Pub Date : 2024-04-02DOI: 10.3390/separations11040110
Katsuhiro Horata, Tsubasa Yoshio, Ryuto Miyazaki, Yohei Adachi, M. Kanezashi, T. Tsuru, J. Ohshita
New polysilsesquioxane (PSQ)-based CO2 separation membranes with succinic anhydride and monoalkylurea units as thermally degradable CO2-philic units were prepared by the copolymerization of a 1:1 mixture of [3-(triethoxysilyl)propyl]succinic anhydride (TESPS) or [3-(triethoxysilyl)propyl]urea (TESPU) and bis(triethoxysilyl)ethane (BTESE). The succinic anhydride and monoalkylurea units underwent thermal degradation to form ester and dialkylurea units, respectively, with the liberation of small molecules (e.g., CO2 and NH3) under N2 atmosphere. The effects of thermal degradation on the performance of the obtained membranes were investigated. The TESPS-BTESE- and TESPU-BTESE-based membranes calcined at 250 °C and 200 °C exhibited good CO2/N2 permselectivities of 20.2 and 14.4, respectively, with CO2 permeances of 7.7 × 10−8 and 7.9 × 10−8 mol m−2·s−1·Pa−1, respectively. When the membranes were further calcined at elevated temperatures of 350 °C and 300 °C, respectively, to promote the thermal degradation of the organic units, the CO2 permeances increased to 1.3 × 10−7 and 1.2 × 10−6 mol m−2·s−1·Pa−1 (3.9 × 102 and 3.6 × 103 GPU), although the CO2/N2 permselectivities decreased to 19.5 and 8.4, respectively. These data indicate that the controlled thermal degradation of the organic units provides a new methodology for possible tuning of the CO2 separation performance of PSQ membranes.
{"title":"Preparation of Polysilsesquioxane-Based CO2 Separation Membranes with Thermally Degradable Succinic Anhydride and Urea Units","authors":"Katsuhiro Horata, Tsubasa Yoshio, Ryuto Miyazaki, Yohei Adachi, M. Kanezashi, T. Tsuru, J. Ohshita","doi":"10.3390/separations11040110","DOIUrl":"https://doi.org/10.3390/separations11040110","url":null,"abstract":"New polysilsesquioxane (PSQ)-based CO2 separation membranes with succinic anhydride and monoalkylurea units as thermally degradable CO2-philic units were prepared by the copolymerization of a 1:1 mixture of [3-(triethoxysilyl)propyl]succinic anhydride (TESPS) or [3-(triethoxysilyl)propyl]urea (TESPU) and bis(triethoxysilyl)ethane (BTESE). The succinic anhydride and monoalkylurea units underwent thermal degradation to form ester and dialkylurea units, respectively, with the liberation of small molecules (e.g., CO2 and NH3) under N2 atmosphere. The effects of thermal degradation on the performance of the obtained membranes were investigated. The TESPS-BTESE- and TESPU-BTESE-based membranes calcined at 250 °C and 200 °C exhibited good CO2/N2 permselectivities of 20.2 and 14.4, respectively, with CO2 permeances of 7.7 × 10−8 and 7.9 × 10−8 mol m−2·s−1·Pa−1, respectively. When the membranes were further calcined at elevated temperatures of 350 °C and 300 °C, respectively, to promote the thermal degradation of the organic units, the CO2 permeances increased to 1.3 × 10−7 and 1.2 × 10−6 mol m−2·s−1·Pa−1 (3.9 × 102 and 3.6 × 103 GPU), although the CO2/N2 permselectivities decreased to 19.5 and 8.4, respectively. These data indicate that the controlled thermal degradation of the organic units provides a new methodology for possible tuning of the CO2 separation performance of PSQ membranes.","PeriodicalId":510456,"journal":{"name":"Separations","volume":"279 ","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140754215","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 : 2024-04-01DOI: 10.3390/separations11040107
Meng-Hua Wang, Zhi-Fan Wang, Man Yuan, Chun-Guo Yang, Dong-Liang Wang, Shu-Qi Wang
Edible bird’s nests have a variety of biological activities, the main components of which are sialic acids. Sialic acids are a group of nine-carbon N-acetylated derivatives of neuraminic acid containing a keto group at position C2 and play important roles in many biological processes. To verify whether the oral administration of edible bird’s nests would change the content and distribution of sialic acid components in vivo, a liquid chromatography–mass spectrometry method for the quantitative analysis of sialic acid levels in serum and tissues was developed. In the negative ion mode, the mobile phases consist of 0.1% formic acid in water (A) and acetonitrile (v/v) (B). Isocratic elution was performed with 60% B for 0−15 min. The chromatographic separation was performed on a Morphling HILIC Amide column (2.1 mm × 150 mm, 5 μm) at a flow rate of 0.5 mL min−1. The results showed that the correlation coefficients of the typical calibration curves were all higher than 0.995, exhibiting good linearity. The levels of free and conjugated forms of N-glycolylneuraminic acid (Neu5Gc), N-acetylneuraminic acid (Neu5Ac), and 2-keto-3-deoxy-D-glycero-D-galactonononic acid (KDN) in the serum and different tissues were simultaneously detected after the oral administration of the edible bird’s nests at a daily dose of 300 and 700 mg Kg−1 for seven days in mice. Our study found that the oral administration of edible bird’s nests can significantly increase the concentration of total sialic acids (Neu5Gc + Neu5Ac + KDN) in serum and spleen and lungs tissues, which may be related to the anti-inflammatory and immune function of edible bird’s nest, but further studies are needed to verify this. Neu5Ac was the dominant sialic acid in brain tissue, and Neu5Gc was the dominant sialic acid in serum and other tissues, including heart, liver, spleen, lungs, and kidney. Moreover, we found that the forms of Neu5Ac and Neu5Gc were mainly conjugated in all groups except liver tissue. In conclusion, the method we established had good linearity and accuracy; it allowed the analytes to be effectively separated from the matrix and endogenous substances in serum or tissues, so it could effectively detect the distribution and concentration of free and conjugated forms of sialic acids in serum and tissues, which was beneficial to the research and exploitation of edible bird’s nests and sialic acids.
