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Separation and recovery of rare earth from waste nickel-metal hydride batteries by phosphate based extraction-precipitation

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Journal of Rare Earths 2022年第6期40卷 974-980,I0005页

作者： Hailan Zhi Shuainan Ni Xiang Su Wenqi Xie hepeng zhang Xiaoqi Sun College of Chemistry and Materials Science Fujian Normal UniversityFuzhou 350007China Fujian CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Fujian Research Center for RE Engineering Technology Xiamen Institute of RE MaterialsHaixi InstituteChinese Academy of SciencesXiamen 36102JChina Jiangxi Province Key Laboratory of Cleaner Production of Rare Earths Ganjiang Innovation AcademyChinese Academy of SciencesGanzhou 341000China Ganzhou Rare Earth Group Co. Ltd.China Southern Rare EarthGanzhou 341000China

A novel type of extraction-precipitation strategy based on phosphate was developed to recover rare earth(RE,i.e.,La,Ce,Nd,and Pr)from waste nickel-metal hydride(NiMH)batteries.This method does not require saponification and organic solvents.The novel phosphates,i.e.,dibenzyl phosphate(DBP),diphenyl phosphate(DPP),triphenyl phosphate(TPP)were studied as extraction-precipitants.DBP has high precipitation efficiencies for RE^(3+),which can reach 97.84%,100%,100%and 99.77%,respectively.In addition,the precipitation efficiencies of Mn^(2+),Co^(2+)and Ni^(2+)are less than 1.75%.DBP-RE has the largest particle size(D10=52.6μm,D50=135.35μm,D90=296.08μm),which is much larger than the precipitations formed by NH_(4)HCO_(3),H_(2)C2O_(4),CaO and MgO.The larger precipitation particle sizes contribute to improving the solid-liquid separation efficiency.With 3 mol/L hydrochloric acid,the stripping efficiency of DBP-RE reaches 98.60%,and the purity of recovered RE is 99.85%.The regenerated DBP can be directly used for the recycling extraction.Therefore,the novel extraction-precipitation strategy is a green and sustainable separation method.

关键词： Waste nickel-metal hydride battery Rare earth Extraction-precipitation Phosphonic acid(ester)

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Separation of aluminum from rare earth by solvent extraction with 4-octyloxybenzoic acid

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Journal of Rare Earths 2023年第2期41卷 290-299页

作者： Gaoshan Yu Zhiyuan Zeng Yun Gao Shuainan Ni hepeng zhang Xiaoqi Sun CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Fujian Research Center for Rare Earth Engineering Technology Xiamen Institute of Rare Earth MaterialsHaixi InstituteChinese Academy of SciencesXiamen 361021China University of Chinese Academy of Sciences Beijing 100039China Jiangxi Province Key Laboratory of Cleaner Production of Rare Earths Ganjiang Innovation AcademyChinese Academy of SciencesGanzhou 341000China

Leaching method is usually used to extract rare earth(RE)elements from ion adsorbed RE ores.In the leaching process,some impurities such as aluminum(Al)enter the leaching solution.The separation of Al from RE by carboxylic acid extractant 4-octyloxybenzoic acid(POOA)was studied in this article.By changing the pH value,temperature,solvent,saponification degree and other parameters,the extraction and separation performance of POOA in chloride system was systematically studied.Through specific extraction experiments and slope analysis,it can be seen that the stoichiometric ratio of POOA to Al is 3:1during the extraction process.The separation factor of Al^(3+)and Pr^(3+)can reach about 160.00.Compared with easily emulsified naphthenic acid,POOA achieves better phase separation.The above results show that saponified POOA(S-POOA)has a good separation effect on Al and RE.Under the condition of low concentration stripping acid of 0.60 mol/L HCl,the developed extraction system can be almost completely stripped,and the stripping rate reaches 97.52%.The regenerated POOA can be directly used for the recycling extraction.

关键词： Rare earths Aluminium 4-octyoxybenzoic acid Solvent extraction Separation

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Identifying the roles of Ce^(3+)-OH and Ce-H in the reverse water-gas shift reaction over highly active Ni-doped CeO_(2) catalyst

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Nano Research 2022年第7期15卷 5831-5841页

作者： Haidong Shen Yujuan Dong Shaowei Yang Yuan He Qimeng Wang Yueling Cao Wenbin Wang Tianshuai Wang Qiuyu zhang hepeng zhang Xi’an Key Laboratory of Functional Organic Porous Materials School of Chemistry and Chemical EngineeringNorthwestern Polytechnical UniversityXi’an 710129China Research&Development Institute of Northwestern Polytechnical University in Shenzhen Shenzhen 518057China

