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Removal and recovery of fluoride from wastewater via mixed calcium salts by fluidized bed induced crystallization technology
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-23 DOI: 10.1016/j.seppur.2025.131773
Zhipeng Gao, Yuming Tian, Jianglei Xiong, Hong Yu, Qiuhong Xiang, Jigang Shen, Cheng Liu
To overcome the disadvantages of high sludge production and the inability to collect calcium fluoride caused by chemical precipitation for defluoridation, the performance of fluidized bed induced crystallization (FBC) with fluorite particles as crystal seeds was investigated for the removal and resource recovery of fluoride (F-) from wastewater. The effects of parametric factors were explored, and the optimal operating conditions were: [Ca2+]:[F-] molar ratio of 0.5, fluoride load of influent of 4 kg/(m2·h), up-flow velocity of 6.5 m/h and initial bed height of 0.6 m. The pilot-scale experiment showed that the mixed calcium salts scheme and the automated system could overcome the adverse impacts caused by influent pH fluctuations. Fluoride removal and recovery were achieved through the heterogeneous crystallization of Ca2+ and F- on the surface of seeds to form CaF2. XRD and EDX Mapping results confirmed that the main ingredient of the product was calcium fluoride (CaF2) with a purity of 89 %, which met the standard for ceramic grade fluorspar. SEM indicated that the crystal seeds transformed from fine lumpy powder to spherical particles. The fluidized bed induced crystallization technology recovered 55 % F- as fluorspar and reduced wastewater treatment costs by 3.0 ∼ 3.5 RMB/m3, making it a more environmentally friendly and more economical technique compared with chemical precipitation.
{"title":"Removal and recovery of fluoride from wastewater via mixed calcium salts by fluidized bed induced crystallization technology","authors":"Zhipeng Gao, Yuming Tian, Jianglei Xiong, Hong Yu, Qiuhong Xiang, Jigang Shen, Cheng Liu","doi":"10.1016/j.seppur.2025.131773","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131773","url":null,"abstract":"To overcome the disadvantages of high sludge production and the inability to collect calcium fluoride caused by chemical precipitation for defluoridation, the performance of fluidized bed induced crystallization (FBC) with fluorite particles as crystal seeds was investigated for the removal and resource recovery of fluoride (F<sup>-</sup>) from wastewater. The effects of parametric factors were explored, and the optimal operating conditions were: [Ca<sup>2+</sup>]:[F<sup>-</sup>] molar ratio of 0.5, fluoride load of influent of 4 kg/(m<sup>2</sup>·h), up-flow velocity of 6.5 m/h and initial bed height of 0.6 m. The pilot-scale experiment showed that the mixed calcium salts scheme and the automated system could overcome the adverse impacts caused by influent pH fluctuations. Fluoride removal and recovery were achieved through the heterogeneous crystallization of Ca<sup>2+</sup> and F<sup>-</sup> on the surface of seeds to form CaF<sub>2</sub>. XRD and EDX Mapping results confirmed that the main ingredient of the product was calcium fluoride (CaF<sub>2</sub>) with a purity of 89 %, which met the standard for ceramic grade fluorspar. SEM indicated that the crystal seeds transformed from fine lumpy powder to spherical particles. The fluidized bed induced crystallization technology recovered 55 % F<sup>-</sup> as fluorspar and reduced wastewater treatment costs by 3.0 ∼ 3.5 RMB/m<sup>3</sup>, making it a more environmentally friendly and more economical technique compared with chemical precipitation.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"74 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143026487","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}
引用次数: 0
Multi-pathway and multiple-mechanism in action together: High-efficient visible-light photocatalytic oxidation and hydrolysis of CEES by a ligand-differentiated Zr-MOF
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-23 DOI: 10.1016/j.seppur.2025.131794
Xin Hu, Ying Yang, Nan Li, Chengcheng Huang, Yunshan Zhou, Lijuan Zhang, Yuxu Zhong, Pingjing Wang, Yunfan Cheng
It is always important to develop materials that are capable of fast catalytically degrading sulfur mustard (HD) by selective oxidation and/or hydrolysis to its nontoxic form. In this paper, ligand-defected UiO-66-NH2 is firstly prepared using acetic acid as a coordinating modifier, and then 5,10,15,20-tetrakis(4-carboxyphenyl)porphyrin molecules are introduced by coordination and amidation reactions to form a new ligand-differentiated MOF UiO-66-NH-AA −TCPP. The new MOF achieves round-the-clock degradation of 2-chloroethyl ethyl sulfide (CEES, HD simulant) by visible-light photocatalytic oxidation and hydrolysis. Notably, the MOF degrades 97.8 % of CEES within 1 h with a half-life of 9.12 min via the cooperation of oxidation and hydrolysis. It is demonstrated that while TCPP increases the number of photoexcited electrons by enhancing visible-light absorption, the electron push–pull effect between –NH2 and –COOH groups of TCPP through the coordination reaction facilitates electron transfer along the ligand–metal cluster–ligand direction, which improves photocatalytic yield of 1O2 for selective oxidation of CEES to sulfoxide. Meanwhile, the MOF shows a stronger ability to hydrolyze CEES than UiO-66-NH2 due to the lipophilicity of porphyrin increasing the contact with CEES. Noteworthily, it is concluded that the MOF achieves efficient decontamination of CEES through a multi-pathway and multi-mechanism co-action strategy.
