achieving a CO<sub>2</sub> conversion rate of 95.23 % and a methanol yield of 99.69 %. The liquid-phase process is further optimized by incorporating reactive distillation technology (Process 3), to enhance reaction efficiency and reduce energy consumption. Following the techno-economic evaluation, the energy efficiency of Process 3 is 7.79 % and 4.99 % higher than that of Process 1 and Process 2, respectively. The product cost of Process 3 is reduced by 8.75 % compared to Process 1 and by 4.25 % compared to Process 2. This research offers insights into the challenges associated with the development of the liquid-phase method.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"90 ","pages":"Article 102976"},"PeriodicalIF":7.2,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142658502","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}
Capturing CO2 and converting it into valuable chemicals and fuels have been regarded as a pivotal strategy in addressing the environmental challenges of ever-growing CO2 emissions. Combining CO2 capture and conversion through material or process integration can eliminate the energy-intensive steps such as separation, compression, and transportation across a wide range of space and temperatures. The flue gas at high temperatures > 300 °C can be handled with dual-function materials consisting of sorbents and catalysts. The dual-function materials combine CO2 capture and conversion through material integration, converting CO2 with reactions such as methanation, reverse water-gas shift, dry reforming of CH4, and oxidative dehydrogenation of propane. On the other hand, capturing CO2 from air directly requires a long time to collect enough CO2 for the subsequent conversion reaction. Consequently, direct air capture will likely combine with the conversion reactions in stepwise operations. The low latent heat in CO2 from direct air capture makes it more suitable for reactions at a mild condition (< 250 °C), and stepwise operation allows the separate control of the capture and conversion conditions. Herein, we reviewed recent advancements in coupling CO2 capture from flue gas and ambient air with thermal catalytic conversion. We discussed the requirements for materials, reactor configuration, and process operation for capturing and converting CO2 from these sources and proposed that future research should focus on enhancing the efficiency, scalability, and sustainability of CO2 capture and conversion technologies and optimizing the process design.
捕获二氧化碳并将其转化为有价值的化学品和燃料，一直被视为应对二氧化碳排放量不断增长所带来的环境挑战的关键战略。通过材料或工艺集成将二氧化碳捕集和转化结合起来，可以省去分离、压缩和跨空间、跨温度运输等高能耗步骤。由吸附剂和催化剂组成的双功能材料可处理 300 °C 高温烟气。双功能材料通过材料集成将二氧化碳捕获和转化结合在一起，通过甲烷化、反向水气变换、CH4 干重整和丙烷氧化脱氢等反应转化二氧化碳。另一方面，直接从空气中捕获二氧化碳需要很长时间才能收集到足够的二氧化碳进行后续转化反应。因此，直接从空气中捕获二氧化碳可能会与转化反应相结合，分步进行。直接从空气中捕获二氧化碳的潜热较低，因此更适合在温和的条件下（250 °C）进行反应，而且分步操作可以分别控制捕获和转化条件。在此，我们回顾了从烟道气和环境空气中捕集二氧化碳并进行热催化转化的最新进展。我们讨论了从这些来源捕集和转化二氧化碳对材料、反应器配置和工艺操作的要求，并建议未来的研究应侧重于提高二氧化碳捕集和转化技术的效率、可扩展性和可持续性，以及优化工艺设计。