{"title":"Changes in the Serum and Tissue Levels of Free and Conjugated Sialic Acids, Neu5Ac, Neu5Gc, and KDN in Mice after the Oral Administration of Edible Bird’s Nests: An LC–MS/MS Quantitative Analysis","authors":"Meng-Hua Wang, Zhi-Fan Wang, Man Yuan, Chun-Guo Yang, Dong-Liang Wang, Shu-Qi Wang","doi":"10.3390/separations11040107","DOIUrl":"https://doi.org/10.3390/separations11040107","url":null,"abstract":"Edible bird’s nests have a variety of biological activities, the main components of which are sialic acids. Sialic acids are a group of nine-carbon N-acetylated derivatives of neuraminic acid containing a keto group at position C2 and play important roles in many biological processes. To verify whether the oral administration of edible bird’s nests would change the content and distribution of sialic acid components in vivo, a liquid chromatography–mass spectrometry method for the quantitative analysis of sialic acid levels in serum and tissues was developed. In the negative ion mode, the mobile phases consist of 0.1% formic acid in water (A) and acetonitrile (v/v) (B). Isocratic elution was performed with 60% B for 0−15 min. The chromatographic separation was performed on a Morphling HILIC Amide column (2.1 mm × 150 mm, 5 μm) at a flow rate of 0.5 mL min−1. The results showed that the correlation coefficients of the typical calibration curves were all higher than 0.995, exhibiting good linearity. The levels of free and conjugated forms of N-glycolylneuraminic acid (Neu5Gc), N-acetylneuraminic acid (Neu5Ac), and 2-keto-3-deoxy-D-glycero-D-galactonononic acid (KDN) in the serum and different tissues were simultaneously detected after the oral administration of the edible bird’s nests at a daily dose of 300 and 700 mg Kg−1 for seven days in mice. Our study found that the oral administration of edible bird’s nests can significantly increase the concentration of total sialic acids (Neu5Gc + Neu5Ac + KDN) in serum and spleen and lungs tissues, which may be related to the anti-inflammatory and immune function of edible bird’s nest, but further studies are needed to verify this. Neu5Ac was the dominant sialic acid in brain tissue, and Neu5Gc was the dominant sialic acid in serum and other tissues, including heart, liver, spleen, lungs, and kidney. Moreover, we found that the forms of Neu5Ac and Neu5Gc were mainly conjugated in all groups except liver tissue. In conclusion, the method we established had good linearity and accuracy; it allowed the analytes to be effectively separated from the matrix and endogenous substances in serum or tissues, so it could effectively detect the distribution and concentration of free and conjugated forms of sialic acids in serum and tissues, which was beneficial to the research and exploitation of edible bird’s nests and sialic acids.","PeriodicalId":510456,"journal":{"name":"Separations","volume":"20 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140797270","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 : 2024-04-01DOI: 10.3390/separations11040109
Li Xu, J. Quan, Li Xu, Meihua Li, Chenglong Li, Saqib Mujtaba, Xingming Ning, Pei Chen, Qiang Weng, Zhongwei An, Xinbing Chen
Surface-coupled transition metal oxyhydroxide (TMOOH) on semiconductor (SC)-based photoanodes are effective strategies for improving photoelectrochemical (PEC) performance. However, there is a substantial difference between the current density and theoretical value due to the inevitable interfacial charge recombination of SC/TMOOH. Here, we employ BiVO4/FeNiOOH as a model, constructing the BiVO4/MnOx/CoOx/FeNiOOH integrated system by introducing a novel hetero-interface regulation unit, i.e., MnOx/CoOx. As expected, the optimized integrated system demonstrates a photocurrent density as high as 5.0 mA/cm2 at 1.23 V versus the reversible hydrogen electrode (RHE) under 1 sun AM 1.5G illumination, accompanied by 12-h stability. The detailed electrochemical analysis and intensity modulated photocurrent spectroscopy (IMPS) have confirmed that the high PEC performance mainly originates from the hetero-interface structure, which not only suppresses the interfacial charge recombination by accelerating the photogenerated hole transfer kinetics from BiVO4 to FeNiOOH but promotes the kinetics of surface oxygen evolution reaction (OER). Notably, these findings can also be extended to other structures (CeOx/CoOx), reflecting its universality. This finding has provided a new insight into the highly efficient solar energy conversion in the SC/TMOOH system.
