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}
Pub Date : 2024-10-24DOI: 10.1016/j.gce.2024.10.005
Yiru Zou , Chao Wang , Haiyan Ji , Peiwen Wu , Yanhong Chao , Xiaoxiao Yu , Zhendong Yu , Haiyan Liu , Zhichang Liu , Wenshuai Zhu
Since the advantages of simple preparation, low-priced, environmental friendliness, and high absorption capacity, deep eutectic solvents (DESs) are considered to have eminent application potential in terms of SO2 absorption. However, the absorption rate, selectivity, and reversibility of DESs urgently need to be further improved to meet the requirements of industrialization. In this work, five purine-based DESs were designed and synthesized through the use of 1-ethyl-3-methylimidazolium chloride (EmimCl) as hydrogen bond acceptors (HBAs) plus 6-aminopurine (6-AmP), 6-hydroxypurine (6-HoP), and 6-chloropurine (6-ChP) as hydrogen bond donors (HBDs), respectively. The results indicated that the optimal molar ratio of HBAs to HBDs is 7:1, and the absorption capacity of EmimCl + 6-AmP-7 can reach up to 18.118 mol/kg, at 298.15 K and 1.0 bar. Notably, the present purine-based DESs not only achieve gas-liquid equilibrium within 40 s, but also exhibit outstanding reversibility (absorb-desorb more than 30 times) and remarkable selectivity of SO2/CO2. Furthermore, a reaction equilibrium thermodynamic model (RETM) equation was employed to investigate the absorption behavior by combining the absorption data under different SO2 partial pressures and temperatures. Finally, Fourier-transform infrared (FT-IR) spectroscopy and 1H nuclear magnetic resonance (NMR) were conducted to explore further the formation and SO2 absorption mechanism of purine-based DESs. It is revealed that the former is mainly hydrogen bonding interaction among HBAs and HBDs, and the latter is mainly Lewis acid-base interaction plus strong charge-transfer interaction among DESs and SO2. Based on the obtained data, it could be confirmed that the SO2 absorption includes both physical and chemical absorption.
{"title":"Rapid, selectivity, and reversibility absorption of SO2 via purine-based deep eutectic solvents and thermodynamic analysis","authors":"Yiru Zou , Chao Wang , Haiyan Ji , Peiwen Wu , Yanhong Chao , Xiaoxiao Yu , Zhendong Yu , Haiyan Liu , Zhichang Liu , Wenshuai Zhu","doi":"10.1016/j.gce.2024.10.005","DOIUrl":"10.1016/j.gce.2024.10.005","url":null,"abstract":"<div><div>Since the advantages of simple preparation, low-priced, environmental friendliness, and high absorption capacity, deep eutectic solvents (DESs) are considered to have eminent application potential in terms of SO<sub>2</sub> absorption. However, the absorption rate, selectivity, and reversibility of DESs urgently need to be further improved to meet the requirements of industrialization. In this work, five purine-based DESs were designed and synthesized through the use of 1-ethyl-3-methylimidazolium chloride (EmimCl) as hydrogen bond acceptors (HBAs) plus 6-aminopurine (6-AmP), 6-hydroxypurine (6-HoP), and 6-chloropurine (6-ChP) as hydrogen bond donors (HBDs), respectively. The results indicated that the optimal molar ratio of HBAs to HBDs is 7:1, and the absorption capacity of EmimCl + 6-AmP-7 can reach up to 18.118 mol/kg, at 298.15 K and 1.0 bar. Notably, the present purine-based DESs not only achieve gas-liquid equilibrium within 40 s, but also exhibit outstanding reversibility (absorb-desorb more than 30 times) and remarkable selectivity of SO<sub>2</sub>/CO<sub>2</sub>. Furthermore, a reaction equilibrium