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Efficient and selective recovery of Gd(Ⅲ)via polyethyleneimine modification of lanthanum-based metal-organic frameworks

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Journal of Rare Earths 2024年第1期42卷 210-219,I0007页

作者： Wenhao Li Lijinhong huang Bin Xiao Xiaoguang Duan Haike Li Lang Li wanfu huang Ganzhou Key Laboratory of Basin Pollution Simulation and Control Jiangxi University of Science and TechnologyGanzhou341000China Innovation Center for Water Quality Security Technology at Ganjiang River Basin Jiangxi University of Science and TechnologyGanzhou341000China Faculty of Science and Engineering WA School of Mines:MineralsEnergy and Chemical EngineeringCurtin UniversityWAAustralia School of Architecture and Design Jiangxi University of Science and TechnologyGanzhou341000China School of Resources and Architectural Engineering Gannan University of Science and TechnologyGanzhou341000China School of Chemical Engineering and Advanced Materials The University of AdelaideAdelaideSA5005Australia School of Resource and Environmental Engineering Jiangxi University of Science and TechnologyGanzhou341000China

With the development of the economy and the increasing demand for environmental protection,the efficient and selective recovery of Gd(Ⅲ)from actual wastewater is of critical *** this work,lanthanum-based metal-organic framework(LaBDC)materials were prepared by a hydrothermal method,and then polyethyleneimine(PEI)and LaBDC were combined by an impregnation method to form a novel LaBDC@xPEI *** prepared materials were characterized using Fourier transfo rm infrared spectroscopy(FTIR),X-ray diffraction(XRD),scanning electron microscopy(SEM),energy dispersive X-ray spectroscopy(EDX),B runauer-Emmett-Teller(BET),thermogravimetric analysis(TGA)and X-ray photoelectron spectroscopy(XPS).Experiments show that LaBDC@50%PEI has the highest adsorption capacity(181.77 mg/g)among lanthanum-based MOFs with different PEI loadings at pH=5.5,which is about 5.1 times that of bare *** adsorption isotherm analysis shows that LaBDC@50%PEI follows the Langmuir *** addition,the adsorption kinetics of LaBDC@50%PEI follows a pseudo-second-order kinetic model,indicating that the adsorption process is chemical *** is worth noting that LaBDC@50%PEI maintains good adsorption performance and stability after three recycling tests,and exhibits excellent selectivity in cation interference ***,the LaBDC@50%PEI composites possess good stability and hold great promises in rapid recovery of Gd(Ⅲ)from practical aqueous environments.

关键词： Wet-impregnation method Polyethylene imine Metaleorganic frameworks Lanthanum Recovery of Gd(Ⅲ) Rare earths

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Ultrathin organic solvent nanofiltration membrane with polydopamine-HKUST-1 interlayer for organic solvent separation

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Journal of Environmental Sciences 2024年第7期141卷 182-193页

作者： Haike Li Xindong Li Guozai Ouyang Lijinhong huang Lang Li Wenhao Li wanfu huang Duokun Li Ganzhou Key Laboratory of Basin Pollution Simulation and Control Jiangxi University of Science and TechnologyGanzhou 341000China Innovation Center for Water Quality Security Technology at Ganjiang River Basin Jiangxi University of Science and TechnologyGanzhou 341000China School of Architecture and Design Jiangxi University of Science and TechnologyGanzhou 341000China WA School of Mines:Minerals Energy and Chemical EngineeringCurtin UniversityWA 6845Australia School of Materials Science and Engineering Tiangong UniversityTianjin 300387China

Polydopamine(PDA)and metal-organic skeleton HKUST-1 were co-deposited on the base membrane of hexamethylenediamine(HDA)-crosslinked polyetherimide(PEI)ultrafiltration membrane as the interlayer,and high-throughput organic solvent nanofiltration membrane(OSN)was prepared by interfacial polymerization and solvent activation *** polyamide(PA)layer surface roughness from 28.4 nm in PA/PEI to 78.3 nm in PA/PDA-HKUST-10.6/PEI membrane,reduced the thickness of the separation layer from 79 to 14 nm,and significantly improved the hydrophilic,thermal and mechanical *** flux of the PA/PDA-HKUST-10.6/PEI membrane in a 0.1 g/L Congo Red(CR)ethanol solution at 0.6 MPa test pressure reached 21.8 L/(m^(2)·hr)and the rejection of CR was 92.8%.Solvent adsorption test,N,N-dimethylformamide(DMF)immersion experiment,and long-term operation test in ethanol showed that the membranes had high solvent *** solvent flux test demonstrated that,under the test pressure of 0.6 MPa,the flux of different solvents ranked as follows:methanol(56.9 L/(m^(2)·hr))>DMF(39.6 L/(m^(2)·hr))>ethanol(31.2 L/(m^(2)·hr))>IPA(4.5 L/(m^(2)·hr))>N-hexane(1.9 L/(m^(2)·hr)).The ability of the membranes to retain dyes in IPA/water dyes solution was also *** flux of the membrane was 30.4 L/(m^(2)·hr)and the rejection of CR was 91.6%when the IPA concentration reached 50%.This OSN membrane-making strategy is economical,environment-friendly and efficient,and has a great application prospect in organic solvent separation systems.