基于半导体（SC）的光阳极表面耦合过渡金属氧氢氧化物（TMOOH）是提高光电化学（PEC）性能的有效策略。然而，由于 SC/TMOOH 不可避免的界面电荷重组，其电流密度与理论值之间存在很大差异。在此，我们以 BiVO4/FeNiOOH 为模型，通过引入新型异质界面调节单元（即 MnOx/CoOx），构建了 BiVO4/MnOx/CoOx/FeNiOOH 集成系统。正如预期的那样，优化后的集成系统在 1 sun AM 1.5G 光照条件下，相对于可逆氢电极（RHE），在 1.23 V 电压下的光电流密度高达 5.0 mA/cm2，并且具有 12 小时的稳定性。详细的电化学分析和强度调制光电流光谱（IMPS）证实，高 PEC 性能主要源于异质界面结构，它不仅通过加速从 BiVO4 到 FeNiOOH 的光生空穴传输动力学抑制了界面电荷重组，还促进了表面氧进化反应（OER）动力学。值得注意的是，这些发现还可以扩展到其他结构（CeOx/CoOx），反映了其普遍性。这一发现为在 SC/TMOOH 系统中实现高效太阳能转换提供了新的视角。
{"title":"Modulating Interfacial Charge Transfer Behavior through the Construction of a Hetero-Interface for Efficient Photoelectrochemical Water Splitting","authors":"Li Xu, J. Quan, Li Xu, Meihua Li, Chenglong Li, Saqib Mujtaba, Xingming Ning, Pei Chen, Qiang Weng, Zhongwei An, Xinbing Chen","doi":"10.3390/separations11040109","DOIUrl":"https://doi.org/10.3390/separations11040109","url":null,"abstract":"Surface-coupled transition metal oxyhydroxide (TMOOH) on semiconductor (SC)-based photoanodes are effective strategies for improving photoelectrochemical (PEC) performance. However, there is a substantial difference between the current density and theoretical value due to the inevitable interfacial charge recombination of SC/TMOOH. Here, we employ BiVO4/FeNiOOH as a model, constructing the BiVO4/MnOx/CoOx/FeNiOOH integrated system by introducing a novel hetero-interface regulation unit, i.e., MnOx/CoOx. As expected, the optimized integrated system demonstrates a photocurrent density as high as 5.0 mA/cm2 at 1.23 V versus the reversible hydrogen electrode (RHE) under 1 sun AM 1.5G illumination, accompanied by 12-h stability. The detailed electrochemical analysis and intensity modulated photocurrent spectroscopy (IMPS) have confirmed that the high PEC performance mainly originates from the hetero-interface structure, which not only suppresses the interfacial charge recombination by accelerating the photogenerated hole transfer kinetics from BiVO4 to FeNiOOH but promotes the kinetics of surface oxygen evolution reaction (OER). Notably, these findings can also be extended to other structures (CeOx/CoOx), reflecting its universality. This finding has provided a new insight into the highly efficient solar energy conversion in the SC/TMOOH system.","PeriodicalId":510456,"journal":{"name":"Separations","volume":"45 2","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140783716","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 : 2024-03-02DOI: 10.3390/separations11030079
Jong Gu Kim, B. Bai
This study investigates lyocell-based activated carbon fibers (ACFs) for their suitability in adsorbing and electrochemically detecting toxic HCl gas. ACFs were prepared via steam activation, varying temperature (800–900 °C) and time (40–240 min) to assess their adsorption and sensing capabilities. The adjustment of activation temperature and reaction time aimed to regulate the uniformity of the pore structure and pore size of the active reaction area, as well as the number of reaction sites in the ACFs. Optimal ACFs were achieved at 900 °C for 50 min, exhibiting the highest specific surface area (1403 m2/g) and total pore volume (0.66 cm3/g). Longer reaction times resulted in pore formation and disorder, reducing mechanical strength. The ACFs prepared under optimal conditions demonstrated a rapid increase in resistance during sensor measurement, indicating a significant sensitivity to HCl gas. These findings suggest the potential of ACFs for efficient HCl gas adsorption (1626.20 mg/g) and highlight the importance of activation parameters in tailoring their properties for practical applications.