{"title":"Multi-pathway and multiple-mechanism in action together: High-efficient visible-light photocatalytic oxidation and hydrolysis of CEES by a ligand-differentiated Zr-MOF","authors":"Xin Hu, Ying Yang, Nan Li, Chengcheng Huang, Yunshan Zhou, Lijuan Zhang, Yuxu Zhong, Pingjing Wang, Yunfan Cheng","doi":"10.1016/j.seppur.2025.131794","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131794","url":null,"abstract":"It is always important to develop materials that are capable of fast catalytically degrading sulfur mustard (HD) by selective oxidation and/or hydrolysis to its nontoxic form. In this paper, ligand-defected UiO-66-NH<sub>2</sub> is firstly prepared using acetic acid as a coordinating modifier, and then 5,10,15,20-tetrakis(4-carboxyphenyl)porphyrin molecules are introduced by coordination and amidation reactions to form a new ligand-differentiated MOF UiO-66-NH-AA −TCPP. The new MOF achieves round-the-clock degradation of 2-chloroethyl ethyl sulfide (CEES, HD simulant) by visible-light photocatalytic oxidation and hydrolysis. Notably, the MOF degrades 97.8 % of CEES within 1 h with a half-life of 9.12 min via the cooperation of oxidation and hydrolysis. It is demonstrated that while TCPP increases the number of photoexcited electrons by enhancing visible-light absorption, the electron push–pull effect between –NH<sub>2</sub> and –COOH groups of TCPP through the coordination reaction facilitates electron transfer along the ligand–metal cluster–ligand direction, which improves photocatalytic yield of <sup>1</sup>O<sub>2</sub> for selective oxidation of CEES to sulfoxide. Meanwhile, the MOF shows a stronger ability to hydrolyze CEES than UiO-66-NH<sub>2</sub> due to the lipophilicity of porphyrin increasing the contact with CEES. Noteworthily, it is concluded that the MOF achieves efficient decontamination of CEES through a multi-pathway and multi-mechanism co-action strategy.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"2 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143026491","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}
引用次数: 0
Resorcin[4]arene-derived hierarchical porous organic polymer modulated polyamide TFC membrane for effective ion separation
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-23 DOI: 10.1016/j.seppur.2025.131599
Meng You, Qianlong Sun, Bingbing Yuan, Chao Xia, Jianqiang Meng
Fine-customized structure and morphology of the thin-film-composite polyamide membranes (TFC-PA) play an essential role in obtaining high water permeance and solute–solute selectivity. Herein we fabricated a TFC-PA nanofiltration membrane with excellent separation performance by the regulation of the interfacial polymerization process via a resorcin[4]arene-derived hierarchical POPs intermediate layer (RA-POPs). The RA-POPs interlayer was constructed on the PSF substrate surface through in situ covalent assembly by the azo-coupling reaction, followed by the formation of the PA layer on top of this porous layer. The effect of azo-coupling reaction conditions on the morphologies and performance of the prepared TFC-PA-POPs membranes was investigated. The constructed RA-POPs layer interlayer increased the hydrophilicity of the substrates. This hydrophilic RA-POPs interlayer facilitated the uniform distribution of the amine solution and slowed down the PIP diffusion into the organic phase by the supramolecular interactions. Consequently, the formed PA layer exhibited a thinner thickness, a high degree of crosslinking, a crumpled structure and an enhanced negatively charged surface. The obtained TFC-PA-POPs membranes possessed high water permeance of 21.0 L m−2 h−1 bar−1, comparable Na2SO4 rejection of 99.35 % and excellent mixed ion selectivity (Cl/SO42−) of 340 in the high salt concentration, which is superior to the commercial and the state-of-the-art polyamide-based NF membranes. The reduced pore size, narrowed pore size distribution and enhanced surface negative charge endowed the TFC-PA-POPs membranes with high mono/multivalent anions selectivity. Our approach for modulating the polyamide microstructure by incorporating macrocycle-derived hierarchical porous organic polymer interlayer has provided insight into the design of TFC-PA NF membranes with high water permeance and precise ion separation for high-salinity wastewater treatment and water purification.
