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Spatiotemporally optimized dual-stage electro-Fenton system with etched Fe⁰-Fe3O4/CF cathode for efficient sulfadiazine degradation 具有蚀刻Fe⁰-Fe3O4/CF阴极的时空优化双级电fenton系统,用于有效的磺胺嘧啶降解
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-23 DOI: 10.1016/j.seppur.2025.131756
Yanshi Zheng, Jinyan Yang, Mei Li, Jiayu Liang, Dehai Yu, Ziyao Wang, Xiao Shan, Gaofeng Pan, Jianchuan Pei
Sulfadiazine (SDZ), a potent antibiotic resistant to conventional biological treatment, presents considerable environmental risks if discharged untreated. Electro-Fenton (EF) is a promising technology in SDZ removal. However, oxygen reduction reaction (ORR) performance deterioration caused by iron deposition and the diverse optimal operating conditions for ORR and ferric reduction reaction (FRR) significantly affect the durability and the SDZ removal efficiency in EF system. In this study, a dual-stage spatiotemporal separation heterogeneous EF system was constructed, employing an air-breathing cathode (ABC) in the first stage and a Fe0-Fe3O4/CF cathode in the second stage, which effectively addresses the inherent limitations of EF systems by separating the ORR, H2O2 activation, and FRR spatiotemporally. A novel K2FeO4 etching method was employed to fabricate the Fe0-Fe3O4/CF cathode, ensuring uniformly dispersed active sites within pores. Under optimal operating conditions, the system achieved complete SDZ degradation in 10 min and 80.42 % total organic carbon (TOC) removal. High Fe(II) retention (55.12 %) on Fe0-Fe3O4/CF25 after reaction was observed due to effective FRR. Mechanism studies confirmed that ·OH generated from heterogeneous Fenton dominated SDZ degradation, with DFT analysis confirming electron transfer from SDZ to ·OH. The system demonstrated high durability and low energy consumption, maintaining the ability to completely degrade SDZ in 30 min after six uses, with an energy consumption of 8.48 kWh (kg SDZ)-1 and 0.26 kWh (g TOC)-1. These findings provide ideas for constructing EF systems with higher SDZ removal efficiency and durability.
磺胺嘧啶(SDZ)是一种对常规生物处理具有耐药性的强效抗生素,如果未经治疗就排放,会带来相当大的环境风险。电fenton (EF)是一种很有前途的SDZ去除技术。然而,铁沉积引起的氧还原反应(ORR)性能下降以及ORR和铁还原反应(FRR)的不同最佳操作条件显著影响了EF系统的耐久性和SDZ去除效率。本研究构建了一种双级时空分离异质EF系统,第一级采用吸气式阴极(ABC),第二级采用Fe0-Fe3O4/CF阴极,有效地解决了EF系统的固有局限性,实现了ORR、H2O2活化和FRR的时空分离。采用一种新颖的K2FeO4刻蚀方法制备Fe0-Fe3O4/CF阴极,保证了孔内活性位点的均匀分散。在最佳操作条件下,系统在10 min内实现了SDZ的完全降解,总有机碳(TOC)去除率为80.42 %。反应后Fe0-Fe3O4/CF25上Fe(II)保留率较高(55.12 %)。机理研究证实,非均相Fenton产生的·OH主导了SDZ的降解,DFT分析证实了SDZ向·OH的电子转移。该系统表现出高耐用性和低能耗,在6次使用后保持在30 min内完全降解SDZ的能力,能耗为8.48 kWh (kg SDZ)-1和0.26 kWh (g TOC)-1。这些发现为构建具有更高SDZ去除效率和耐久性的EF系统提供了思路。
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引用次数: 0
Series of halogen engineered well-mixed oxides derived from layered double hydroxides for highly efficient NH3-SCR catalysts: Improvement of the oxygen vacancies 从层状双氢氧化物衍生的卤素工程混合氧化物系列,用于高效NH3-SCR催化剂:改善氧空位
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-23 DOI: 10.1016/j.seppur.2025.131775
Yu Zhang, Rui Wang
Reinforcing the development of efficient catalysts is crucial for addressing the challenges associated with NOx removal technologies. Herein, we present a unique method for the in situ production of halogen-doped NiCoMoOx catalysts utilizing a crystallization-thermal decomposition mechanism and the use of such catalysts for the selective catalytic reduction of NOx with NH3 (NH3-SCR). The formation of lattice defect (oxygen vacancies) and surface acid sites on Br-doped NiCoMoOx catalyst was considerably enhanced compared with that on pure NiCoMoOx, resulting in highly efficient reduction of NOx and a broader temperature operating range. The 2Br-NiCoMoOx catalyst achieved the highest NOx conversion of 97.2 % at 250°C, while NiCoMoOx was only 83 %, and the NOx conversion was always above 80 % in a wide temperature window of 200 to 350 °C. Through comprehensive characterization, it was also revealed that the introduction of Br enhanced the low temperature redox performance and the adsorption and activation of NO and NH3 on the catalyst surface, which played a crucial role in facilitating the reaction between NO and NH3. Furthermore, we achieved broad temperature window NOx reduction by ingeniously utilizing a tandem catalyst system composed of V2O5-WO3/TiO2 and 2Br-NiCoMoOx, with the optimal mass ratio of the two phases being 1:3. This research presents novel design approaches that offer a new approach to the creation of high-performance SCR catalysts.
