Pub Date : 2024-09-27DOI: 10.1016/j.seppur.2024.129875
The capture and conversion of low-concentration CO2 into high value-added products under mild conditions remains a major challenge. In this work, an additive/metal/solvent-free catalytic transformation between epoxides and low-concentration CO2 under atmospheric conditions is achieved by using hypercrosslinked ionic polymers (IMPy-HIP or BPy-HIP) as catalysts prepared by an one-pot Friedel–Crafts alkylation between an imidazolium-based ionic linker and 1, 1′-binaphthyl-2, 2′-diyl hydrogenphosphate (BNDHP, a Bronsted acid, strong hydrogen bond donor). The HIPs bearing a strong hydrogen bonding site (ArPO3OH), active cations (imidazolium) and nucleophilic counterion (Cl−) demonstrate highly catalytic efficiency and stable recyclability for low-concentration CO2-epoxide cycloaddition. The experiment results combining with DFT theoretical calculations reveal that the high performance of this catalyst attributes to the cooperation of the Bronsted acid site (P-OH), basic pyridine N and ionic site. In addition, the catalyst shows excellent structural stability and substrate universality, and it can be easily separated by centrifugation and reused for five runs without significant decrease in catalytic performance.
{"title":"Hypercrosslinked ionic polymers constructed by ionic cross-linkers and Bronsted acid for catalytic cycloaddition of low-concentration CO2 with epoxide under atmospheric pressure","authors":"","doi":"10.1016/j.seppur.2024.129875","DOIUrl":"10.1016/j.seppur.2024.129875","url":null,"abstract":"<div><div>The capture and conversion of low-concentration CO<sub>2</sub> into high value-added products under mild conditions remains a major challenge. In this work, an additive/metal/solvent-free catalytic transformation between epoxides and low-concentration CO<sub>2</sub> under atmospheric conditions is achieved by using hypercrosslinked ionic polymers (IMPy-HIP or BPy-HIP) as catalysts prepared by an one-pot Friedel–Crafts alkylation between an imidazolium-based ionic linker and 1, 1′-binaphthyl-2, 2′-diyl hydrogenphosphate (BNDHP, a Bronsted acid, strong hydrogen bond donor). The HIPs bearing a strong hydrogen bonding site (ArPO<sub>3</sub>OH), active cations (imidazolium) and nucleophilic counterion (Cl<sup>−</sup>) demonstrate highly catalytic efficiency and stable recyclability for low-concentration CO<sub>2</sub>-epoxide cycloaddition. The experiment results combining with DFT theoretical calculations reveal that the high performance of this catalyst attributes to the cooperation of the Bronsted acid site (P-OH), basic pyridine N and ionic site. In addition, the catalyst shows excellent structural stability and substrate universality, and it can be easily separated by centrifugation and reused for five runs without significant decrease in catalytic performance.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":null,"pages":null},"PeriodicalIF":8.1,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142358782","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-27DOI: 10.1016/j.seppur.2024.129902
The novel strategy of thin-film nanocomposite loose nanofiltration (LNF) membranes incorporating an interlayer of nanomaterials has raised growing interests for the high-performance membrane design. Although the effects of membrane structure on separation performance have been elucidated for a long time, however, the quantitative structure-performance relationship of interlayer-based LNF membranes has not been established. In this study, we established the structure-performance relationship of TA-MoS2 interlayer based LNF membranes from a quantitative level for the first time. The correlation heat map analysis identified four key structural parameters (e.g. selective layer thickness, crosslinking degree, water contact angle, and zeta potential) for water permeability as well as dye rejection, and three key structural parameters (e.g. selective layer thickness, crosslinking degree, and zeta potential) for salts rejection, respectively. Furthermore, the multiple linear regression analysis revealed the rigorous mathematic modeling of key structural parameters-separation performance relationships with all R2 values above 0.899, and determined the contributions of each key structural parameter to the separation performance in a quantitative level. Finally, the optimal TA-MoS2 interlayer based LNF membrane exhibited a high water permeability of 80.2 LMH·bar−1, effective separation of dye/salts (rejection rate: congo red (99.0%), methyl blue (95.1%), Na2SO4 (1.5%) and NaCl (0.5%)), good stability and antifouling properties (i.e. water flux recovery rate (FRR) of 96% for humic acid). This study can pave the way of quantitatively design of interlayer-based LNF membrane with targeted performance.
