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Journal of Environmental Sciences 2024年第3期137卷 395-406页

作者： Fangzhi Duan Yongfeng Zhu Yan Liu Aiqin Wang key laboratory of clay mineral applied research of gansu province Center of Eco-material and Green ChemistryLanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China

Porous materials applied in environmental remediation have received researchers'extensive attention recently,but the related green and convenient preparation method is rarely reported.Here,we recommended a green and convenient strategy for the fabrication of porous material via aqueous foam templates,which was synergistically stabilized by Codonopsis pilosula(CP)and clay minerals of attapulgite(APT).The characterization results revealed that the APT was modified by organic molecules leached from CP and anchored at the air-water interface,which improved the foam stability significantly.The novel porous material of polyacrylamide/Codonopsis pilosula/attapulgite(PAM/CP/APT)templated from the aqueous foam via a polymerization reaction had excellent adsorption capacity for the cationic dyes methyl violet(MV)and methylene blue(MB),and the adsorption capacity can reach 755.85 mg/g and557.64 mg/g,respectively.More importantly,the adsorption capacity of spent adsorbent material was still over 200 mg/g after being recycled five times through a simple carbonization process,and then it was added to the plant pot,the total biomass was increased by about86.42%.This study provided a green and sustainable pathway for the preparation,application and subsequent processing of porous materials.

关键词： Porous material Aqueous foam Atapulgite Adsorption Cationic dyes Sustainable utilization

Review on the effect of isomorphic replacement on the structure and application performance of typical clay minerals

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Progress in Natural Science:Materials International 2024年第2期34卷 251-262页

作者： Ritong Huang Limei Wu Xiaolong Wang Ning Tang Lili Gao Aiqin Wang Yushen Lu School of Materials Science and Engineering Shenyang Jianzhu University School of Mechanical Engineering Shenyang Jianzhu University key laboratory of clay mineral applied research of gansu province Center of Eco-material and Green Chemistry Lanzhou Institute of Chemical Physics Chinese Academy of Sciences

clay minerals represent a class of hydrated phyllosilicates making up the fine-grained portions of rocks, sediments, and soils. Due to the advantages of abundant reserves, low prices, and wide applications, the development and utilization of clay minerals have received increasing attention in recent years. Isomorphic replacement is a common phenomenon in clay minerals, which is one of the main causes of changes in mineral chemical composition and physical and chemical properties. This article briefly describes the crystal structure of several clay minerals such as montmorillonite, vermiculite, palygorskite, kaolinite, and halloysite. It summarized the research status of the effect of isomorphic replacement on their structure and application performance. The research results can provide theoretical basis for the structural research and efficient resource utilization of clay minerals.

关键词： clay minerals Crystal structure Isomorphism Application performance

Natural attapulgite supported nano-Ni catalysts for the efficient reductive amination of biomass-derived aldehydes and ketones

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Green Synthesis and Catalysis

Green Synthesis and Catalysis 2024年第1期5卷 42-50页

作者： Jia Zhang Jian Yang Xuemei Li Bin Mu Hailong Liu Chungu Xia Aiqin Wang Zhiwei Huang State key laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China key laboratory of clay mineral applied research of gansu province Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China University of Chinese Academy of Sciences Beijing 100049China

The efficient synthesis of useful primary amines via reductive amination of biomass-based aldehydes and ketones over earth-abundant base metal catalysts is an attractive biomass value-adding technology yet facing lots of challenges.Herein,natural attapulgite(ATP)was applied as support for the fabrication of active Ni catalysts with different Ni loadings(5–30 wt%)by the deposition-precipitation method.The Ni/ATP-550 catalyst with 10–15 wt%Ni loadings was found to present the highest catalytic performance for the synthesis of valuable 5-amino-1-pentanol(5-AP)via reductive amination of biofurfural-derived 2-hydroxytetrahydropyran among a variety of commonly used oxide supports loaded Ni catalysts,as well as ATP supported nickel catalysts with other loadings,achieving 5-AP yield up to 94%.The intrinsic activity of the Ni/ATP catalysts was found to depend strongly on the Ni^(0) crystallite size and Ni^(0) fraction of the catalysts,which generally increased with increasing Ni^(0) crystallite size and fraction,owing probably to the hydrogenation of imine intermediate is a structure-sensitive reaction.The efficient 10Ni/ATP-550 catalyst also exhibited good activity and stability in the reductive amination of several other biomass-derived aldehydes and ketones to their corresponding primary amines with good to excellent yields(81%–99%).This work provided a clean and efficient natural ATP-supported non-noble metal nickel-based catalytic system for the reductive amination of aldehydes and ketones to synthesize high-value-added primary amines,which could be a promising candidate for the industrial production of amines.