加强高效催化剂的开发对于解决与NOx去除技术相关的挑战至关重要。在此,我们提出了一种独特的方法,利用结晶-热分解机制原位生产卤素掺杂NiCoMoOx催化剂,并使用这种催化剂与NH3选择性催化还原NOx (NH3- scr)。与纯NiCoMoOx相比,br掺杂NiCoMoOx催化剂的晶格缺陷(氧空位)和表面酸位的形成明显增强,从而实现了NOx的高效还原和更宽的温度工作范围。在250℃时,2Br-NiCoMoOx催化剂的NOx转化率最高,达到97.2% %,而NiCoMoOx仅为83 %,在200 ~ 350 ℃的宽温度窗内,NOx转化率始终保持在80 %以上。通过综合表征,还发现Br的引入增强了催化剂的低温氧化还原性能以及NO和NH3在催化剂表面的吸附和活化,对促进NO和NH3的反应起着至关重要的作用。此外,我们巧妙地利用由V2O5-WO3/TiO2和2Br-NiCoMoOx组成的串联催化剂体系,实现了宽温度窗的NOx还原,两相的最佳质量比为1:3。本研究提出了新颖的设计方法,为创造高性能SCR催化剂提供了新的途径。
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引用次数: 0
Investigation of tribo-electrostatic separation mechanism for thermoplastics in e-waste based on functional group distribution and surface potential 基于官能团分布和表面电位的电子垃圾中热塑性塑料摩擦-静电分离机理研究
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-23 DOI: 10.1016/j.seppur.2025.131764
Xin He, Zhongxin Zhong, Yixuan Ouyang, Jianbo Wang
With the global dramatic increase in e-waste, recycling thermoplastics in e-waste through tribo-electrostatic separation has become essential. In this study, the internal and external functional group distribution of four typical thermoplastics including polyvinyl chloride (PVC), high impact polystyrene (HIPS), polypropylene (PP) and acrylonitrile–butadiene–styrene (ABS) were analyzed by Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS). A certain degree of oxidation, mainly exhibited as –OH, existed in all thermoplastics. For the first time, atomic force microscopy (AFM) was employed to assess surface potentials of thermoplastics, and their total electronegativity was calculated by integrating the content and electronegativity of various functional groups. The order of surface potential and total electronegativity in four thermoplastics is consistent: PVC (−4.08 V, 2.74) > HIPS (−8.36 V, 2.59) > PP (−9.18 V, 2.57) > ABS (−11.30 V, 2.56). Both content and electronegativity of functional groups in thermoplastics significantly influence surface potential levels. The variations in volume resistivity and relative dielectric constant (RDC) of thermoplastics under different environmental conditions suggested that low relative humidity and low temperature (particularly lower temperature) are more conducive to separation. Effective separation and recycling of binary mixed thermoplastics could be accomplished via tribo-electrostatic method. Thermoplastics with higher surface potential are more inclined to gain electrons and negatively charged, finally enriched in positive electrode. The greater the surface potential difference between two thermoplastics, the higher purity of their separation products. For instance, both positive and negative product purities of the ABS-PVC exceeded 97 % (surface potential difference of 7.22 V).