{"title":"Quantitative assessment of structure-performance relationship of loose nanofiltration membranes with TA-MoS2 interlayer for effective dye/salt separation","authors":"","doi":"10.1016/j.seppur.2024.129902","DOIUrl":"10.1016/j.seppur.2024.129902","url":null,"abstract":"<div><div>The novel strategy of thin-film nanocomposite loose nanofiltration (LNF) membranes incorporating an interlayer of nanomaterials has raised growing interests for the high-performance membrane design. Although the effects of membrane structure on separation performance have been elucidated for a long time, however, the quantitative structure-performance relationship of interlayer-based LNF membranes has not been established. In this study, we established the structure-performance relationship of TA-MoS<sub>2</sub> interlayer based LNF membranes from a quantitative level for the first time. The correlation heat map analysis identified four key structural parameters (e.g. selective layer thickness, crosslinking degree, water contact angle, and zeta potential) for water permeability as well as dye rejection, and three key structural parameters (e.g. selective layer thickness, crosslinking degree, and zeta potential) for salts rejection, respectively. Furthermore, the multiple linear regression analysis revealed the rigorous mathematic modeling of key structural parameters-separation performance relationships with all R<sup>2</sup> values above 0.899, and determined the contributions of each key structural parameter to the separation performance in a quantitative level. Finally, the optimal TA-MoS<sub>2</sub> interlayer based LNF membrane exhibited a high water permeability of 80.2 LMH·bar<sup>−1</sup>, effective separation of dye/salts (rejection rate: congo red (99.0%), methyl blue (95.1%), Na<sub>2</sub>SO<sub>4</sub> (1.5%) and NaCl (0.5%)), good stability and antifouling properties (i.e. water flux recovery rate (FRR) of 96% for humic acid). This study can pave the way of quantitatively design of interlayer-based LNF membrane with targeted performance.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":null,"pages":null},"PeriodicalIF":8.1,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142358720","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-27DOI: 10.1016/j.seppur.2024.129911
Cobalt-based catalysts are the most promising catalysts for the catalytic oxidation of volatile organic compounds (VOCs). Metal doping is considered to be a valuable strategy to improve the catalytic activity of metal oxide catalysts. Here, a small amount of Sm doped SmyCoOx spinel oxides with walnut-like shape were successfully prepared by solvothermal method and applied for oxidation of toluene and o-xylene. Their physiochemical properties were studied by various characterization, DFT calculation and in situ DRIFIS tests. Sm0.09CoOx substituted by Sm at six-coordination cobalt shows the best oxidation ability on toluene (T90 = 228 °C) and o-xylene (T90 = 268 °C). This is because doping Sm in Co3O4 causes the lattice distortion, and generates Sm-O-Co bonds to weaken the bond energy of Co-O bonds, thus inducing the generation of active oxygen by improving the mobility of lattice oxygen. These results are of great significance for constructing metal–oxygen bonds through metal-doped cobalt oxide catalysts to improve catalytic performance.
钴基催化剂是催化氧化挥发性有机化合物 (VOC) 的最有前途的催化剂。金属掺杂被认为是提高金属氧化物催化剂催化活性的重要策略。本文采用溶热法成功制备了少量掺杂 Sm 的核桃状 SmyCoOx 尖晶石氧化物，并将其用于甲苯和邻二甲苯的氧化。通过各种表征、DFT 计算和原位 DRIFIS 试验研究了它们的理化性质。由 Sm 取代六配位钴的 Sm0.09CoOx 对甲苯（T90 = 228 ℃）和邻二甲苯（T90 = 268 ℃）的氧化能力最佳。这是因为在 Co3O4 中掺杂 Sm 会导致晶格畸变，并生成 Sm-O-Co 键，削弱 Co-O 键的键能，从而通过提高晶格氧的流动性来诱导活性氧的生成。这些结果对于通过金属掺杂氧化钴催化剂构建金属氧键以提高催化性能具有重要意义。
{"title":"Promoting the catalytic activity of SmyCoOx on oxidation of toluene and o-xylene by Sm doped Co3O4 to weaken the Co–O bonds","authors":"","doi":"10.1016/j.seppur.2024.129911","DOIUrl":"10.1016/j.seppur.2024.129911","url":null,"abstract":"<div><div>Cobalt-based catalysts are the most promising catalysts for the catalytic oxidation of volatile organic compounds (VOCs). Metal doping is considered to be a valuable strategy to improve the catalytic activity of metal oxide catalysts. Here, a small amount of Sm doped Sm<sub>y</sub>CoO<sub>x</sub> spinel oxides with walnut-like shape were successfully prepared by solvothermal method and applied for oxidation of toluene and o-xylene. Their physiochemical properties were studied by various characterization, DFT calculation and in situ DRIFIS tests. Sm<sub>0.09</sub>CoO<sub>x</sub> substituted by Sm at six-coordination cobalt shows the best oxidation ability on toluene (T<sub>90</sub> = 228 °C) and o-xylene (T<sub>90</sub> = 268 °C). This is because doping Sm in Co<sub>3</sub>O<sub>4</sub> causes the lattice distortion, and generates Sm-O-Co bonds to weaken the bond energy of Co-O bonds, thus inducing the generation of active oxygen by improving the mobility of lattice oxygen. These results are of great significance for constructing metal–oxygen bonds through metal-doped cobalt oxide catalysts to improve catalytic performance.