Pub Date : 2024-12-13DOI: 10.1016/j.gce.2024.12.001
Zhenyu Zhao , Jiayi Bai , Han Tao , Shenyao Wang , Kaili Wang , Wenjun Lin , Lili Jiang , Haoran Li , Congmin Wang
Due to the strong hydrophobicity of PET, chemical catalysts usually require harsh conditions. Herein, inspired by the catalytic sites of PETase, we reported a metal-free catalyst with both high stability and activity, which could achieve almost complete hydrolysis of PET (≥ 99%) under relatively mild conditions (100 °C, PH ≈ 8). Mechanistic investigations showed that hydrogen bonds played an important role. With the increase of hydrogen bond multiplicity and strength, the reaction barrier decreased gradually. We believe that this work might provide a direction for the development of efficient metal-free catalysts and have great industrial application prospects.
{"title":"Ionic liquids with multiple hydrogen bonds as metal-free catalysts for efficient hydrolysis of PET under relatively mild conditions","authors":"Zhenyu Zhao , Jiayi Bai , Han Tao , Shenyao Wang , Kaili Wang , Wenjun Lin , Lili Jiang , Haoran Li , Congmin Wang","doi":"10.1016/j.gce.2024.12.001","DOIUrl":"10.1016/j.gce.2024.12.001","url":null,"abstract":"<div><div>Due to the strong hydrophobicity of PET, chemical catalysts usually require harsh conditions. Herein, inspired by the catalytic sites of PETase, we reported a metal-free catalyst with both high stability and activity, which could achieve almost complete hydrolysis of PET (≥ 99%) under relatively mild conditions (100 °C, PH ≈ 8). Mechanistic investigations showed that hydrogen bonds played an important role. With the increase of hydrogen bond multiplicity and strength, the reaction barrier decreased gradually. We believe that this work might provide a direction for the development of efficient metal-free catalysts and have great industrial application prospects.</div></div>","PeriodicalId":66474,"journal":{"name":"Green Chemical Engineering","volume":"7 2","pages":"Pages 219-224"},"PeriodicalIF":7.6,"publicationDate":"2024-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145814417","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Valorization of nitrous oxide (N2O), a potent greenhouse gas, through the oxidative dehydrogenation of light alkanes such as methane and propane to produce light olefins (ethylene and propylene), presents a promising technique for both environmental mitigation and valuable chemical production. This review provides a systematic analysis of the differences between N2O and O2 as oxidants, emphasizing the distinctive advantages of N2O as a mild oxidant for olefin production. It delves into key technologies, such as oxidative dehydrogenation of propane (ODHP) to propylene and oxidative coupling of methane (OCM) to ethylene, focusing on the underlying reaction mechanisms and recent advancements in catalyst development. A major challenge in these reactions is the trade-off between activity and selectivity. To address this, we propose an innovative strategy–redox center separation–to enhance catalytic performance. This comprehensive review offers valuable insights for the rational design of catalysts, advancing sustainable chemical engineering processes that utilize N2O, while addressing critical environmental and industrial challenges.
