Project Details

Student Name Mohd Amirul Bin Md Zain

Student ID 2015836448

Faculty Faculty of Chemical Engineering

Project Title Preparation of Cellulose- Based Hydrogel

Prepared Via Pre-Cooled Dissolving Method and

Optimising of Hydrogel

Project Description This experiment focuses on the optimizing of

cellulose- based hydrogel which is the best

condition in production of cellulose- based

hydrogel. In this experiment we will use chemical

such as cellulose powder, Epichlorohydrin (ECH),

an aqueous solution of sodium hydroxide NaOH,

urea and distilled water. The parameter of this

experiment is the formation of hydrogel and

percentage yield in the hydrogel.

Supervisor Dr Sarifah Fauziah Binti Syed Draman

Research Area Cellulose- based Hydrogel

Project Duration (Semester) Semester 5 (September 2017- January 2018)

Research/ Project Base/ Location UITM Bukit Besi

PROJECT EXECUTIVE SUMMARY

Introduction

Hydrogel consist of three-dimensional hydrophilic polymer network which able to absorb

large amount of water and solution. Because of their sorption capacity, hydrogels have been
massively used as water retaining devices, mostly the field of personal hygiene products and
in agriculture pharmaceutical, biomedical and catalysis. Hydrogels derived from natural
polymers, especially polysaccharides. Among polysaccharides, cellulose is the most abundant
one, obtainable worldwide and it combines hydrophilicity with good mechanical properties. It
is a biodegradable and biocompatible material, which could be extracted from plants,
bacteria, algae and even animals. From literature, in the present study, cellulose from was
used to produce cellulose hydrogel. The effect of cellulose on the new dissolving system
using NaOH/urea was investigated. The formation and optimisation of cellulose hydrogel
produced using epichlorohydrin agent was studied.

Objective of Study
The main objective is:
1. To prepare cellulose based-hydrogel from using NaOH/urea and cellulose powder.
2. To optimise condition to find the higher yield of hydrogel.

Scope of Study
This experiment focuses on the optimizing of cellulose- based hydrogel which is the best
condition in production of cellulose- based hydrogel. In this experiment we will use chemical
such as cellulose powder, Epichlorohydrin (ECH), an aqueous solution of sodium hydroxide
NaOH, urea and distilled water. The parameter of this experiment is the formation of
hydrogel and percentage yield in the hydrogel. The experiment is conduct in 12 experiment
with the different percentage of concentration of NaOH/urea.

Instrumentation

 Stirrer hot plate

 Magnetic stirrer bar
 100ml beaker
 100ml measuring cylinder
 Spatula
 Freezer/Refrigerator
 Fourier transform infrared spectroscopy (FTIR)
 Thermometer
EXTRACTION OF CELLULOSE AND PREPARATION OF CELLULOSE- BASED
HYDROGEL PREPARED VIA PRE-COOLED DISSOLVING METHOD AND
OPTIMISING OF HYDROGEL

Bleaching Process
(DEDEDED)

Stage D

(NaOH + Acetic Acid + Distilled Water)

Conducted at 80◦C for 2

hour in water both
Stage E

1 : 20

(NaOH + Lepironia Conifera)

Lepironia Conifera was washed with

distilled water Dried at 105◦C for 24
hour

Pure cellulose

Prepared different ratio 1. Pre-cooled to -13◦C in a

freezer
NaOH l Urea l LC or Pure 2. The mixture was thawed for
Cellulose 10 minutes

Cellulose Solution
Stirred for 3 hour at room
temperature

ECH (Epichlorohydrin)

Hydrogel
 Weekly Progress Report

Commencing Week: 1
Date : 14.9.17
Planning/Work Done

Each of team members do the research to find the suitable method in producing cellulose
based hydrogel. The suitable journals for our purpose are list down.

The first journal is title “Highly porous regenerated cellulose hydrogel and aerogel prepared
from hydrothermal synthesized cellulose carbamate”. The main finding is the preparation
method to produce hydrogel. The method is kenaf core powder is dissolved in LiOH/urea
solution at -13ᵒC low temperature. According to the rapid dissolution method, resulting
mixture was stirred rapidly for 5 min to obtain the homogeneous cellulose solution compared
to pre-cooled method that required several cooling process. The solution was then centrifuged
at 10000 rpm for 5 min at 5ᵒC to remove any air bubbles and to separate the cellulose
solution and undissolved cellulose. In a typical hydrogel synthesis procedure, the cross-
linking agent epichlorohydrin solution (5%) was added drop wise into the cellulose solution.
The resulting viscous cellulose solution was stirred at room temperature for approximately 1
h until the hydrogel was formed.