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":null,"pages":null},"PeriodicalIF":8.1,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142358877","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-26DOI: 10.1016/j.seppur.2024.129845
Improper use of neonicotinoid insecticides (NNIs) can cause serious harm to aquatic ecosystems and human health. Despite the demonstrated excellent reactivity of nonradical persulfate activation in complex aquatic environments, the relationship between defect engineering and catalytic activity, as well as the construction of nonradical directed activation systems, remains uncertain. In this study, we synthesized and characterized Al-doped NiCoAl-LDO layered metal oxide catalysts for the first time. These catalysts were then used to activate peroxydisulfate (PDS) for degrading imidacloprid (IMI) in wastewater. Through degradation experiments and characterization analysis, singlet oxygen (1O2) and electron transfer were identified as the primary mechanisms responsible for IMI removal. Under optimized conditions (0.5 g/L catalyst loading, 1 mM PDS dosage, pH = 7.0), the degradation rate of IMI reached 0.06 min−1. The NiCo2Al1-LDO/PDS system exhibited efficient IMI degradation over a wide pH range (pH = 4–10) (> 73.6 %) and demonstrated excellent resistance against interference from anions such as Cl−, SO42−, HCO3−, CO32−, as well as Humic acid (HA). Our findings confirm that Al doping induces lattice distortion and enhances interfacial electron transfer processes in the catalyst structure, thereby facilitating the transformation from radical to nonradical pathway during the degradation process. This study not only advances our fundamental understanding of metal oxide active site doping regulation, but also presents a novel defect engineering strategy for nonradical oxidation of IMI, offering valuable insights for future research and practical applications of persulfate.
{"title":"Imidacloprid degradation activated by peroxydisulfate with NiCoAl layered metal oxide catalysts: The unique role of Al","authors":"","doi":"10.1016/j.seppur.2024.129845","DOIUrl":"10.1016/j.seppur.2024.129845","url":null,"abstract":"<div><div>Improper use of neonicotinoid insecticides (NNIs) can cause serious harm to aquatic ecosystems and human health. Despite the demonstrated excellent reactivity of nonradical persulfate activation in complex aquatic environments, the relationship between defect engineering and catalytic activity, as well as the construction of nonradical directed activation systems, remains uncertain. In this study, we synthesized and characterized Al-doped NiCoAl-LDO layered metal oxide catalysts for the first time. These catalysts were then used to activate peroxydisulfate (PDS) for degrading imidacloprid (IMI) in wastewater. Through degradation experiments and characterization analysis, singlet oxygen (<sup>1</sup>O<sub>2</sub>) and electron transfer were identified as the primary mechanisms responsible for IMI removal. Under optimized conditions (0.5 g/L catalyst loading, 1 mM PDS dosage, pH = 7.0), the degradation rate of IMI reached 0.06 min<sup>−1</sup>. The NiCo<sub>2</sub>Al<sub>1</sub>-LDO/PDS system exhibited efficient IMI degradation over a wide pH range (pH = 4–10) (> 73.6 %) and demonstrated excellent resistance against interference from anions such as Cl<sup>−</sup>, SO<sub>4</sub><sup>2−</sup>, HCO<sub>3</sub><sup>−</sup>, CO<sub>3</sub><sup>2−</sup>, as well as Humic acid (HA). Our findings confirm that Al doping induces lattice distortion and enhances interfacial electron transfer processes in the catalyst structure, thereby facilitating the transformation from radical to nonradical pathway during the degradation process. This study not only advances our fundamental understanding of metal oxide active site doping regulation, but also presents a novel defect engineering strategy for nonradical oxidation of IMI, offering valuable insights for future research and practical applications of persulfate.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":null,"pages":null},"PeriodicalIF":8.1,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142327385","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-26DOI: 10.1016/j.seppur.2024.129899