随着全球电子垃圾的急剧增加,通过摩擦静电分离回收电子垃圾中的热塑性塑料已成为必不可少的。采用傅里叶变换红外光谱(FTIR)和x射线光电子能谱(XPS)分析了聚氯乙烯(PVC)、高冲击聚苯乙烯(HIPS)、聚丙烯(PP)和丙烯腈-丁二烯-苯乙烯(ABS)四种典型热塑性塑料的内外官能团分布。所有热塑性塑料都存在一定程度的氧化,主要表现为-OH。首次采用原子力显微镜(AFM)评价热塑性塑料的表面电位,并通过对各种官能团的含量和电负性进行积分计算其总电负性。表面电位和总电负性的顺序在四个热塑性塑料是一致的:PVC(−4.08 V, 2.74) 祝辞 臀部(−8.36 V, 2.59) 祝辞 PP(−9.18 V, 2.57) 祝辞 ABS(−11.30 V, 2.56)。热塑性塑料中官能团的含量和电负性都显著影响表面电位水平。不同环境条件下热塑性塑料的体积电阻率和相对介电常数(RDC)的变化表明,低相对湿度和低温(特别是低温)更有利于分离。摩擦静电法可以有效地分离和回收二元混合热塑性塑料。表面电位高的热塑性塑料更倾向于获得电子并带负电荷,最终富集在正极。两种热塑性塑料的表面电位差越大,其分离产物的纯度越高。例如,ABS-PVC的正负产品纯度均超过97 %(表面电位差为7.22 V)。
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引用次数: 0
Simultaneous deep purification of fluoride and trivalent arsenic by a bimetallic composite xerogel coagulant 双金属复合干凝胶混凝剂同时深度净化氟和三价砷
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-23 DOI: 10.1016/j.seppur.2025.131779
Yonghai Gan, Le Qu, Zihao Cang, Xinhe Ding, Jun Luo, Zhe Li, Zheng Wang, Chengcheng Ding, Yibin Cui, Bin Xu, Bingdang Wu
Arsenic-fluoride (As-F) co-existence pollution seriously threatened the drinking water safety of residents using groundwater as water sources. At present, coagulation technology was widely used in the removal of arsenic and fluoride due to its economic efficiency and simple operation. While traditional aluminum (Al) and iron (Fe) coagulants could not remove fluoride and As(III) simultaneously, and high metal residues would bring additional risks. Based on the hydrolysis properties and pollution removal performance of zirconium (Zr) and titanium (Ti) salts, here we developed a new bimetallic composite xerogel coagulant (ZTXC) for simultaneous deep purification of fluoride and As(III). The characterization of physicochemical properties showed that ZTXC was a high-polymerization amorphous hydroxide similar to titanium xerogel coagulant (TXC) and zirconium xerogel coagulant (ZXC). ZTXC with a Zr/Ti molar ratio of 4:1 could effectively purify fluoride and As(III) at the same time, reducing fluoride and As(III) to 0.45 mg/L and 9.07 μg/L at pH 5.0 with dosage of 0.4 mM, respectively. Combining the advantages of Zr and Ti salts, ZTXC showed better coagulation performance and lower metal residues than PAC and PFS. Through the analysis of hydrolysis precipitation species and charge differences, fluoride removal mainly relied on the electrostatic attraction by positively charged hydrolysates, while neutral As(III) was mainly removed through hydroxyl coordination. This study could provide reference and theoretical guidance for the development and application of materials and technologies for As-F co-contaminated drinking water treatment.
氟化砷共存污染严重威胁着以地下水为水源的居民的饮用水安全。目前,混凝技术以其经济高效、操作简单等优点被广泛应用于除砷除氟。而传统的铝(Al)和铁(Fe)混凝剂不能同时去除氟化物和砷(III),并且金属残留量高会带来额外的风险。基于锆(Zr)和钛(Ti)盐的水解性能和除污性能,研制了一种新型双金属复合干凝胶混凝剂(ZTXC),可同时深度净化氟化物和砷(III)。理化性质表征表明,ZTXC是一种类似于钛干凝胶混凝剂(TXC)和锆干凝胶混凝剂(ZXC)的高聚合无定形氢氧化物。ZTXC在Zr/Ti摩尔比为4:1时,可同时有效地净化氟化物和As(III),在pH为5.0、用量为0.4 mM时,氟化物和As(III)的还原浓度分别为0.45 mg/L和9.07 μg/L。结合Zr和Ti盐的优点,ZTXC比PAC和PFS具有更好的混凝性能和更低的金属残留。通过对水解沉淀种类和电荷差异的分析,除氟主要依靠带正电的水解产物的静电吸引,而中性As(III)主要通过羟基配位去除。本研究可为砷-氟共污染饮用水处理材料和技术的开发与应用提供参考和理论指导。
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引用次数: 0
Impact and removal of fluorine impurity in the comprehensive recovery of spent LiFePO4/C 废LiFePO4/C综合回收中氟杂质的影响及去除
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-23 DOI: 10.1016/j.seppur.2025.131766
Yang Jiang, Changhong Peng, Kanggen Zhou, Hao Zhou, Tangmiaoqin Chen, Guopeng Zhang, Wei Chen
The comprehensive recovery of spent lithium iron phosphate powder (LFP/C) remains challenging in industry due to the difficulty in impurity removal. Specifically, the impact of fluorine impurity on the recovery process is unclear. In this work, the specific effects of fluorine on the removal of aluminum impurities and the subsequent recovery of FePO4·2H2O from spent LFP/C were investigated, and an acid-assisted pyrolysis process was proposed to transfer fluorine species into the gas phase for fluorine removal. The results indicate that due to the coordination reactions between F- with Al3+ and Fe2+/Fe3+, the presence of F- in increased the difficulty of aluminum removal and reduced the precipitation efficiency of FePO4·2H2O. Additionally, F- accelerated the aging of LFP/C cathode materials, increasing resistance to lithium-ion migration, which ultimately resulted in an irreversible decline in electrochemical performance. The acid-assisted pyrolysis process achieved a fluorine removal rate of approximately 98 % under the optimal condition (pyrolysis temperature 600-700°C, reaction time 4.0h, H3PO4 dosage 1.2 times of theoretic amount, and solid/liquid ratio 4.0), reducing the fluorine content from 1.69 wt% to 0.05 wt%. This work presents a potential strategy for fluorine removal, contributing to the comprehensive recovery of valuable elements from spent LFP/C.