The second journal is “Properties of Cellulose Hydrogel from Kenaf Core Prepared via Pre-
cooled Dissolving Method”. This journal used pre-cooled dissolving method to produce
hydrogel. KC powder was added into an aqueous mixture of NaOH/urea. The mixture was
pre-cooled to −13ᵒC in a freezer. The mixture was thawed and vigorously stirring for 10 min
to obtain the transparent solution and was subjected to centrifugation at 10000 rpm for 10
min for degassing and excluding the undissolved cellulose fraction. The cellulose solution
obtained in the previous section was used to produce hydrogel using epichlorohydrin (ECH),
as crosslinking agent. The mixture of the cellulose solution and ECH was stirred for 3 h to
produce hydrogel at room temperature.

The third journal is “Synthesis and Characterization of Cellulose-Based Hydrogels to Be

Used as Gel Electrolytes”. Solution contain Cellulose, urea and NaOH is undergoes low
temperature (between −13 and −15 °C) by several freezing-thawing cycles up to the
achievement of a transparent 4 wt. % cellulose solution. The solution was then poured into a
Petri dish and ECH 5 vol. % was added dropwise at room temperature (RT) under magnetic
stirring. After 1 h, the Petri dish was placed into freezer at −30 °C for 20 h. After thawing the
solid at RT, the hydrogel was obtained within 24 h.

Prepared By: Checked By

 Weekly Progress Report

Commencing Week: 2
Date : 21.9.17
Planning/Work Done

Meeting with the supervisor to show the proper method to use in our experiment for
production of cellulose based hydrogel.

PRE-COOLING DISSOLUTION OF KC POWDER

1. The cellulose solution prepared with different ratio of NaOH/urea/KC powder.
2. KC powder was added into an aqueous mixture of NaOH/urea.
3. The mixture was pre-cooled to −13ᵒC in a freezer.
4. The mixture was thawed and vigorously stirring for 10 min to obtain the transparent
solution and was subjected to centrifugation at 10000 rpm for 10 min for degassing
and excluding the undissolved cellulose fraction.
5. The undissolved cellulose was washed with excess of water

FORMATION OF HYDROGEL
1. The cellulose solution obtained in the previous section was used to produce hydrogel
using epichlorohydrin (ECH), as crosslinking agent.
2. The mixture of the cellulose solution and ECH was stirred for 3 h to produce hydrogel
at room temperature.
3. The hydrogel obtained was washed with deionized water to remove excess NaOH and
urea and oven dried before further characterizations.

Supervisor approved the method but we need to change the kenaf core powder to pure
cellulose powder because the laboratories do not provide them.

Prepared By: Checked By

 Weekly Progress Report

Commencing Week: 3
Date : 24.9.17
Planning/Work Done

All the material and chemical has been checked in the laboratory. We confirmed the material
and chemical with En. Zam and Pn. Aida. However, the first experiment cannot be done
because the lab had some maintenance because of leaking. The maintenance occurred for the
whole weeks.

Prepared By: Checked By

 Weekly Progress Report

Commencing Week: 4
Date : 5.10.17
Planning/Work Done

Find more information regarding the process flow. This is because we still not understand the
experiment fully. The pre-cooling dissolution method part is the confusing part and need
some guideline from supervisor. We decided to make an appointment with the supervisor to
get more clarify about the experiment.

Prepared By: Checked By

 Weekly Progress Report

Commencing Week: 5
Date :8.10.17
Planning/Work Done

Second meeting with supervisor. Our supervisor briefly explains the detail process flow of
production of hydrogel. So we can plan when we can run the experiment. First of all,
supervisor asked us to make a trial sample to make sure our method that we used can produce
hydrogel. This is because our laboratory has limited cellulose powder and epichlorohydrin.
The first trial experiment will be conduct on week 6 after the semester break.

Prepared By: Checked By

 Weekly Progress Report

Commencing Week: 6
Date : 22.10.17- 26.10.17
Planning/Work Done

The first experiment we run with 2g NaOH, 1g Urea and 1g cellulose in different beaker.
Then we put them in 50ml of distilled water to be stir on magnetic stirrer. The solution is stir
until homogenous colourless liquid formed. We stir for almost 4 days but the homogenous
colourless liquid do not formed. We realized that we made a mistake because the solution
need to stir in low temperature condition to produce the homogenous solution.

The first experiment is fail.

Prepared By: Checked By

 Weekly Progress Report

Commencing Week: 7
Date : 30.10.17
Planning/Work Done

Third meeting with supervisor at Makmal Kimia. Supervisor look at our previous result of
experiment and we have some discussion.

1. Redo the experiment with 3g NaOH, 3g Urea, 2g cellulose and 50ml distilled water.
2. Stir in low temperature solution of NaOH and Urea while cellulose solution are stir on
magnetic stirrer with ice.
3. After 2 hours, solution of NaOH and Urea is pour into cellulose solution and stir with
ice until homogenous colourless liquid formed.