Humidification/dehumidification desalination presents a promising method for small-scale water production due to its ability to utilize solar energy and minimal technological requirements. This research examines the performance of solar-assisted humidification/dehumidification (SA-HDH) desalination system, which is designed to treat seawater from Dumas Beach in Surat city of India. The system integrates a solar air heater, a packed humidifier, and a dehumidifier with an indirect evaporative cooler. Through comprehensive energy, exergy, sustainability, and economic assessments, the study aims to assess system efficiency and viability. Results demonstrate that increasing airflow rates significantly enhances heat transfer efficiency within the humidifier and dehumidifier, boosting system performance and increasing yield by 5.4–7.7 %. The average energy efficiency of 35.5 % is observed at an airflow rate of 125 kg/h. The system effectively removed 99.7 % of total dissolved solids, total hardness, and chloride from the seawater, producing high-quality freshwater. The cost of water production ranging from 0.025 to 0.028 $/L, with a sustainability index ranging from 1.052 to 1.064. These findings underscore the SA-HDH system’s potential as an efficient, sustainable, and cost-effective solution for mitigating water scarcity.
{"title":"Performance evaluation of solar-assisted humidification dehumidification system for seawater desalination: An experimental approach","authors":"","doi":"10.1016/j.seppur.2024.129899","DOIUrl":"10.1016/j.seppur.2024.129899","url":null,"abstract":"<div><div>Humidification/dehumidification desalination presents a promising method for small-scale water production due to its ability to utilize solar energy and minimal technological requirements. This research examines the performance of solar-assisted humidification/dehumidification (SA-HDH) desalination system, which is designed to treat seawater from Dumas Beach in Surat city of India. The system integrates a solar air heater, a packed humidifier, and a dehumidifier with an indirect evaporative cooler. Through comprehensive energy, exergy, sustainability, and economic assessments, the study aims to assess system efficiency and viability. Results demonstrate that increasing airflow rates significantly enhances heat transfer efficiency within the humidifier and dehumidifier, boosting system performance and increasing yield by 5.4–7.7 %. The average energy efficiency of 35.5 % is observed at an airflow rate of 125 kg/h. The system effectively removed 99.7 % of total dissolved solids, total hardness, and chloride from the seawater, producing high-quality freshwater. The cost of water production ranging from 0.025 to 0.028 $/L, with a sustainability index ranging from 1.052 to 1.064. These findings underscore the SA-HDH system’s potential as an efficient, sustainable, and cost-effective solution for mitigating water scarcity.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":null,"pages":null},"PeriodicalIF":8.1,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142358973","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-26DOI: 10.1016/j.seppur.2024.129878
Global warming induced by greenhouse gas emissions represents one of the most significant challenges of our time. In response to this issue, extensive research is being conducted on capture and storage of carbon dioxide (CO2) from stationary carbon sources. Metal-organic Frameworks (MOFs) are widely recognized for their efficacy in gas adsorption and separation due to their remarkable structural integrity, high porosity, and versatility. However, the crystalline and powdered forms of MOFs often limit their practical applications because of their inherent hardness and brittleness. Lignocellulose composite aerogels (LCG) possess high porosity and a substantial specific surface area. Their three-dimensional network facilitates the effective embedding of MOFs crystals within the pores, thereby minimizing the loss of MOFs. This characteristic positions LCG as ideal substrates for enhancing the separation and adsorption performance of CO2 capture. This paper reviews the recent advancements in MOFs@Lignocellulose-based composite aerogel (MOFs@LCG), focusing on the preparation method, interaction mechanisms, strategies for improving adsorption performance, and applications in CO2 capture. This review presented herein are significant for advancing research and development in the field of CO2 adsorption and separation.