废磷酸铁锂粉(LFP/C)的综合回收由于杂质去除困难,在工业上一直是一个挑战。具体来说,氟杂质对回收过程的影响尚不清楚。本文研究了氟对铝杂质的去除和废LFP/C中FePO4·2H2O的回收的具体影响,并提出了一种酸助热解工艺,将氟转移到气相中进行除氟。结果表明:由于F-与Al3+和Fe2+/Fe3+的配位反应,F- in的存在增加了除铝的难度,降低了FePO4·2H2O的沉淀效率;此外,F-加速了LFP/C正极材料的老化,增加了对锂离子迁移的抵抗力,最终导致电化学性能不可逆转地下降。在最佳条件下(热解温度600 ~ 700℃,反应时间4.0h, H3PO4投加量为理论投加量的1.2倍,料液比4.0),酸助热解工艺的氟去除率约为98 %,氟含量由1.69 wt%降至0.05 wt%。这项工作提出了一种潜在的除氟战略,有助于从废LFP/C中全面回收有价值元素。
{"title":"Impact and removal of fluorine impurity in the comprehensive recovery of spent LiFePO4/C","authors":"Yang Jiang, Changhong Peng, Kanggen Zhou, Hao Zhou, Tangmiaoqin Chen, Guopeng Zhang, Wei Chen","doi":"10.1016/j.seppur.2025.131766","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131766","url":null,"abstract":"The comprehensive recovery of spent lithium iron phosphate powder (LFP/C) remains challenging in industry due to the difficulty in impurity removal. Specifically, the impact of fluorine impurity on the recovery process is unclear. In this work, the specific effects of fluorine on the removal of aluminum impurities and the subsequent recovery of FePO<sub>4</sub>·2H<sub>2</sub>O from spent LFP/C were investigated, and an acid-assisted pyrolysis process was proposed to transfer fluorine species into the gas phase for fluorine removal. The results indicate that due to the coordination reactions between F<sup>-</sup> with Al<sup>3+</sup> and Fe<sup>2+</sup>/Fe<sup>3+</sup>, the presence of F<sup>-</sup> in increased the difficulty of aluminum removal and reduced the precipitation efficiency of FePO<sub>4</sub>·2H<sub>2</sub>O. Additionally, F<sup>-</sup> accelerated the aging of LFP/C cathode materials, increasing resistance to lithium-ion migration, which ultimately resulted in an irreversible decline in electrochemical performance. The acid-assisted pyrolysis process achieved a fluorine removal rate of approximately 98 % under the optimal condition (pyrolysis temperature 600-700°C, reaction time 4.0h, H<sub>3</sub>PO<sub>4</sub> dosage 1.2 times of theoretic amount, and solid/liquid ratio 4.0), reducing the fluorine content from 1.69 wt% to 0.05 wt%. This work presents a potential strategy for fluorine removal, contributing to the comprehensive recovery of valuable elements from spent LFP/C.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"51 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143020963","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
Highly selective and rapid sequential degradation of venlafaxine-class antidepressants using a novel BiOCl-based two-dimensional molecularly imprinted photocatalyst 高选择性和快速顺序降解文拉法辛类抗抑郁药使用新型biocl为基础的二维分子印迹光催化剂
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-23 DOI: 10.1016/j.seppur.2025.131777
Lin Liu, Songsong Zhi, Runan Chen, Yang Yang, Chenshi Luo, Pengfei Liang, Yongli Liu, Guifen Zhu
Photocatalytic degradation is an effective technology for the removal of organic compounds. However, the lack of selectivity limits its practical application for harmful substances in complex systems. Herein, a novel molecularly imprinted photocatalyst (MI-BiOCl) was prepared using two-dimensional nanosheet BiOCl as a matrix. Based on the superior degradation activity and charge carrier transfer of BiOCl, along with an imprinting layer with selectivity, MI-BiOCl can selectively adsorb and rapidly and sequentially degrade venlafaxine (VEN) and its analogue fluoxetine (FLU) in mixtures. MI-BiOCl can adsorb 32.27 mg/g of VEN within 5 min, with an imprinting factor of 4.72. Within pH range of 3–9, the degradation efficiency of VEN by MI-BiOCl remained above 98.8 %, unaffected by coexisting humic acid, and after four cycles, it was still higher than 98 %. Moreover, over 88.8 % of VEN and 99.3 % of FLU in municipal wastewater were degraded by MI-BiOCl, and the degradation intermediates tended to be non-toxic. DFT simulations verified that the highly selective degradation was due to the synergistic effect of imprinting sites, catalytic active sites and non-covalent bonding forces including van der Waals, hydrogen bonding and electrostatic interaction between MI-BiOCl and VEN and FLU. FLU, with stronger binding affinity, has the advantage of being preferentially degraded. The strategy provides a method for the highly selective degradation of drug pollutants in complex media.
