A Unique Interactive Nanostructure Knitting based Passive Sampler Adsorbent for Monitoring of Hg2+ in Water

This work reports the development of ultralight interwoven ultrathin graphitic carbon nitride (g-CN) nanosheets for use as a potential adsorbent in a passive sampler (PAS) designed to bind Hg2+ ions. The g-CN nanosheets were prepared from bulk g-CN synthesised via a modified high-temperature short-time (HTST) polycondensation process. The crystal structure, surface functional groups, and morphology of the g-CN nanosheets were characterised using a battery of instruments. The results confirmed that the as-synthesized product is composed of few-layered nanosheets. The adsorption efficiency of g-CN for binding Hg2+ (100 ng mL−1) in sea, river, rain, and Milli-Q quality water was 89%, 93%, 97%, and 100%, respectively, at natural pH. Interference studies found that the cations tested (Co2+, Ca2+, Zn2+, Fe2+, Mn2+, Ni2+, Bi3+, Na+, and K+) had no significant effect on the adsorption efficiency of Hg2+. Different parameters were optimised to improve the performance of g-CN such as pH, contact time, and amount of adsorbent. Optimum conditions were pH 7, 120 min incubation time and 10 mg of nanosheets. The yield of nanosheets was 72.5%, which is higher compared to other polycondensation processes using different monomers. The g-CN sheets could also be regenerated up to eight times with only a 20% loss in binding efficiency. Overall, nano-knitted g-CN is a promising low-cost green adsorbent for use in passive samplers or as a transducing material in sensor applications.

[1]  Bicai Pan,et al.  Enhanced photoresponsive ultrathin graphitic-phase C3N4 nanosheets for bioimaging. , 2013, Journal of the American Chemical Society.

[2]  Marcello M. Veiga,et al.  Processing centres in artisanal gold mining , 2014 .

[3]  Y. Long,et al.  A Sensitive Sensor for trace Hg2+ Determination Based on Ultrathin g-C3N4 Modified Glassy Carbon Electrode , 2015 .

[4]  D. Han.  Synthesis, Characterization, And Application Of Pyrite For Removal Of Mercury , 2013 .

[5]  Yao Zheng,et al.  Graphitic carbon nitride materials: controllable synthesis and applications in fuel cells and photocatalysis , 2012 .

[6]  M. Antonietti,et al.  Synthesis of bulk and nanoporous carbon nitride polymers from ammonium thiocyanate for photocatalytic hydrogen evolution , 2011 .

[7]  M. Karim,et al.  Ligand field effect for Dysprosium(III) and Lutetium(III) adsorption and EXAFS coordination with novel composite nanomaterials , 2017 .

[8]  M. Antonietti,et al.  A metal-free polymeric photocatalyst for hydrogen production from water under visible light. , 2009, Nature materials.

[9]  S. Cao,et al.  Rapid and high-yield production of g-C3N4 nanosheets via chemical exfoliation for photocatalytic H2 evolution , 2015 .

[10]  A. Sari,et al.  Adsorption of Pb(II) and Cr(III) from aqueous solution on Celtek clay. , 2007, Journal of hazardous materials.

[11]  M. R. Awual.  New type mesoporous conjugate material for selective optical copper(II) ions monitoring & removal from polluted waters , 2017 .

[12]  M. Anbia,et al.  Adsorption studies of Pb(II) and Cu(II) ions on mesoporous carbon nitride functionalized with melamine-based dendrimer amine , 2015, International Journal of Environmental Science and Technology.

[13]  Nikolaos Koukouzas,et al.  Removal of heavy metals from wastewater using CFB-coal fly ash zeolitic materials. , 2010, Journal of hazardous materials.

[14]  A. Vollmer,et al.  Alkynyl Ethers of Glucans : Substituent Distribution in Propargyl-, Pentynyl- and Hexynyldextrans and -amyloses and Support for Silver Nanoparticle Formation , 2010 .

[15]  P. Ajayan,et al.  Exfoliated Graphitic Carbon Nitride Nanosheets as Efficient Catalysts for Hydrogen Evolution under Visible Light. , 2013 .

[16]  M. Soleimani,et al.  Elimination of mercury by adsorption onto activated carbon prepared from the biomass material , 2012 .

[17]  M. Sillanpää,et al.  EDTA-Cross-Linked β-Cyclodextrin: An Environmentally Friendly Bifunctional Adsorbent for Simultaneous Adsorption of Metals and Cationic Dyes. , 2015, Environmental science & technology.