关键词： Interfacial polymerization Organic solvent nanofiltration Interlayer Metal-organic frameworks Polydopamine

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Glycine functionalized activated carbon derived from navel orange peel for enhancement recovery of Gd(Ⅲ)

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Journal of Rare Earths 2022年第11期40卷 1794-1802,I0005页

作者： Bin Xiao Lijinhong huang wanfu huang Dongmei Zhang Xiangrong Zeng Xiaohui Yao School of Resource and Environmental Engineering Jiangxi University of Science and TechnologyGanzhou 341000China Jiangxi College of Applied Technology Ganzhou 341000China Faculty of Science and Engineering WA School of Mines:MineralsEnergy and Chemical EngineeringCurtin UniversityWAAustralia School of Architecture and Design Jiangxi University of Science and TechnologyGanzhou 341000China

Glycine functionalized activated carbon adsorption material(NOPAC-GLY-X)was successfully prepared by one-step thermal decomposition using agricultural waste navel orange peel as a *** batch adsorption experiments,it is found that the adsorption performance of Gd(Ⅲ)on activated carbon can be significantly enhanced by glycine *** adsorption isotherms of the NOPACs conform to the Langmuir isotherm model,and the maximum adsorption capacity of the activated carbon sample NOPAC-Gly-60 is approximately 48.5 mg/*** Gd(Ⅲ)adsorption capacity of navel orange peel activated carbon can be doubled after glycine modification,and the adsorption efficiency of gadolinium can reach99%at pH=*** physicochemical properties of the prepared adsorbents were characterized by Brunauer-Emmett-Teller(BET),Fourier transform infrared spectroscopy(FTIR),elemental analysis(EA),and X-ray photoelectron spectroscopy(XPS).The characterization test shows that the specific surface area of the sample increases from 1121 to 1523 m^(2)/g,and the ratio of(N+O)/C increases from 10.8%to 30.0%by the glycine *** five cycles of adsorption-desorption,the adsorption capacity can still be maintained at 88%of the initial ***-GLY-60 has excellent adsorption selectivity for Gd(Ⅲ).With the obvious advantages of simple synthesis steps and low cost,the activated carbon modification method adopted in this study has great application value in the field of rare earth adsorption and recovery.

关键词： Glycine functionalized One-step thermal decomposition Navel orange peel Gd(Ⅲ)adsorption Rare earths

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Synthesis of N,O-rich active site porous polymers and their efficient recovery of Gd(Ⅲ) from solution

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稀土学报:英文版 2023年第9期41卷 1419-1428,I0006页

作者： Bin Xiao Lijinhong huang Jiacai Ou Bin Zeng Zhiqiang Zou Xiangrong Zeng wanfu huang School of Resource and Environmental Engineering Jiangxi University of Science and TechnologyGanzhou 341000China School of Resources and Architectural Engineering Gannan University of Science and TechnologyGanzhou 341000China Faculty of Science and Engineering WA School of Mines:MineralsEnergy and Chemical EngineeringCurtin UniversityWAAustralia School of Architecture and Design Jiangxi University of Science and TechnologyGanzhou 341000China