光催化降解是一种有效的去除有机化合物的技术。然而,选择性的不足限制了其在复杂体系中对有害物质的实际应用。本文以二维纳米片BiOCl为基质制备了一种新型分子印迹光催化剂(MI-BiOCl)。基于BiOCl优越的降解活性和电荷载体转移,加上具有选择性的印迹层,MI-BiOCl可以选择性吸附并快速顺序降解混合物中的文拉法辛(VEN)及其类似物氟西汀(FLU)。MI-BiOCl可在5 min内吸附32.27 mg/g的VEN,印迹因子为4.72。在3 ~ 9的pH范围内,MI-BiOCl对VEN的降解效率保持在98.8 %以上,不受腐植酸共存的影响,4个循环后仍高于98 %。此外,MI-BiOCl可降解城市污水中超过88.8% %的VEN和99.3% %的FLU,且降解中间体趋于无毒性。DFT模拟验证了高选择性降解是由于印迹位点、催化活性位点以及MI-BiOCl与VEN和FLU之间的非共价键作用力(包括范德华、氢键和静电相互作用)的协同作用。流感具有较强的结合亲和力,具有优先降解的优势。该策略为复杂介质中药物污染物的高选择性降解提供了一种方法。
{"title":"Highly selective and rapid sequential degradation of venlafaxine-class antidepressants using a novel BiOCl-based two-dimensional molecularly imprinted photocatalyst","authors":"Lin Liu, Songsong Zhi, Runan Chen, Yang Yang, Chenshi Luo, Pengfei Liang, Yongli Liu, Guifen Zhu","doi":"10.1016/j.seppur.2025.131777","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131777","url":null,"abstract":"Photocatalytic degradation is an effective technology for the removal of organic compounds. However, the lack of selectivity limits its practical application for harmful substances in complex systems. Herein, a novel molecularly imprinted photocatalyst (MI-BiOCl) was prepared using two-dimensional nanosheet BiOCl as a matrix. Based on the superior degradation activity and charge carrier transfer of BiOCl, along with an imprinting layer with selectivity, MI-BiOCl can selectively adsorb and rapidly and sequentially degrade venlafaxine (VEN) and its analogue fluoxetine (FLU) in mixtures. MI-BiOCl can adsorb 32.27 mg/g of VEN within 5 min, with an imprinting factor of 4.72. Within pH range of 3–9, the degradation efficiency of VEN by MI-BiOCl remained above 98.8 %, unaffected by coexisting humic acid, and after four cycles, it was still higher than 98 %. Moreover, over 88.8 % of VEN and 99.3 % of FLU in municipal wastewater were degraded by MI-BiOCl, and the degradation intermediates tended to be non-toxic. DFT simulations verified that the highly selective degradation was due to the synergistic effect of imprinting sites, catalytic active sites and non-covalent bonding forces including van der Waals, hydrogen bonding and electrostatic interaction between MI-BiOCl and VEN and FLU. FLU, with stronger binding affinity, has the advantage of being preferentially degraded. The strategy provides a method for the highly selective degradation of drug pollutants in complex media.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"54 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143020873","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
A photocatalytic system for the Alleviation of ocean acidification and antibiotic pollution 缓解海洋酸化和抗生素污染的光催化系统
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-23 DOI: 10.1016/j.seppur.2025.131771
Jiangnan Huang, Jiali Huang, Xugang Shu, Xingan Cheng, Hao Yu, Yonghai Cao, Zhuofeng Hu, Jimmy C. Yu
Ocean acidification from the uptake of CO2 and antibiotic pollution from a consequence of inshore mariculture are two serious threats to marine ecosystems. In this work, a novelty oxygen-doping carbon nitride (O-CN) photocatalyst are designed for the release of CO2 and degradation of a targeted antibiotic (ofloxacin, OFL) in acidified seawater. Notably, this photocatalytic system can take advantage of ocean acidification as more CO3•- radicals were produced in the seawater. The catalyst could degrade OFL rapidly (k = 0.039 min−1) in the presence of CO32– and HCO3, which derive from the dissolved CO2 in the seawater, much higher than that of pristine CN (k = 0.013 min−1). Mechanism study revealed that the existence of CO32– and HCO3 would facilitate the generation of new N-C-O (O1) groups on the O-CN surface. These O1 groups are the active sites for the formation of •OH radicals that can oxidize OFL and release CO2. This investigation offers a novel strategy for alleviating two environmental threats simultaneously.