{"title":"Recent advancements in integrating CO2 capture from flue gas and ambient air with thermal catalytic conversion for efficient CO2 utilization","authors":"Ruoyu Zhang , Zhenwei Xie , Qingfeng Ge , Xinli Zhu","doi":"10.1016/j.jcou.2024.102973","DOIUrl":"10.1016/j.jcou.2024.102973","url":null,"abstract":"<div><div>Capturing CO<sub>2</sub> and converting it into valuable chemicals and fuels have been regarded as a pivotal strategy in addressing the environmental challenges of ever-growing CO<sub>2</sub> emissions. Combining CO<sub>2</sub> capture and conversion through material or process integration can eliminate the energy-intensive steps such as separation, compression, and transportation across a wide range of space and temperatures. The flue gas at high temperatures > 300 °C can be handled with dual-function materials consisting of sorbents and catalysts. The dual-function materials combine CO<sub>2</sub> capture and conversion through material integration, converting CO<sub>2</sub> with reactions such as methanation, reverse water-gas shift, dry reforming of CH<sub>4</sub>, and oxidative dehydrogenation of propane. On the other hand, capturing CO<sub>2</sub> from air directly requires a long time to collect enough CO<sub>2</sub> for the subsequent conversion reaction. Consequently, direct air capture will likely combine with the conversion reactions in stepwise operations. The low latent heat in CO<sub>2</sub> from direct air capture makes it more suitable for reactions at a mild condition (< 250 °C), and stepwise operation allows the separate control of the capture and conversion conditions. Herein, we reviewed recent advancements in coupling CO<sub>2</sub> capture from flue gas and ambient air with thermal catalytic conversion. We discussed the requirements for materials, reactor configuration, and process operation for capturing and converting CO<sub>2</sub> from these sources and proposed that future research should focus on enhancing the efficiency, scalability, and sustainability of CO<sub>2</sub> capture and conversion technologies and optimizing the process design.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"89 ","pages":"Article 102973"},"PeriodicalIF":7.2,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142654236","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}
Pub Date : 2024-11-01DOI: 10.1016/j.jcou.2024.102975
Marcus Carter , Huong Giang T. Nguyen , Andrew J. Allen , Feng Yi , Wei-Chang D. Yang , Avery E. Baumann , W. Sean McGivern , Jeffrey A. Manion , Ivan Kuzmenko , Zois Tsinas , Charlotte M. Wentz , Malia Wenny , Daniel W. Siderius , Roger D. van Zee , Christopher M. Stafford , Craig M. Brown
As part of U.S. national efforts to combat the detrimental effect of global climate change, the National Institute of Standards and Technology (NIST) was recently tasked to support efforts in direct air capture (DAC) of carbon dioxide research and deployment. In order to develop test procedures, materials, and documentary standards, key characterization methods relevant to DAC materials have been investigated and used to identify desirable properties for a potential Standard Reference Material (SRM). Select amine-supported materials that previously showed potential for DAC applications have been characterized using commonly available laboratory methods. Further insights into the adsorption characteristics have been gained from developing and applying more specialized characterization tools ideal for probing low concentrations of carbon dioxide. A broad suite of capabilities that examine relevant properties under appropriate conditions gives the most profound insights into a material’s specific performance. We advocate for even more specialized capabilities to be developed and standardized to quantitatively monitor the interactions of CO2 with molecular species in complex and often disordered systems to advance DAC and support carbon dioxide reduction (CDR) in general.