Our previous study found that the adsorption performance of porous carbon for Gd(Ⅲ) could be significantly improved by increasing the N,and O functional groups on its ***,the adsorption capacity of porous carbon is low due to the limited number of N,and O functional groups that can be loaded on its *** to the advantage of customizable functional groups of porous organic polymers(POPs),the triazine-based Tb-MEL and hydroxyl-modified triazine-based Tp-MEL were synthesized by a one-step hydrothermal method using nitrogen-rich melamine as the raw material and triformylbenzene(Tb) and 2,4,6-triformylphloroglucinol(Tp),*** Gd(Ⅲ) adsorption isotherms and kinetic curves of Tb-MEL,and Tp-MEL at pH=6 and T=25℃ are in high agreement with the Langmuir isotherm(R^(2)>0.998) and pseudo-second-order kinetics(R^(2)>0.993),*** fitted maximum adsorption capacity(q_(max)) is about 136.05 mg/g,much higher than 58.38 mg/g of *** adsorption efficiency for Gd(Ⅲ) at pH=7 is close to 100%,and Tp-MEL maintains 62.4% of the initial adsorption capacity after ten cycle s of sorption/desorption of Gd(Ⅲ),with an average elution efficiency of more than 90%.Adsorption selection performance tests show that Tp-MEL has good adsorption selectivity for HREE ions,and the selectivity is as follows:Lu^(3+)>Y^(3+)>Gd^(3+)>Nd^(3+)>La^(3+)>Al^(3+)>Ca^(2+)>Mg^(2+).Batch adsorption,Brunauer-Emmett-Teller(BET) method,and X-ray photoelectron spectrometer(XPS)tests show that hydroxyl modifications lose the specific surface area of the polymer,and the functional groups contribute more to the adsorption performance than the specific surface area.

关键词： N O functional groups Triazine-based Hydroxyl-modified Adsorption performance Rare earths

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Tannic acid/Fe^(3+)interlayer for preparation of high-permeability polyetherimide organic solvent nanofiltration membranes for organic solvent separation

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Chinese Journal of Chemical Engineering 2023年第5期57卷 17-29页

作者： Haike Li Xindong Li Guozai Ouyang Lang Li Zhaohuang Zhong Meng Cai Wenhao Li wanfu huang Ganzhou Key Laboratory of Basin Pollution Simulation and Control Jiangxi University of Science and TechnologyGanzhou 341000China Innovation Center for Water Quality Security Technology at Ganjiang River Basin Jiangxi University of Science and TechnologyGanzhou 341000China School of Civil and Surveying&Mapping Engineering Jiangxi University of Science and TechnologyGanzhou 341000JiangxiChina

Organic solvent nanofiltration(OSN)membranes have a great application prospect in organic solvent separation,but the development of OSN membranes is mainly restricted by trade-off between permeability and rejection *** this work,a TA/Fe^(3+)polymer was introduced into polyetherimide(PEI)ultrafiltration membranes crosslinked with hexamethylene diamine as the intermediate layer,and OSN membranes with high separation performance and solvent permeability were obtained through interfacial polymerization and solvent *** interlayer with high surface hydrophilicity and a fixed pore structure controlled the adsorption/diffusion of the amine monomer during interfacial polymerization,forming a smooth(average surface roughness<5.5 nm),ultra-thin(separation layer thickness reduced from 150 to 16 nm)and dense surface structure polyamide(PA)*** PA-Fe^(3+)_3-HDA/PEI membrane retained more than 94%of methyl blue(BS)in 0.1 g·L^(-1)BS ethanol solution at 0.6 MPa,and the ethanol permeation reached 28.56 L^(-1)·m^(-2)·h^(-1).The average flux recovery ratio(FRR)of PA-Fe^(3+)_(3)-HDA/PEI membrane was found to be 84%,which has better fouling resistance than PA-HDA/PEI membrane,and it was found to have better stability performance through different solvent immersion experiments and continuous operation in 0.1 g·L^(-1)BS ethanol *** with thin-film composite nanofiltration membranes,the PA-Fe^(3+)_(3)-HDA/PEI membrane can be manufactured from an economical and environment-friendly method and overcomes the trade-off between permeability and rejection rate,showing great application potential in organic solvent separation systems.

关键词： Nanofiltration membrane Waste treatment Surface Filtration Tannic acid Interfacial polymerization

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钨冶炼渣中锡的回收工艺研究

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有色金属（选矿部分） 2024年第6期 57-63页

作者：阳晨黄万抚张文译刘观发王泽凯江西理工大学资源与环境工程学院江西赣州341000

随着冶炼工艺的不断演变和发展,冶炼技术也逐渐趋于成熟。通过冶炼工艺提取钨后剩余的钨冶炼渣大量堆存,给人类的生产生活带来了负面影响。钨冶炼渣成分较为复杂,表面残留有浸出药剂,其中富含大量的有价金属,因此选取合适的工艺回收钨... 详细信息