{"title":"Design strategies and advantages of metal-organic frameworks@ lignocellulose-based composite aerogel for CO2 capture: A review","authors":"","doi":"10.1016/j.seppur.2024.129878","DOIUrl":"10.1016/j.seppur.2024.129878","url":null,"abstract":"<div><div>Global warming induced by greenhouse gas emissions represents one of the most significant challenges of our time. In response to this issue, extensive research is being conducted on capture and storage of carbon dioxide (CO<sub>2</sub>) from stationary carbon sources. Metal-organic Frameworks (MOFs) are widely recognized for their efficacy in gas adsorption and separation due to their remarkable structural integrity, high porosity, and versatility. However, the crystalline and powdered forms of MOFs often limit their practical applications because of their inherent hardness and brittleness. Lignocellulose composite aerogels (LCG) possess high porosity and a substantial specific surface area. Their three-dimensional network facilitates the effective embedding of MOFs crystals within the pores, thereby minimizing the loss of MOFs. This characteristic positions LCG as ideal substrates for enhancing the separation and adsorption performance of CO<sub>2</sub> capture. This paper reviews the recent advancements in MOFs@Lignocellulose-based composite aerogel (MOFs@LCG), focusing on the preparation method, interaction mechanisms, strategies for improving adsorption performance, and applications in CO<sub>2</sub> capture. This review presented herein are significant for advancing research and development in the field of CO<sub>2</sub> adsorption and separation.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":null,"pages":null},"PeriodicalIF":8.1,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142358971","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-26DOI: 10.1016/j.seppur.2024.129871
Piezoelectric materials can induce strain due to the fluid turbulent force produced during fluid shaking, which may be used to activate peroxymonosulfate (PMS). In this study, the effective interfacial interaction of few-odd-numbered layered MoS2 nanosheets and hydrochar (HC) nanocomposites as the piezoelectric material was used in a hydrodynamics energy-driven piezoelectric catalytic PMS activation process (piezo-PMS activation process) for Eriochrome Black T dye degradation. The results showed that Black T dye was efficiently degraded with an efficiency of 99.23 % within 15 min and a pseudo-first-order rate constant of 3.10 min−1 in the MoS2@HC-(6.5:3.5)/PMS/Shaking system. To clearly see the influence of hydraulic gradient (G) value, the hydrodynamics energy-driven piezo-PMS activation process for Black T dye degradation was performed at different shaking frequencies. The results indicated an optimal G value of (14.106 s−1) for Black T dye degradation. Notably, the MoS2@HC-(6.5:3.5)/ PMS/Shaking system produced the lowest EE/O value (34.05 kWhm−3 order−1), resulting in energy savings over 127 times of HC and 9 times of MoS2. Furthermore, piezoelectrochemical measurements of MoS2@HC-(6.5:3.5) indicated that these superior performances primarily resulted from the synergistic effects of MoS2 and HC. This led to a stronger piezoelectric response with effective piezo-generated charge separation, which in turn improved the efficiency of producing reactive species. Combining the scavenger test, FT-IR, and zeta potential analysis, we determined that •OH and SO4•− played a major role, while O2•− and 1O2 played a secondary role in Black T dye degradation. The steady-state concentrations of [•OH]ss, and [SO4•−]ss were 14.52 × 10−14 M and 20.00 × 10−14 M, respectively in the fluid turbulent force driven piezo-PMS activation process. Furthermore, a plausible degradation pathway of Black T dye was proposed based on the assessment of carbon number reduction, the mean oxidation number of organic carbon (MOC) and the predicted TOC/color index.