Nickel-CeO_(2)-based materials are commonly used for the thermal catalytic hydrogenation of CO_(2).However,high Ni loadings and low CO selectivity restrict their use in the reverse water–gas shift(RWGS)reaction.Herein,we demonstrate a highly active,robust,and low-Ni-doped(1.1 wt.%)CeO_(2) catalyst(1.0-Ni-CeO_(2)).The Ni-based-mass-specific CO formation rate reaches up to 1,542 mmol·gNi^(−1)·h^(−1) with 100%CO selectivity at 300°C for 100 h,among the best values reported in the literature.Density functional theory(DFT)and diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)results reveal that the enhanced catalytic activity is attributed to the abundant Ce–H species,while the high selectivity results from low CO affinity.More importantly,a new reaction mechanism is proposed,which involves the reduction of bicarbonate to generate formate intermediate and CO by the H−released from Ce–H species.The new findings in this work will benefit the design of economic,efficient,and robust catalysts for low-temperature RWGS reactions.

关键词： CO_(2)hydrogenation Ni-doped CeO_(2) reverse water-gas shift(RWGS)reaction cerium hydride mechanism investigation

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RuCo alloy nanoparticles embedded within N-doped porous two-dimensional carbon nanosheets:a high-performance hydrogen evolution reaction catalyst

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Tungsten 2024年第1期6卷 114-123页

作者： Jin-Hui Wang Shao-Wei Yang Fu-Bin Ma Yi-Ke Zhao Shi-Nuo Zhao Zheng-Yu Xiong Dong Cai Hai-Dong Shen Kai Zhu Qiu-Yu zhang Yue-Ling Cao Tian-Shuai Wang He-Peng zhang Research and Development Institute of Northwestern Polytechnical University in Shenzhen Shenzhen 518057China Xi’an Key Laboratory of Functional Organic Porous Materials School of Chemistry and Chemical EngineeringNorthwestern Polytechnical UniversityXi’an 710129China School of Power and Energy Northwestern Polytechnical UniversityXi’an 710129China Chongqing Science and Technology Innovation Center of Northwestern Polytechnical University Chongqing 401135China

Developing cost-effective electrocatalysts with high activity and stability especially at high current density is of great significance for the large-scale commercial application of electrochemical water splitting to hydrogen production but still remains challenging.Herein,we report an effective confinement pyrolysis strategy to fabricate embedded ruthenium-cobalt nanoclusters supported on N-doped porous two-dimensional carbon nanosheets(RuCo@CN).Markedly,the embedded structure can effectively prevent the migration,agglomeration,and leaching of nanoparticles,thus endowing the RuCo@CN catalyst with high stability.To be exact,high stability with up to 650 h can be achieved at high current density(-500 and-1000 mA·cm^(-2)).Besides,the RuCo@CN catalysts also exhibit highly reactive with low overpotentials of only 11mV at-10 mA·cm^(-2).Density functional theory calculations reveal that the introduction of cobalt reduces the decomposition barrier of H_(2)O for RuCo@CN alloy,thus promoting hydrogen evolution reaction.

关键词： Hydrogen evolution reaction Confinement pyrolysis strategy Mosaic structure Stability

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Injectable hybrid inorganic nanoscaffold as rapid stem cell assembly template for cartilage repair

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National Science Review 2022年第4期9卷 116-127页

作者： Shenqiang Wang Letao Yang Bolei Cai Fuwei Liu Yannan Hou Hua Zheng Fang Cheng hepeng zhang Le Wang Xiaoyi Wang Qianxin Lv Liang Kong Ki-Bum Lee Qiuyu zhang Key Laboratory of Special Functional and Smart Polymer Materials of Ministry of Industry and Information Technology School of Chemistry and Chemical EngineeringNorthwestern Polytechnical University Xi'an Key Laboratory of Functional Organic Porous Materials School of Chemistry and Chemical EngineeringNorthwestern Polytechnical University Department of Chemistry and Chemical Biology Rutgers University Department of Biomedical Engineering Columbia University State Key Laboratory of Military Stomatology & National Clinical Research Center for Oral Diseases & Shaanxi Key Laboratory of Oral Diseases Department of Oral and Maxillofacial SurgerySchool of StomatologyThe Fourth Military Medical University Research & Development Institute of Northwestern Polytechnical University in Shenzhen