{"title":"Advances and challenges in N2O valorization for alkane oxidative dehydrogenation to olefins","authors":"Yunshuo Wu , Xuanhao Wu , Haiqiang Wang , Zhongbiao Wu","doi":"10.1016/j.gce.2024.11.005","DOIUrl":"10.1016/j.gce.2024.11.005","url":null,"abstract":"<div><div>Valorization of nitrous oxide (N<sub>2</sub>O), a potent greenhouse gas, through the oxidative dehydrogenation of light alkanes such as methane and propane to produce light olefins (ethylene and propylene), presents a promising technique for both environmental mitigation and valuable chemical production. This review provides a systematic analysis of the differences between N<sub>2</sub>O and O<sub>2</sub> as oxidants, emphasizing the distinctive advantages of N<sub>2</sub>O as a mild oxidant for olefin production. It delves into key technologies, such as oxidative dehydrogenation of propane (ODHP) to propylene and oxidative coupling of methane (OCM) to ethylene, focusing on the underlying reaction mechanisms and recent advancements in catalyst development. A major challenge in these reactions is the trade-off between activity and selectivity. To address this, we propose an innovative strategy–redox center separation–to enhance catalytic performance. This comprehensive review offers valuable insights for the rational design of catalysts, advancing sustainable chemical engineering processes that utilize N<sub>2</sub>O, while addressing critical environmental and industrial challenges.</div></div>","PeriodicalId":66474,"journal":{"name":"Green Chemical Engineering","volume":"7 2","pages":"Pages 137-146"},"PeriodicalIF":7.6,"publicationDate":"2024-11-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145814409","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-21DOI: 10.1016/S2666-9528(24)00070-0
{"title":"OFC: Outside Front Cover","authors":"","doi":"10.1016/S2666-9528(24)00070-0","DOIUrl":"10.1016/S2666-9528(24)00070-0","url":null,"abstract":"","PeriodicalId":66474,"journal":{"name":"Green Chemical Engineering","volume":"6 1","pages":"Page OFC"},"PeriodicalIF":9.1,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142704748","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 : 2024-11-21DOI: 10.1016/S2666-9528(24)00079-7
{"title":"Outside Back Cover","authors":"","doi":"10.1016/S2666-9528(24)00079-7","DOIUrl":"10.1016/S2666-9528(24)00079-7","url":null,"abstract":"","PeriodicalId":66474,"journal":{"name":"Green Chemical Engineering","volume":"6 1","pages":"Page OBC"},"PeriodicalIF":9.1,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142704747","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 : 2024-11-17DOI: 10.1016/j.gce.2024.11.003
Mood Mohan , Nikhitha Gugulothu , Sreelekha Guggilam , T. Rajitha Rajeshwar , Michelle K. Kidder , Jeremy C. Smith
The polarity of solvents plays a critical role in various research applications, particularly in their solubilities. Polarity is conveniently characterized by the Kamlet-Taft parameters that is, the hydrogen bonding acidity (α), the basicity (β), and the polarizability (π∗). Obtaining Kamlet-Taft parameters is very important for designer solvents, namely ionic liquids (ILs) and deep eutectic solvents (DESs). However, given the unlimited theoretical number of combinations of ionic pairs in ILs and hydrogen-bond donor/acceptor pairs in DESs, experimental determination of their Kamlet-Taft parameters is impractical. To address this, the present study developed two different machine learning (ML) algorithms to predict Kamlet-Taft parameters for designer solvents using quantum chemically derived input features. The ML models developed in the present study showed accurate predictions with high determination coefficient (R2) and low root mean square error (RMSE) values. Further, in the context of present interest in the circular bioeconomy, the relationship between the basicities and acidities of designer solvents and their ability to dissolve lignin and carbon dioxide (CO2) is discussed. Our method thus guides the design of effective solvents with optimal Kamlet-Taft parameter values dissolving and converting biomass and CO2 into valuable chemicals.
{"title":"Physics-informed machine learning to predict solvatochromic parameters of designer solvents with case studies in CO2 and lignin dissolution","authors":"Mood Mohan , Nikhitha Gugulothu , Sreelekha Guggilam , T. Rajitha Rajeshwar , Michelle K. Kidder , Jeremy C. Smith","doi":"10.1016/j.gce.2024.11.003","DOIUrl":"10.1016/j.gce.2024.11.003","url":null,"abstract":"<div><div>The polarity of solvents plays a critical role in various research applications, particularly in their solubilities. Polarity is conveniently characterized by the Kamlet-Taft parameters that is, the hydrogen bonding acidity (<em>α</em>), the basicity (<em>β</em>), and the polarizability (<em>π∗</em>). Obtaining Kamlet-Taft parameters is very important for designer solvents, namely ionic liquids (ILs) and deep eutectic solvents (DESs). However, given the unlimited theoretical number of combinations of ionic pairs in ILs and hydrogen-bond donor/acceptor pairs in DESs, experimental determination of their Kamlet-Taft parameters is impractical. To address this, the present study developed two different machine learning (ML) algorithms to predict Kamlet-Taft parameters for designer solvents using quantum chemically derived input features. The ML models developed in the present study showed accurate predictions with high determination coefficient (R<sup>2</sup>) and low root mean square error (RMSE) values. Further, in the context of present interest in the circular bioeconomy, the relationship between the basicities and acidities of designer solvents and their ability to dissolve lignin and carbon dioxide (CO<sub>2</sub>) is discussed. Our method thus guides the design of effective solvents with optimal Kamlet-Taft parameter values dissolving and converting biomass and CO<sub>2</sub> into valuable chemicals.</div></div>","PeriodicalId":66474,"journal":{"name":"Green Chemical Engineering","volume":"6 2","pages":"Pages 275-287"},"PeriodicalIF":9.1,"publicationDate":"2024-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143594166","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 : 2024-11-06DOI: 10.1016/j.gce.2024.11.002