{"title":"A Chemical Safety Assessment of Lyocell-Based Activated Carbon Fiber with a High Surface Area through the Evaluation of HCl Gas Adsorption and Electrochemical Properties","authors":"Jong Gu Kim, B. Bai","doi":"10.3390/separations11030079","DOIUrl":"https://doi.org/10.3390/separations11030079","url":null,"abstract":"This study investigates lyocell-based activated carbon fibers (ACFs) for their suitability in adsorbing and electrochemically detecting toxic HCl gas. ACFs were prepared via steam activation, varying temperature (800–900 °C) and time (40–240 min) to assess their adsorption and sensing capabilities. The adjustment of activation temperature and reaction time aimed to regulate the uniformity of the pore structure and pore size of the active reaction area, as well as the number of reaction sites in the ACFs. Optimal ACFs were achieved at 900 °C for 50 min, exhibiting the highest specific surface area (1403 m2/g) and total pore volume (0.66 cm3/g). Longer reaction times resulted in pore formation and disorder, reducing mechanical strength. The ACFs prepared under optimal conditions demonstrated a rapid increase in resistance during sensor measurement, indicating a significant sensitivity to HCl gas. These findings suggest the potential of ACFs for efficient HCl gas adsorption (1626.20 mg/g) and highlight the importance of activation parameters in tailoring their properties for practical applications.","PeriodicalId":510456,"journal":{"name":"Separations","volume":"13 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-03-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140081880","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 : 2024-03-01DOI: 10.3390/separations11030078
B. Arwenyo, Prashan M. Rodrigo, O. Olabode, Hashani P. Abeysinghe, Jessie N. Tisdale, Rose C. Azuba, T. Mlsna
Copper is a non-biodegradable heavy metal, and high levels in water bodies cause serious environmental and health issues. Douglas fir biochar has a higher number of carboxylic, phenolic, and lactonic groups, which provide suitable active sites for copper removal. Douglas fir biochar (BC) was modified using 20% solutions of KOH (KOH/BC), H2SO4, (H2SO4/BC), and Na2CO3 (Na2CO3/BC). All materials were characterized using SEM, SEM-EDS, FTIR, TGA, XRD, BET, and elemental analysis. These modifications were done to compare the activations of those sites by measuring copper removal efficiencies. KOH/BC, H2SO4/BC, and Na2CO3/BC materials gave surface areas of 389.3, 326.7, and 367.9 m2 g−1, respectively, compared with pristine biochar with a surface area of 578.9 m2 g−1. The maximum Langmuir adsorption capacities for Na2CO3/BC, KOH/BC, BC, and H2SO4/BC were 24.79, 18.31, 17.38, and 9.17 mg g−1, respectively. All three modifications gave faster kinetics at 2 mg/L initial copper concentrations (pH 5) compared with pristine BC. The copper removal efficiency was demonstrated in four different spiked real water matrices. The copper removals of all four water matrices were above 90% at 2 mg/L initial concentration with a 2 g/L biochar dosage. The competitive effects of Pb2+, Zn2+, Cd2+, and Mg2+ were studied at equimolar concentrations of Cu2+ and competitive ions for all four materials.