{"title":"Progress in development of characterization capabilities to evaluate candidate materials for direct air capture applications","authors":"Marcus Carter , Huong Giang T. Nguyen , Andrew J. Allen , Feng Yi , Wei-Chang D. Yang , Avery E. Baumann , W. Sean McGivern , Jeffrey A. Manion , Ivan Kuzmenko , Zois Tsinas , Charlotte M. Wentz , Malia Wenny , Daniel W. Siderius , Roger D. van Zee , Christopher M. Stafford , Craig M. Brown","doi":"10.1016/j.jcou.2024.102975","DOIUrl":"10.1016/j.jcou.2024.102975","url":null,"abstract":"<div><div>As part of U.S. national efforts to combat the detrimental effect of global climate change, the National Institute of Standards and Technology (NIST) was recently tasked to support efforts in direct air capture (DAC) of carbon dioxide research and deployment. In order to develop test procedures, materials, and documentary standards, key characterization methods relevant to DAC materials have been investigated and used to identify desirable properties for a potential Standard Reference Material (SRM). Select amine-supported materials that previously showed potential for DAC applications have been characterized using commonly available laboratory methods. Further insights into the adsorption characteristics have been gained from developing and applying more specialized characterization tools ideal for probing low concentrations of carbon dioxide. A broad suite of capabilities that examine relevant properties under appropriate conditions gives the most profound insights into a material’s specific performance. We advocate for even more specialized capabilities to be developed and standardized to quantitatively monitor the interactions of CO<sub>2</sub> with molecular species in complex and often disordered systems to advance DAC and support carbon dioxide reduction (CDR) in general.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"89 ","pages":"Article 102975"},"PeriodicalIF":7.2,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142654305","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}
Pub Date : 2024-11-01DOI: 10.1016/j.jcou.2024.102971
Xiaojiao Cheng , Hu Wen , Shixing Fan , Bocong Liu , Rijun Li , Yanhui Xu , Wen Wang
Liquid CO2 enhancing coalbed methane recovery (CO2-ECBM) is an effective and intrinsically reliable gas drainage technology. Injection of liquid CO2 into coal seam has the dual effect of increasing the permeability of the coal and rock and strengthening the recovery of gas, which is manifested primarily as “pressure cracking, low temperature frostbite, physical extraction and chemical corrosion, phase change pressurization, low viscosity permeability, competitive adsorption”. In this paper, the acidification and corrosion of CO2-H2O-coal was studied in physical and chemical extraction by experimental test and comparative analysis. The liquid CO2 acidification reference group and the variable group experiment were designed. On the basis of the pH value of the aqueous solution, the content of major elements and minerals in coal, the minerals involved in chemical reaction, and their specific gravity were deduced. Variation in pore volume, specific surface area, and pore fractal characteristics were quantitatively and qualitatively analyzed. The experimental results show that the higher the pressure, the higher the content of carbonic acid dissolved in water and the amount of H+ ionized by carbonic acid. The longer the reaction time, the greater the mineral content involved in the chemical reaction, and the H+ in the water sample is consumed in large quantities. The elements of Na, K, Ca, Mg, Al, Si, S, P, and Ti decreased with increasing pressure, and the maximum decreases were 0.004 %, 0.024 %, 1.095 %, 0.028 %, 0.220 %, 0.304 %, 0.006 %, 0.003 % and 0.029 %, respectively. The decrease in Ca element was the largest, indicating that Ca-bearing minerals participate in the reaction. Calcite, kaolinite, and illite were the main minerals involved in the chemical reaction of CO2-H2O-coal. The pores (d > 100 nm) and transition pores (10 < d < 100 nm) in the sample were further developed, and the pore volume increased significantly, forming a good gas migration channel. In addition, the number of new micropores (2 < d < 10 nm) increases, the specific surface area increases significantly, and the complexity of the pores increases, forming a good reservoir.
