AU2020101505A4 - Method for Preparing Magnetically-Responsive Aminated Cellulose-Based Material for Adsorption of Heavy Metals and Application Method Thereof - Google Patents

Method for Preparing Magnetically-Responsive Aminated Cellulose-Based Material for Adsorption of Heavy Metals and Application Method Thereof Download PDF

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AU2020101505A4
AU2020101505A4 AU2020101505A AU2020101505A AU2020101505A4 AU 2020101505 A4 AU2020101505 A4 AU 2020101505A4 AU 2020101505 A AU2020101505 A AU 2020101505A AU 2020101505 A AU2020101505 A AU 2020101505A AU 2020101505 A4 AU2020101505 A4 AU 2020101505A4
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cellulose
adsorption
magnetically
responsive
based material
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Meixiao CHENG
Hui He
Yanping Hou
Wenyu Huang
Yunhua Li
Zhuo Sun
Fei Xue
Hongxiang Zhu
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Guangxi University
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Abstract

The present invention discloses a preparation method of a magnetically-responsive aminated cellulose-based material for adsorption of heavy metals and application method thereof, where the preparation method includes the following steps of: S1. crushing the cellulose, and dissolving the cellulose in an alkaline/urea aqueous solution under stirring to obtain a transparent cellulose solution; S2. adding an aminating reagent and a superparamagnetic material into the cellulose solution, followed by mixing uniformly, and then adding a cross-linking agent to graft the aminating reagent onto a cellulose chain to obtain modified cellulose; S3. by adjusting a reaction temperature and pH value of the modified cellulose system or adding ethanol, changing the modified cellulose from a liquid state to a solid state to obtain a magnetically-responsive aminated cellulose-based material for adsorption of heavy metals. The magnetically-responsive aminated cellulose-based material for adsorption of heavy metals obtained by the method in the present invention has the characteristics of high amino group density and magnetically-responsiveness, which not only can realize a rapid solid-liquid separation in an external magnetic field, but also has good removal effect and regeneration performance on various heavy metal ions in waterbodies, and can be applied to the field of treatment of heavy metal wastewater.

Description

I METHOD FOR PREPARING MAGNETICALLY-RESPONSIVE AMINATED CELLULOSE-BASED MATERIAL FORADSORPTIONOF HEAVY METALSAND APPLICATION METHOD THEREOF TECHNICAL FIELD
The present invention relates to the technical field of adsorption materials, in
particular to a preparation method of a magnetically-responsive aminated
cellulose-based material for adsorption of heavy metals and an application method
thereof.
BACKGROUND
The prevalence of pollution incidents such as cadmium-polluted rice, blood lead,
and arsenic poisoning have made heavy metal pollution became one of the most
concerned public events; and the treatment of heavy metal ion pollution in water is
difficult and costly due to the characteristics of various types, wide range easy
diffusion, etc. The heavy metal ions pollution in water comes from industrial
wastewater such as mining and metallurgy, mechanical manufacturing, chemical
industry, and electronics industry, primarily including mercury (Hg), nickel (Ni),
copper (Cu), lead (Pb), arsenic (As), chromium (Cr), cadmium (Cd), etc. These
heavy metal ions cannot be degraded by microorganisms in water bodies, but can
only migrate and transform among water, substrates and organisms in different
valence states. When heavy metal ions enter organisms through drinking water
and food chain and accumulate to a certain level through continuous enrichment, it
will cause various diseases and bring irreversible losses to human health and
nature.
At present, the method for removing heavy metal ions from the waterbodies
mainly includes electrolysis, biological wastewater treatment, chemical
precipitation, ion exchange, membrane filtration and the like. Although these methods have good effects on the treatment of heavy metal ions, there are still some shortcomings, for example, the chemical precipitation and electrolysis are not suitable for the treatment of heavy metal ion wastewater with a low concentration, as it is difficult to meet the discharge standard for the wastewater, and sludge or other pollutants will also be generated during the treatment process, resulting in higher treatment cost; the biological wastewater treatment has no universal applicability due to a long period and high requirements on the external environment; although the membrane filtration and the ion exchange are good in treatment effect, they are easily affected by factors such as processing conditions and other impurities in water, with small treatment capacity, and high maintenance cost of equipment. It is worth mentioning that the adsorption process has received wide attention in the field of treating heavy metal ion wastewater due to its advantages of various raw materials, simple operation, and high plasticity. As treatment effect mainly depends on the performance of the adsorption material, the research emphasis in this field is to design and prepare green, efficient, economical, and renewable adsorption materials.