{"title":"Comparison of Acid- and Base-Modified Biochar Derived from Douglas Fir for Removal of Copper (II) from Wastewater","authors":"B. Arwenyo, Prashan M. Rodrigo, O. Olabode, Hashani P. Abeysinghe, Jessie N. Tisdale, Rose C. Azuba, T. Mlsna","doi":"10.3390/separations11030078","DOIUrl":"https://doi.org/10.3390/separations11030078","url":null,"abstract":"Copper is a non-biodegradable heavy metal, and high levels in water bodies cause serious environmental and health issues. Douglas fir biochar has a higher number of carboxylic, phenolic, and lactonic groups, which provide suitable active sites for copper removal. Douglas fir biochar (BC) was modified using 20% solutions of KOH (KOH/BC), H2SO4, (H2SO4/BC), and Na2CO3 (Na2CO3/BC). All materials were characterized using SEM, SEM-EDS, FTIR, TGA, XRD, BET, and elemental analysis. These modifications were done to compare the activations of those sites by measuring copper removal efficiencies. KOH/BC, H2SO4/BC, and Na2CO3/BC materials gave surface areas of 389.3, 326.7, and 367.9 m2 g−1, respectively, compared with pristine biochar with a surface area of 578.9 m2 g−1. The maximum Langmuir adsorption capacities for Na2CO3/BC, KOH/BC, BC, and H2SO4/BC were 24.79, 18.31, 17.38, and 9.17 mg g−1, respectively. All three modifications gave faster kinetics at 2 mg/L initial copper concentrations (pH 5) compared with pristine BC. The copper removal efficiency was demonstrated in four different spiked real water matrices. The copper removals of all four water matrices were above 90% at 2 mg/L initial concentration with a 2 g/L biochar dosage. The competitive effects of Pb2+, Zn2+, Cd2+, and Mg2+ were studied at equimolar concentrations of Cu2+ and competitive ions for all four materials.","PeriodicalId":510456,"journal":{"name":"Separations","volume":" 8","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140091356","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 : 2024-03-01DOI: 10.3390/separations11030077
Da Li, Zhan Yang, Kun Wang, Lan Zhang, Linglong Shi, Abdul Qadeer, Jiao Dong, Haoyu Ren
Nickel titanate (NiTiO3) semiconductors and graphitic carbon nitride (g-C3N4) have attracted great attention as photocatalysts in the degradation of environmental pollutants because of their visible-light-driven activity. But the utilizations of both semiconductors are limited by their low specific surface area. In this study, a nano-NiTiO3/g-C3N4 photocatalyst was successfully synthesized by optimizing the preparation method of photocatalyst precursors. Compared with the bulk g-C3N4 and bulk NiTiO3/g-C3N4 composite photocatalysts, the nano-NiTiO3/g-C3N4 composite catalyst displayed a larger specific surface area, a more abundant pore size structure, and superior carrier separation capabilities. According to the pseudo-first-order, the degradation rate of MB was more than 2.5–19.7 times higher than that of previous studies. The superoxide radicals (·O2−) and holes (h+) played significant roles in the photocatalytic reaction of MB. This study provides a new idea for the synthesis of photocatalysts and the improvement in photocatalytic performance.
{"title":"Construction of High-Activity Nano-NiTiO3/g-C3N4 Composite Catalysts for Enhanced Photodegradation Activities under Visible Light","authors":"Da Li, Zhan Yang, Kun Wang, Lan Zhang, Linglong Shi, Abdul Qadeer, Jiao Dong, Haoyu Ren","doi":"10.3390/separations11030077","DOIUrl":"https://doi.org/10.3390/separations11030077","url":null,"abstract":"Nickel titanate (NiTiO3) semiconductors and graphitic carbon nitride (g-C3N4) have attracted great attention as photocatalysts in the degradation of environmental pollutants because of their visible-light-driven activity. But the utilizations of both semiconductors are limited by their low specific surface area. In this study, a nano-NiTiO3/g-C3N4 photocatalyst was successfully synthesized by optimizing the preparation method of photocatalyst precursors. Compared with the bulk g-C3N4 and bulk NiTiO3/g-C3N4 composite photocatalysts, the nano-NiTiO3/g-C3N4 composite catalyst displayed a larger specific surface area, a more abundant pore size structure, and superior carrier separation capabilities. According to the pseudo-first-order, the degradation rate of MB was more than 2.5–19.7 times higher than that of previous studies. The superoxide radicals (·O2−) and holes (h+) played significant roles in the photocatalytic reaction of MB. This study provides a new idea for the synthesis of photocatalysts and the improvement in photocatalytic performance.","PeriodicalId":510456,"journal":{"name":"Separations","volume":"104 26","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140089183","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 : 2024-02-23DOI: 10.3390/separations11030066
Calogero Cuttaia, Barbara Di Stefano, Solange Sorçaburu Ciglieri, Raffaella Vetrini, C. Previderè, P. Fattorini
Body fluid identification is fundamental in forensic science as it links a specific biological source to a genetic profile, thus providing critical clues for crime scene reconstruction. Blood is one of the most common body fluids found on the crime scene, and several strategies have been developed for its identification in recent decades. Usually, after a preliminary (or presumptive) test to determine the presence of blood (both human and non-human), a confirmatory test is needed to prove that the sample is human blood. Out of the confirmatory tests, immunochromatographic (IC) assays are the most commonly and widely used. This work gives a review of the use of commercial kits specifically developed to detect human hemoglobin or glycophorin A (a surface protein of human red cells) in forensics. Claimed sensitivity varies broadly (ranging from 0.06 to 75 nanoliters of fresh blood), but different values (as low as 0.002 nL) were found during validation procedures. Specificities are high, and the possibility of cross-reaction (with the risk of false-positive results) is so low that it can be considered negligible. False-negative results, however, can be found due to the so-called “hook effect” as well as to the target degradation/modification, which interferes with the Ag-Ab binding. In addition, the chemical compositions of the presumptive test, detergents, and washing can also promote false negative outcomes in peculiar situations. Although IC assays are rapid, inexpensive, specific, and easy to use even on the crime scene, their major limitation is represented by the destructive approach required by this kind of confirmatory test. Since the final goal of the forensic investigation is the genetic typing of a bloodstain, we will describe the strategies developed for IC assays of faint stains as well as the strategies adopted to ensure that exactly the same sample undergoes human blood identification and DNA typing.