随着冶炼工艺的不断演变和发展,冶炼技术也逐渐趋于成熟。通过冶炼工艺提取钨后剩余的钨冶炼渣大量堆存,给人类的生产生活带来了负面影响。钨冶炼渣成分较为复杂,表面残留有浸出药剂,其中富含大量的有价金属,因此选取合适的工艺回收钨冶炼渣中的有价金属不仅可以从源头上减少排放量,减轻对土壤和水资源的污染,还能提高有价金属的资源利用率并降低钨冶炼渣处理成本。钨冶炼渣的减量化、环保化和资源化处理是钨行业碳减排的关键一环,对某黑白混合钨冶炼渣中金属锡的回收进行了试验研究,该钨冶炼渣中约有87.59%的锡分布在-0.045 mm粒级中,分选难度较大。选择尼尔森立式离心选矿机作为粗选设备,通过逐步优化实验确定粗选流程的最佳条件,分别为磨矿细度为-0.038 mm粒级含量占78.15%、给矿浓度15%、分选锥转速90 G/s、反冲水流量2.60 L/min。为进一步提高粗精矿锡品位,对四种精选方法进行了对比试验,最终在“离心选矿机一粗一精+摇床、离心选矿机分级精选”的重选工艺下,当给矿浓度15%、分选锥转速90 G/s、反冲水流量2.75 L/min时,获得了锡精矿锡品位4.03%、锡回收率52.41%,实现了钨冶炼渣中有价金属锡的有效回收,为钨冶炼渣的减量化及资源化利用提供了一定的参考。

关键词：钨冶炼渣锡回收重选联合工艺

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PREPARATION OF FERROFLUID FOR MINERAL PROCESSING AND ITS PROPERTIES

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中国有色金属学会会刊：英文版 1998年第3期8卷 169-173页

作者： huang, wanfu Wang, Dianzuo Xu, Sunqu Univ of Science and Technology Beijing Beijing China

１ＩＮＴＲＯＤＵＣＴＩＯＮＢｅｃａｕｓｅｏｆｉｔｓｅｓｐｅｃｉａｌｙｈｉｇｈｓｅｐａｒａｔｉｎｇｄｅｎｓｉｔｙａｎｄｓｅｐａｒａｔｉｎｇｐｒｅｃｉｓｉｏｎ，ｔｈｅｆｅｒｏｆｌｕｉｄｉｃｓｅｐａｒａｔｉｏｎｈａｓａｔａ... 详细信息

１ＩＮＴＲＯＤＵＣＴＩＯＮＢｅｃａｕｓｅｏｆｉｔｓｅｓｐｅｃｉａｌｙｈｉｇｈｓｅｐａｒａｔｉｎｇｄｅｎｓｉｔｙａｎｄｓｅｐａｒａｔｉｎｇｐｒｅｃｉｓｉｏｎ，ｔｈｅｆｅｒｏｆｌｕｉｄｉｃｓｅｐａｒａｔｉｏｎｈａｓａｔａｃｔｅｄｓｃｉｅｎｔｉｓｔ’ｓｇｒ...

关键词： mineral processing ferrofluid preparation properties

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钨冶炼除磷渣中浸出钼和钨研究

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材料导报 2023年第15期37卷 203-207页

作者：曾斌曾祥荣黄万抚江西理工大学资源与环境工程学院江西赣州341000 信丰华锐钨钼新材料有限公司江西赣州341000

钨冶炼除磷渣是重要的钼和钨二次资源。采用热压浸出法从钨冶炼除磷渣中浸出Mo和WO_(3),考察碳酸钠用量、氢氧化钠用量、浸出时间、浸出温度、液固比、搅拌速度对Mo和WO_(3)浸出率的影响。研究结果显示,碳酸钠用量和氢氧化钠用量是影响M... 详细信息

钨冶炼除磷渣是重要的钼和钨二次资源。采用热压浸出法从钨冶炼除磷渣中浸出Mo和WO_(3),考察碳酸钠用量、氢氧化钠用量、浸出时间、浸出温度、液固比、搅拌速度对Mo和WO_(3)浸出率的影响。研究结果显示,碳酸钠用量和氢氧化钠用量是影响Mo和WO_(3)浸出率的关键因素,采用碳酸钠-氢氧化钠协同浸出,Mo和WO_(3)的浸出率显著提高。确定较优试验条件为:碳酸钠的用量为理论用量的2.5倍,氢氧化钠用量为理论用量的0.15倍,浸出时间2 h,浸出温度188℃,浸出液固比3∶1,浸出搅拌速度80 r·min^(-1),此条件下,Mo和WO_(3)浸出率分别为99.19%、99.11%。按优化条件进行工业试验,Mo浸出率大于98.50%,WO_(3)浸出率大于98.40%,浸出渣中Mo含量小于0.16%,WO_(3)含量小于0.20%。