[18]  T. Hayat,et al.  Application of graphitic carbon nitride for the removal of Pb(II) and aniline from aqueous solutions , 2015 .

[19]  H. Znad,et al.  A ligand anchored conjugate adsorbent for effective mercury(II) detection and removal from aqueous media , 2018 .

[20]  R. Rajar,et al.  Spatial variations of mercury in sediment of Minamata Bay, Japan. , 2006, The Science of the total environment.

[21]  Abdullah M. Asiri,et al.  Using of g-C 3 N 4 nanosheets for the highly efficient scavenging of heavy metals at environmental relevant concentrations , 2018, Journal of Molecular Liquids.

[22]  M. R. Awual.  Novel conjugated hybrid material for efficient lead(II) capturing from contaminated wastewater. , 2019, Materials science & engineering. C, Materials for biological applications.

[23]  M. R. Abukhadra,et al.  Geochemical evaluation and environmental application of Yemeni natural zeolite as sorbent for Cd2+ from solution: kinetic modeling, equilibrium studies, and statistical optimization , 2017, Environmental Earth Sciences.

[24]  Jinshui Zhang,et al.  Polycondensation of thiourea into carbon nitride semiconductors as visible light photocatalysts , 2012 .

[25]  G. Zou,et al.  Nitrogen-rich carbon nitride hollow vessels: synthesis, characterization, and their properties. , 2010, The journal of physical chemistry. B.

[26]  Shin'ichi Suzuki,et al.  Radioactive cesium removal from nuclear wastewater by novel inorganic and conjugate adsorbents , 2014 .

[27]  M. R. Awual.  Mesoporous composite material for efficient lead(II) detection and removal from aqueous media , 2019, Journal of Environmental Chemical Engineering.

[28]  Jae-Hyuk Yu,et al.  Chemically functionalized silica gel with alkynyl terminated monolayers as an efficient new material for removal of mercury ions from water , 2016 .

[29]  M. Awual,et al.  Solid phase sensitive palladium(II) ions detection and recovery using ligand based efficient conjugate nanomaterials , 2016 .

[30]  Miao Yu,et al.  Ultrasensitive detection of toxic cations through changes in the tunnelling current across films of striped nanoparticles. , 2012, Nature materials.

[31]  Abdullah M. Asiri,et al.  Ultrathin graphitic carbon nitride nanosheets: a low-cost, green, and highly efficient electrocatalyst toward the reduction of hydrogen peroxide and its glucose biosensing application. , 2013, Nanoscale.

[32]  P. Ajayan,et al.  Exfoliated Graphitic Carbon Nitride Nanosheets as Efficient Catalysts for Hydrogen Evolution Under Visible Light , 2013, Advanced materials.

[33]  Xiangke Wang,et al.  Polyaniline Multiwalled Carbon Nanotube Magnetic Composite Prepared by Plasma-Induced Graft Technique and Its Application for Removal of Aniline and Phenol , 2010 .

[34]  Walter Z. Tang,et al.  Green Synthesis of Magnetic EDTA- and/or DTPA-Cross-Linked Chitosan Adsorbents for Highly Efficient Removal of Metals , 2015 .

[35]  M. Sillanpää,et al.  Polyethylenimine-cross-linked cellulose nanocrystals for highly efficient recovery of rare earth elements from water and a mechanism study , 2017 .

[36]  Hui‐Ming Cheng,et al.  Graphene‐Like Carbon Nitride Nanosheets for Improved Photocatalytic Activities , 2012 .

[37]  Li Xu,et al.  Graphene-analogue carbon nitride: novel exfoliation synthesis and its application in photocatalysis and photoelectrochemical selective detection of trace amount of Cu²⁺. , 2014, Nanoscale.

[38]  Qian Liu,et al.  Ultrathin graphitic carbon nitride nanosheet: a highly efficient fluorosensor for rapid, ultrasensitive detection of Cu(2+). , 2013, Analytical chemistry.

[39]  Jun He,et al.  Enhancement of photocatalytic activity of Bi2WO6 hybridized with graphite-like C3N4 , 2012 .

[40]  M. R. Awual.  Assessing of lead(III) capturing from contaminated wastewater using ligand doped conjugate adsorbent , 2016 .

[41]  Shubin Yang,et al.  Highly efficient enrichment of radionuclides on graphene oxide-supported polyaniline. , 2013, Environmental science & technology.