In recent years, cellulose-based adsorbents have attracted much attention in
the field of heavy metal ion adsorption due to wide raw material sources and
environmental friendliness. In order to improve the adsorption properties of
untreated cellulose materials which generally have poor adsorption of heavy metal
ions, various functional groups with adsorption properties, such as-COOH, -OH,
-NH2and -SH, may be introduced into cellulose chains by initiating free radicals,
oxidation, crosslinking, etc. The modified cellulose-based adsorbents has a great
improvement in the adsorption performance of heavy metal ions. However, in most
researches, there are some problems such as low content of functional groups,
slow adsorption rate for heavy metal ions, poor regeneration effect and difficult
recovery of adsorbents. Therefore, designing and synthesizing a cellulose-based adsorbents which is convenient to recover and has good adsorption performance and regeneration performance on heavy metal ions is still the research focus in the art, and problems faced by researchers.
SUMMARY
The present invention aims to solve the technical problems of slow adsorption
rate of heavy metal ions, poor regeneration effect and difficult recovery of
adsorbents in the conventional cellulose-based material for adsorption of heavy
metals, and provides a preparation method of renewable and environment-friendly
magnetically-responsive aminated cellulose-based material for adsorption of
heavy metals which is fast in adsorption rate for multiple heavy metal ions, good in
regeneration performance, convenient in recovery and high in amino group density
and application method thereof.
The present invention solves the technical problems by the following technical
schemes:
The present invention discloses a preparation method of a
magnetically-responsive aminated cellulose-based material for adsorption of
heavy metals, which includes the following steps of:
S1. dissolution of cellulose: crushing the cellulose, and dissolving the cellulose
in an alkaline/urea aqueous solution under stirring to obtain a transparent cellulose
solution;
S2. grafting reaction: adding an aminating reagent and a superparamagnetic
material into the cellulose solution, followed by mixing uniformly, and then adding
a cross-linking agent to graft the aminating reagent onto a cellulose chain to obtain
modified cellulose;
S3. curing: by adjusting a reaction temperature and pH value of the modified
cellulose system or adding ethanol, changing the modified cellulose from a liquid
state to a solid state to obtain a magnetically-responsive aminated cellulose-based material for adsorption of heavy metals.
In step S1, the cellulose comes from bagasse pulp, bamboo pulp, eucalyptus
pulp or cotton; the cellulose is ground and sieved through a 200-mesh screen.
In step S1, the alkaline/urea aqueous solution is prepared by mixing NaOH or
LiOH, urea or thiourea and H20 at a mass ratio of 7:12:81, the mixture is frozen for
8 h at -160 C, and the cellulose and alkaline/urea aqueous solution are dissolved at
a mass ratio of 1:25.
In step S2, a molar ratio of the added aminating agent to the cellulose is
1:1-2:1, the amountof added superparamagnetic material is 0.1% of the mass of
cellulose, and a molar ratio of the added crosslinking agent to the cellulose is
:1-10:1; the reaction is carried out for 2 h at room temperature after the
crosslinking agent is added.
In step S2, the aminating agent is polyethyleneimine, polyamide or branched
polyamines; the superparamagnetic material is Fe304 or y-Fe203; and the
cross-linking agent is epichlorohydrin or glycidyl methacrylate.
In step S3, a reaction temperature of the modified cellulose system is adjusted
in a range of 50°C-70 0C, and the pH value is adjusted in a range of 5-8, so that an
amino group density of the prepared magnetically-responsive aminated
cellulose-based material for adsorption of heavy metals is more than 7.0 mmol/g.
