Self-assembled CuS porous grade sub-nanoflowers as efficient nano-adsorbents for adsorption/self-deposition characteristics research

Zhao Xian-Tuo; Xu Lin-Lin; Tian Yue; Jiao An-Xin; Ma Hui; Zhang Meng-Ya; Cui Qing-Qiang

doi:10.7498/aps.70.20211152

Abstract

In recent decades, growing population and industrial development have led to releasing huge amounts of highly toxic chemical pollutants into the environment globally. Several approaches to handling the removal of contaminants from wastewater for environmental remediation, including biological, chemical, physical, and advanced oxidation processes have been employed. Among them, using nano-adsorbents as a tool for effectively removing organic contaminants represents a promising strategy in sewage purification field. More importantly, the nano-adsorbents with auto-deposition property can greatly improve the efficiency of sewage treatment. Therefore, the developing of environment friendly nano-adsorbents is thus an important issue to remove organic contaminants in water via simply adsorbing. Here in this work, porous flower-like copper sulfide (CuS) grade sub-nanomaterials are successfully fabricated by simply mixing two inorganic salts. Furthermore, the as-prepared nano-adsorbents with auto-deposition property can create a super adsorption capability for organic contaminants in wastewater. We further study the adsorption/auto-deposition characteristics of porous flower-like CuS grade sub-nanomaterials systematically by using various organic dyes (methyl blue, crystal violet, lemon yellow, sunset yellow and amaranth) as target molecules. For instance, in a typical procedure, 0.8-mg methyl blue can be removed 100% via adding 10-mg porous flower-like CuS grade sub-nanomaterials sample in 30 min. Therefore, the adsorption efficiency can be enhanced by 55% and 26% in comparison with the adsorption efficiency of CuS micro pompons and micron particles, respectively. Additionally, the porous flower-like CuS grade sub-nanomaterials can self-deposite on the bottom of the solution within 3 h after adsorption has finished, and the deposition efficiency can be improved by 95% and 3.17 times in comparison with the deposition efficiency of CuS micro pompons and micron particles, respectively. Comparing with micron particles, the unique self-depositing characteristics of porous flower-like grade sub-nanomaterials are attributed to larger specific surface area, greater porosity and stronger electrostatic adsorption capacity. Remarkably, this work provides an effective method of effectively removing various organic dyes from wastewater.

Keywords:

Authors and contacts

School of Physics, Shandong University, Jinan 250100, China

Corresponding author: Cui Qing-Qiang, cuiqingqiang@sdu.edu.cn

Funds: Project supported by the 2021 Laboratory Construction and Management Research Project of Shandong University, China (Grant No. sy20213202)

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References

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Cited By

图 1 (a), (b)多孔级次纳米花; (c), (d)微米绒球; (e), (f)微米颗粒的SEM

Figure 1. (a), (b) SEM image of porous grade sub-nanoflowers; (c), (d) SEM image of micron pompon; (e), (f) SEM image of micron particles.

DownLoad: Full-Size Img PowerPoint

图 2 (a) 多孔级次纳米花的S和Cu的能量散射谱; (b) mapping选区SEM图; (c), (d) 分别为S和Cu元素分布

Figure 2. (a) Energy scattering spectra of S and Cu in porous grade sub-nanoflowers; (b) mapping selected SEM image; (c), (d) S and Cu elements mapping, respectively.

DownLoad: Full-Size Img PowerPoint

图 3 多孔级次纳米花CuS的TEM图　(a), (b), (c) 分辨率依次增大; (d) 选区电子衍图谱

Figure 3. (a), (b), (c) The typical low and enlarged TEM image of porous grade sub-nanoflowers CuS; (d) the corresponding selected area electron diffraction (SAED) pattern.

DownLoad: Full-Size Img PowerPoint

图 4 CuS微米颗粒、微米绒球、多孔级次纳米花的XRD谱

Figure 4. XRD spectra of CuS micron pompon、micron particles and porous grade sub-nanoflowers.

DownLoad: Full-Size Img PowerPoint

图 5 级次纳米花的XPS谱　(a) Cu; (b) S

Figure 5. XPS spectra of grade sub-nanoflowers: (a) Cu; (b) S.

DownLoad: Full-Size Img PowerPoint

图 6 (a), (b), (c) 分别为多孔级次纳米花、微米颗粒、微米绒球的氮气吸脱附曲线; (d), (e), (f)为对应的孔径分布曲线

Figure 6. (a), (b), (c) Nitrogen desorption curve of porous grade sub-nanoflowers, micron pompon and micron particles, respectively; (d), (e), (f) the corresponding aperture distribution curve.