吸收二氧化碳造成的海洋酸化和近海海水养殖造成的抗生素污染是对海洋生态系统的两大严重威胁。在这项工作中,设计了一种新型氧掺杂氮化碳(O-CN)光催化剂,用于在酸化海水中释放CO2和降解靶向抗生素(氧氟沙星,OFL)。值得注意的是,这种光催化系统可以利用海洋酸化,因为海水中产生了更多的CO3•-自由基。在海水中溶解CO2产生的CO32 -和HCO3 -存在的情况下,催化剂对OFL的降解速度(k = 0.039 min−1)远高于原始CN (k = 0.013 min−1)。机理研究表明,CO32 -和HCO3 -的存在有利于在O-CN表面生成新的N-C-O (O1)基团。这些O1基团是形成•OH自由基的活性位点,可以氧化OFL并释放CO2。这项研究为同时减轻两种环境威胁提供了一种新的策略。
{"title":"A photocatalytic system for the Alleviation of ocean acidification and antibiotic pollution","authors":"Jiangnan Huang, Jiali Huang, Xugang Shu, Xingan Cheng, Hao Yu, Yonghai Cao, Zhuofeng Hu, Jimmy C. Yu","doi":"10.1016/j.seppur.2025.131771","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131771","url":null,"abstract":"Ocean acidification from the uptake of CO<sub>2</sub> and antibiotic pollution from a consequence of inshore mariculture are two serious threats to marine ecosystems. In this work, a novelty oxygen-doping carbon nitride (O-CN) photocatalyst are designed for the release of CO<sub>2</sub> and degradation of a targeted antibiotic (ofloxacin, OFL) in acidified seawater. Notably, this photocatalytic system can take advantage of ocean acidification as more CO<sub>3</sub><sup>•-</sup> radicals were produced in the seawater. The catalyst could degrade OFL rapidly (<em>k</em> = 0.039 min<sup>−1</sup>) in the presence of CO<sub>3</sub><sup>2–</sup> and HCO<sub>3</sub><sup>–</sup>, which derive from the dissolved CO<sub>2</sub> in the seawater, much higher than that of pristine CN (<em>k</em> = 0.013 min<sup>−1</sup>). Mechanism study revealed that the existence of CO<sub>3</sub><sup>2–</sup> and HCO<sub>3</sub><sup>–</sup> would facilitate the generation of new N-C-O (O1) groups on the O-CN surface. These O1 groups are the active sites for the formation of •OH radicals that can oxidize OFL and release CO<sub>2</sub>. This investigation offers a novel strategy for alleviating two environmental threats simultaneously.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"33 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143020877","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
Enhanced toluene adsorption selectivity of Fe-MFI zeolite under humid conditions using tetrasodium iminodisuccinate as ligand 以亚氨基二磺酸四钠为配体增强Fe-MFI沸石在湿润条件下对甲苯的吸附选择性
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-23 DOI: 10.1016/j.seppur.2025.131772
Haoran Sun, Jie Zhong, Hengxu Guo, Yipu Xu, Ziyang Liu, Anmin Zheng, Peng Peng, Zifeng Yan
It is of vital importance to selectively adsorb volatile organic compounds (VOC) via zeolite in order to alleviate their threats to both the public health and environment. However, practical VOC removal processes are often conducted under humid conditions where competitive water adsorption is always unavoidable. In this study, a Fe-containing MFI zeolite sample with less water affinity was prepared via an impregnation method with the help of tetrasodium iminodisuccinate (IDS) as a ligand. The breakthrough analysis of the Fe-containing MFI zeolite using toluene as a model compound for VOC showed that it has a significant increase in toluene adsorption selectivity under humid conditions compared to its high water affinity counterparts. Various characterization techniques confirmed that the iron species can heal the silanol nests related defects within Si-MFI zeolite by embedding into the framework via forming Fe-O-Si interaction.