An application method of the magnetically-responsive aminated
cellulose-based material for adsorption of heavy metals prepared by the method
provided by the present invention includes the following operation steps of:
S1. adsorption of heavy metal ions: dispersing a certain amount of
magnetically-responsive aminated cellulose-based material for adsorption of
heavy metals in an aqueous solution containing single or multiple heavy metal ions,
and adsorbing for a period of time to achieve adsorption equilibrium; or placing the
adsorption material in an adsorption column to form a fixed bed, and allowing the aqueous solution containing the heavy metal ions to pass through the fixed bed from top to bottom to realize the adsorption of heavy metal ions in waterbodies;
S2. recovery of adsorption material: after the adsorption of heavy metal ions in
water achieves equilibrium, placing the magnetically responsive aminated
cellulose-based material for adsorption of heavy metals in an external magnetic
field, which will gather to the strongest position of the magnetic field, and
recovering the adsorption materials by a rapid solid-liquid separation without
filtration;
S3. regeneration of adsorption material: placing the recovered adsorption
material in the eluent, desorbing heavy metal ions on the material to realize the
regeneration of the material for being reused.
The heavy metal ions include anionic Cr (VI) and heavy metal ions with
metallicity weaker than Fe (III).
According to the present invention, starting from a homogeneous reaction
system of cellulose, simultaneously introducing amino groups at C2, C 3 and C6
positions of the cellulose, dissolving the cellulose by using an alkaline/urea
aqueous solution, adding a superparamagnetic material and an aminating agent,
grafting the aminating agent onto the cellulose chain through a cross-linking agent,
and coating the superparamagnetic material in the cellulose-based material
through a sol-gel phase inversion method, and preparing the
magnetically-responsive aminated cellulose-based material for adsorption of
heavy metals.
Compared with the prior art, the present invention has the following beneficial
effects:
(1) In the present invention, the cellulose is grafted and modified in a
homogeneous system, and the amination reagent is a macromolecular polyamine,
which effectively overcomes the deficiency of low grafting rate of heterogeneous graft modification of the cellulose; in addition, amino groups may be simultaneously introduced at C2, C 3 and C6 positions of the cellulose, which increases the density of functional groups of the material and effectively improves the adsorption performance of the material for heavy metal ions.
(2) In the present invention, the superparamagnetic materials are introduced
simultaneously in the process of cellulose modification to make the materials
magnetically responsive, which not only facilitates recycling in an external
magnetic field, but also helps to increase the adsorption rate and adsorption
capacity of the material for heavy metal ions.
(3) The magnetically-responsive aminated cellulose-based material for
adsorption of heavy metals prepared by the present invention is applied to the
treatment of heavy metal ion wastewater, which not only has good adsorption
performance, but also can complete adsorption within 10 min, and also has good
regeneration performance, with regeneration rate still remaining above 96% after
times of desorption-regeneration cycling.
(4) The magnetically-responsive aminated cellulose-based material for
adsorption of heavy metals obtained by the method may be applied in the field of
adsorption and concentration of heavy metal ions and environmental treatment in
waterbodies, and the field of the treatment of industrial wastewater generated in
the production and processes of mining, metallurgy, mechanical manufacturing,
chemical industry and electronics, as well as domestic wastewater and the like.
DETAILED DESCRIPTION
The present invention is further described below with reference to specific
examples, which are not to be construed as limiting the present invention. Without
departing from the spirit and essence of the present invention, simple
modifications or replacements to the methods, steps or conditions of the present
invention are within the scope of the present invention; unless otherwise specified, the technical means used in the examples are conventional means well known to those skilled in the art.
Unless otherwise specified, the reagents, methods and apparatus employed in
the present invention are conventional in the art. Unless otherwise specified, the
reagents and materials used in the present invention are commercially available.
