以小麦秸秆生物炭(BC)作为载体,采用原位聚合法,通过控制BC热解温度和N-苯基甘氨酸/生物炭(NPG/BC)质量比等合成条件,制备了一系列生物炭/聚(N-苯基甘氨酸)(BC/PNPG)复合吸附剂,研究合成条件对Sb(Ⅲ)吸附性能的影响,并通过SEM、FT-IR和XPS等表征手段揭示吸附机理。结果表明,BC对Sb(Ⅲ)的吸附量随热解温度的升高而增大,最大为7.55mg/g。热解温度为800℃、NPG/BC质量比为5∶5、合成环境为酸性条件下,制备的BC3/PNPG-5∶5-S对Sb(Ⅲ)的吸附量为17.65mg/g,是BC的2.3倍。该复合吸附剂对Sb(Ⅲ)的吸附机制包括苯胺基与Sb(Ⅲ)的螯合作用、带正电荷的质子化双极化子对Sb(Ⅲ)的氧化作用和带正电的PNPG与Sb(OH)-6之间的静电相互作用。
A series of biochar/poly(N-phenylglycine) (BC/PNPG) composite adsorbents were prepared by in-situ polymerization method through controlling the biochar pyrolysis temperature and N-phenylglycine/biochar (NPG/BC) mass ratio.The influence of the synthesis conditions on the adsorption performance of Sb(Ⅲ) was studied,and the adsorption mechanism was revealed by SEM,FT-IR and XPS.The results showed that the adsorption capacity of Sb(Ⅲ) increased with the increase of pyrolysis temperature,and the maximum was 7.55mg·g-1.The adsorption capacity of BC3/PNPG prepared under the conditions of pyrolysis temperature of 800℃,NPG/BC mass ratio of 5∶5,and acidic environment was 17.65mg·g-1,which was 2.3 times that of the pristine BC.The adsorption mechanism of the composite adsorbent for Sb(Ⅲ) included the chelation of aniline group with Sb(Ⅲ),the oxidation of Sb(Ⅲ) by protonated bipolarizers with positive charge,and the electrostatic interaction between positively charged PNPG with Sb(OH)-6.
[1] Sundar S,Chakravarty J.Antimony toxicity[J].International Journal of Environmental Research and Public Health,2010,7(12):4267-4277.
[2] Tao Y R,Su H L,Li H X,et al.Ecological and human health risk assessment of antimony (Sb) in surface and drinking water in China[J].Journal of Cleaner Production,2021,318:128514.
[3] Liu Y L,Lou Z M,Yang K L,et al.Coagulation removal of Sb(Ⅴ) from textile wastewater matrix with enhanced strategy:comparison study and mechanism analysis[J].Chemosphere,2019,237:124494.
[4] Xu S,Zhong Z Q,Liu W Z,et al.Removal of Sb(Ⅲ) from wastewater by magnesium oxide and the related mechanisms[J].Environmental Research,2020,186:109489.
[5] Deng Y L,Mao Q M,Luo S,et al.Adsorption-based removal of Sb(Ⅲ) from wastewater by graphene oxide-modified zirconium-based metal-organic framework composites[J].Adsorption Science & Technology,2022,2022:1-13.
[6] 贾祥苓,闵奇,白仁碧,等.聚合物负载铁-锰双金属氧化物去除水中锑的研究[J].化工新型材料,2023,51(4):231-237.
[7] 刘鑫,施浙炎,卢佳业,等.碳纤维负载二元锆铁氧化物复合材料对水中锑的吸附研究[J].化工新型材料,2023,51(9):278-281,284.
[8] Dong W J,Gu X R,Shu Y,et al.Pulse electrocoagulation combined with a coagulant to remove antimony in wastewater[J].Journal of Water Process Engineering,2022,47:102749.
[9] Meng L J,Wu M J,Chen H S,et al.Rejection of antimony in dyeing and printing wastewater by forward osmosis[J].Science of the Total Environment,2020,745(prepublish):141015.
[10] 洪思奇,牛梦娴,覃璇,等.吸附法去除印染废水中锑的研究进展[J].西安工程大学学报,2022,36(3):63-70.
[11] 刘凯楠,李国峰,云梁,等.农业废弃生物质在废水处理中的应用研究进展[J].合成材料老化与应用,2023,52(3):119-121.
[12] 聂若楠,王旺民,曹丽娟,等.关于生物炭的四重功能化改性及其吸附环境污染物机制的综述[J].材料导报,2023,37(22):242-250.
[13] 崔灿,牛姣姣,杨莲,等.β-环糊精改性磁性生物炭高效去除水中Pb(Ⅱ)[J/OL].复合材料学报,1-16[2024-01-19]https://doi.org/10.13801/j.cnki.fhclxb.20230706.002.
[14] Mao W J,Wu P,Zhang Y Q,et al.Manganese oxide-modified biochar derived from discarded mushroom-stick for the removal of Sb(Ⅲ) from aqueous solution[J].Environmental Science and Pollution Research,2022,29(32):49322-49334.