{"title":"Evolution law of the pore structure of CO2-H2O-coal in liquid CO2-ECBM","authors":"Xiaojiao Cheng , Hu Wen , Shixing Fan , Bocong Liu , Rijun Li , Yanhui Xu , Wen Wang","doi":"10.1016/j.jcou.2024.102971","DOIUrl":"10.1016/j.jcou.2024.102971","url":null,"abstract":"<div><div>Liquid CO<sub>2</sub> enhancing coalbed methane recovery (CO<sub>2</sub>-ECBM) is an effective and intrinsically reliable gas drainage technology. Injection of liquid CO<sub>2</sub> into coal seam has the dual effect of increasing the permeability of the coal and rock and strengthening the recovery of gas, which is manifested primarily as “pressure cracking, low temperature frostbite, physical extraction and chemical corrosion, phase change pressurization, low viscosity permeability, competitive adsorption”. In this paper, the acidification and corrosion of CO<sub>2</sub>-H<sub>2</sub>O-coal was studied in physical and chemical extraction by experimental test and comparative analysis. The liquid CO<sub>2</sub> acidification reference group and the variable group experiment were designed. On the basis of the pH value of the aqueous solution, the content of major elements and minerals in coal, the minerals involved in chemical reaction, and their specific gravity were deduced. Variation in pore volume, specific surface area, and pore fractal characteristics were quantitatively and qualitatively analyzed. The experimental results show that the higher the pressure, the higher the content of carbonic acid dissolved in water and the amount of H<sup>+</sup> ionized by carbonic acid. The longer the reaction time, the greater the mineral content involved in the chemical reaction, and the H<sup>+</sup> in the water sample is consumed in large quantities. The elements of Na, K, Ca, Mg, Al, Si, S, P, and Ti decreased with increasing pressure, and the maximum decreases were 0.004 %, 0.024 %, 1.095 %, 0.028 %, 0.220 %, 0.304 %, 0.006 %, 0.003 % and 0.029 %, respectively. The decrease in Ca element was the largest, indicating that Ca-bearing minerals participate in the reaction. Calcite, kaolinite, and illite were the main minerals involved in the chemical reaction of CO<sub>2</sub>-H<sub>2</sub>O-coal. The pores (<em>d</em> > 100 nm) and transition pores (10 < <em>d</em> < 100 nm) in the sample were further developed, and the pore volume increased significantly, forming a good gas migration channel. In addition, the number of new micropores (2 < <em>d</em> < 10 nm) increases, the specific surface area increases significantly, and the complexity of the pores increases, forming a good reservoir.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"89 ","pages":"Article 102971"},"PeriodicalIF":7.2,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142553887","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}
Pub Date : 2024-11-01DOI: 10.1016/j.jcou.2024.102974
Ying-chao Wang , Ming-ming Zhai , He-xiang Huang , Zheng-hui Shi , Yuan-zhe Li , Cheng-cheng Zhao , Kang-ning Xie , Xiu-yuan Li , Yan-fei Hu , Zhi-hua Qiao , Chi Tang , Chen-xu Zhang
Carbon dioxide (CO2) capture has become a hot topic in recent years because of global warming issues. However, most research has focused primarily on gas capture, with limited methods available for achieving both CO2 capture and conversion within a single material. Here, we synthesized FMU-101, a metal-organic framework (MOF) with metal-open sites, through the self-assembly of [1,1′-Biphenyl]-3,3′,5-tricarboxylic acid and lanthanide ions in a solvothermal environment. FMU-101 features hexagonal one-dimensional pores with a diameter of 1.4 nm. The presence of free dimethylamine cations and metal open sites in the channel contributes to its remarkable capability for selectively enriching CO2 from CO2/CH4 mixtures in dynamic breakthrough experiments. Furthermore, the metal-open sites in FMU-101 play a crucial role in CO2 fixation, serving as effective catalytic sites for converting the adsorbed CO2 into high-value chloropropylene carbonate, a versatile chemical intermediate. The segregation and conversion mechanisms were further elucidated through density-functional theory (DFT) calculations and Grand Canonical Monte Carlo (GCMC) simulations, which highlighted the critical role of metal-open sites in CO2 adsorption and transformation.