Ruichen Liu, Miao Wang, Jiaxin Zheng, Xinli Tong
The heterogeneous photocatalysis for the oxidative cleavage of C–C bond is significant to the transformation of biomass feedstock. In this work, a heterojunction photocatalyst based on the conductor ZnS and C3N4 (CN) material is prepared and employed in the aerobic oxidative cleavage reaction of vicinal diol under visible light irradiation. As a result, it is found that 3ZnS/CN catalyst obtained by a mechanical grinding method shows a high photocatalytic activity. In the photocatalytic oxidative cleavage process of 1-phenyl-1,2-glycol, more than 98.7% conversion of substrate with a 96.2% selectivity of benzaldehyde was attained using O2 as oxidant. In addition, the photocatalyst recycling experiments exhibited that the 3ZnS/CN catalyst still kept a good activity and stability even after being recycled for 5 times. Finally, the active reaction intermediates were investigated by the control experiments and the relative electron paramagnetic resonance (EPR) detection. According to the obtained results and photocatalytic principle, the mechanism for the selective oxidative transformatioin of 1-phenyl-1,2-glycol has been proposed. It gives a promising approach for the catalytic utilization of biomass-based lignin and cellulose.
{"title":"Visible light-driven selective oxidative transformation of vicinal diols using ZnS-based photocatalyst in the presence of molecular oxygen","authors":"Ruichen Liu, Miao Wang, Jiaxin Zheng, Xinli Tong","doi":"10.1016/j.gce.2024.11.002","DOIUrl":"10.1016/j.gce.2024.11.002","url":null,"abstract":"<div><div>The heterogeneous photocatalysis for the oxidative cleavage of C–C bond is significant to the transformation of biomass feedstock. In this work, a heterojunction photocatalyst based on the conductor ZnS and C<sub>3</sub>N<sub>4</sub> (CN) material is prepared and employed in the aerobic oxidative cleavage reaction of vicinal diol under visible light irradiation. As a result, it is found that 3ZnS/CN catalyst obtained by a mechanical grinding method shows a high photocatalytic activity. In the photocatalytic oxidative cleavage process of 1-phenyl-1,2-glycol, more than 98.7% conversion of substrate with a 96.2% selectivity of benzaldehyde was attained using O<sub>2</sub> as oxidant. In addition, the photocatalyst recycling experiments exhibited that the 3ZnS/CN catalyst still kept a good activity and stability even after being recycled for 5 times. Finally, the active reaction intermediates were investigated by the control experiments and the relative electron paramagnetic resonance (EPR) detection. According to the obtained results and photocatalytic principle, the mechanism for the selective oxidative transformatioin of 1-phenyl-1,2-glycol has been proposed. It gives a promising approach for the catalytic utilization of biomass-based lignin and cellulose.</div></div>","PeriodicalId":66474,"journal":{"name":"Green Chemical Engineering","volume":"7 2","pages":"Pages 209-218"},"PeriodicalIF":7.6,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145814415","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Alcohol industry residues (AIRs) are protein-rich lignocellulosic biowastes from a major industry, having the dual traits of renewable biomass and organic waste. They mainly consist of Brewer's spent grains (BSG) and Baijiu distiller's grains (BDG), with annual production totaling tens of millions of tons. Recycling these residues effectively is crucial for the environment, society, and industry. Given their unique characteristic of concentrated carbon and nitrogen sources, valorizing AIRs into biocarbon products through thermochemistry is the most sustainable method for waste management, resource recycling, and green ecology. In this review, the preparation and properties of AIRs-derived biocarbon products are systematically discussed. Recent advancements in the green thermochemical valorization of AIRs into biocarbon products for various applications like thermal utilization, environmental remediation, and energy storage are comprehensively reviewed. It is suggested that hydrothermal carbonization, coupled with necessary chemical functionalization (e.g., using metal oxides and oxysalts), would be a preferable strategy for producing desired functionalized biocarbon for use as carbon adsorbents (for wastewater treatment) and carbon fertilizers (for soil conservation). The yield and quality of functionalized biocarbon can be ensured through the directional regulation of the migration of essential elements like carbon and nitrogen. The co-generation of nitrogen-doped biochar and nitrogen-enriched liquid fertilizer using innovative hydrothermal strategies is identified as a potential research avenue to achieve the full and cascading utilization of AIRs. This review aims to provide an overview and insights into thermochemically valorizing AIRs alongside other light industrial residues for relevant researchers.