Cartilage injuries are o?ten devastating and most cannot be cured because of the intrinsically low regenerative capacity of cartilage tissues. Although stem-cell therapy has shown enormous potential for cartilage repair, the therapeutic outcome has been restricted by low survival rates and poor chondrocyte differentiation in vivo. Here, we report an injectable hybrid inorganic(IHI) nanoscaffold that facilitates fast assembly, enhances survival and regulates chondrogenic differentiation of stem cells. IHI nanoscaffolds that strongly bind to extracellular matrix(ECM) proteins assemble stem cells through synergistic 3 D cell–cell and cell–matrix interactions, creating a favorable physical microenvironment for stem-cell survival and differentiation in vitro and in vivo. Additionally, chondrogenic factors can be loaded into nanoscaffolds with a high capacity, which allows deep, homogenous drug delivery into assembled 3 D stem-cell-derived tissues for effective control over the soluble microenvironment of stem cells. The developed IHI nanoscaffolds that assemble with stem cells are injectable. They also scavenge reactive oxygen species and timely biodegrade for proper integration into injured cartilage tissues. Implantation of stem-cell-assembled IHI nanoscaffolds into injured cartilage results in accelerated tissue regeneration and functional recovery. By establishing our IHI nanoscaffold-templated 3 D stem-cell assembly method, we provide a promising approach to better overcoming the inhibitory microenvironment associated with cartilage injuries and to advance current stem-cell-based tissue engineering.

关键词： injectable nanoscaffold 3D cell culture tissue engineering cartilage repair stem-cell therapy

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基于生成对抗网络的跨分辨率拓扑优化方法的比较研究

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振动与冲击 2024年第6期43卷 132-140页

作者：朱赫鹏丁喆张严李小白武汉科技大学机械传动与制造工程湖北省重点实验室武汉430081 武汉科技大学冶金装备及其控制教育部重点实验室武汉430081 武汉科技大学精密制造研究院武汉430081

拓扑优化的迭代过程涉及大量有限元分析与灵敏度更新步骤,且随着划分网格数目的增加,其优化过程将耗费大量的计算成本。利用深度学习方法,通过建立低分辨率中间构型与高分辨率拓扑结构之间的映射关系,可实现结构的跨分辨率拓扑优化设计... 详细信息

拓扑优化的迭代过程涉及大量有限元分析与灵敏度更新步骤,且随着划分网格数目的增加,其优化过程将耗费大量的计算成本。利用深度学习方法,通过建立低分辨率中间构型与高分辨率拓扑结构之间的映射关系,可实现结构的跨分辨率拓扑优化设计,从而大幅提高其计算效率。该文基于两种不同的生成对抗网络,构建了可实现跨分辨率预测的拓扑优化方法,并将其扩展至三维结构的优化预测。首先,以柔顺度最小化为目标函数,利用各向同性材料惩罚法生成不同载荷条件、初始位移和体积分数下的优化结构数据集;然后,分别利用Pix2pix和Esrgan网络解决其跨分辨率预测问题,其中对于Pix2pix网络,使用了残差模块代替其生成器内部的卷积模块,以增强网络对低层信息的复用;最后,通过二维和三维算例验证了所提方法的有效性,并与现有基于CGAN(conditional generative adversarial network)网络的方法进行了比较研究。结果表明,综合考虑计算精度和计算效率,基于Esrgan网络的方法表现更优,最适合应用于跨分辨率拓扑优化设计。

关键词：拓扑优化柔顺度跨分辨率预测 Pix2pix Esrgan

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Molecular simulation of oligomer inhibitors for calcite scale

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Particuology 2012年第3期10卷 266-275页

作者： Qiuyu zhang Hua Ren Wenwen Wang Junping zhang hepeng zhang School of Science Northwestern Polytechnical UniversityXi'an 710072China

Molecular simulation was performed to study the interaction between CaCO3 crystal and several oligomer inhibitors, by using the equilibrium morphology method to calculate the growth morphology of CaCO3 without inhibitors. The calculated morphology agreed well with SEM photographs. Then, a double-layer model was built to investigate the interaction between calcite crystal and oligomer inhibitors containing maleic anhydride （MA） and acrylic acid （AA）. Interaction energy per gram of an oligomer inhibitor was introduced as a scale of inhibition efficiency of different monomers. The results indicated that, for calcite scale inhibition, acrylamide （AM） and vinyl phosphonic acid （VPA） were the most efficient monomers, while allylsulfonic acid （AS） was the poorest. Increasing proportion of AM in dimer inhibitor molecule would improve the inhibition efficiency of MA, though, for a trimer, such as MA-AA-AM, certain sequence of monomers in the inhibitor molecule was necessary besides higher proportion of AM.