{"title":"A stable dual-function lanthanum MOF: Simultaneous CO2 capture and catalysis","authors":"Ying-chao Wang , Ming-ming Zhai , He-xiang Huang , Zheng-hui Shi , Yuan-zhe Li , Cheng-cheng Zhao , Kang-ning Xie , Xiu-yuan Li , Yan-fei Hu , Zhi-hua Qiao , Chi Tang , Chen-xu Zhang","doi":"10.1016/j.jcou.2024.102974","DOIUrl":"10.1016/j.jcou.2024.102974","url":null,"abstract":"<div><div>Carbon dioxide (CO<sub>2</sub>) capture has become a hot topic in recent years because of global warming issues. However, most research has focused primarily on gas capture, with limited methods available for achieving both CO<sub>2</sub> capture and conversion within a single material. Here, we synthesized FMU-101, a metal-organic framework (MOF) with metal-open sites, through the self-assembly of [1,1′-Biphenyl]-3,3′,5-tricarboxylic acid and lanthanide ions in a solvothermal environment. FMU-101 features hexagonal one-dimensional pores with a diameter of 1.4 nm. The presence of free dimethylamine cations and metal open sites in the channel contributes to its remarkable capability for selectively enriching CO<sub>2</sub> from CO<sub>2</sub>/CH<sub>4</sub> mixtures in dynamic breakthrough experiments. Furthermore, the metal-open sites in FMU-101 play a crucial role in CO<sub>2</sub> fixation, serving as effective catalytic sites for converting the adsorbed CO<sub>2</sub> into high-value chloropropylene carbonate, a versatile chemical intermediate. The segregation and conversion mechanisms were further elucidated through density-functional theory (DFT) calculations and Grand Canonical Monte Carlo (GCMC) simulations, which highlighted the critical role of metal-open sites in CO<sub>2</sub> adsorption and transformation.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"89 ","pages":"Article 102974"},"PeriodicalIF":7.2,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142654308","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}
Pub Date : 2024-11-01DOI: 10.1016/j.jcou.2024.102969
Belén Bachiller-Baeza , João Elias F.S. Rodrigues , Maricarmen Capel-Sanchez , Javier Gainza , Victoria E. García-Sánchez , Ignacio J. Villar-García , Virginia Perez-Dieste , Carlo Marini , M. Teresa Fernández-Diaz , José A. Alonso , Consuelo Álvarez-Galván
In this work, key factors that affect catalytic activity of Ni/La-doped ceria catalysts for the reverse water gas shift reaction (RWGS) have been revealed by applying in situ advanced synchrotron techniques, such as X-ray Absorption Spectroscopy (XAS) and Near-ambient pressure X-ray Photoelectron spectroscopy (NAP-XPS). Complementary ex situ characterization techniques have been also used, adding valuable insights on different physicochemical properties of the catalysts. Lanthanum incorporates into the ceria lattice, increasing oxygen mobility, which has a role in the formation of H2O during the reaction. The optimum substitution degree of Ce by La that maximizes CO yield is close to 10 %. It is found that both bulk and surface Ce3+ proportions depend on the proportion of La, increasing with La content. At a reaction temperature of 873 K, bulk Ce3+ proportions are higher than surface ones. These differences are due to oxidative phenomena, associated to the reactive mixture that take place on the surface, such as CO2 adsorption and H2O formation. Concerning Ni phase, NiO bulk reduction to metallic Ni is very fast (in the range 573–623 K), however, Ni0 and Ni2+ species coexist on the surface during the reaction. It is found that a higher proportion of surface metallic Ni promotes the selectivity towards the RWGS, inhibiting the competing methanation reaction. On the other hand, La doping is relevant for the formation of lanthanum oxycarbonate, which has a role gasifying carbon deposits.
在这项研究中，通过应用 X 射线吸收光谱（XAS）和近常压 X 射线光电子能谱（NAP-XPS）等原位先进同步辐射技术，揭示了影响用于反向水煤气变换反应（RWGS）的掺镍/掺镭铈催化剂催化活性的关键因素。此外，还使用了补充性的原位表征技术，为催化剂的不同物理化学特性增添了宝贵的见解。镧加入到铈晶格中，增加了氧的流动性，从而在反应过程中形成 H2O。铈对镧的最佳取代度接近 10%，可使 CO 产率最大化。研究发现，体积和表面 Ce3+ 的比例都取决于 La 的比例，随着 La 含量的增加而增加。在 873 K 的反应温度下，块状 Ce3+ 的比例高于表面 Ce3+ 的比例。这些差异是由于氧化现象造成的，与表面发生的反应混合物有关，如 CO2 吸附和 H2O 形成。关于镍相，NiO 体积还原成金属镍的速度非常快（在 573-623 K 范围内），但在反应过程中，Ni0 和 Ni2+ 物种在表面共存。研究发现，表面金属镍的比例越高，对 RWGS 的选择性越大，从而抑制了竞争性的甲烷化反应。另一方面，La 掺杂与氧碳酸镧的形成有关，而氧碳酸镧具有气化碳沉积物的作用。