关键词： Attapulgite Nano-Ni catalyst Reductive amination 5-Amino-1-pentanol Structure-activity relationship

Novel eco-friendly spherical porous adsorbent fabricated from Pickering middle internal phase emulsions for removal of Pb(Ⅱ) and Cd(Ⅱ)

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Journal of Environmental Sciences 2022年第2期34卷 320-330页

作者： Hui Yu Yongfeng Zhu Aiping Hui Aiqin Wang key laboratory of clay mineral applied research of gansu province Center of Eco-material and Green ChemistryLanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China

Spherical porous materials prepared from the emulsion template used in the water treatment have displayed a vast prospect, as the high surface area, abundant porous structure, convenient operation and excellent adsorption performance. But the tedious fabrication process, high consumption of organic solvent and surfactant limited the application widely. Herein, a facile and eco-friendly spherical porous adsorbent(SPA) is fabricated from the green surfactant-free(corn oil)-in-water Pickering medium internal phase emulsions(Pickering MIPEs) via the convenient ion crosslinking procedure. The Pickering MIPEs synergistically stabilized with the semi-coke(SC), which is the natural particle produced from the shale oil distillation, and sodium alginate(SA) has excellent storage and anti-coalescence stability. The as-prepared porous adsorbent possessed the abundant pore structure, which provided favorable conditions for effective mass transfer in adsorption, and could be tuned by varying the SA dosage. The saturation adsorption capacities of Pb(II) and Cd(II) can be achieved with 460.54 and 278.77 mg/g within 45 min at 25 ℃, respectively. Overall, this study supplied a viable and eco-friendly route for fabricating the spherical porous adsorbent with a tunable porous structure for heavy metal ion wastewater.

关键词： Spherical porous adsorbent(SPA) Emulsion template Semi-coke Adsorption Heavy metal ion

Fabrication porous adsorbents templated from aqueous foams using astragalus membranaceus and attapulgite as stabilizer for efficient removal of cationic dyes

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Journal of Environmental Sciences 2023年第5期127卷 855-865页

作者： Fangzhi Duan Yongfeng Zhu Yushen Lu Jiang Xu Aiqin Wang key laboratory of clay mineral applied research of gansu province Center of Eco-material and Green ChemistryLanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China

The water-based foam stabilized by the natural surfactant applied in the fabrication of porous materials has attracted extensive attention,as the advantages of cleanness,convenience and low cost.Particularly,the development of a green preparation method has became themain research focus and frontier.In thiswork,a green liquid foamwith high stability was prepared by synergistic stabilization of natural plant astragalus membranaceus(AMS)and attapulgite(APT),and then a novel porous material with sufficient hierarchical pore structure was templated from the foam via a simple free radical polymerization of acrylamide(AM).The characterization results revealed that the amphiphilic molecules from AMS adsorbed onto thewater-air interface and formed a protective shell to prevent the bubble breakup,and APT gathered in the plateau border and formed a three-dimensional network structure,which greatly slowed down the drainage rate.The porous material polyacrylamide/astragalus membranaceus/attapulgite(PAM/AMS/APT)showed the excellent adsorption performance for cationic dyes of Methyl Violet(MV)and Methylene Blue(MB)in water,and the maximum adsorption capacity could reach to 709.13 and 703.30 mg/g,respectively.Furthermore,the polymer material enabled to regenerate and cycle via a convenient calcination process,and the adsorption capacitywas still higher than 200 mg/g after five cycles.In short,this research provided a new idea for the green preparation of porous materials and the treatment of water pollution.