{"title":"Resorcin[4]arene-derived hierarchical porous organic polymer modulated polyamide TFC membrane for effective ion separation","authors":"Meng You, Qianlong Sun, Bingbing Yuan, Chao Xia, Jianqiang Meng","doi":"10.1016/j.seppur.2025.131599","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131599","url":null,"abstract":"Fine-customized structure and morphology of the thin-film-composite polyamide membranes (TFC-PA) play an essential role in obtaining high water permeance and solute–solute selectivity. Herein we fabricated a TFC-PA nanofiltration membrane with excellent separation performance by the regulation of the<!-- --> <!-- -->interfacial polymerization process via a resorcin[4]arene-derived hierarchical POPs intermediate layer (RA-POPs). The RA-POPs interlayer was constructed on the PSF substrate surface through in situ covalent assembly by the azo-coupling reaction, followed by the formation of the PA layer on top of this porous layer. The effect of azo-coupling reaction conditions on the morphologies and performance of the prepared TFC-PA-POPs membranes was investigated. The constructed RA-POPs layer interlayer increased the hydrophilicity of the substrates. This hydrophilic RA-POPs interlayer facilitated the uniform distribution of the amine solution and slowed down the PIP diffusion into the organic phase by the supramolecular interactions. Consequently, the formed PA layer exhibited a thinner thickness, a high degree of crosslinking, a crumpled structure and an enhanced negatively charged surface. The obtained TFC-PA-POPs membranes possessed high water permeance of 21.0 L m<sup>−2</sup> h<sup>−1</sup> bar<sup>−1</sup>, comparable Na<sub>2</sub>SO<sub>4</sub> rejection of 99.35 % and excellent mixed ion selectivity (Cl<sup>−</sup>/SO<sub>4</sub><sup>2−</sup>) of 340 in the high salt concentration, which is superior to the commercial and the state-of-the-art polyamide-based NF membranes. The reduced pore size, narrowed pore size distribution and enhanced surface negative charge endowed the TFC-PA-POPs membranes with high mono/multivalent anions selectivity. Our approach for modulating the polyamide microstructure by incorporating macrocycle-derived hierarchical porous organic polymer interlayer has provided insight into the design of TFC-PA NF membranes with high water permeance and precise ion separation for high-salinity wastewater treatment and water purification.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"38 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143026493","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}
引用次数: 0
Scalable sewing textiles with optimized electrothermal utilization for efficient all-day desalination 可伸缩的缝纫纺织品与优化的电热利用,高效的全天脱盐
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-23 DOI: 10.1016/j.seppur.2025.131782
Wei Li, Bin Chen, Haipeng Ren, Shichang Yang, Ruicheng Zhang, Duo Xu, Keshuai Liu, Can Ge, Hao Yu
Solar steam generation (SSG) has been considered a promising technology to address the worldwide water crisis through desalination and condensation. However, the strong dependence on solar radiation leads to evaporation instability and discontinuity in evaporation rates. Hence, it is critical to develop sustainable electrothermal coupled solar steam generation (ESSG) systems and improve energy conversion efficiencies. Herein, a scalable sewing photo-electro-thermal textile (SPET) is customized to enhance energy utilization efficiency during each step of the electrothermal conversion process. Specifically, the moderate voltage input is manipulated to match evaporation energy requirements. Sewing patterns are modified to improve electrothermal conversion efficiency and thermal distribution uniformity. Hence, an outstanding ESSG rate of 2.43 kg m−2·h−1 is realized under 2 V DC input and 1 sun radiation. The daily condensate mass reaches about 19.8 L·m−2 during 30 days of desalination (continuous operation for 24 h per day) without salt accumulation or galvanic corrosion. Overall, SPET with rational electrothermal conversion, thermal distribution, and evaporation utilization efficiencies demonstrate continuous, durable, and efficient ESSG.
太阳能蒸汽发电(SSG)被认为是一种很有前途的技术,通过淡化和冷凝来解决世界范围内的水危机。然而,对太阳辐射的强烈依赖导致蒸发不稳定和蒸发速率的不连续性。因此,开发可持续的电热耦合太阳能蒸汽发电(ESSG)系统,提高能量转换效率至关重要。在此,定制了一种可伸缩的缝纫光电热电纺织品(SPET),以提高电热转换过程中每个步骤的能源利用效率。具体来说,中压输入被操纵以匹配蒸发能量需求。修改缝纫图案以提高电热转换效率和热分布均匀性。因此,在2 V直流输入和1太阳辐射下,实现了2.43 kg m−2·h−1的出色ESSG速率。脱盐30 天(每天连续运行24 h),无积盐和电偶腐蚀,日凝结水质量约19.8 L·m−2。总体而言,具有合理电热转换、热分布和蒸发利用效率的SPET表现出连续、持久和高效的ESSG。
{"title":"Scalable sewing textiles with optimized electrothermal utilization for efficient all-day desalination","authors":"Wei Li, Bin Chen, Haipeng Ren, Shichang Yang, Ruicheng Zhang, Duo Xu, Keshuai Liu, Can Ge, Hao Yu","doi":"10.1016/j.seppur.2025.131782","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131782","url":null,"abstract":"Solar steam generation (SSG) has been considered a promising technology to address the worldwide water crisis through desalination and condensation. However, the strong dependence on solar radiation leads to evaporation instability and discontinuity in evaporation rates. Hence, it is critical to develop sustainable electrothermal coupled solar steam generation (ESSG) systems and improve energy conversion efficiencies. Herein, a scalable sewing photo-electro-thermal textile (SPET) is customized to enhance energy utilization efficiency during each step of the electrothermal conversion process. Specifically, the moderate voltage input is manipulated to match evaporation energy requirements. Sewing patterns are modified to improve electrothermal conversion efficiency and thermal distribution uniformity. Hence, an outstanding ESSG rate of 2.43 kg m<sup>−2</sup>·h<sup>−1</sup> is realized under 2 V DC input and 1 sun radiation. The daily condensate mass reaches about 19.8 L·m<sup>−2</sup> during 30 days of desalination (continuous operation for 24 h per day) without salt accumulation or galvanic corrosion. Overall, SPET with rational electrothermal conversion, thermal distribution, and evaporation utilization efficiencies demonstrate continuous, durable, and efficient ESSG.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"17 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143020896","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}