关键词：钨冶炼除磷渣碳酸钠-氢氧化钠协同浸出浸出率

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PDA夹层调控的荷正电纳滤膜的制备及在水处理中的应用

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材料导报 2023年第6期37卷 202-209页

作者：包亚晴黄李金鸿李新冬黄彪林黄万抚江西理工大学土木与测绘工程学院江西赣州341000 江西理工大学建筑与设计工程学院江西赣州341000 江西理工大学资源与环境工程学院江西赣州341000

当前商用纳滤膜在溶液中多显示荷负电,而根据道南效应,荷正电纳滤膜在分离废水中的荷正电物质时更具优势。本工作在掺杂金属有机骨架(MOF)的混合基质基膜上构建聚多巴胺(PDA)中间层,再通过聚乙烯亚胺(PEI)和均苯三甲酰氯(TMC)的交联反... 详细信息

当前商用纳滤膜在溶液中多显示荷负电,而根据道南效应,荷正电纳滤膜在分离废水中的荷正电物质时更具优势。本工作在掺杂金属有机骨架(MOF)的混合基质基膜上构建聚多巴胺(PDA)中间层,再通过聚乙烯亚胺(PEI)和均苯三甲酰氯(TMC)的交联反应制备了荷正电聚酰胺复合纳滤膜。对多巴胺(DA)沉积浓度和时间及TMC有机相的添加条件进行优化;对比了PDA中间层添加前后两种复合纳滤膜对1 g/L的MgCl2、NaCl、MgSO4、Na2SO4溶液的渗透截留情况;重点考察了改性膜对含Cu2+、Ni2+和Pb2+的重金属溶液及五种阴阳离子染料的处理情况,最后评估了膜的耐污染性能。结果表明,将2 g/L的DA在超滤支撑层上沉积90 min,PEI水相浓度为1.2%、浸没时间为7 min、TMC有机相浓度为0.5%、交联时间为120 s时,所制备的改性膜的综合性能最佳,膜的接触角为51.5°,表面粗糙度下降,等电点在pH为9左右,在溶液中显示荷正电。改性膜对MgCl2的截留率上升到94.26%,在0.8 MPa下,其对Cu2+、Ni2+、Pb2+溶液的水通量均在40 L/(m2·h)以上,且离子截留率分别为96.57%、95.23%、94.73%;同时,其对几种染料的截留率均能达到90%以上。因此,PDA中间层改性的荷正电纳滤膜在废水处理中具有良好的应用前景。

关键词：聚多巴胺(PDA) 聚乙烯亚胺(PEI) 荷正电纳滤膜重金属染料

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具有PDA-UiO-66中间层耐溶剂复合纳滤膜的制备及性能

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精细化工 2023年第2期40卷 388-397页

作者：李浪李新冬李海柯李文豪黄万抚江西理工大学赣州市赣江流域水质安全保障技术创新中心江西赣州341000 江西理工大学赣州市流域污染模拟与控制重点实验室江西赣州341000

将多巴胺和Ui O-66纳米颗粒共沉积在经1,6-己二胺交联的聚醚酰亚胺(PEI)基膜上构建了纳米复合中间层(PDA-UiO-66),并在中间层上进行界面聚合反应制备了耐溶剂复合纳滤膜(TFN-U)。通过FTIR、XRD、SEM、AFM、水接触角测量仪对膜结构进行... 详细信息

将多巴胺和Ui O-66纳米颗粒共沉积在经1,6-己二胺交联的聚醚酰亚胺(PEI)基膜上构建了纳米复合中间层(PDA-UiO-66),并在中间层上进行界面聚合反应制备了耐溶剂复合纳滤膜(TFN-U)。通过FTIR、XRD、SEM、AFM、水接触角测量仪对膜结构进行了表征和测试,探究了Ui O-66质量浓度对TFN-U膜耐溶剂性、耐污染性以及运行稳定性的影响。结果表明,PDA-Ui O-66纳米复合中间层的引入能提高TFN-U膜的渗透通量,当Ui O-66纳米颗粒质量浓度为0.2 g/L时,TFN-U2膜水通量为63.83 L/(m^(2)·h),甲醇通量为28.50L/(m^(2)·h),对刚果红水溶液和刚果红甲醇溶液的截留率为98.2%和93.2%,经无水乙醇、丙酮、乙酸乙酯、正己烷及N,N-二甲基甲酰胺(DMF)浸泡48h后,其对刚果红的截留率均>94%,通量恢复率达到78.1%,在连续24 h过滤刚果红甲醇溶液后,该膜的甲醇通量为14.13L/(m^(2)·h),截留率为98.3%,表明TFN-U2膜具有良好的耐溶剂性、耐污染性以及一定的运行稳定性。

关键词：聚多巴胺 Ui O-66 中间层耐溶剂复合纳滤膜水处理技术

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