Example 1
1. A preparation method includes the following steps:
(1) firstly bagasse pulp cellulose was crushed and sieved through a 200-mesh
screen, a NaOH/urea/H20solution was mixed at a mass ratio of 7:12:81, and then
frozen at -16 0 C for 8 h to obtain an alkaline/urea aqueous solution; the bagasse
pulp cellulose and alkaline/urea aqueous solution were weighed at a mass ratio of
1:25, and the bagasse pulp cellulose was dissolved in the alkaline/urea aqueous
solution under high-speed stirring to obtain a transparent cellulose solution;
(2) polyethyleneimine and Fe304 were added to the cellulose solution at a
molar ratio of 1:1, stirred uniformly, epichlorohydrin was slowly added to the
cellulose at a molar ratio of 5:1, and the mixture was reacted at room temperature
for 2 h to obtain modified cellulose, where the amount of added Fe304 is 0.1% of
the mass of cellulose;
(3) the reaction system was adjusted to 50 0C, and stirred for 2 h to obtain a
granular magnetically-responsive aminated cellulose-based material for
adsorption of heavy metals, where the amino group density was 8.18 mmol/g
measured by elemental analysis.
2. An application method is as follows:
(1) a certain amount of magnetically-responsive aminated cellulose-based
material for adsorption of heavy metals was dispersed in an aqueous solution
containing anionic Cr (VI), achieving adsorption equilibrium within 8 min; or the
adsorption material was placed in an adsorption column to form a fixed bed, and an aqueous solution containing Cr (VI) was allowed to pass through the fixed bed from top to bottom to realize adsorption of Cr (VI) in waterbodies;
(2) the material after adsorption was placed in an external magnetic field,
which would gather to the strongest position of the magnetic field, a solid-liquid
separation was realized within 30 s, and the adsorption material was recovered;
(3) the recovered adsorption material was placed in a NaOH solution to desorb
the heavy metal ions on the material to realize regeneration and utilization of the
material, where the regeneration rate still remained above 98% after 10 times of
regeneration cycling.
Example 2
1. A preparation method includes the following steps:
(1) firstly bamboo pulp cellulose was crushed and sieved through a 200-mesh
screen, a LiOH/thiourea/H20solution was mixed at a mass ratio of 7:12:81, and
then frozen at -16 0 C for 8 h to obtain an alkaline/urea aqueous solution; the
bamboo pulp cellulose and alkaline/urea aqueous solution were weighed at a mass
ratio of 1:25, and the bamboo pulp cellulose was dissolved in the alkaline/urea
aqueous solution under high-speed stirring to obtain a transparent cellulose
solution;
(2) polyamide and y-Fe203were added to the cellulose solution at a molar ratio
of 1:1, stirred uniformly, epichlorohydrin was slowly added to the cellulose at a
molar ratio of 5:1, and the mixture was reacted at room temperature for 2 h to
obtain modified cellulose, where the amount of added y-Fe203 is 0.1% of the mass
of cellulose;
(3) the reaction system was adjusted to 70 0C, and stirred for 2 h to obtain a
granular magnetically-responsive aminated cellulose-based material for
adsorption of heavy metals, where the amino group density was 7.50 mmol/g
measured by elemental analysis.
2. An application method is as follows:
(1) a certain amount of magnetically-responsive aminated cellulose-based
material for adsorption of heavy metals was dispersed in an aqueous solution
containing single or multiple heavy metal ions with metal properties weaker than
Fe (III), such as Cu (II), Pb (II), Cd (II), Ni (II), Hg (II), Ag (I) and the like,
achieving adsorption equilibrium within 10 min; or the adsorption material was
placed in an adsorption column to form a fixed bed, and an aqueous solution
containing heavy metal ions was allowed to pass through the fixed bed from top to
bottom to realize the adsorption of heavy metal ions;
(2) the material after adsorption was placed in an external magnetic field,
which would gather to the strongest position of the magnetic field, a solid-liquid
separation was realized within 30 s, and the adsorption material was recovered;
(3) the recovered adsorption material was placed in a HCI solution to desorb
heavy metal ions on the material so as to realize regeneration and utilization of the
material, where the regeneration rate still remained above 96% after 10 times of
regeneration cycling.