引用次数: 0
Advances and challenges in recycling spent LiFePO4 batteries
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-23 DOI: 10.1016/j.seppur.2025.131780
Biyun Luo, Bing Xu, Qunxuan Yan, Yujiuan Zhou, Zhongling Dong, Xujiao Huang, Zixiang Zhao
The intensive growth and finite lifespan of electric vehicle have brought about the concomitantly exponential generation of scrapped lithium-ion batteries (LIB). Lithium iron phosphate (LFP) batteries account for a large proportion of spent LIB. However, their actual recycling volume is relatively low due to the limited economic value of recycling. With the increasing environmental and economic benefits of recycling spent LIB, the recovery of spent lithium iron phosphate (sLFP) batteries is becoming a hot research field, with a variety of innovative green recycling technologies emerging.This review described the leaching mechanism of LIB, and evaluated the advantages and limitations of various recycling technologies for sLFP batteries (Pyrometallurgy, Hydrometallurgy, Direct regeneration, Electrochemical technology). In addition, the recycling method, challenges, and developing tendency of battery recycling are put presented and analyzed.
{"title":"Advances and challenges in recycling spent LiFePO4 batteries","authors":"Biyun Luo, Bing Xu, Qunxuan Yan, Yujiuan Zhou, Zhongling Dong, Xujiao Huang, Zixiang Zhao","doi":"10.1016/j.seppur.2025.131780","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131780","url":null,"abstract":"The intensive growth and finite lifespan of electric vehicle have brought about the concomitantly exponential generation of scrapped lithium-ion batteries (LIB). Lithium iron phosphate (LFP) batteries account for a large proportion of spent LIB. However, their actual recycling volume is relatively low due to the limited economic value of recycling. With the increasing environmental and economic benefits of recycling spent LIB, the recovery of spent lithium iron phosphate (sLFP) batteries is becoming a hot research field, with a variety of innovative green recycling technologies emerging.This review described the leaching mechanism of LIB, and evaluated the advantages and limitations of various recycling technologies for sLFP batteries (Pyrometallurgy, Hydrometallurgy, Direct regeneration, Electrochemical technology). In addition, the recycling method, challenges, and developing tendency of battery recycling are put presented and analyzed.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"138 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143026496","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}
引用次数: 0
Adsorption mechanism of SDBS collector in flotation separation of K2SO4/[Kx(NH4)(1-x)]2SO4 and NH4Cl generated via double decomposition
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-23 DOI: 10.1016/j.seppur.2025.131789
Yanyu Zheng, Haipeng Wu, Pan Wu, Changjun Liu, Jian He, Wei Jiang
Potassium sulfate (K2SO4) is an essential potassium fertilizer, and its production entailing the double decomposition reaction of KCl and (NH4)2SO4 is a crucial industrial process. However, the subsequent separation of K2SO4 and NH4Cl from the mixed products via crystallization necessitates high amounts of energy. In this study, flotation was introduced to achieve an efficient separation of K2SO4 and NH4Cl at a lower cost, and sodium dodecyl benzene sulfonate (SDBS) was used as the collector for K2SO4 flotation. After one flotation, the K2O yield reached 81.20 %; however, the K2O and Cl- contents of the obtained product were only 37.12 % and 10.18 %, respectively, which did not meet fertilizer product requirements. This resulted from the inevitable presence of the [Kx(NH4)(1-x)]2SO4 complex salt, produced in the economically acceptable concentration range during the double decomposition reaction. Molecular dynamics (MD) simulations confirmed that the interaction between SDBS and the surfaces of K2SO4 and [Kx(NH4)(1-x)]2SO4 (x = 0.75) was stronger than that of their ion hydration layer, allowing it to be adsorbed onto their surfaces, whereas its adsorption onto the surface of NH4Cl was impeded, which enabled the flotation separation of K2SO4/[K0.75(NH4)0.25]2SO4 and NH4Cl. However, the adsorption of SDBS onto the surfaces of K2SO4 and [Kx(NH4)(1-x)]2SO4 occurred simultaneously without significant differences, which hindered their effective separation and resulted in a low K2O content in the product. Based on this mechanistic understanding, a secondary decomposition reaction-flotation process was introduced, enabling a final K2SO4 yield of 91.78 %, with an increased K2O content of 42.06 %–44.29 %, and reduced Cl- content of 2.97 %–4.05 %, meeting the requirements of compound fertilizer products.