[42]  M. R. Awual.  Novel nanocomposite materials for efficient and selective mercury ions capturing from wastewater , 2017 .

[43]  M. Naushad,et al.  Functional ligand anchored nanomaterial based facial adsorbent for cobalt(II) detection and removal from water samples , 2015 .

[44]  Masaaki Nagatsu,et al.  Carbon nanotubes as adsorbents in environmental pollution management: A review , 2011 .

[45]  M. Khaleque,et al.  Treatment of copper(II) containing wastewater by a newly developed ligand based facial conjugate materials , 2016 .

[46]  Shu-quan Zhu,et al.  Mercury enrichment in coal fire sponge in Wuda coalfield, Inner Mongolia of China , 2018 .

[47]  G. Dong,et al.  A fantastic graphitic carbon nitride (g-C3N4) material: Electronic structure, photocatalytic and photoelectronic properties , 2014 .

[48]  M. R. Awual.  A novel facial composite adsorbent for enhanced copper(II) detection and removal from wastewater , 2015 .

[49]  Jiaxing Li,et al.  Few-layered graphene oxide nanosheets as superior sorbents for heavy metal ion pollution management. , 2011, Environmental science & technology.

[50]  M. Antonietti,et al.  Polymeric Graphitic Carbon Nitride for Heterogeneous Photocatalysis , 2012 .

[51]  M. Awual,et al.  Encapsulation of cesium from contaminated water with highly selective facial organic–inorganic mesoporous hybrid adsorbent , 2016 .

[52]  M. Hashmi,et al.  Vibrational properties of carbon nitride films by Raman spectroscopy , 1998 .

[53]  Abdullah M. Asiri,et al.  Ultrathin graphitic carbon nitride nanosheets: a novel peroxidase mimetic, Fe doping-mediated catalytic performance enhancement and application to rapid, highly sensitive optical detection of glucose. , 2013, Nanoscale.

[54]  Yixue Chen,et al.  Sorption of copper(II) onto super-adsorbent of bentonite-polyacrylamide composites. , 2010, Journal of hazardous materials.

[55]  A. Heidari,et al.  Thiol-incorporated activated carbon derived from fir wood sawdust as an efficient adsorbent for the removal of mercury ion: Batch and fixed-bed column studies , 2016 .

[56]  M. Khraisheh,et al.  Efficient detection and adsorption of cadmium(II) ions using innovative nano-composite materials , 2018, Chemical Engineering Journal.

[57]  Jinyun Liu,et al.  A 2D-g-C3N4 nanosheet as an eco-friendly adsorbent for various environmental pollutants in water. , 2017, Chemosphere.

[58]  M. Awual,et al.  Facile mercury detection and removal from aqueous media involving ligand impregnated conjugate nanomaterials , 2016 .

[59]  W. Hu,et al.  Low-temperature plasma synthesis of carbon nanotubes and graphene based materials and their fuel cell applications. , 2013, Chemical Society reviews.

[60]  M. Karim,et al.  Inorganic-organic based novel nano-conjugate material for effective cobalt(II) ions capturing from wastewater , 2017 .

[61]  Shin'ichi Suzuki,et al.  Selective cesium removal from radioactive liquid waste by crown ether immobilized new class conjugate adsorbent. , 2014, Journal of hazardous materials.

[62]  Yongqiang Dong,et al.  Graphitic Carbon Nitride Materials: Sensing, Imaging and Therapy. , 2016, Small.

[63]  G. Mckay,et al.  Removal of cobalt (II) ions from aqueous solutions utilizing the pre-treated 2-Hypnea Valentiae algae: Equilibrium, thermodynamic, and dynamic studies , 2018 .

[64]  İ. Tosun,et al.  Lead removal from aqueous solution by natural and pretreated clinoptilolite: adsorption equilibrium and kinetics. , 2007, Journal of hazardous materials.

[65]  A. Alsaedi,et al.  Interaction mechanism of radionickel on Na-montmorillonite: Influences of pH, electrolyte cations, humic acid and temperature , 2016 .

[66]  M. Dinu,et al.  Kinetics, equilibrium modeling, and thermodynamics on removal of Cr(VI) ions from aqueous solution using novel composites with strong base anion exchanger microspheres embedded into chitosan/poly(vinyl amine) cryogels , 2017 .

[67]  Qing Zhou,et al.  The ultra-rapid synthesis of 2D graphitic carbon nitride nanosheets via direct microwave heating for field emission. , 2016, Chemical communications.