{"title":"In situ evolution of surface and bulk properties of Ni/La-doped CeO2 catalysts for CO2 reduction with hydrogen","authors":"Belén Bachiller-Baeza , João Elias F.S. Rodrigues , Maricarmen Capel-Sanchez , Javier Gainza , Victoria E. García-Sánchez , Ignacio J. Villar-García , Virginia Perez-Dieste , Carlo Marini , M. Teresa Fernández-Diaz , José A. Alonso , Consuelo Álvarez-Galván","doi":"10.1016/j.jcou.2024.102969","DOIUrl":"10.1016/j.jcou.2024.102969","url":null,"abstract":"<div><div>In this work, key factors that affect catalytic activity of Ni/La-doped ceria catalysts for the reverse water gas shift reaction (RWGS) have been revealed by applying in situ advanced synchrotron techniques, such as X-ray Absorption Spectroscopy (XAS) and Near-ambient pressure X-ray Photoelectron spectroscopy (NAP-XPS). Complementary ex situ characterization techniques have been also used, adding valuable insights on different physicochemical properties of the catalysts. Lanthanum incorporates into the ceria lattice, increasing oxygen mobility, which has a role in the formation of H<sub>2</sub>O during the reaction. The optimum substitution degree of Ce by La that maximizes CO yield is close to 10 %. It is found that both bulk and surface Ce<sup>3+</sup> proportions depend on the proportion of La, increasing with La content. At a reaction temperature of 873 K, bulk Ce<sup>3+</sup> proportions are higher than surface ones. These differences are due to oxidative phenomena, associated to the reactive mixture that take place on the surface, such as CO<sub>2</sub> adsorption and H<sub>2</sub>O formation. Concerning Ni phase, NiO bulk reduction to metallic Ni is very fast (in the range 573–623 K), however, Ni<sup>0</sup> and Ni<sup>2+</sup> species coexist on the surface during the reaction. It is found that a higher proportion of surface metallic Ni promotes the selectivity towards the RWGS, inhibiting the competing methanation reaction. On the other hand, La doping is relevant for the formation of lanthanum oxycarbonate, which has a role gasifying carbon deposits.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"89 ","pages":"Article 102969"},"PeriodicalIF":7.2,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142654306","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}
Pub Date : 2024-11-01DOI: 10.1016/j.jcou.2024.102966
Xin Li, Ning Gao, Fei Yuan, Lucheng Huang
In the context of carbon neutrality, carbon-negative technology is considered a crucial technology for reducing carbon emissions and achieving carbon neutrality. Carbon-negative technology has gained attention from governments, businesses and academia. To comprehend the overall development status of carbon-negative technology, including the core technologies, the patent landscape, competition, and cooperation among major countries and regions, this paper proposes an analytical framework for the patent landscape of carbon-negative technology. The research results demonstrate the rapid overall development of carbon-negative technology. The R&D strategies of major competing countries in the field of carbon-negative technology focus on specific technology areas, and their core technologies exhibit similarities as well as differences. In the field of technology-based solutions, the United States and China dominate with their leaders and active contributors in various technology domains. The collaboration largely revolves around the United States, while other nations engage in less partnership and interaction. Countries have not yet established technological leadership in carbon sinks technology, and the cooperation network is relatively limited. These findings contribute to our understanding of the current global development status of carbon-negative technology, as well as the competitive levels and positions of major countries in this field. These findings also provide a decision-making basis and support for the development of carbon-negative technology.