DownLoad: Full-Size Img PowerPoint

图 7 (a), (b)分别为纳米枝晶正在生长为纳米花瓣时的TEM图和SEM图; (c)硫源释放S^2– 速率过快导致CuS直接团聚而未能得到纳米花瓣; (d)自组装过程因能量不足导致大量纳米片散落

Figure 7. (a), (b) TEM and SEM images when nanocrystals are growing into nanocrystals, respectively; (c) the S^2– release rate of sulfur source is too fast, which leads to direct aggregation of CuS and fails to obtain nanopetals; (d) a large number of nanosheets were scattered due to lack of energy during the self-assembly process.

DownLoad: Full-Size Img PowerPoint

图 8 (a) CuS多孔级次纳米花, (b) CuS微米绒球, (c) CuS微米颗粒材料吸附MB溶液后上清液吸收谱随吸附时间的变化曲线; (d)表征三份材料对MB的吸附过程

Figure 8. The varied absorption spectra of supernatant after adding (a) porous grade sub-nanoflowers, (b) micron pompon and (c) micron particle material to adsorb MB with changing adsorption time; (d) the adsorption process of MB by adding three materials, respectively.

DownLoad: Full-Size Img PowerPoint

图 9 溶液体系的吸收谱　(a)静置1 h, (b)静置3 h. 插图为吸附体系实物照片（批注：需要把曲线的文字注释和右上角插图中的文字注释中的“微米球”改为“微米绒球”，把“微米椭球”改为“微米颗粒”）

Figure 9. The absorption spectra of the solution system after standing for (a)1 h and (b)3 h; The inset is a physical photo of the adsorption system.

DownLoad: Full-Size Img PowerPoint

图 10 (a)多孔级次纳米花, (b)微米绒球和(c)微米颗粒吸附MB染料分子后的SEM

Figure 10. SEM images of (a) porous grade sub-nanoflowers, (b) micron pompon, and (c) micron particle material after adsorbing MB dye molecules.

DownLoad: Full-Size Img PowerPoint

图 11 (a)多孔级次纳米花对结晶紫, (b)柠檬黄, (c)日落黄, (d)苋菜红的吸附过程中测试离心液的吸收谱线

Figure 11. The absorption spectra of (a) crystal violet, (b) lemon yellow, (c)sunset yellow and (d)amaranth by adding porous grade sub-nanoflowers as nano-adsorbents via centrifugal treatment.

DownLoad: Full-Size Img PowerPoint

图 12 (a)为苋菜红、日落黄、柠檬黄和结晶紫的原始吸收谱; (b), (c)分别为加入多孔级次纳米花材料静置30 min和3 h后溶液吸收谱

Figure 12. (a) The original absorption spectra of amaranth, sunset yellow, lemon yellow and crystal violet; (b), (c) the absorption spectra of the solution after adding porous grade sub-nanoflowers materials for 30 min and 3 h, respectively.

DownLoad: Full-Size Img PowerPoint

表 1 三份样品的Zeta电势

Table 1. Zeta potential of three samples.

