Wood-derived nanocellulose hydrogel incorporating gold nanoclusters using in situ multistep reactions for efficient sorption and sensitive detection of mercury ion
Graphical abstract
Introduction
Heavy metal pollution has become a well-known environmental concern due to its severe toxicity to living organisms (Ma et al., 2019). Among these heavy metals, Hg2+ ion is considered one of the most hazardous metal ions and can easily convert to higher toxic methylmercury via biological methylation. Hg2+ ion cause irreversible damages such as neurological abnormalities, gingivitis and tumor formation even at low concentrations (Geng et al., 2015). Various methods such as chemical precipitation, membrane filtration, electrochemical separation, ion exchange and adsorption have been developed to remove Hg2+ ion. Adsorption is a useful strategy due to its high efficiency and ease of handling (Berglund and Wieser, 2011; Pu et al., 2018). Designing and synthesising green and highly effective adsorbents is urgently required based on the environmental and sustainable development strategy.
Wood machining residues are a type of forestry waste, and making appropriate use of them is critical for clean, efficient and high-value-added utilisation (Cai et al., 2020). Using wood and wood machining residues, nanocellulose can be derived with good physical, chemical, and biological properties (Xiong et al., 2017). Some high-performance hydrogels for removing heavy metal ions have been developed using nanocellulose, such as nanofibrillated cellulose/polyethyleneimine composite hydrogel for removing copper ion (Li et al., 2018), nanocellulose hydrogel coated titanate-bismuth oxide membrane for efficient anion/cation/oily-water treatment (Xiong et al., 2018) and cellulose nanofibrils/polyurethane hydrogel for removing cadmium ion (Hong et al., 2018). Hence, WCNs are promising candidates for synthesising green and highly effective adsorbents.
Gold nanoclusters (Au NCs) are zero-dimensional nanomaterials used as functional fluorescent probes (Zhang et al., 2015). They own many advanced performances, including unique optical and non-toxic features (Wang et al., 2017). Au NCs have been used to detect Hg2+ in numerous reports (Ansari et al., 2020; Sarkar et al., 2016; Yang et al., 2017). Qiao et al. (2016) synthesised L-amino acid oxidase capped Au NCs using the ‘one-pot’ method in an aqueous solution and showed that these Au NCs could be used as a probe to develop a highly selective and sensitive method for Hg2+. Wei et al. (2010) prepared lysozyme-stabilised Au NCs in basic aqueous solution and found that these Au NCs could be used as a sensor for sensitive and selective Hg2+ detection. However, Au NCs used in the liquid phase are easy to agglomerate with increased detection and storage time (Li et al., 2019). One possible solution to overcome this problem is to develop a stable matrix for incorporating Au NCs, such as WCNs-based hydrogel.
Here, we are interested in producing WNH for Hg2+ detection and sorption. The morphology, structure, fluorescence features, adsorption and detection characteristics of the WNH were investigated. Additionally, the sorption and detection mechanism was confirmed. The economic analysis of the WNH was also explored.
Section snippets
Reagents
Acrylamide (AM, 99 %), N,N’-Methylenebis(acrylamide) (MBA, 99 %), ammonium persulfate (APS, 98 %), 2,2,6,6-Tetramethylpiperidinooxy (TEMPO, 97 %), albumin from bovine serum (BSA, 96 %), chloroauric acid (HAuCl4, 98 %) and sodium hypochlorite pentahydrate (NaClO·5H2O, 40 %) were bought from J&K Scientific Co., Ltd. (China).
Fabrication of WCNs
A mass ratio of 1:50 was used for 20-g of bleached Eucalyptus urophylla pulp with water. Then, 0.16-g TEMPO, 0.8-g NaBr and 12-mL NaClO (5 % chlorine solution) were added and
Preparation of WNH
Fig. 1 shows the fabrication of a schematic of the novel WNH. WCNs were one of the most important materials. First, WCNs, BSA, AM, MBA and HAuCl4 were mixed well. The HAuCl4 underwent a progressive reduction to form Au NCs in situ, and the formed Au NCs were fixed on BSA scaffolds to construct BSA-Au NCs; BSA-Au NCs was connected with WCNs by hydrogen bonding. After that, the PPS initiator was added and AM monomer and MBA cross-linker formed chemical bonds with WCNs to build WNH. Meanwhile, in
Conclusions
A novel wood-derived nanocellulose hydrogel (WNH) was successfully prepared with in situ synthesised Au NCs. The WCNs provided a skeleton for accelerating 3D porous structure and improved the sorption ability for Hg2+; moreover, Au NCs acted as a fluorescent probe for Hg2+ and provided adsorption sites. With a maximum adsorption capacity of 234.4 mg/g, the WNH possessed efficient adsorption properties. Meanwhile, this hydrogel was employed for selective and quantitative Hg2+ detection with a
CRediT authorship contribution statement
Qiuyan Luo: Investigation. Yifeng Huang: Software. Zihua Lei: Investigation. Junwen Peng: Software. Dong Xu: Software. Xin Guo: Conceptualization, Writing - original draft, Validation. Yiqiang Wu: Validation, Supervision.