{"title":"Thermochemical valorization of alcohol industry residues into biocarbon for energy and environmental applications: a review","authors":"Hao Zhan , Tianle Xu , Hao Jiang , Mingjie Chen , Zonghao Lai , Wenjian Zhao , Lijian Leng , Zhiyong Zeng , Xinming Wang","doi":"10.1016/j.gce.2024.11.001","DOIUrl":"10.1016/j.gce.2024.11.001","url":null,"abstract":"<div><div>Alcohol industry residues (AIRs) are protein-rich lignocellulosic biowastes from a major industry, having the dual traits of renewable biomass and organic waste. They mainly consist of Brewer's spent grains (BSG) and Baijiu distiller's grains (BDG), with annual production totaling tens of millions of tons. Recycling these residues effectively is crucial for the environment, society, and industry. Given their unique characteristic of concentrated carbon and nitrogen sources, valorizing AIRs into biocarbon products through thermochemistry is the most sustainable method for waste management, resource recycling, and green ecology. In this review, the preparation and properties of AIRs-derived biocarbon products are systematically discussed. Recent advancements in the green thermochemical valorization of AIRs into biocarbon products for various applications like thermal utilization, environmental remediation, and energy storage are comprehensively reviewed. It is suggested that hydrothermal carbonization, coupled with necessary chemical functionalization (<em>e.g.</em>, using metal oxides and oxysalts), would be a preferable strategy for producing desired functionalized biocarbon for use as carbon adsorbents (for wastewater treatment) and carbon fertilizers (for soil conservation). The yield and quality of functionalized biocarbon can be ensured through the directional regulation of the migration of essential elements like carbon and nitrogen. The co-generation of nitrogen-doped biochar and nitrogen-enriched liquid fertilizer using innovative hydrothermal strategies is identified as a potential research avenue to achieve the full and cascading utilization of AIRs. This review aims to provide an overview and insights into thermochemically valorizing AIRs alongside other light industrial residues for relevant researchers.</div></div>","PeriodicalId":66474,"journal":{"name":"Green Chemical Engineering","volume":"6 4","pages":"Pages 456-472"},"PeriodicalIF":7.6,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144917211","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-01DOI: 10.1016/j.gce.2024.10.008
Long Chen , Zhanjun Zhang , Songtao Xiao , Xinyan Li , Shangjie Zhao , Yaolin Zhao , Chenxi Yu , Zhaoning Feng , Ke Ma , Xiaojuan Liu , Xiaofan Ding , Jing Zhao , Jinping Liu
Since the continuous development of nuclear energy, substantial amounts of radioactive thorium wastewater are inevitably produced. The discharge of radioactive thorium wastewater not only pollutes the natural environment but also endangers human health. Due to its affordability, simplicity, and high effectiveness, the adsorption method has emerged as the most often used method for treatment. Covalent organic framework (COF) materials are excellent adsorbents with various characteristics, including superior chemical stability, design flexibility, and various architectures, and thus are widely used in separating radioactive nuclides. Herein, we synthesized two structurally similar COFs that vary in their pore dimensions and the connectivity of their modules. After incorporating hydroxyl groups into the structure of Tb-TMT formed by benzene-1,3,5-tricarbaldehyde (Tb) and 2,4,6-trimethyl-1,3,5-triazine (TMT), the uptake capacity of thorium ions is significantly enhanced. The differences in solution pH, contact time, initial concentration, and competitive ion experiments between the materials before and after hydroxyl functionalization were studied. Additionally, the research assessed their reuse capabilities. In this research, the Hb-TMT exhibits an outstanding adsorption capacity for Th(IV) ions, with a remarkable adsorptive capacity reaching 543.5 mg g−1, and it showes good uptake efficiency within 5 min with excellent selectivity (Kd = 1.2 × 104). After three cycles of regeneration, Hb-TMT still maintains a high level of adsorption capacity for Th(IV) (> 80%) and has good reusability. Furthermore, the role of nitrogen-oxygen synergistic effect on hydroxyl-functionalized COF is highlighted by density functional theory (DFT) calculations. This study provides fresh insights for choosing functional groups in functionalized COFs, specifically for radionuclide adsorption.