样品 Zeta电势/mV

级次纳米花 –13.3
微米绒球 –2.29
微米颗粒 –1.15

DownLoad: CSV

map

[1]	Srivastava S, Sinha R, Roy D 2004 Aquat. Toxicol. 66 319 Google Scholar
[2]	Wu Y, Su M, Chen J, Xu Z, Tang J, Chang X, Chen D 2019 Dyes Pigm. 170 107591 Google Scholar
[3]	Zhang H, Chen M, Wang D M, Xu L L, Liu X D 2016 Opt. Mater. Express 6 2573 Google Scholar
[4]	Miao X, Tang Y, Wong C W 2015 Nature 518 483
[5]	Ghorai S, Sarkar A, Raoufi M, Panda A B, Schönherr H, Pal S 2014 ACS Appl. Mater. Interfaces 6 4766 Google Scholar
[6]	Wu Z, Joo H, Lee K 2005 Chem. Eng. J. 112 227 Google Scholar
[7]	Xie Y J, Yan B, Xu H L, Chen J, Liu Q X, Deng Y H, Zeng H B 2014 ACS Appl. Mater. Interfaces 6 8845 Google Scholar
[8]	Feng M, You W, Wu Z S, Chen Q D, Zhan H B 2013 ACS Appl. Mater. Interfaces 5 12654 Google Scholar
[9]	Yousefi M, Villar-Rodil S, Paredes J I, Moshfegh A Z 2019 J. Alloy. Compd. 809 151783 Google Scholar
[10]	Zhan Y, Wan X, He S, Yang Q, He Y 2018 Chem. Eng. J. 333 132 Google Scholar
[11]	Reddy P A K, Reddy P V L, Kwon E, Kim K, Akter T, Kalagara S 2016 Environ. Int. 91 94 Google Scholar
[12]	Verdin A, Sahraoui A L H, Durand R 2004 Int. Biodeterior. Biodegrad. 53 65 Google Scholar
[13]	Zhang X, Zhang P Y, Wu Z, Zhang L, Zeng G M, Zhou C J 2013 Colloids Surf., A 435 85 Google Scholar
[14]	Yagub M T, Sen T K, Afroze S, Ang H M 2014 Adv. Colloid. Interfaces Sci. 209 172 Google Scholar
[15]	Feng M, You W, Wu Z S, Chen Q D, Zhan H B 2013 ACS Appl. Mater. Inter. 5 12654
[16]	Massey A T, Gusain R, Kumari S, Khatri O P 2016 Ind. Eng. Chem. Res. 55 7124 Google Scholar
[17]	Xie Y J, Yan B, Xu H L, et al. 2014 ACS Appl. Mater. Inter. 6 8845
[18]	Liao W L, Ma Y Q, Chen A Y, Yang Y L 2015 Chem. Eng. J. 271 232 Google Scholar
[19]	Song H J, You S, Jia X H, Yang J 2015 Ceram. Int. 8 23
[20]	Bobbitt N S, Mendonca M L, Howarth A J, et al. 2017 Chem. Soc. Rev. 46 3357 Google Scholar
[21]	Zhao W, Wang Z H, Zhou L, Liu N Q, Wang H X 2016 Front. Mater. Sci. Chin. 10 290 Google Scholar
[22]	赵娟, 胡慧芳, 曾亚萍, 程彩萍 2013 62 158104 Google Scholar Zhao J, Hu H F, Zeng Y P, Cheng C P 2013 Acta Phys. Sin 62 158104 Google Scholar
[23]	Mazaheri H, Ghaedi M, Asfaram A, Hajati S 2016 J. Mol. Liq. 219 667 Google Scholar
[24]	Okpalugo T I T, Papakonstantinou P, Murphy H, McLaughlin J, Brown N M D 2005 Carbon 43 153 Google Scholar
[25]	Dettlaff-Weglikowska U, Skakalova V, Graupner R, et al. 2005 J. Am. Chem. Soc. 127 5125 Google Scholar
[26]	Tseng C H, Wang C C, Chen C Y 2006 Nanotechnology 17 5602 Google Scholar
[27]	Nduna M K, Lewis A E, Nortier P 2014 Colloids Surf., A 441 643 Google Scholar
[28]	Borthakur P, Boruah P K, Das M R 2021 J. Environ. Chem. Eng. 9 104635 Google Scholar
[29]	Gqebe S, Rodriguez-Pascual M, Lewis A 2016 J. S. Afr. Inst. Min. Metall. 116 575 Google Scholar
[30]	Zha Z B, Wang S M, Zhang S H, Qu E Z, Ke H T, Wang J R, Dai Z F 2013 Nanoscale 5 3216 Google Scholar
[31]	Ayodhya D, Venkatesham M, Kumari A S, et al. 2016 J. Exp. Nanosci. 11 418 Google Scholar
[32]	Wang T J, Zhang H, Xu L L, Wang X L, Chen M 2017 Opt. Mater. Express 7 3863 Google Scholar
[33]	Fan Y, Liu P F, Huang Z Y, Jiang T W, Yao K L, Han R 2015 J. Power Sources 280 30 Google Scholar
[34]	Velasco L F, Guillet-Nicolas R, Dobos G, Thommes M, Lodewyckx P 2016 Carbon 96 753 Google Scholar
[35]	Gao S Y, Liu H Y, Geng K R, Wei X J 2015 Nano Energy 12 785 Google Scholar
[36]	Eid K, Wang H J, He P, Wang K M, Ahamad T, Alshehri S M, Yamauchi Y, Wang L 2015 Nanoscale 7 16860 Google Scholar
[37]	Wu K, Zhang Q, Sun D M, Zhu X S, Chen Y, Lu T H, Tang Y W 2015 Int. J. Hydrogen Energy 40 6530 Google Scholar
[38]	Fu G T, Wu K, Lin J, Tang Y W, Chen Y, Zhou Y M, Lu T H 2013 J. Phys. Chem. C. 117 9826 Google Scholar
[39]	Wang T J, Wang D M, Zhang H, Wang X L, Chen M 2017 Opt. Mater. Express 7 924 Google Scholar
[40]	Gao P X, Ding Y, Mai W, Hughes W L, Lao C S, Wang Z L 2005 Science 309 1700 Google Scholar

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