关键词： Astragalus membranaceus Pickering foam Porous material Adsorption Biochar

Facile fabrication of the porous adsorbent from natural plant Angelica Sinensis stabilized liquid foam for dye removal

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Green Chemical Engineering 2022年第1期3卷 83-91页

作者： Fangzhi Duan Yongfeng Zhu Hui Yu Aiqin Wang key laboratory of clay mineral applied research of gansu province Center of Eco-material and Green ChemistryLanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou730000China Certer of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing100049China

Porous materials as emerging high-efficiency adsorbents have attracted increasing attention in recent years,due to the high specific surface area,fast adsorption rate,favorable adsorption capacity to heavy metal,dyes,and other pollutants,etc.Among various approaches,the foam template method with the advantage of flexible operation and controllable pores structure is proposed to prepare net type of porous adsorbents with superior adsorption capacity and rapid adsorption rate.In this process,natural plant Angelica Sinensis(AS)was treated with a simple alkalineheat process,and the resultant product was used firstly to prepare foam with high stability,and the positive effect of the cellulose dissociation and the conversion of ligustilide into amphiphilic moleculars on improving the stability of Pickering foam was revealed.The liquid foam can serve as pore-foaming template and precursor of polymerization for synthesizing porous adsorbent by one-step integrated process of free radical polymerization and silane hydrolysis.The porous adsorbent showed the sufficient porous structure and excellent adsorption performance for cationic dye,with maximum adsorption capacities of 386.13 mg g^(-1) and 284.20 mg g^(-1) for methyl violet(MV)and malachite green(MG).In a word,the novel approach can provide an important reference for green synthesis of high stable foam and the superporous material,and the adsorbent showed great application potential in the field of water treatment.

关键词： Adsorbent Angelica Sinensis Pickering foam Adsorption Dye

From waste hot-pot oil as carbon precursor to development of recyclable attapulgite/carbon composites for wastewater treatment

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Journal of Environmental Sciences 2019年第1期31卷 346-358页

作者： Jie Tang Bin Mu Li Zong Aiqin Wang key laboratory of clay mineral applied research of gansu province Center of Eco-material and Green Chemistry Lanzhou Institute of Chemical Physics Chinese Academy of Sciences University of Chinese Academy of Sciences Center of Xuyi Palygorskite applied Technology Lanzhou Institute of Chemical Physics Chinese Academy of Sciences

The utilization of waste products as valuable materials was a technical imperative for waste management. In this study, the cost-effective attapulgite/carbon(APT/C) composite was developed for wastewater treatment using waste hot-pot oil as a carbon precursor through a facile one-step calcination process. The APT/C composite prepared at 300°C exhibited the excellent adsorption capacity and rapid equilibrium rate over a broad p H range for the removal of various pollutants. More importantly, the removal ratios of the composites toward Methyl Violet and tetracycline still remained 77.6% and 60.2% of the initial adsorption capacity after ten adsorption–regeneration cycles via a facile thermal regeneration strategy, respectively.Beyond all doubt, this research provided a feasible and economical way for the sustainable utilization of waste hot-pot oil in wastewater treatment, achieving the concept of disposal waste with waste and recycling.

关键词： Waste hot-pot oil Calcination Attapulgite/carbon composites Adsorption Thermal regeneration

Removal of antibiotics from aqueous solution by using porous adsorbent templated from eco-friendly Pickering aqueous foams

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Journal of Environmental Sciences 2021年第4期33卷 352-362页

作者： Hui Yu Yongfeng Zhu Aiping Hui Fangfang Yang Aiqin Wang key laboratory of clay mineral applied research of gansu province Center of Eco-material and Green ChemistryLanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China