体液鉴定是法医学的基础，因为它将特定的生物来源与遗传特征联系起来，从而为重建犯罪现场提供重要线索。血液是在犯罪现场发现的最常见体液之一，近几十年来已开发出多种体液鉴定策略。通常情况下，在进行初步（或推定）检验以确定血液（包括人类和非人类血液）存在之后，需要进行确证检验以证明样本为人类血液。在确证检验中，免疫层析（IC）检验是最常用和最广泛使用的。本研究综述了法医学中使用的专门用于检测人类血红蛋白或糖蛋白 A（人类红细胞的一种表面蛋白）的商业试剂盒。声称的灵敏度差别很大（从 0.06 到 75 纳升新鲜血液不等），但在验证过程中发现了不同的数值（低至 0.002 nL）。特异性很高，交叉反应的可能性（假阳性结果的风险）很低，可以忽略不计。然而，由于所谓的 "钩子效应 "以及目标降解/修饰干扰了 Ag-Ab 结合，可能会出现假阴性结果。此外，在特殊情况下，推定试验的化学成分、洗涤剂和洗涤也会导致假阴性结果。虽然集成电路检测快速、廉价、特异，而且即使在犯罪现场也很容易使用，但其主要局限性在于这种确证检验所需的破坏性方法。由于法医调查的最终目标是对血迹进行基因分型，我们将介绍针对微弱血迹的 IC 检测所开发的策略，以及为确保对完全相同的样本进行人体血液鉴定和 DNA 分型所采取的策略。
{"title":"Immunochromatographic Detection of Human Blood: A Forensic Review","authors":"Calogero Cuttaia, Barbara Di Stefano, Solange Sorçaburu Ciglieri, Raffaella Vetrini, C. Previderè, P. Fattorini","doi":"10.3390/separations11030066","DOIUrl":"https://doi.org/10.3390/separations11030066","url":null,"abstract":"Body fluid identification is fundamental in forensic science as it links a specific biological source to a genetic profile, thus providing critical clues for crime scene reconstruction. Blood is one of the most common body fluids found on the crime scene, and several strategies have been developed for its identification in recent decades. Usually, after a preliminary (or presumptive) test to determine the presence of blood (both human and non-human), a confirmatory test is needed to prove that the sample is human blood. Out of the confirmatory tests, immunochromatographic (IC) assays are the most commonly and widely used. This work gives a review of the use of commercial kits specifically developed to detect human hemoglobin or glycophorin A (a surface protein of human red cells) in forensics. Claimed sensitivity varies broadly (ranging from 0.06 to 75 nanoliters of fresh blood), but different values (as low as 0.002 nL) were found during validation procedures. Specificities are high, and the possibility of cross-reaction (with the risk of false-positive results) is so low that it can be considered negligible. False-negative results, however, can be found due to the so-called “hook effect” as well as to the target degradation/modification, which interferes with the Ag-Ab binding. In addition, the chemical compositions of the presumptive test, detergents, and washing can also promote false negative outcomes in peculiar situations. Although IC assays are rapid, inexpensive, specific, and easy to use even on the crime scene, their major limitation is represented by the destructive approach required by this kind of confirmatory test. Since the final goal of the forensic investigation is the genetic typing of a bloodstain, we will describe the strategies developed for IC assays of faint stains as well as the strategies adopted to ensure that exactly the same sample undergoes human blood identification and DNA typing.","PeriodicalId":510456,"journal":{"name":"Separations","volume":"19 8","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-02-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139957396","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}
The widespread use of tetracycline (TC) poses potential hazards to ecosystems and human health. In this study, ZIF-67 was successfully synthesized using a room-temperature static synthesis method and applied to the efficient removal of TC from water. It was shown that the maximum adsorption of TC by ZIF-67 could reach 1583.128 mg·g−1 at pH = 5.0, an initial TC concentration of 450 mg·g−1, an adsorption time of 720 min, and a temperature of 308K.The pseudo-second-order kinetic model and Langmuir’s isothermal adsorption model could describe the adsorption process better, which proved that the adsorption of ZIF-67 on TC was mainly monolayer adsorption dominated by chemisorption. Mechanistic studies showed that the adsorption process of ZIF-67 on TC was mainly through electrostatic interactions, pore adsorption, π–π interactions, and framework coordination of ZIF-67 surface cations with TC.