{"title":"The development trends, technological competition situations and cooperation status of carbon-negative technology: A patent landscape analysis","authors":"Xin Li, Ning Gao, Fei Yuan, Lucheng Huang","doi":"10.1016/j.jcou.2024.102966","DOIUrl":"10.1016/j.jcou.2024.102966","url":null,"abstract":"<div><div>In the context of carbon neutrality, carbon-negative technology is considered a crucial technology for reducing carbon emissions and achieving carbon neutrality. Carbon-negative technology has gained attention from governments, businesses and academia. To comprehend the overall development status of carbon-negative technology, including the core technologies, the patent landscape, competition, and cooperation among major countries and regions, this paper proposes an analytical framework for the patent landscape of carbon-negative technology. The research results demonstrate the rapid overall development of carbon-negative technology. The R&D strategies of major competing countries in the field of carbon-negative technology focus on specific technology areas, and their core technologies exhibit similarities as well as differences. In the field of technology-based solutions, the United States and China dominate with their leaders and active contributors in various technology domains. The collaboration largely revolves around the United States, while other nations engage in less partnership and interaction. Countries have not yet established technological leadership in carbon sinks technology, and the cooperation network is relatively limited. These findings contribute to our understanding of the current global development status of carbon-negative technology, as well as the competitive levels and positions of major countries in this field. These findings also provide a decision-making basis and support for the development of carbon-negative technology.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"89 ","pages":"Article 102966"},"PeriodicalIF":7.2,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142654304","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}
Aqueous carbonation of end-of-life concrete fines is a promising method to alleviate greenhouse gas emissions by CO2 sequestration from point-source emitters. This produces a valuable material that can be utilized in new cement formulations. This study investigates effects of the composition of cement pastes and of the carbonation conditions on the reactivity and phase assemblage for aqueous carbonated Portland cement pastes incorporating silica fume, fly ash, and blast furnace slag. Results from 27Al and 29Si NMR show that hydration of the carbonated pastes under reactivity test conditions lead to phase assemblages dominated by a C-(A)-S-H phase, with reduced Al/Si ratio, as well as by ettringite and hemi/monocarbonate AFm phases. The results from the reactivity tests demonstrate that the carbonated blended cement pastes exhibit superior reactivity compared to carbonated neat Portland cement paste because of their increased fraction of reactive alumina and silica species. The variations in carbonation conditions (i.e., temperature, CO2 gas concentration, and solution composition) do not alter significantly the reactivity of the carbonated pastes. These findings demonstrate the robustness of aqueous carbonation of concrete fines and support its wider application as a mean to reduce CO2 emissions and enhance circularity of cement-based materials.
{"title":"Reactivity of aqueous carbonated cement pastes: Effect of chemical composition and carbonation conditions","authors":"Fábio Maia Neto , Ruben Snellings , Jørgen Skibsted","doi":"10.1016/j.jcou.2024.102970","DOIUrl":"10.1016/j.jcou.2024.102970","url":null,"abstract":"<div><div>Aqueous carbonation of end-of-life concrete fines is a promising method to alleviate greenhouse gas emissions by CO<sub>2</sub> sequestration from point-source emitters. This produces a valuable material that can be utilized in new cement formulations. This study investigates effects of the composition of cement pastes and of the carbonation conditions on the reactivity and phase assemblage for aqueous carbonated Portland cement pastes incorporating silica fume, fly ash, and blast furnace slag. Results from <sup>27</sup>Al and <sup>29</sup>Si NMR show that hydration of the carbonated pastes under reactivity test conditions lead to phase assemblages dominated by a C-(A)-S-H phase, with reduced Al/Si ratio, as well as by ettringite and hemi/monocarbonate AFm phases. The results from the reactivity tests demonstrate that the carbonated blended cement pastes exhibit superior reactivity compared to carbonated neat Portland cement paste because of their increased fraction of reactive alumina and silica species. The variations in carbonation conditions (<em>i.e</em>., temperature, CO<sub>2</sub> gas concentration, and solution composition) do not alter significantly the reactivity of the carbonated pastes. These findings demonstrate the robustness of aqueous carbonation of concrete fines and support its wider application as a mean to reduce CO<sub>2</sub> emissions and enhance circularity of cement-based materials.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"89 ","pages":"Article 102970"},"PeriodicalIF":7.2,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142577950","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}
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