{"title":"Efficient capture of thorium ions by the hydroxyl-functionalized sp2c-COF through nitrogen-oxygen cooperative mechanism","authors":"Long Chen , Zhanjun Zhang , Songtao Xiao , Xinyan Li , Shangjie Zhao , Yaolin Zhao , Chenxi Yu , Zhaoning Feng , Ke Ma , Xiaojuan Liu , Xiaofan Ding , Jing Zhao , Jinping Liu","doi":"10.1016/j.gce.2024.10.008","DOIUrl":"10.1016/j.gce.2024.10.008","url":null,"abstract":"<div><div>Since the continuous development of nuclear energy, substantial amounts of radioactive thorium wastewater are inevitably produced. The discharge of radioactive thorium wastewater not only pollutes the natural environment but also endangers human health. Due to its affordability, simplicity, and high effectiveness, the adsorption method has emerged as the most often used method for treatment. Covalent organic framework (COF) materials are excellent adsorbents with various characteristics, including superior chemical stability, design flexibility, and various architectures, and thus are widely used in separating radioactive nuclides. Herein, we synthesized two structurally similar COFs that vary in their pore dimensions and the connectivity of their modules. After incorporating hydroxyl groups into the structure of Tb-TMT formed by benzene-1,3,5-tricarbaldehyde (Tb) and 2,4,6-trimethyl-1,3,5-triazine (TMT), the uptake capacity of thorium ions is significantly enhanced. The differences in solution pH, contact time, initial concentration, and competitive ion experiments between the materials before and after hydroxyl functionalization were studied. Additionally, the research assessed their reuse capabilities. In this research, the Hb-TMT exhibits an outstanding adsorption capacity for Th(IV) ions, with a remarkable adsorptive capacity reaching 543.5 mg g<sup>−1</sup>, and it showes good uptake efficiency within 5 min with excellent selectivity (<em>K</em><sub>d</sub> = 1.2 × 10<sup>4</sup>). After three cycles of regeneration, Hb-TMT still maintains a high level of adsorption capacity for Th(IV) (> 80%) and has good reusability. Furthermore, the role of nitrogen-oxygen synergistic effect on hydroxyl-functionalized COF is highlighted by density functional theory (DFT) calculations. This study provides fresh insights for choosing functional groups in functionalized COFs, specifically for radionuclide adsorption.</div></div>","PeriodicalId":66474,"journal":{"name":"Green Chemical Engineering","volume":"7 2","pages":"Pages 191-199"},"PeriodicalIF":7.6,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145814413","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-01DOI: 10.1016/j.gce.2024.10.007
Jinhui Liu , Xiaolong Sun , Fei Teng , Qibin Xia , Zhong Li , Ying Wu , Xin Zhou
Efficient recovery of ethane (C2H6) from natural gas is of industrial importance, yet it poses considerable challenges. Herein, we report the two-step green preparation of asphalt-based carbon adsorbent Asphalt-based Carbon adsorbents (AsCs) with exceptional C2H6/CH4 selectivity and high capacity, where the KOH usage can be significantly reduced by 75% than conventional chemical activation processes. More importantly, the resulting AsC-0.75-900 exhibits exceptional C2H6/CH4 separation performance with the ideal adsorbed solution theory (IAST) selectivity of 30.74 and C2H6 capacity of 4.53 mmol/g at 298 K and 100 kPa. Notably, even at the low pressure of 10 kPa, its C2H6 uptake remains high at 2.25 mmol/g, comparable to many advanced metal-organic frameworks (MOFs). Molecular simulation was used to elucidate the adsorption mechanism. Fixed-bed experiments further demonstrate dynamic separation performance, achieving complete separation of a C2H6/CH4 binary mixture (10:90, v/v) at ambient condition. In addition to superior separation performance, AsC-0.75-900 offers inherent structural stability and cost-effectiveness, positioning it a highly promising candidate for C2H6 recovery from natural gas.