压电材料可在流体晃动过程中因流体湍流力而产生应变，从而可用于活化过一硫酸盐（PMS）。在本研究中，利用少偶数层 MoS2 纳米片和水碳（HC）纳米复合材料作为压电材料的有效界面相互作用，将其用于流体力学能量驱动的压电催化 PMS 激活过程（压电-PMS 激活过程），以降解 Eriochrome Black T 染料。结果表明，MoS2@HC-(6.5:3.5)/PMS/振荡体系能在 15 分钟内高效降解黑 T 染料，降解效率为 99.23%，伪一阶速率常数为 3.10 min-1。为了清楚地了解水力梯度（G）值的影响，在不同的振荡频率下对 Black T 染料降解进行了流体力学能量驱动的压电-PMS 激活过程。结果表明，黑 T 染料降解的最佳 G 值为（14.106 s-1）。值得注意的是，MoS2@HC-(6.5:3.5)/ PMS/Shaking 系统产生了最低的 EE/O 值（34.05 kWhm-3 阶-1），从而节省了超过 127 倍的 HC 能耗和 9 倍的 MoS2 能耗。此外，MoS2@HC-(6.5:3.5) 的压电化学测量结果表明，这些优异性能主要来自于 MoS2 和 HC 的协同效应。MoS2@HC-(6.5:3.5)的电化学测量结果表明，这些优异的性能主要来自于 MoS2 和 HC 的协同效应，这导致了更强的压电响应和有效的压电电荷分离，进而提高了产生活性物种的效率。结合清道夫测试、傅立叶变换红外光谱和 zeta 电位分析，我们确定 -OH 和 SO4--在 Black T 染料降解中起主要作用，而 O2--和 1O2 起次要作用。在流体湍流力驱动的压电-PMS活化过程中，[-OH]ss 和 [SO4--]ss 的稳态浓度分别为 14.52 × 10-14 M 和 20.00 × 10-14 M。此外，根据碳数减少、有机碳平均氧化数（MOC）和预测的 TOC/ 颜色指数的评估，提出了黑 T 染料的合理降解途径。
{"title":"MoS2@Hydrochar nanocomposites with cost-effective fluid turbulent eddies induced piezoelectric catalytic peroxymonosulfate utilization efficiency for water polluted dye degradation","authors":"","doi":"10.1016/j.seppur.2024.129871","DOIUrl":"10.1016/j.seppur.2024.129871","url":null,"abstract":"<div><div>Piezoelectric materials can induce strain due to the fluid turbulent force produced during fluid shaking, which may be used to activate peroxymonosulfate (PMS). In this study, the effective interfacial interaction of few-odd-numbered layered MoS<sub>2</sub> nanosheets and hydrochar (HC) nanocomposites as the piezoelectric material was used in a hydrodynamics energy-driven piezoelectric catalytic PMS activation process (piezo-PMS activation process) for Eriochrome Black T dye degradation. The results showed that Black T dye was efficiently degraded with an efficiency of 99.23 % within 15 min and a pseudo-first-order rate constant of 3.10 min<sup>−1</sup> in the MoS<sub>2</sub>@HC-(6.5:3.5)/PMS/Shaking system. To clearly see the influence of hydraulic gradient (G) value, the hydrodynamics energy-driven piezo-PMS activation process for Black T dye degradation was performed at different shaking frequencies. The results indicated an optimal G value of (14.106 s<sup>−1</sup>) for Black T dye degradation. Notably, the MoS<sub>2</sub>@HC-(6.5:3.5)/ PMS/Shaking system produced the lowest EE/O value (34.05 kWhm<sup>−3</sup> order<sup>−1</sup>), resulting in energy savings over 127 times of HC and 9 times of MoS<sub>2</sub>. Furthermore, piezoelectrochemical measurements of MoS<sub>2</sub>@HC-(6.5:3.5) indicated that these superior performances primarily resulted from the synergistic effects of MoS<sub>2</sub> and HC. This led to a stronger piezoelectric response with effective piezo-generated charge separation, which in turn improved the efficiency of producing reactive species. Combining the scavenger test, FT-IR, and zeta potential analysis, we determined that •OH and SO<sub>4</sub><sup>•−</sup> played a major role, while O<sub>2</sub>•− and <sup>1</sup>O<sub>2</sub> played a secondary role in Black T dye degradation. The steady-state concentrations of [•OH]<sub>ss</sub>, and [SO<sub>4</sub><sup>•−</sup>]<sub>ss</sub> were 14.52 × 10<sup>−14</sup> M and 20.00 × 10<sup>−14</sup> M, respectively in the fluid turbulent force driven piezo-PMS activation process. Furthermore, a plausible degradation pathway of Black T dye was proposed based on the assessment of carbon number reduction, the mean oxidation number of organic carbon (MOC) and the predicted TOC/color index.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":null,"pages":null},"PeriodicalIF":8.1,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142358722","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-26DOI: 10.1016/j.seppur.2024.129861
Greywater (GW) treatment is recognized as a more efficient alternative to blackwater treatment, particularly for reuse applications, due to its lower pathogen content and higher concentrations of chemical oxygen demand (COD) and surfactants. In this study, the adsorption performance of woodchip biochar (BC) and activated carbon (AC) was compared for the removal of COD, anionic surfactants (ASU), and non-ionic surfactants (NISU) from GW. Response Surface Methodology (RSM) was employed to optimize the removal efficiency of both organic matter and surfactants. AC demonstrated higher adsorption capacities for COD and ASU, with KL = 0.007 L/mg and Qmax = 0.95 mg/g for COD, and KL = 1.4 × 104 L/mg and Qmax = 0.08 mg/g for ASU. In contrast, BC showed a significantly higher affinity for NISU, with KL = 8.4 × 103 L/mg and Qmax = 0.01 mg/g. Breakthrough curves and pseudo-first-order (PFO) kinetics provided insights into adsorption dynamics, with AC showing delayed breakthrough and greater longevity, while BC offered rapid adsorption and cost-effectiveness. The treated GW achieved substantial reductions in contaminant levels, with final COD and surfactant concentrations reduced to approximately 10 mg/L and 0.05 mg/L, respectively, meeting Italian and Australian regulatory standards. The study highlights the potential of woodchip BC as a cost-effective and sustainable alternative to AC, particularly for short-term adsorption applications, and offers valuable insights into the treatment of GW for reuse.