Example 3
1. A preparation method includes the following steps:
(1) firstly eucalyptus pulp cellulose was crushed and sieved through a
200-mesh screen, a NaOH/thiourea/H20 solution was mixed at a mass ratio of
7:12:81, and then frozen at -16 0 C for 8 h to obtain an alkaline/urea aqueous
solution; the eucalyptus pulp cellulose and alkaline/urea aqueous solution were
weighed at a mass ratio of 1:25, and the eucalyptus pulp cellulose was dissolved in
the alkaline/urea aqueous solution under high-speed stirring to obtain a
transparent cellulose solution;
(2) branched polyethyleneimine and y-Fe203 were added to the cellulose
solution at a molar ratio of 2:1, stirred uniformly, glycidyl methacrylate was slowly
.LU
added to the cellulose at a molar ratio of 10:1, and the mixture was reacted at
room temperature for 2 h to obtain modified cellulose, where the amount of added
y-Fe203 is 0.1% of the mass of cellulose;
(3) the pH value of the system was adjusted to 5 by using hydrochloric acid,
and continuously stirred for 2 h to obtain a granular magnetically-responsive
aminated cellulose-based material for adsorption of heavy metals, where the
amino group density was 11.42 mmol/g measured by elemental analysis.
2. An application method is as follows:
(1) a certain amount of magnetically-responsive aminated cellulose-based
material for adsorption of heavy metals was dispersed in an aqueous solution
containing anionic Cr (VI), achieving adsorption equilibrium within 5 min; or the
adsorption material was placed in an adsorption column to form a fixed bed, and an
aqueous solution containing Cr (VI) was allowed to pass through the fixed bed from
top to bottom to realize adsorption of Cr (VI) in waterbodies;
(2) the material after adsorption was placed in an external magnetic field,
which would gather to the strongest position of the magnetic field, a solid-liquid
separation was realized within 30 s, and the adsorption material was recovered;
(3) the recovered adsorption material was placed in a NaOH solution to desorb
the heavy metal ions on the material to realize regeneration and utilization of the
material, where the regeneration rate still remained above 98% after 10 times of
regeneration cycling.
Example 4
1. A preparation method includes the following steps:
(1) firstly cotton cellulose was crushed and sieved through a 200-mesh screen,
a LiOH/urea/H20solution was mixed at a mass ratio of 7:12:81, and then frozen at
-16 0 C for 8 h to obtain an alkaline/urea aqueous solution; the cotton cellulose and
alkaline/urea aqueous solution were weighed at a mass ratio of 1:25, and the
II
cotton cellulose was dissolved in the alkaline/urea aqueous solution under
high-speed stirring to obtain a transparent cellulose solution;
(2) branched polyamide and Fe304were added to the cellulose solution at a
molar ratio of 2:1, stirred uniformly, glycidyl methacrylate was slowly added to the
cellulose at a molar ratio of 10:1, and the mixture was reacted at room
temperature for 2 h to obtain modified cellulose, where the amount of added Fe304
is 0.1% of the mass of cellulose;
(3) the pH value of the system was adjusted to 8 by using hydrochloric acid,
and continuously stirred for 2 h to obtain a granular magnetically-responsive
aminated cellulose-based material for adsorption of heavy metals, where the
amino group density was 10.85 mmol/g measured by elemental analysis.
2. An application method is as follows:
(1) a certain amount of magnetically-responsive aminated cellulose-based
material for adsorption of heavy metals was dispersed in an aqueous solution
containing single or multiple heavy metal ions with metal properties weaker than
Fe (III), such as Cu (II), Pb (II), Cd (II), Ni (II), Hg (II), Ag (I) and the like,
achieving adsorption equilibrium within 8 min; or the adsorption material was
placed in an adsorption column to form a fixed bed, and an aqueous solution
containing heavy metal ions was allowed to pass through the fixed bed from top to
bottom to realize the adsorption of heavy metal ions;
(2) the material after adsorption was placed in an external magnetic field,
which would gather to the strongest position of the magnetic field, a solid-liquid
separation was realized within 30 s, and the adsorption material was recovered;
(3) the recovered adsorption material was placed in a HCI solution to desorb
heavy metal ions on the material so as to realize regeneration and utilization of the
material, where the regeneration rate still remained above 97% after 10 times of
regeneration cycling.