{"title":"Efficient Removal of Tetracycline by Metal–Organic Framework ZIF-67 and Its Mechanism","authors":"Shengyang Zheng, Yaping Xu, Xu Yao, Chenzhe Wang, Ping Liu, Haitao Zhao, Jianbing Lu, Jing Ju","doi":"10.3390/separations11020063","DOIUrl":"https://doi.org/10.3390/separations11020063","url":null,"abstract":"The widespread use of tetracycline (TC) poses potential hazards to ecosystems and human health. In this study, ZIF-67 was successfully synthesized using a room-temperature static synthesis method and applied to the efficient removal of TC from water. It was shown that the maximum adsorption of TC by ZIF-67 could reach 1583.128 mg·g−1 at pH = 5.0, an initial TC concentration of 450 mg·g−1, an adsorption time of 720 min, and a temperature of 308K.The pseudo-second-order kinetic model and Langmuir’s isothermal adsorption model could describe the adsorption process better, which proved that the adsorption of ZIF-67 on TC was mainly monolayer adsorption dominated by chemisorption. Mechanistic studies showed that the adsorption process of ZIF-67 on TC was mainly through electrostatic interactions, pore adsorption, π–π interactions, and framework coordination of ZIF-67 surface cations with TC.","PeriodicalId":510456,"journal":{"name":"Separations","volume":"93 14","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139959705","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 : 2024-02-16DOI: 10.3390/separations11020060
P. Vareltzis, Panagiota Karatsioli, Ioannis Kazakos, Anna-Maria Menelaou, Konstantina Parmaxi, Vangelis Economou
The food industry is seeking a stable, non-toxic red dye as a substitute for synthetic pigments. This can result from the reaction between 5-O-Caffeoylquinic acid (5-CQA) and tryptophan (TRP). This study explores the reaction kinetics under ultrasound conditions and investigates reaction parameters, such as pH, temperature, and reactants’ concentrations, to accelerate the reaction. At the end of the reaction, the solution was either spray-dried or acidified to isolate the pigment, which was evaluated for its potential as a food dye. Using ultrasound at 40 °C led to a significant acceleration of the reaction that was completed in 8.5 h, marking a 300% improvement compared to literature. The caffeic acid, and not the quinic acid, moiety of 5-CQA seems to be partly responsible for the formation of the red pigment. The pH had a profound impact on the reaction rate, with an optimal value of pH = 9.5. Increased TRP concentrations led to increased reaction rates, while higher 5-CQA concentrations led to significant deviations from redness (a* value). The pigment, lacking significant antimicrobial activity, exhibited remarkable thermal stability (pH 3–9), delaying food oxidation and color deterioration. The results indicate that the reaction can be significantly accelerated by ultrasound, which will be useful for the scale-up of the process and giving the produced pigment the potential for use as an alternative to artificial coloring.