The aqueous foam template without any solvent and only using the particles stabilizer has attracted much attention for preparation of the porous adsorbents.Herein,a novel porous adsorbent was fabricated via thermal-initiated polymerization of Pickering aqueous foams,which was stabilized by the natural sepiolite(Sep)and pine pollen,and utilized for the removal of antibiotic from aqueous solution.The stabilizing mechanism of Pickering aqueous foam of that the Sep was modified with the leaching substance from pine pollen and arranged orderly around the bubble to form a dense"shell"structure was revealed.The adsorbents possessed the hierarchical porous structure and excellent adsorption performance for antibiotic of chlorotetracycline hydrochloride(CTC)and tetracycline hydrochloride(TC).The equilibrium adsorption capacities of CTC and TC were achieved with 465.59 and 330.59 mg/g within 60 min at 25℃,respectively.The adsorption process obeyed Langmuir model and pseudo-second-order adsorption kinetic model.This work provided eco-friendly approach for fabricate porous adsorbents for wastewater treatment.

关键词： Porous adsorbent Adsorption Antibiotic Pickering aqueous foams Pollen Sepiolite

Preparation of porous adsorbent via Pickering emulsion template for water treatment: A review

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Journal of Environmental Sciences 2020年第2期32卷 217-236页

作者： Yongfeng Zhu Wenbo Wang Hui Yu Aiqin Wang key laboratory of clay mineral applied research of gansu province Center of Eco-material and Green ChemistryLanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China

Porous materials as emerging potential adsorbents have received much more attention because they are capable of capturing various pollutants with fast adsorption rate, high adsorption capacity, good selectivity and excellent reusability.In order to prepare porous materials with decent porous structure, Pickering emulsion template method has been proved to be one of the most effective technologies to create pore structure.This paper reviewed comprehensively the latest research progress on the preparation of porous materials from various Pickering emulsions and their applications in the decontamination of pollutants(e.g., heavy metal ions, organic pollutants) and in the oil/water separation.It was expected that the summaries and discussions in this review will provide insights into the design and fabrication of new efficient porous adsorbents, and also give us a better understanding of the subject.

关键词： Pickering emulsion Porous material Soft template Water treatment

From illite/smectite clay to mesoporous silicate adsorbent for efficient removal of chlortetracycline from water

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Journal of Environmental Sciences 2017年第1期29卷 31-43页

作者： Wenbo Wang Guangyan Tian Li Zong Yanmin Zhou Yuru Kang Qin Wang Aiqin Wang Center of Eco-materials and Green Chemistry Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China University of the Chinese Academy of Sciences Beijing 100049China key laboratory of clay mineral applied research of gansu province Lanzhou 730000China College of Animal Science and Technology Nanjing Agricultural UniversityNanjing 210095China

A series of mesoporous silicate adsorbents with superior adsorption performance for hazardous chlortetracycline（CTC） were sucessfully prepared via a facile one-pot hydrothermal reaction using low-cost illite/smectite（IS） clay,sodium silicate and magnesium sulfate as the starting materials.In this process,IS clay was ＂teared up＂ and then ＂rebuilt＂ as new porous silicate adsorbent with high specific surface area of 363.52 m^2/g（about 8.7 folds higher than that of IS clay） and very negative Zeta potential（- 34.5 mV）.The inert Si- O- Si（Mg,Al） bonds in crystal framework of IS were broken to form Si（Al）- O^- groups with good adsorption activity,which greatly increased the adsorption sites served for holding much CTC molecules.Systematic evaluation on adsorption properties reveals the optimal silicate adsorbent can adsorb 408.81 mg/g of CTC（only 159.7 mg/g for raw IS clay） and remove 99.3%（only 46.5%for raw IS clay） of CTC from 100 mg/L initial solution（pH 3.51;adsorption temperature 30℃;adsorbent dosage,3 g/L）.The adsorption behaviors of CTC onto the adsorbent follows the Langmuir isotherm model,Temkin equation and pseudo second-order kinetic model.The mesopore adsorption,electrostatic attraction and chemical association mainly contribute to the enhanced adsorption properties.As a whole,the high-efficient silicate adsorbent could be candidates to remove CTC from the wastewater with high amounts of CTC.

关键词： Illite/smectite clay Hybrid silicate adsorbent Chlortetracycline Removal