{"title":"Adsorption mechanism of SDBS collector in flotation separation of K2SO4/[Kx(NH4)(1-x)]2SO4 and NH4Cl generated via double decomposition","authors":"Yanyu Zheng, Haipeng Wu, Pan Wu, Changjun Liu, Jian He, Wei Jiang","doi":"10.1016/j.seppur.2025.131789","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131789","url":null,"abstract":"Potassium sulfate (K<sub>2</sub>SO<sub>4</sub>) is an essential potassium fertilizer, and its production entailing the double decomposition reaction of KCl and (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub> is a crucial industrial process. However, the subsequent separation of K<sub>2</sub>SO<sub>4</sub> and NH<sub>4</sub>Cl from the mixed products via crystallization necessitates high amounts of energy. In this study, flotation was introduced to achieve an efficient separation of K<sub>2</sub>SO<sub>4</sub> and NH<sub>4</sub>Cl at a lower cost, and sodium dodecyl benzene sulfonate (SDBS) was used as the collector for K<sub>2</sub>SO<sub>4</sub> flotation. After one flotation, the K<sub>2</sub>O yield reached 81.20 %; however, the K<sub>2</sub>O and Cl<sup>-</sup> contents of the obtained product were only 37.12 % and 10.18 %, respectively, which did not meet fertilizer product requirements. This resulted from the inevitable presence of the [K<sub>x</sub>(NH<sub>4</sub>)<sub>(1-x)</sub>]<sub>2</sub>SO<sub>4</sub> complex salt, produced in the economically acceptable concentration range during the double decomposition reaction. Molecular dynamics (MD) simulations confirmed that the interaction between SDBS and the surfaces of K<sub>2</sub>SO<sub>4</sub> and [K<sub>x</sub>(NH<sub>4</sub>)<sub>(1-x)</sub>]<sub>2</sub>SO<sub>4</sub> (x = 0.75) was stronger than that of their ion hydration layer, allowing it to be adsorbed onto their surfaces, whereas its adsorption onto the surface of NH<sub>4</sub>Cl was impeded, which enabled the flotation separation of K<sub>2</sub>SO<sub>4</sub>/[K<sub>0.75</sub>(NH<sub>4</sub>)<sub>0.25</sub>]<sub>2</sub>SO<sub>4</sub> and NH<sub>4</sub>Cl. However, the adsorption of SDBS onto the surfaces of K<sub>2</sub>SO<sub>4</sub> and [K<sub>x</sub>(NH<sub>4</sub>)<sub>(1-x)</sub>]<sub>2</sub>SO<sub>4</sub> occurred simultaneously without significant differences, which hindered their effective separation and resulted in a low K<sub>2</sub>O content in the product. Based on this mechanistic understanding, a secondary decomposition reaction-flotation process was introduced, enabling a final K<sub>2</sub>SO<sub>4</sub> yield of 91.78 %, with an increased K<sub>2</sub>O content of 42.06 %–44.29 %, and reduced Cl<sup>-</sup> content of 2.97 %–4.05 %, meeting the requirements of compound fertilizer products.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"76 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143026494","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}
引用次数: 0
Bioinspired porous spindle-knotted sponge evaporator prepared with a chemically reactive ink coating for efficient solar desalination
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-23 DOI: 10.1016/j.seppur.2025.131781
Yiting Yao, Jiehao Du, Xue Yan, Bin Shang, Ruquan Zhang, Jingjing Huang, Shaojin Gu
The multi-scale structural design of solar evaporators was considered one of the methods to improve the photothermal performance by enhancing light absorption and optimizing the water transport pathways. Nonetheless, development of simple and effective technologies to regulate the structure of evaporators remain challenging. In this study, we developed a bioinspired robust porous spindle-knotted solar evaporator by directly spraying a layer of ink-containing polyethyleneimine-pentaerythritol pentaacrylate (BPEI-5Acl) reactive coating onto a hydrophilic melamine sponge (MS). Additionally, the reactive coating exhibits secondary reactive properties, enabling it to further react with octadecylamine (ODA) to effectively adjust the surface microstructure and wettability, forming a three-dimensional core–shell structure with hydrophilic interior and hydrophobic exterior. Benefiting from the porous spindle-knotted microstructure, the evaporator achieves a light absorption rate exceeding 93 %. Coupled with its inner hydrophilic and outer hydrophobic properties, the evaporator achieves an evaporation rate of 2.04 kg m-2h−1 and the conversion efficiency of 94.7 %. Furthermore, the reactive coating on the surface of the evaporator has robust adhesion with the ink, effectively achieving durability in desalination and removal of heavy metals and dyes during the evaporation process. This simple and effective reactive coating strategy provides a model for the large-scale production of solar evaporators.