{"title":"Optimization of the Reaction between 5-O-Caffeoylquinic Acid (5-CQA) and Tryptophan—Isolation of the Product and Its Evaluation as a Food Dye","authors":"P. Vareltzis, Panagiota Karatsioli, Ioannis Kazakos, Anna-Maria Menelaou, Konstantina Parmaxi, Vangelis Economou","doi":"10.3390/separations11020060","DOIUrl":"https://doi.org/10.3390/separations11020060","url":null,"abstract":"The food industry is seeking a stable, non-toxic red dye as a substitute for synthetic pigments. This can result from the reaction between 5-O-Caffeoylquinic acid (5-CQA) and tryptophan (TRP). This study explores the reaction kinetics under ultrasound conditions and investigates reaction parameters, such as pH, temperature, and reactants’ concentrations, to accelerate the reaction. At the end of the reaction, the solution was either spray-dried or acidified to isolate the pigment, which was evaluated for its potential as a food dye. Using ultrasound at 40 °C led to a significant acceleration of the reaction that was completed in 8.5 h, marking a 300% improvement compared to literature. The caffeic acid, and not the quinic acid, moiety of 5-CQA seems to be partly responsible for the formation of the red pigment. The pH had a profound impact on the reaction rate, with an optimal value of pH = 9.5. Increased TRP concentrations led to increased reaction rates, while higher 5-CQA concentrations led to significant deviations from redness (a* value). The pigment, lacking significant antimicrobial activity, exhibited remarkable thermal stability (pH 3–9), delaying food oxidation and color deterioration. The results indicate that the reaction can be significantly accelerated by ultrasound, which will be useful for the scale-up of the process and giving the produced pigment the potential for use as an alternative to artificial coloring.","PeriodicalId":510456,"journal":{"name":"Separations","volume":"21 5","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139961121","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 : 2024-02-14DOI: 10.3390/separations11020059
Zeinab Rabiei, Andrew Simons, Magdalena Folkmanova, Tereza Vesela, O. Uhlík, E. Kozliak, Alena Kubátová
Lignin, a complex and abundant biopolymer, is a major constituent of plant cell walls. Due to its chemical and structural complexity, lignin degradation is a challenging task for both natural and engineered systems. Therefore, investigation of lignin degradation using so called “model compounds” has been the focus of many research efforts in recent years. This study addresses the utility of guaiacylglycerol-β-guaiacyl ether (Gβ2) as a model compound for evaluating the β-O-4 bond cleavage under diverse thermal and aqueous medium conditions. Experimental conditions included varied pH (3–10), microbial biodegradation, subcritical water environment (150–250 °C), and mild pyrolysis (150–250 °C). A high-performance liquid chromatography with high-resolution mass spectrometry was employed for accurate detection and quantification of both Gβ2 and its degradation/modification products in an aqueous environment. Pyrolysis experiments were performed using gas chromatography-mass spectrometry analysis with a pyrolyzer. The results showed that Gβ2 remained stable under exposure to moderate pH and several bacterial strains, which were successfully used previously for biodegradation of other recalcitrant pollutants. We report, for the first time, differing Gβ2 breakdown pathways for subcritical water treatment vs. pyrolysis under an inert atmosphere. The scientific novelty lies in the presentation of differences in the degradation pathways of Gβ2 during subcritical water treatment compared to pyrolysis in an inert atmosphere, with water playing a key role. The observed differences are ascribed to the suppression of homolytic reactions by water as a solvent.
{"title":"Stability and Reactivity of Guaiacylglycerol-β-Guaiacyl Ether, a Compound Modeling β-O-4 Linkage in Lignin","authors":"Zeinab Rabiei, Andrew Simons, Magdalena Folkmanova, Tereza Vesela, O. Uhlík, E. Kozliak, Alena Kubátová","doi":"10.3390/separations11020059","DOIUrl":"https://doi.org/10.3390/separations11020059","url":null,"abstract":"Lignin, a complex and abundant biopolymer, is a major constituent of plant cell walls. Due to its chemical and structural complexity, lignin degradation is a challenging task for both natural and engineered systems. Therefore, investigation of lignin degradation using so called “model compounds” has been the focus of many research efforts in recent years. This study addresses the utility of guaiacylglycerol-β-guaiacyl ether (Gβ2) as a model compound for evaluating the β-O-4 bond cleavage under diverse thermal and aqueous medium conditions. Experimental conditions included varied pH (3–10), microbial biodegradation, subcritical water environment (150–250 °C), and mild pyrolysis (150–250 °C). A high-performance liquid chromatography with high-resolution mass spectrometry was employed for accurate detection and quantification of both Gβ2 and its degradation/modification products in an aqueous environment. Pyrolysis experiments were performed using gas chromatography-mass spectrometry analysis with a pyrolyzer. The results showed that Gβ2 remained stable under exposure to moderate pH and several bacterial strains, which were successfully used previously for biodegradation of other recalcitrant pollutants. We report, for the first time, differing Gβ2 breakdown pathways for subcritical water treatment vs. pyrolysis under an inert atmosphere. The scientific novelty lies in the presentation of differences in the degradation pathways of Gβ2 during subcritical water treatment compared to pyrolysis in an inert atmosphere, with water playing a key role. The observed differences are ascribed to the suppression of homolytic reactions by water as a solvent.","PeriodicalId":510456,"journal":{"name":"Separations","volume":"81 2","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139779438","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}
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