thermodynamic model (RETM) equation was employed to investigate the absorption behavior by combining the absorption data under different SO<sub>2</sub> partial pressures and temperatures. Finally, Fourier-transform infrared (FT-IR) spectroscopy and <sup>1</sup>H nuclear magnetic resonance (NMR) were conducted to explore further the formation and SO<sub>2</sub> absorption mechanism of purine-based DESs. It is revealed that the former is mainly hydrogen bonding interaction among HBAs and HBDs, and the latter is mainly Lewis acid-base interaction plus strong charge-transfer interaction among DESs and SO<sub>2</sub>. Based on the obtained data, it could be confirmed that the SO<sub>2</sub> absorption includes both physical and chemical absorption.</div></div>","PeriodicalId":66474,"journal":{"name":"Green Chemical Engineering","volume":"7 2","pages":"Pages 180-190"},"PeriodicalIF":7.6,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145814412","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 : 2024-10-18DOI: 10.1016/j.gce.2024.10.004
Ruilong Zhang , Jun Zhao , Qiangqiang Jia , Jian Ye , Xiaohua Tian , Lulu Wang , Ifunanya R. Akaniro , Prince N. Amaniampong , Jianming Pan , Jiangdong Dai
The rapid expansion of the chemical and pharmaceutical industries has resulted in the introduction of various sources of micropollutants into the environment, posing threats to drinking water quality and public health. Membrane separation technology offers a promising solution with low energy use, high-quality effluent, and operational simplicity. Here, we developed fluffy layered double hydroxides (LDH)/graphene oxide (GO) 2D membranes, specifically tannic acid-mediated LDH-GO/GO-TA composite membranes (LG/GT). The integration of GO nanosheets regulated the growth of LDH, enhancing electron transfer and adsorption-driven catalytic performance. This design enabled LDH-GO to activate peroxymonosulfate (PMS) and completely degraded Rhodamine B (RhB) within 10 min. The Gaussian calculation was combined with this finding, which could explain the catalytic self-cleaning in the separation process. The TA-mediated enhancement further increased the RhB rejection of LG/GT-7.5 to 99.23%. Additionally, the needle/sheet structure significantly improved permeance to 358.28 L m−2 h−1 bar−1, surpassing the L/GT-7.5 performance (e.g. 338.53 L m−2 h−1 bar−1), indicating superior pore formation and water mass transfer. The heterostructure between GO and LDH greatly improved cycling stability, with the membrane maintaining a permeance of 282.71 L m−2 h−1 bar−1 and a rejection of 97.97% despite 20 cycles. This work demonstrated the potential of fluffy layered LDH 2D membranes for enhanced wastewater treatment applications. These findings suggested significant potential for practical implementation in industrial wastewater treatment processes, offering a sustainable and efficient solution to water pollution challenges.
化学和制药工业的迅速扩张导致各种微污染物进入环境，对饮用水质量和公众健康构成威胁。膜分离技术具有低能耗、高质量出水、操作简单等优点。在这里，我们开发了蓬松的层状双氢氧化物(LDH)/氧化石墨烯（GO） 2D膜，特别是单宁酸介导的LDH-GO/GO- ta复合膜（LG/GT）。氧化石墨烯纳米片的集成调节了LDH的生长，增强了电子转移和吸附驱动的催化性能。该设计使LDH-GO能够在10分钟内激活过氧单硫酸盐（PMS）并完全降解罗丹明B （RhB）。将高斯计算与这一发现相结合，可以解释分离过程中的催化自清洁现象。ta介导的增强进一步使LG/GT-7.5的RhB排斥反应增加到99.23%。此外，针/片结构显著提高了渗透率，达到358.28 L m−2 h−1 bar−1，超过了L/GT-7.5的性能（例如338.53 L m−2 h−1 bar−1），表明优越的孔隙形成和水质量传递。氧化石墨烯和LDH之间的异质结构极大地提高了循环稳定性，在循环20次后，膜的渗透率保持在282.71 L m−2 h−1 bar−1，截留率为97.97%。这项工作证明了蓬松层状LDH 2D膜在增强废水处理应用方面的潜力。这些发现表明了在工业废水处理过程中实际应用的巨大潜力，为水污染挑战提供了可持续和高效的解决方案。
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