Example 5
1. A preparation method includes the following steps:
(1) firstly bagasse pulp cellulose was crushed and sieved through a 200-mesh
screen, a LiOH/thiourea/H20 solution was mixed at a mass ratio of 7:12:81, and
then frozen at -16 0 C for 8 h to obtain an alkaline/urea aqueous solution; the
bagasse pulp cellulose and alkaline/urea aqueous solution were weighed at a mass
ratio of 1:25, and the bagasse pulp cellulose was dissolved in the alkaline/urea
aqueous solution under high-speed stirring to obtain a transparent cellulose
solution;
(2) branched polyethyleneimine and Fe304 were added to the cellulose solution
at a molar ratio of 1.5:1, stirred uniformly, glycidyl methacrylate was slowly added
to the cellulose at a molar ratio of 7.5:1, and the mixture was reacted at room
temperature for 2 h to obtain modified cellulose, where the amount of added Fe304
is 0.1% of the mass of cellulose;
(3) the pH value of the system was adjusted to 7 by using hydrochloric acid,
and continuously stirred for 2 h to obtain a granular magnetically-responsive
aminated cellulose-based material for adsorption of heavy metals, where the
amino group density was 9.15 mmol/g measured by elemental analysis.
2. An application method is as follows:
(1) a certain amount of magnetically-responsive aminated cellulose-based
material for adsorption of heavy metals was dispersed in an aqueous solution
containing anionic Cr (VI), to achieving adsorption equilibrium within 5 min; or the
adsorption material was placed in an adsorption column to form a fixed bed, and an
aqueous solution containing Cr (VI) was allowed to pass through the fixed bed from
top to bottom to realize adsorption of Cr (VI) in waterbodies;
(2) the material after adsorption was placed in an external magnetic field,
which would gather to the strongest position of the magnetic field, a solid-liquid
-I__
separation was realized within 30 s, and the adsorption material was recovered;
(3) the recovered adsorption material was placed in a NaOH solution to desorb
the heavy metal ions on the material to realize regeneration and utilization of the
material, where the regeneration rate still remained above 98% after 10 times of
regeneration cycling.
Example 6
1. A preparation method includes the following steps:
(1) firstly eucalyptus pulp cellulose was crushed and sieved through a
200-mesh screen, a NaOH/urea/H20solution was mixed at a mass ratio of 7:12:81,
and then frozen at -16 0 C for 8 h to obtain an alkaline/urea aqueous solution; the
eucalyptus pulp cellulose and alkaline/urea aqueous solution were weighed at a
mass ratio of 1:25, and the eucalyptus pulp cellulose was dissolved in the
alkaline/urea aqueous solution under high-speed stirring to obtain a transparent
cellulose solution;
(2) polyamide and Fe304were added to the cellulose solution at a molar ratio of
1.5:1, stirred uniformly, epichlorohydrin was slowly added to the cellulose at a
molar ratio of 7.5:1, and the mixture was reacted at room temperature for 2 h to
obtain modified cellulose, where the amount of added Fe304 is 0.1% of the mass of
cellulose;
(3) a proper amount of ethanol was added into the system, and continuously
stirred for 2 h to obtain a granular magnetically-responsive aminated
cellulose-based material for adsorption of heavy metals, where the amino group
density was 8.92 mmol/g measured by elemental analysis.