Declaration of Competing Interest
We declare that we have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
Acknowledgements
Research is financially supported by Hunan Youth Science and Technology Innovation Talent Project (2020RC3043), Training Plan of Young Backbone Teachers in Colleges and Universities of Hunan Province, China (71), Postgraduate Scientific Research Innovation Project of Hunan Province (CX20210880), and National Innovation and Entrepreneurship Training Program for College Students (202110538001).
References (53)
- et al.
A ligand anchored conjugate adsorbent for effective mercury(II) detection and removal from aqueous media
Chem. Eng. J.
(2018) - et al.
Facile synthesis of polyphenol mediated metal nanocomposites for selective sensing of methylmercury
J. Environ. Chem. Eng.
(2020) - et al.
Facile mercury detection and removal from aqueous media involving ligand impregnated conjugate nanomaterials
Chem. Eng. J.
(2016) - et al.
Nonconventional biocompatible macromolecular AEEgens for sensitive detections and removals of Cu(II) and Fe(III): N and/ or O donor(s) selective coordinations of metal ions
Sensor. Actuat. B-Chem.
(2021) - et al.
Carboxymethlyated cellulose nanofibrils(CMCNFs) embedded in polyurethane foam as a modular adsorbent of heavy metal ions
Carbohyd. Polym.
(2018) - et al.
Chitosan nanoparticle hydrogel based sebacoyl moiety with remarkable capability for metal ion removal from aqueous systems
Int. J. Biol. Macromol.
(2019) - et al.
Pectin-grafted terpolymer superadsorbent via N-H activated strategic protrusion of monomer for removals of Cd(II), Hg(II), and Pb(II)
Carbohyd. Polym.
(2019) - et al.
Shape memory aerogels from nanocellulose and polyethyleneimine as a novel adsorbent for removal of Cu(II) and Pb(II)
Carbohyd. Polym.
(2018) - et al.
Immobilization of two polyelectrolytes leading to a novel hydrogel for high-performance Hg2+ removal to ppb and sub-ppb levels
Chem. Eng. J.
(2018) - et al.
Synthesis and characterization of a new starch/SnO2 nanocomposite for efficient adsorption of toxic Hg2+ metal ion
Chem. Eng. J.
(2016)
Catalyst-free synthesis of triazine-based porous organic polymers for Hg2+ adsorptive removal from aqueous solution
Chem. Eng. J.
Water-soluble gold nanoclusters-based fluorescence probe for highly selective and sensitive detection of Hg2+
Sensor. Actuat. B-Chem.
Detoxification of Hg(II) from aqueous and enzyme media: pristine vs. Tailored calcium alginate hydrogels
Int. J. Biol. Macromol.
Pb2+ and Hg2+ removal from polluted milk by di-acrylated Pluronic P123 hydrogels
Food Chem.
PH dependence and thermodynamics of Hg(II) adsorption onto chitosan-poly(vinyl alcohol) hydrogel adsorbent
Colloid. Surface. A.
Nano-cellulose hydrogel coated flexible titanate-bismuth oxide membrane for trinity synergistic treatment of super-intricate anion/cation/oily-water
Chem. Eng. J.
Sulfathiazole-based novel UV-cured hydrogel sorbents for mercury removal from aqueous solutions
Radiat. Phys. Chem.
Gold nanocluster embedded bovine serum albumin nanofibers-graphene hybrid membranes for the efficient detection and separation of mercury ion
Chem. Eng. J.
Luminescent golden silk and fabric through in situ chemically coating pristine-silk with gold nanoclusters
Biomaterials
A highly efficient polyampholyte hydrogel sorbent based fixed-bed process for heavy metal removal in actual industrial effluent
Water Res.
A renewable, sustainable and low-cost adsorbent for ibuprofen removal
Water Sci. Technol.
Isotopic compositions of the elements 2009 (IUPAC Technical Report)
Pure Appl. Chem.
Full factorial design approach to Hg(II) adsorption onto hydrogels
Arab. J. Sci. Eng.
Synthesis of Pt-loaded NiFe-LDH nanosheets on wood veneer for efficient gaseous formaldehyde degradation
ACS Appl. Mater. Inter.
Nonconjugated biocompatible macromolecular luminogens for sensing and removals of Fe(III) and Cu(II): DFT studies on selective coordination(s) and On-Off sensing
Macromol. Rapid Comm.
Adsorption-assisted decontamination of Hg(II) from aqueous solution by multi-functionalized corncob-derived biochar
RSC Adv.
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