{"title":"Comparative study of greywater treatment using activated carbon and woodchip biochar for surfactant and organic matter removal","authors":"","doi":"10.1016/j.seppur.2024.129861","DOIUrl":"10.1016/j.seppur.2024.129861","url":null,"abstract":"<div><div>Greywater (GW) treatment is recognized as a more efficient alternative to blackwater treatment, particularly for reuse applications, due to its lower pathogen content and higher concentrations of chemical oxygen demand (COD) and surfactants. In this study, the adsorption performance of woodchip biochar (BC) and activated carbon (AC) was compared for the removal of COD, anionic surfactants (ASU), and non-ionic surfactants (NISU) from GW. Response Surface Methodology (RSM) was employed to optimize the removal efficiency of both organic matter and surfactants. AC demonstrated higher adsorption capacities for COD and ASU, with K<sub>L</sub> = 0.007 L/mg and Qmax = 0.95 mg/g for COD, and K<sub>L</sub> = 1.4 × 10<sup>4</sup> L/mg and Qmax = 0.08 mg/g for ASU. In contrast, BC showed a significantly higher affinity for NISU, with K<sub>L</sub> = 8.4 × 10<sup>3</sup> L/mg and Qmax = 0.01 mg/g. Breakthrough curves and pseudo-first-order (PFO) kinetics provided insights into adsorption dynamics, with AC showing delayed breakthrough and greater longevity, while BC offered rapid adsorption and cost-effectiveness. The treated GW achieved substantial reductions in contaminant levels, with final COD and surfactant concentrations reduced to approximately 10 mg/L and 0.05 mg/L, respectively, meeting Italian and Australian regulatory standards. The study highlights the potential of woodchip BC as a cost-effective and sustainable alternative to AC, particularly for short-term adsorption applications, and offers valuable insights into the treatment of GW for reuse.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":null,"pages":null},"PeriodicalIF":8.1,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142358663","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-26DOI: 10.1016/j.seppur.2024.129831
An effective strategy to enhance the photocatalytic hydrogen evolution activity is to rationally guide the photogenerated carrier migration. In this work, a novel carbon-based material CuS/Graphdiyne (CuS-GDY), was synthesized via a Cu-surface mediated method. Subsequently, the peanut-shaped LaCoO3 is distributed uniformly on the surface of the layered CuS-GDY via electrostatic self-assembly, forming stepped heterojunctions that accelerate the transfer of photogenerated carriers. The modified CuS-GDY facilitated further optimization of the electrical conductivity and electron transfer capabilities of GDY. Furthermore, the formation of a Schottky junction between CuS and LaCoO3 facilitates electron egress from the conduction band of LaCoO3, thereby enriching the catalyst with active sites. The combined effect of the S-scheme and Schottky junctions within the composite catalysts facilitates the separation and transfer of photogenerated carriers, as evidenced by in situ XPS, DFT theoretical calculations, and complementary characterization techniques. This study presents novel insights into the modification of GDY and a deeper comprehension of the heterojunction dynamics in catalyst systems.