{"title":"Two-step preparation of asphalt-based porous carbon adsorbent with superior C2H6/CH4 selectivity for ethane recovery from natural gas","authors":"Jinhui Liu , Xiaolong Sun , Fei Teng , Qibin Xia , Zhong Li , Ying Wu , Xin Zhou","doi":"10.1016/j.gce.2024.10.007","DOIUrl":"10.1016/j.gce.2024.10.007","url":null,"abstract":"<div><div>Efficient recovery of ethane (C<sub>2</sub>H<sub>6</sub>) from natural gas is of industrial importance, yet it poses considerable challenges. Herein, we report the two-step green preparation of asphalt-based carbon adsorbent Asphalt-based Carbon adsorbents (AsCs) with exceptional C<sub>2</sub>H<sub>6</sub>/CH<sub>4</sub> selectivity and high capacity, where the KOH usage can be significantly reduced by 75% than conventional chemical activation processes. More importantly, the resulting AsC-0.75-900 exhibits exceptional C<sub>2</sub>H<sub>6</sub>/CH<sub>4</sub> separation performance with the ideal adsorbed solution theory (IAST) selectivity of 30.74 and C<sub>2</sub>H<sub>6</sub> capacity of 4.53 mmol/g at 298 K and 100 kPa. Notably, even at the low pressure of 10 kPa, its C<sub>2</sub>H<sub>6</sub> uptake remains high at 2.25 mmol/g, comparable to many advanced metal-organic frameworks (MOFs). Molecular simulation was used to elucidate the adsorption mechanism. Fixed-bed experiments further demonstrate dynamic separation performance, achieving complete separation of a C<sub>2</sub>H<sub>6</sub>/CH<sub>4</sub> binary mixture (10:90, v/v) at ambient condition. In addition to superior separation performance, AsC-0.75-900 offers inherent structural stability and cost-effectiveness, positioning it a highly promising candidate for C<sub>2</sub>H<sub>6</sub> recovery from natural gas.</div></div>","PeriodicalId":66474,"journal":{"name":"Green Chemical Engineering","volume":"7 2","pages":"Pages 200-208"},"PeriodicalIF":7.6,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145814414","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-28DOI: 10.1016/j.gce.2024.10.006
Qun Huang, Zhibing Zhang
Microcapsules containing various flavour/fragrance oils with different properties were fabricated using gelatine and gum arabic by complex coacervation. The surface properties (surface polarity and the spreading coefficients) of core oils were investigated in order to evaluate their effects on the capsule morphology and encapsulation efficiency based on a spreading coefficient and two component surface energy theory. Contact angles, interfacial tensions, and surface polarities were measured, and results were discussed with respect to the internal structure as well as encapsulation efficiency of different oil microcapsules. The thermodynamic spreading coefficients theory did not give an exactly accurate prediction of capsule morphology using high molecular weight biopolymer as the wall material in this work. Notwithstanding, the morphology predictions for different oil microcapsules are holistically consistent with the values of their encapsulation efficiency. Also, it has been found that the encapsulation efficiency increased with the decreasing surface polarity of the core oil holistically.
{"title":"Evaluation of gum arabic and gelatine coacervated microcapsule morphology and core oil encapsulation efficiency by combining the spreading coefficient and two component surface energy theory","authors":"Qun Huang, Zhibing Zhang","doi":"10.1016/j.gce.2024.10.006","DOIUrl":"10.1016/j.gce.2024.10.006","url":null,"abstract":"<div><div>Microcapsules containing various flavour/fragrance oils with different properties were fabricated using gelatine and gum arabic by complex coacervation. The surface properties (surface polarity and the spreading coefficients) of core oils were investigated in order to evaluate their effects on the capsule morphology and encapsulation efficiency based on a spreading coefficient and two component surface energy theory. Contact angles, interfacial tensions, and surface polarities were measured, and results were discussed with respect to the internal structure as well as encapsulation efficiency of different oil microcapsules. The thermodynamic spreading coefficients theory did not give an exactly accurate prediction of capsule morphology using high molecular weight biopolymer as the wall material in this work. Notwithstanding, the morphology predictions for different oil microcapsules are holistically consistent with the values of their encapsulation efficiency. Also, it has been found that the encapsulation efficiency increased with the decreasing surface polarity of the core oil holistically.</div></div>","PeriodicalId":66474,"journal":{"name":"Green Chemical Engineering","volume":"6 3","pages":"Pages 420-429"},"PeriodicalIF":9.1,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144116664","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}