{"title":"Bioinspired porous spindle-knotted sponge evaporator prepared with a chemically reactive ink coating for efficient solar desalination","authors":"Yiting Yao, Jiehao Du, Xue Yan, Bin Shang, Ruquan Zhang, Jingjing Huang, Shaojin Gu","doi":"10.1016/j.seppur.2025.131781","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131781","url":null,"abstract":"The multi-scale structural design of solar evaporators was considered one of the methods to improve the photothermal performance by enhancing light absorption and optimizing the water transport pathways. Nonetheless, development of simple and effective technologies to regulate the structure of evaporators remain challenging. In this study, we developed a bioinspired robust porous spindle-knotted solar evaporator by directly spraying a layer of ink-containing polyethyleneimine-pentaerythritol pentaacrylate (BPEI-5Acl) reactive coating onto a hydrophilic melamine sponge (MS). Additionally, the reactive coating exhibits secondary reactive properties, enabling it to further react with octadecylamine (ODA) to effectively adjust the surface microstructure and wettability, forming a three-dimensional core–shell structure with hydrophilic interior and hydrophobic exterior. Benefiting from the porous spindle-knotted microstructure, the evaporator achieves a light absorption rate exceeding 93 %. Coupled with its inner hydrophilic and outer hydrophobic properties, the evaporator achieves an evaporation rate of 2.04 kg m<sup>-2</sup>h<sup>−1</sup> and the conversion efficiency of 94.7 %. Furthermore, the reactive coating on the surface of the evaporator has robust adhesion with the ink, effectively achieving durability in desalination and removal of heavy metals and dyes during the evaporation process. This simple and effective reactive coating strategy provides a model for the large-scale production of solar evaporators.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"18 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143026498","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}
引用次数: 0
High-graphitization carbon layers coated with Fe − N − C sites for efficient and robust catalytic CO2 decomposition of amine-solvent 高石墨化碳层涂有铁 − N − C位点,用于高效和稳健的催化CO2分解胺溶剂
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-23 DOI: 10.1016/j.seppur.2025.131785
Xing Li, Lei Xing, Chunyu Zhang, Shudan He, Fanghua Liu, Zhen Chen, Huazhen Chang, Junhua Li
Catalytic solvent regeneration is widely considered a promising solution for addressing the intensive heat duty of amine-based carbon dioxide (CO2) capture. This highly challenging application has motivated researchers to develop excellent catalysts with high activity and durability. In this study, we engineered active and durable Fe − N − C catalyst coated with high-graphitization carbon layers (labeled Phen − Fe − N − C) through a secondary thermal pyrolysis treatment. The multiple graphite layers and atomic metal sties were verified by experimental characterization and coordination structure analysis. The improved graphite layers further enhanced the activity of Fe − N − C sites, providing more acid sites for proton-electron transfer and C − N breaking during solvent regeneration (or CO2 desorption). Thus, the maximal CO2 desorption rate increased by 50 % when Fe − N − C was used compared with that of the blank case, and the rate further increased by 27 % when Phen − Fe − N − C was used. After 15 days of hydrothermal testing, the single Fe atom over the spent catalysts presented no significant aggregation or dissolution in the solvent, validating the durability of Phen − Fe − N − C. This work demonstrates a feasible and novel strategy to improve M − N − C materials for efficient and robust CO2 desorption from amine solvents toward energy-saving CO2 capture.
催化溶剂再生被广泛认为是解决胺基二氧化碳(CO2)捕获的高热负荷的有前途的解决方案。这种极具挑战性的应用促使研究人员开发出具有高活性和耐用性的优异催化剂。在这项研究中,我们设计积极和持久的Fe − N − C催化剂涂层high-graphitization碳层(标记为苯酚的 − Fe − N − C)通过二次热裂解处理。通过实验表征和配位结构分析验证了多层石墨层和原子金属层。改进后的石墨层进一步增强了Fe − N − C位的活性,在溶剂再生(或CO2解吸)过程中为质子电子转移和C − N断裂提供了更多的酸位。因此,最大二氧化碳解吸率增加了50 %当菲 − N − C使用空白的情况下,价格相比,进一步增加了27 %时苯酚的 − Fe − N − C使用。经过15 天的水热测试,废催化剂上的单个Fe原子在溶剂中没有明显的聚集或溶解,验证了Phen − Fe − N − C的耐久性。这项工作证明了一种可行和新颖的策略,可以改善M - N - C材料,使其从胺溶剂中高效和稳健地解吸二氧化碳,从而实现节能的二氧化碳捕获。
{"title":"High-graphitization carbon layers coated with Fe − N − C sites for efficient and robust catalytic CO2 decomposition of amine-solvent","authors":"Xing Li, Lei Xing, Chunyu Zhang, Shudan He, Fanghua Liu, Zhen Chen, Huazhen Chang, Junhua Li","doi":"10.1016/j.seppur.2025.131785","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131785","url":null,"abstract":"Catalytic solvent regeneration is widely considered a promising solution for addressing the intensive heat duty of amine-based carbon dioxide (CO<sub>2</sub>) capture. This highly challenging application has motivated researchers to develop excellent catalysts with high activity and durability. In this study, we engineered active and durable Fe − N − C catalyst coated with high-graphitization carbon layers (labeled Phen − Fe − N − C) through a secondary thermal pyrolysis treatment. The multiple graphite layers and atomic metal sties were verified by experimental characterization and coordination structure analysis. The improved graphite layers further enhanced the activity of Fe − N − C sites, providing more acid sites for proton-electron transfer and C − N breaking during solvent regeneration (or CO<sub>2</sub> desorption). Thus, the maximal CO<sub>2</sub> desorption rate increased by 50 % when Fe − N − C was used compared with that of the blank case, and the rate further increased by 27 % when Phen − Fe − N − C was used. After 15 days of hydrothermal testing, the single Fe atom over the spent catalysts presented no significant aggregation or dissolution in the solvent, validating the durability of Phen − Fe − N − C. This work demonstrates a feasible and novel strategy to improve M − N − C materials for efficient and robust CO<sub>2</sub> desorption from amine solvents toward energy-saving CO<sub>2</sub> capture.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"104 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143020878","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}