提高光催化氢气进化活性的有效策略是合理引导光生载流子迁移。本研究通过铜表面介导法合成了一种新型碳基材料 CuS/Graphdiyne（CuS-GDY）。随后，花生状的 LaCoO3 通过静电自组装均匀分布在层状 CuS-GDY 表面，形成阶梯状异质结，加速了光生载流子的转移。改性后的 CuS-GDY 有助于进一步优化 GDY 的导电性和电子转移能力。此外，CuS 和 LaCoO3 之间形成的肖特基结有利于电子从 LaCoO3 的传导带流出，从而使催化剂的活性位点更加丰富。复合催化剂中的 S 型和肖特基结的共同作用促进了光生载流子的分离和转移，原位 XPS、DFT 理论计算和补充表征技术都证明了这一点。这项研究提出了有关 GDY 改性的新见解，并加深了对催化剂系统中异质结动力学的理解。
{"title":"Graphdiyne surface-modified CuS-GDY/LaCoO3 S-scheme heterojunctions for enhanced photocatalytic hydrogen evolution","authors":"","doi":"10.1016/j.seppur.2024.129831","DOIUrl":"10.1016/j.seppur.2024.129831","url":null,"abstract":"<div><div>An effective strategy to enhance the photocatalytic hydrogen evolution activity is to rationally guide the photogenerated carrier migration. In this work, a novel carbon-based material CuS/Graphdiyne (CuS-GDY), was synthesized via a Cu-surface mediated method. Subsequently, the peanut-shaped LaCoO<sub>3</sub> is distributed uniformly on the surface of the layered CuS-GDY via electrostatic self-assembly, forming stepped heterojunctions that accelerate the transfer of photogenerated carriers. The modified CuS-GDY facilitated further optimization of the electrical conductivity and electron transfer capabilities of GDY. Furthermore, the formation of a Schottky junction between CuS and LaCoO<sub>3</sub> facilitates electron egress from the conduction band of LaCoO<sub>3</sub>, thereby enriching the catalyst with active sites. The combined effect of the S-scheme and Schottky junctions within the composite catalysts facilitates the separation and transfer of photogenerated carriers, as evidenced by in situ XPS, DFT theoretical calculations, and complementary characterization techniques. This study presents novel insights into the modification of GDY and a deeper comprehension of the heterojunction dynamics in catalyst systems.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":null,"pages":null},"PeriodicalIF":8.1,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142358721","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-26DOI: 10.1016/j.seppur.2024.129775
Oxygen reduction reaction (ORR), as an important reaction carried out on the cathode of direct methanol fuel cells (DMFC), directly affects the performance of the cell. Previous experimental studies have shown that there are some interactions between the defect structure and N doping to promote the ORR performance of the catalysts. In this work, the binder was first utilized to reduce the lignin content in the cotton straw (CS) system, thereby increasing the defective structure of the carbon substrate. Here, we obtained 5C-NP-Fe catalysts by increasing the defectivity of the carbon substrate through binder. The coordination environment surrounding the Fe-N4 sites is optimized by the synergistic action of the N and P atoms and the faulty structure, as shown by DFT theoretical calculations. In alkaline medium, half-wave potentials as high as 0.88 V in the three-electrode system and a peak power density of 10.8 mW cm−2 in a direct methanol fuel cell at 60℃. Compared to a 20 wt% commercial Pt/C catalyst (0.84 V, 7.5 mW cm−2), 5C-NP-Fe showed good ORR activity. The binder modification strategy provides a simple and green approach to the structural optimization of biomass-based catalysts.
{"title":"Biomass carbon with defective structures as effective ORR catalyst for DMFC","authors":"","doi":"10.1016/j.seppur.2024.129775","DOIUrl":"10.1016/j.seppur.2024.129775","url":null,"abstract":"<div><div>Oxygen reduction reaction (ORR), as an important reaction carried out on the cathode of direct methanol fuel cells (DMFC), directly affects the performance of the cell. Previous experimental studies have shown that there are some interactions between the defect structure and N doping to promote the ORR performance of the catalysts. In this work, the binder was first utilized to reduce the lignin content in the cotton straw (CS) system, thereby increasing the defective structure of the carbon substrate. Here, we obtained 5C-NP-Fe catalysts by increasing the defectivity of the carbon substrate through binder. The coordination environment surrounding the Fe-N<sub>4</sub> sites is optimized by the synergistic action of the N and P atoms and the faulty structure, as shown by DFT theoretical calculations. In alkaline medium, half-wave potentials as high as 0.88 V in the three-electrode system and a peak power density of 10.8 mW cm<sup>−2</sup> in a direct methanol fuel cell at 60℃. Compared to a 20 wt% commercial Pt/C catalyst (0.84 V, 7.5 mW cm<sup>−2</sup>), 5C-NP-Fe showed good ORR activity. The binder modification strategy provides a simple and green approach to the structural optimization of biomass-based catalysts.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":null,"pages":null},"PeriodicalIF":8.1,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142358863","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
扫码关注我们
求助内容：
应助结果提醒方式：
京公网安备 11010802042870号