2. An application method is as follows:
(1) a certain amount of magnetically-responsive aminated cellulose-based
material for adsorption of heavy metals was dispersed in an aqueous solution
containing single or multiple heavy metal ions with metal properties weaker than
Fe (III), such as Cu (II), Pb (II), Cd (II), Ni (II), Hg (II), Ag (I) and the like,
achieving adsorption equilibrium within 10 min; or the adsorption material was
placed in an adsorption column to form a fixed bed, and an aqueous solution
containing heavy metal ions was allowed to pass through the fixed bed from top to
bottom to realize the adsorption of heavy metal ions;
(2) the material after adsorption was placed in an external magnetic field,
which would gather to the strongest position of the magnetic field, a solid-liquid
separation was realized within 30 s, and the adsorption material was recovered;
(3) the recovered adsorption material was placed in a HCI solution to desorb
heavy metal ions on the material so as to realize regeneration and utilization of the
material, where the regeneration rate still remained above 96% after 10 times of
regeneration cycling.

Claims (5)

  1. Claims: 1. A preparation method of a magnetically-responsive aminated cellulose-based material for adsorption of heavy metals, wherein the method comprises the following steps of: S1. dissolution of cellulose: crushing the cellulose, and dissolving the cellulose in an alkaline/urea aqueous solution under stirring to obtain a transparent cellulose solution; S2. grafting reaction: adding an aminating reagent and a superparamagnetic material into the cellulose solution, followed by mixing uniformly, and then adding a cross-linking agent to graft the aminating reagent onto a cellulose chain to obtain modified cellulose; S3. curing: by adjusting a reaction temperature and pH value of the modified cellulose system or adding ethanol, changing the modified cellulose from a liquid state to a solid state to obtain a magnetically-responsive aminated cellulose-based material for adsorption of heavy metals.
  2. 2. The preparation method of a magnetically-responsive aminated cellulose-based material for adsorption of heavy metals according to claim 1, wherein in step S1, the cellulose comes from bagasse pulp, bamboo pulp, eucalyptus pulp or cotton; the cellulose is ground and sieved through a 200-mesh screen, wherein in step S2, the aminating agent is polyethyleneimine, polyamide or branched polyamines; the superparamagnetic material is Fe304 or y-Fe203; the cross-linking agent is epichlorohydrin or glycidyl methacrylate.
  3. 3. The preparation method of a magnetically-responsive aminated cellulose-based material for adsorption of heavy metals according to claim 1 or 2, wherein in step S1, the alkaline/urea aqueous solution is prepared by mixing NaOH or LiOH, urea or thiourea and H20 at a mass ratio of 7:12:81, the mixture is frozen for 8 h at -160 C, and the cellulose and alkaline/urea aqueous solution are dissolved at a mass ratio of 1:25.
  4. 4. The preparation method of a magnetically-responsive aminated cellulose-based
    material for adsorption of heavy metals according to claim 1 or 2, wherein in step S2,
    a molar ratio of the added aminating agent to the cellulose is 1:1-2:1, the amount of
    added superparamagnetic material is 0.1% of the mass of cellulose, and a molar ratio
    of the added crosslinking agent to the cellulose is 5:1-10:1; the reaction is carried out
    for 2 h at room temperature after the crosslinking agent is added.
  5. 5. An application method of the magnetically-responsive aminated cellulose-based
    material for adsorption of heavy metals prepared according to claim 1, comprising the
    following steps:
    S1. adsorption of heavy metal ions: dispersing a certain amount of
    magnetically-responsive aminated cellulose-based material for adsorption of heavy
    metals in an aqueous solution containing single or multiple heavy metal ions, and
    adsorbing for a period of time to achieve adsorption equilibrium; or placing the
    adsorption material in an adsorption column to form a fixed bed, and allowing the
    aqueous solution containing the heavy metal ions to pass through the fixed bed from
    top to bottom to realize adsorption of the heavy metal ions in waterbodies;
    S2. recovery of adsorption material: after the adsorption of heavy metal ions in
    water achieves equilibrium, placing the magnetically responsive aminated
    cellulose-based material for adsorption of heavy metals in an external magnetic field,
    which will gather to the strongest position of the magnetic field, and recovering the
    adsorption materials by a rapid solid-liquid separation without filtration; and
    S3. regeneration of adsorption material: placing the recovered adsorption material
    in an eluent, desorbing heavy metal ions on the material to realize the regeneration of
    the material for being reused.
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