通过沸石选择性吸附挥发性有机化合物(VOC)以减轻其对公众健康和环境的威胁至关重要。然而,实际的VOC去除过程通常在潮湿的条件下进行,在这种条件下,竞争性的水吸附总是不可避免的。本研究以亚氨基二磺酸四钠(IDS)为配体,通过浸渍法制备了一种低亲水性的含铁MFI沸石样品。以甲苯为模型化合物对含铁MFI分子筛进行的突破性分析表明,与高亲水性分子筛相比,含铁MFI分子筛在潮湿条件下对甲苯的吸附选择性显著提高。各种表征技术证实,铁可以通过形成Fe-O-Si相互作用嵌入到Si-MFI分子筛框架中,从而修复硅烷醇巢相关缺陷。
{"title":"Enhanced toluene adsorption selectivity of Fe-MFI zeolite under humid conditions using tetrasodium iminodisuccinate as ligand","authors":"Haoran Sun, Jie Zhong, Hengxu Guo, Yipu Xu, Ziyang Liu, Anmin Zheng, Peng Peng, Zifeng Yan","doi":"10.1016/j.seppur.2025.131772","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131772","url":null,"abstract":"It is of vital importance to selectively adsorb volatile organic compounds (VOC) via zeolite in order to alleviate their threats to both the public health and environment. However, practical VOC removal processes are often conducted under humid conditions where competitive water adsorption is always unavoidable. In this study, a Fe-containing MFI zeolite sample with less water affinity was prepared via an impregnation method with the help of tetrasodium iminodisuccinate (IDS) as a ligand. The breakthrough analysis of the Fe-containing MFI zeolite using toluene as a model compound for VOC showed that it has a significant increase in toluene adsorption selectivity under humid conditions compared to its high water affinity counterparts. Various characterization techniques confirmed that the iron species can heal the silanol nests related defects within Si-MFI zeolite by embedding into the framework via forming Fe-O-Si interaction.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"28 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143020874","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
Synchronizing directional photogenerated electrons and holes through Ag and Bi bimetallic modification toward sustained hydrogenation process in CO2 methanation reaction 通过银和铋双金属改性实现CO2甲烷化反应中定向光电子和空穴的同步化
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-23 DOI: 10.1016/j.seppur.2025.131786
Kai-hua Zhang, Ru-Yue Ding, Xin-Jie Zhao, Xiao-jing Wang, Yu-pei Li, Jun Zhao, Fa-tang Li
Sustained photocatalytic hydrogenation of CO2 molecules is crucial for the CO2 methanation reaction. Synchronizing directional photogenerated charge carriers and regulating the activation and hydrogenation process of CO2 molecules are key to achieving the efficient photocatalytic methanation of CO2. Herein, Ag–Bi bimetallic sites were designed and anchored on the surface of TiO2 via a one-step solution impregnation reduction and applied for the photocatalytic conversion of CO2 to CH4. The optimum 5 %Ag90Bi10-TiO2 composite exhibited excellent photocatalytic performance for the photoreduction of CO2 into CH4. The product selectivity of CH4 reached up to 97.2 %, at a rate of 58.9 μmol·g−1·h−1. In situ Kelvin probe force microscopy and diffuse reflectance infrared Fourier transform spectroscopy attributed the high selectivity of CH4 to the coexistence of metallic Ag and Bi sites, which induced directional photogenerated electrons and hole transfer. Moreover, the synergistic function of Ag–Bi bimetallic active sites on TiO2 facilitated the hydrogenation of *CO2 to CH4. The proposed strategy provides insight into the design of highly selective photocatalysts for the reaction of photocatalytic methanation of CO2.