[15] 周雪.生物炭负载镧掺杂铁氧化物吸附As(Ⅴ)、Sb(Ⅲ)的研究以及对废水中微生物群落结构的影响[D].绍兴:绍兴文理学院,2022.
[16] Mansoor S J,Abbasitabar F.Adsorption behavior of Fe(Ⅱ) and Fe(Ⅲ) ions on polyaniline coated sawdust:batch and fixed-bed studies[J].Acta Chimica Slovenica,2020,67(1):36-46.
[17] Wang N,Feng J T,Yan W,et al.Dual-functional sites for synergistic adsorption of Cr(Ⅵ) and Sb(Ⅴ) by polyaniline-TiO2 hydrate:adsorption behaviors,sites and mechanisms[J].Frontiers of Environmental Science & Engineering,2022,16(8):105.
[18] Zhang L,Niu W Y,Sun J,et al.Efficient removal of Cr(Ⅵ) from water by the uniform fiber ball loaded with polypyrrole:static adsorption,dynamic adsorption and mechanism studies[J].Chemosphere,2020,248:126102.
[19] Bhaumik M,Agarwal S,GuptaV K,et al.Enhanced removal of Cr(Ⅵ) from aqueous solutions using polypyrrole wrapped oxidized MWCNTs nanocomposites adsorbent[J].Journal of Colloid And Interface Science,2016,470:257-267.
[20] Wu T T,Lin Z X,Wu H Y,et al.Adsorption studies on Ag(Ⅰ) using poly(N-phenylglycine) membrane and application in practical silver recycling[J].ACS Applied Polymer Materials,2022,4(5):3333-3342.
[21] Wu T T,Lin Z X,Wu H Y,et al.Selective and sensitive adsorption of Au(Ⅲ) by poly-N-phenylglycine[J].Separation and Purification Technology,2022,287:120604.
[22] 杨育振,高宝龙,黄屹,等.中高热解温度下秸秆基生物炭对铅、镉的吸附特性研究[J].中国地质,2023,50(1):52-60.
[23] 巫丹,范方宇,王昌命,等.温度对澳洲坚果壳生物炭特性影响[J].应用化工,2021,50(5):1282-1286,1291.
[24] 常西亮,胡雪菲,蒋煜峰,等.不同温度下小麦秸秆生物炭的制备及表征[J].环境科学与技术,2017,40(4):24-29.
[25] 张少娜.农林废弃物热解特性及动力学研究[D].北京:中国地质大学(北京),2021.
[26] 肖欣.生物炭的多级结构特征、构效关系及其吸附作用研究[D].杭州:浙江大学,2018.
[27] 范方方,左卫元.制备条件对稻壳生物炭吸附亚甲基蓝性能的影响研究[J].安徽化工,2022,48(6):66-69.
[28] 赵明涛,张婧雯,李冬冬,等.花生壳生物炭的制备、表征及其对邻苯二甲酸二甲酯的吸附特性[J].应用化工,2021,50(9):2415-2417,2423.
[29] 周力.不同热解温度下苜蓿和玉米芯生物炭对水中四环素的吸附特性研究[D].西安:西北大学,2021.
[30] 郑庆福,王永和,孙月光,等.不同物料和炭化方式制备生物炭结构性质的FT-IR研究[J].光谱学与光谱分析,2014,34(4):962-966.
[31] 徐玉娥,邵晓辉,谢军海,等.不同裂解温度下3种豆科植物生物炭理化特性分析[J].热带作物学报,2023,44(12):2528-2536.
[32] Muniraj V K A,Boukherroub R,Shelke M V.Flexible energy storage device based on poly(N-phenylglycine),an incentive-energy pseudocapacitive conducting polymer,and electrochemically exfoliated graphite sheets[J].ACS Sustainable Chemistry & Engineering,2020,8(16):6433-6441.
[33] Wu T T,Lin Z X,Zhang Y,et al.Poly-N-phenylglycine@multi-walled carbon nanotubes composite membrane for improvement of Au(Ⅲ) adsorption[J].Separation and Purification Technology,2023,304:122404.
[34] 赵越.麦秆生物炭对黄绵土热物理性质的影响及机制[D].兰州:兰州交通大学,2020.
[35] Doh J H,Kim J H,Kim H J,et al.Enhanced adsorption of aqueous copper(Ⅱ) ions using dedoped poly-N-phenylglycine nanofibers[J].Chemical Engineering Journal,2015,277:352-359.
[36] Kim H J,Choi H,Sharma A K,et al.Recyclable aqueous metal adsorbent:synthesis and Cu(Ⅱ) sorption characteristics of ternary nanocomposites of Fe3O4 nanoparticles@graphene poly-N-phenylglycine nanofibers[J].Journal of Hazardous Materials,2021,401(prepublish):123283.
[37] Capra L,Manolache M,Ion I,et al.Adsorption of Sb(Ⅲ) on oxidized exfoliated graphite nanoplatelets[J].Nanomaterials(Basel,Switzerland),2018,8(12):992.
基金资助
陕西省重点研发计划项目(2023-YBNY-260);西安工程大学科研计划项目(310/107020511)
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