引用次数: 0
Parametric analysis and prototype development of smog-free tower for sustainable urban environment
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-23 DOI: 10.1016/j.seppur.2025.131776
Muhammad Hamza, Sana Yaqub, Majid Ali, Mustafa Anwar, Awais Bokhari, Muhammad Murtaza, Abeera Ayaz Ansari, Qazi Shahzad Ali
Urban expansion contributes to smog formation by emitting particulate matter (PM) into the atmosphere, threatening overall well-being. Wet scrubbers and spray towers have been employed to mitigate smog through water-based adsorption. The existing technologies face sustainability challenges such as significant water consumption and long-term environmental impact. To combat this issue, an environmentally friendly smog-free tower (SFT) is manufactured. The SFT is constructed from galvanized iron sheets with a height and diameter of 1067 and 381 mm, respectively. SFT uses PM2.5 filters (PMF) made up of activated carbon, polyester fiber, and polypropylene fiber to capture PM from self-generated smog (SGS) produced by coal and cooking oil. In this study, three factors; contact time, contact diameter of filter, and position of filter tray in the SFT are evaluated to examine the performance of SFT. Results revealed that PM2.5 and PM10 pollutants are effectively captured when the contact time is 50 min with removal efficiency of 97.8 % and 98.4 % respectively by a filter having 381 mm diameter. In the case of the filter tray’s position in the SFT, the removal efficiency at the first position exceeded the third position which in turn exceeded the second position. Removal efficiency is dropped at the second position of SFT because of resistance to flow for SGS due to the increased distance of the filter from the bottom suction fan and the inlet compressor. SFT stands as an indicator of cleaner city life, effectively cleansing an area of 113 m2 with an energy consumption of 48.3 kW.h.
{"title":"Parametric analysis and prototype development of smog-free tower for sustainable urban environment","authors":"Muhammad Hamza, Sana Yaqub, Majid Ali, Mustafa Anwar, Awais Bokhari, Muhammad Murtaza, Abeera Ayaz Ansari, Qazi Shahzad Ali","doi":"10.1016/j.seppur.2025.131776","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131776","url":null,"abstract":"Urban expansion contributes to smog formation by emitting particulate matter (PM) into the atmosphere, threatening overall well-being. Wet scrubbers and spray towers have been employed to mitigate smog through water-based adsorption. The existing technologies face sustainability challenges such as significant water consumption and long-term environmental impact. To combat this issue, an environmentally friendly smog-free tower (SFT) is manufactured. The SFT is constructed from galvanized iron sheets with a height and diameter of 1067 and 381 mm, respectively. SFT uses PM2.5 filters (PMF) made up of activated carbon, polyester fiber, and polypropylene fiber to capture PM from self-generated smog (SGS) produced by coal and cooking oil. In this study, three factors; contact time, contact diameter of filter, and position of filter tray in the SFT are evaluated to examine the performance of SFT. Results revealed that PM<sub>2.5</sub> and PM<sub>10</sub> pollutants are effectively captured when the contact time is 50 min with removal efficiency of 97.8 % and 98.4 % respectively by a filter having 381 mm diameter. In the case of the filter tray’s position in the SFT, the removal efficiency at the first position exceeded the third position which in turn exceeded the second position. Removal efficiency is dropped at the second position of SFT because of resistance to flow for SGS due to the increased distance of the filter from the bottom suction fan and the inlet compressor. SFT stands as an indicator of cleaner city life, effectively cleansing an area of 113 m<sup>2</sup> with an energy consumption of 48.3 kW.h.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"34 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143026492","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}
引用次数: 0
Pore structure-domoinated nonradical oxidation activity of self-dispersed Fe doped mesoporous-carbon for boosting antibiotics degradation efficiency 自分散铁掺杂介孔碳在提高抗生素降解效率方面的非自由基氧化活性
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-22 DOI: 10.1016/j.seppur.2025.131742
Yingjie Li, Jiajun Zou, Haoyang Huang, Jiawei Li, Haichuan Zhang, Ji Li
Electron transfer process (ETP) mediated nonradical oxidation pathway exhibits high efficiency/selectivity for removing trace organic pollutants in complex water matrices. Pore structure regulation strategy is feasible for achieving nonradical pathways, but the detail influence of various pore structures was rarely elucidated. Here, three types of Fe doped mesoporous-carbon catalysts (Fe@MNC) with different pore structures were precisely synthesized, including ordered linear mesopores (Fe@o-LMC), disordered spherical mesopores (Fe@d-SMC) and disordered dendritic mesopores (Fe@d-DMC). There was a significant difference in sulfamethoxazole (SMX) degradation performance among three Fe@MNC/peroxymonosulfate (PMS) catalytic systems, with the pseudo first-order reaction rate constants (kobs) followed by Fe@o-LMC (0.818 min−1) > Fe@d-SMC (0.394 min−1) > Fe@d-DMC (0.166 min−1). Importantly, ETP pathway was responsible for SMX degradation, and the electron transfer intensity was the intrinsic reason for the difference in catalytic performance. Subsequently, the pore structure-dominated SMX degradation efficiency was elucidated by analyzing SMX mass-transfer inner the Fe@MNC: the more favorable the pore structure was for reactants mass transfer, the more favorable it was for triggering ETP, thereby leading higher degradation efficiency. Finally, the enhanced ETP of Fe@o-LMC/PMS system also exhibited excellent reactivity for the degradation of other electron-rich antibiotics, as well as adaptability under various water quality and excellent stability. This work reveals the pore structure effect in Fenton-like reaction, and provides a new insight into the design of ETP mediated nonradical based porous catalysts for efficient antibiotic removal from wastewater.