CO2分子的持续光催化加氢对CO2甲烷化反应至关重要。同步定向光生载流子,调控CO2分子的活化和加氢过程是实现CO2高效光催化甲烷化的关键。本文设计了Ag-Bi双金属位点,并通过一步溶液浸渍还原法将其固定在TiO2表面,用于光催化CO2转化为CH4。最佳的5 %Ag90Bi10-TiO2复合材料对CO2光还原成CH4具有优异的光催化性能。CH4的选择性达到97.2 %,反应速率为58.9 μmol·g−1·h−1。原位开尔文探针力显微镜和漫反射红外傅立叶变换光谱分析认为,CH4的高选择性是由于金属Ag和Bi位点的共存,从而诱导了定向光生电子和空穴转移。此外,Ag-Bi双金属活性位点在TiO2上的协同作用促进了*CO2 -加氢成CH4。提出的策略为光催化甲烷化CO2反应的高选择性光催化剂的设计提供了见解。
{"title":"Synchronizing directional photogenerated electrons and holes through Ag and Bi bimetallic modification toward sustained hydrogenation process in CO2 methanation reaction","authors":"Kai-hua Zhang, Ru-Yue Ding, Xin-Jie Zhao, Xiao-jing Wang, Yu-pei Li, Jun Zhao, Fa-tang Li","doi":"10.1016/j.seppur.2025.131786","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131786","url":null,"abstract":"Sustained photocatalytic hydrogenation of CO<sub>2</sub> molecules is crucial for the CO<sub>2</sub> methanation reaction. Synchronizing directional photogenerated charge carriers and regulating the activation and hydrogenation process of CO<sub>2</sub> molecules are key to achieving the efficient photocatalytic methanation of CO<sub>2</sub>. Herein, Ag–Bi bimetallic sites were designed and anchored on the surface of TiO<sub>2</sub> via a one-step solution impregnation reduction and applied for the photocatalytic conversion of CO<sub>2</sub> to CH<sub>4</sub>. The optimum 5 %Ag<sub>90</sub>Bi<sub>10</sub>-TiO<sub>2</sub> composite exhibited excellent photocatalytic performance for the photoreduction of CO<sub>2</sub> into CH<sub>4</sub>. The product selectivity of CH<sub>4</sub> reached up to 97.2 %, at a rate of 58.9 μmol·g<sup>−1</sup>·h<sup>−1</sup>. In situ Kelvin probe force microscopy and diffuse reflectance infrared Fourier transform spectroscopy attributed the high selectivity of CH<sub>4</sub> to the coexistence of metallic Ag and Bi sites, which induced directional photogenerated electrons and hole transfer. Moreover, the synergistic function of Ag–Bi bimetallic active sites on TiO<sub>2</sub> facilitated the hydrogenation of *CO<sub>2</sub><sup>–</sup> to CH<sub>4</sub>. The proposed strategy provides insight into the design of highly selective photocatalysts for the reaction of photocatalytic methanation of CO<sub>2</sub>.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"13 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143020897","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
Efficient and convenient purification strategy using maltodextrin-based nanosponges for rapid removal of cationic dyes 利用麦芽糖糊精基纳米海绵快速去除阳离子染料的高效、便捷的净化策略
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-23 DOI: 10.1016/j.seppur.2025.131702
Chaochao Wen, Yu Huang, Wenjia Zhang, Jiping Tian, Chuan Dong, Cheng Yang, Wenting Liang
Developing new adsorbents and studying their adsorption mechanisms can greatly assist in addressing environmental pollution issues. Herein, the maltodextrin-based nanosponges (MD-SPs) were facilely synthesized by esterification reaction at room temperature. The porous features, nanostructure, and swelling capacities of the resulting MD-SPs can be regulated by altering the crosslinking agent, which controls the adsorption properties. Using nine cationic dyes as model adsorbates, the results showed that MD-SPs could adsorb a large amount of cationic dyes in a short time. Especially, MD-SP-1 could rapidly adsorb over 90 % of most cationic dyes within 3 min, and the maximal adsorption quantity (Qm) of cationic red X-GRL (CRX) was as high as 2137.81 mg/g. The adsorption behaviors were meticulously investigated by multiple adsorption kinetic and thermodynamic models. Furthermore, the integrated analysis of experimental and theoretical calculations results demonstrated that the electrostatic force, hydrogen bonding, hydrophobic interaction, cation-π interaction, and π-π stacking may collectively facilitate the capture of dye molecules. Notably, the absorbent offered excellent anti-interference capabilities, high stability, and reusability, making it an ideal adsorbent for the rapid and batch treatment of dye wastewater. These discoveries may provide valuable references for the theoretical and practical study of adsorbents and offer new insights into the development of advanced maltodextrin-based adsorbents.
开发新型吸附剂并研究其吸附机理对解决环境污染问题具有重要意义。本文在室温下通过酯化反应制备了麦芽糖糊精基纳米海绵(MD-SPs)。通过改变交联剂,可以调节MD-SPs的孔隙特征、纳米结构和膨胀能力,从而控制其吸附性能。以9种阳离子染料为模型吸附剂,结果表明,MD-SPs能在短时间内吸附大量阳离子染料。特别是,MD-SP-1在3 min内可快速吸附90% %以上的阳离子染料,对阳离子红X-GRL (CRX)的最大吸附量(Qm)高达2137.81 mg/g。采用多种吸附动力学和热力学模型对其吸附行为进行了细致的研究。此外,实验和理论计算结果的综合分析表明,静电力、氢键、疏水相互作用、阳离子-π相互作用和π-π堆积共同促进了染料分子的捕获。值得注意的是,该吸附剂具有出色的抗干扰能力,高稳定性和可重复使用性,使其成为染料废水快速批量处理的理想吸附剂。这些发现可为吸附剂的理论和实践研究提供有价值的参考,并为开发先进的麦芽糖糊精基吸附剂提供新的见解。
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Separation and Purification Technology
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