关键词： Molecular simulationCrystal morphology Interaction energy Scale inhibitorScale inhibition efficiency

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Key synthesis of magnetic Janus nanoparticles using a modified facile method

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Particuology 2014年第6期12卷 59-65页

作者： Nisar Ali Baoliang zhang hepeng zhang Wajed Zaman Wei Li Qiuyu zhang Key Laboratory of Applied Physics and Chemistry in Space of Ministry of Education School of ScienceNorthwestern Polytechnical University School of Material Science & Engineering Northwestern Polytechnical University

Inorganic/organic poly（methylmethacrylate-acrylic acid-divinylbenzene） iron oxide Janus magnetic nanoparticles（P（MMA-AA-DVB）/Fe3O4） with strong magnetic domains and unique surface functionalities were prepared using a solvothermal process.The P（MMA-AA-DVB） nanoparticles were prepared via soapfree emulsion polymerization and used as a precursor for preparing Janus nanoparticles.The morphology and magnetic properties of the magnetic Janus nanoparticles formed were characterized using a laser particle size analyzer,transmission electron microscopy,Fourier transform infrared spectroscopy,vibrating sample magnetometry,and thermogravimetric analysis.The synthesized P（MMA-AA-DVB）/Fe3O4 magnetic Janus nanoparticles were characterized by a Janus structure and possessed a stable asymmetric morphology after being dually functionalized.The particle size,magnetic content,and magnetic domain of the P（MMA-AA-DVB）/Fe3O4 magnetic Janus nanoparticles were 200 nm,40%,and 25 emu/g,respectively.The formation mechanism of the Janus nanoparticles was also investigated,and the results revealed that the reduction of Fe3＋ ions and growth of Fe3O4 took place on the surface of the P（MMA-AA-DVB） polymeric precursor particles.The size of the Janus particles could be controlled by narrowing the size distribution of the P（MMA-AA-DVB） precursor nanoparticles.

关键词： Janus Magnetic nanoparticles Solvothermal process Composite Emulsion polymerization

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Preparation of SiO_2/TiO_2 Janus particles by electrostatic assembly,hydrolysis and calcination

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Particuology 2013年第5期11卷 574-580页

作者： Baoliang zhang Qiuyu zhang hepeng zhang Xinlong Fan Dezhong Yin Xiangjie Li Wei Li Department of Applied Chemistry College of ScienceNorthwestern Polytechnical University

This paper describes a novel chemical method for preparing SiO2/TiO2 Janus particles. First, polystyrene （PSt）/SiO2 particles with a raspberry-like structure are prepared by electrostatic assembly. The influences of the reaction time of sulfonation and the treatment times of polyelectrolyte solutions （PDADMAC, PSS） on PSt and SiO2 are investigated with respect to the surface charge density of the particles. SiO2/TiO2 Janus particles are then obtained by hydrolysis of butyl titanate on the surface of PSt/SiO2 particles followed by a calcination process. Particle size analyzer, Zeta potential instrument, FTIR, TEM and SEM are used to characterize the particle size, the amount of charge on the surface of PSt and SiO2 particles and the compositions and morphologies of PSt/SiO2, SiO2/Ti02 and PSt/SiO2/Ti02. The diameters of the PSt, SiO2, PSt/Si02 and SiO2/Ti02 particles are 2.0 t^m, 303 nm, 2.7 bcm and 330 nm, respectively.

关键词： Janus particlesElectrostatic assemblyHydrolysisCalcination

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Synthesis of PS/Ag asymmetric hybrid particles via phase separation and self-assembly

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Particuology 2013年第6期11卷 768-775页

作者： Xinlong Fan Qiuyu zhang hepeng zhang Baoliang zhang Chunmei Li Xiangjie Li Xingfeng Lei Key Laboratory of Applied Physics and Chemistry in Space of Ministry of Education School of ScienceNorthwestern Polytechnical University

This article presents a facile approach to preparation of polystyrene/silver （PS/Ag） asymmetric hybrid par- ticles. In this method, polystyrene/polyglycidyl methacrylate （PS/PGMA） Janus particles were synthesized via internal phase separation triggered by evaporation of dichloromethane （DCM） from PS/PGMA/DCM- in water emulsion droplets. Then, the Janus particles were aminated and sequentially carboxylated to obtain PS/PGMA-NH2 and PS/PGMA-COOH particles. Ag＋ self-assembled on the surface of PGMA hemi- sphere of the functionalized PS/PGMA particles by coordinating with amine/carboxyl. PS/Ag asymmetric hybrid particles with 7.29 wt% of Ag were obtained by reduction of Ag＋, Scanning electron microscopy, energy-dispersive X-ray spectroscopy and transmission electron microscopy results confirmed that Ag was asymmetrically distributed on the surface of polymer particles.

关键词： Phase separation Interracial interaction Amination Carboxylation Coordination Self-assembly

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