电子转移过程(ETP)介导的非自由基氧化途径对复杂水基质中痕量有机污染物的去除具有较高的效率和选择性。孔隙结构调控策略对于实现非自由基途径是可行的,但各种孔隙结构的具体影响很少被阐明。本文精确合成了三种不同孔结构的Fe掺杂介孔碳催化剂(Fe@MNC),包括有序线性介孔(Fe@o-LMC)、无序球形介孔(Fe@d-SMC)和无序枝状介孔(Fe@d-DMC)。有显著差异的磺胺甲恶唑(SMX)降解性能之间的三个Fe@MNC / peroxymonosulfate (PMS)催化系统,与伪一级反应速率常数(水)其次是Fe@o-LMC(0.818 分钟−1) 祝辞 Fe@d-SMC(0.394 分钟−1) 祝辞 Fe@d-DMC(0.166 分钟−1)。重要的是,ETP途径负责SMX的降解,而电子转移强度是催化性能差异的内在原因。随后,通过分析Fe@MNC内部SMX的传质,阐明了孔隙结构主导的SMX降解效率:越有利于反应物传质的孔隙结构越有利于触发ETP,从而导致更高的降解效率。最后,Fe@o-LMC/PMS体系的增强ETP对其他富电子抗生素的降解也表现出优异的反应性,对各种水质的适应性和优异的稳定性。本研究揭示了类fenton反应的孔结构效应,为设计ETP介导的非自由基基多孔催化剂高效去除废水中的抗生素提供了新的思路。
{"title":"Pore structure-domoinated nonradical oxidation activity of self-dispersed Fe doped mesoporous-carbon for boosting antibiotics degradation efficiency","authors":"Yingjie Li, Jiajun Zou, Haoyang Huang, Jiawei Li, Haichuan Zhang, Ji Li","doi":"10.1016/j.seppur.2025.131742","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131742","url":null,"abstract":"Electron transfer process (ETP) mediated nonradical oxidation pathway exhibits high efficiency/selectivity for removing trace organic pollutants in complex water matrices. Pore structure regulation strategy is feasible for achieving nonradical pathways, but the detail influence of various pore structures was rarely elucidated. Here, three types of Fe doped mesoporous-carbon catalysts (Fe@MNC) with different pore structures were precisely synthesized, including ordered linear mesopores (Fe@<em>o</em>-LMC), disordered spherical mesopores (Fe@<em>d</em>-SMC) and disordered dendritic mesopores (Fe@<em>d</em>-DMC). There was a significant difference in sulfamethoxazole (SMX) degradation performance among three Fe@MNC/peroxymonosulfate (PMS) catalytic systems, with the pseudo first-order reaction rate constants (<em>k<sub>obs</sub></em>) followed by Fe@<em>o</em>-LMC (0.818 min<sup>−1</sup>) &gt; Fe@<em>d</em>-SMC (0.394 min<sup>−1</sup>) &gt; Fe@<em>d</em>-DMC (0.166 min<sup>−1</sup>). Importantly, ETP pathway was responsible for SMX degradation, and the electron transfer intensity was the intrinsic reason for the difference in catalytic performance. Subsequently, the pore structure-dominated SMX degradation efficiency was elucidated by analyzing SMX mass-transfer inner the Fe@MNC: the more favorable the pore structure was for reactants mass transfer, the more favorable it was for triggering ETP, thereby leading higher degradation efficiency. Finally, the enhanced ETP of Fe@<em>o</em>-LMC/PMS system also exhibited excellent reactivity for the degradation of other electron-rich antibiotics, as well as adaptability under various water quality and excellent stability. This work reveals the pore structure effect in Fenton-like reaction, and provides a new insight into the design of ETP mediated nonradical based porous catalysts for efficient antibiotic removal from wastewater.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"101 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142992212","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}
引用次数: 0
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Separation and Purification Technology
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