On the next day, we run the experiment on get the homogenous colourless liquid.

After centrifuge for 30 minutes at 4000 rpm, we get the undissolved cellulose. The
undissolved cellulose then crosslinking with epichlorohydrin to produce hydrogel.

Prepared By: Checked By

 Weekly Progress Report

Commencing Week: 8
Date : 5.11.2017- 9.11.2017
Planning/Work Done

We start with the Run 1 until Run 4 which is :

 Run 1 : 4g NaOH, 4g Urea and 2g cellulose
 Run 2 : 8g NaOH, 4g Urea and 2g cellulose
 Run 3 : 4g NaOH, 8g Urea and 2g cellulose
 Run 4 : 8g NaOH, 8g Urea and 2g cellulose

However, only two run able to produce hydrogel at the end which is Run 2 and Run 4. This is
because Run 1 unable to form homogenous colourless liquid while Run 3 (the solution in the
beaker fall while stir). The Run 2 and Run 4 is crosslinking with epichlorohydrin and stir for
3 hours.

After 3 hours, we get the hydrogel. The hydrogel is weigh to get the percent yield.

Prepared By: Checked By

 Weekly Progress Report

Commencing Week: 9
Date : 12.11.2017- 16.11.2017
Planning/Work Done

We run again the experiment of Run 3 and produce the hydrogel but Run 1 still not produce
homogenous colourless solution. Then we proceed to next run which is:

 Run 5 : 6g NaOH, 6g Urea and 2g cellulose

 Run 6 : 6g NaOH, 6g Urea and 2g cellulose
 Run 7 : 6g NaOH, 6g Urea and 2g cellulose
 Run 8 : 6g NaOH, 6g Urea and 2g cellulose

Unfortunately all the run above do not produce homogeneous colourless solution after follow
procedure. We try to further freeze and left for 24 hours the Run 7 and the stir back. It is
work and form homogenous colourless. The Run 7 formed the hydrogel. Some error occur
cause beaker for Run 5 to fall down while stirring. Run 6 and 8 form hydrogel at the end.

Prepared By: Checked By

 Weekly Progress Report

Commencing Week: 10
Date : 19.11.2017- 23.11.2017
Planning/Work Done

We continue experiment with the Run:

 Run 9 : 6g NaOH, 8.8g Urea and 2g cellulose

 Run 10 : 3.2g NaOH, 6g Urea and 2g cellulose
 Run 11 : 3.2g NaOH, 6g Urea and 2g cellulose
 Run 12 : 6g NaOH, 3.2g Urea and 2g cellulose

Run 9-12 form homogenous colourless solution after mixed together the NaOH, Urea and
cellulose. Then, we centrifuge them at 4000 rpm for 30 minutes. The undissolved cellulose
then weight to calculate the solubility. After that, the undissolved cellulose was cross-linking
with epichlorohydrin to produce hydrogel. The hydrogel is weigh to find the yield.

Prepared By: Checked By

 Weekly Progress Report

Commencing Week: 11
Date : 26.11.2017- 30.11.2017
Planning/Work Done

We repeat the experiment that has failure before which is Run 1 and Run 5.

 Run 1 : 4g NaOH, 4g Urea and 2g cellulose

 Run 5 : 6g NaOH, 6g Urea and 2g cellulose

Run 1& 5 form homogenous colourless solution after mixed together the NaOH, Urea and
cellulose. Then, we centrifuge them at 4000 rpm for 30 minutes. The undissolved cellulose
then weight to calculate the solubility. After that, the undissolved cellulose was cross-linking
with epichlorohydrin to produce hydrogel. The hydrogel is weigh to find the yield.

All the weight of hydrogels (yield) is recorded in a table.

Prepared By: Checked By

 Weekly Progress Report

Commencing Week: 12
Date :7.12.2017
Planning/Work Done

Each of team members do the research to find the suitable method in characteristic cellulose
based hydrogel. A suitable article for our purpose are list down:

The article title ‘Synthesis and Characterization of Cellulose-Based Hydrogels to Be Used as

Gel Electrolytes’ use Fourier Transform Infrared spectroscopy (FTIR). FTIR spectra were
recorded using a Bruker ALPHA spectrometer (Billerica, MA, USA) in the 4000–400 cm−1
frequency range, at a resolution of 4 cm−1. Vacuum-dried hydrogel samples were analyzed
by 300 scans in attenuated total reflectance (ATR) mode, while cellulose powder and fibers
were analyzed in KBr discs.

The article also starting by writing the article and methodology first.

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 Weekly Progress Report

Commencing Week: 13
Date : 14.12.2017
Planning/Work Done

12 samples (Run 1- Run 12) in the beaker are transfer to seal glass tube to avoid from
contamination.

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 Weekly Progress Report

Commencing Week: 14
Date :19.12.2017
Planning/Work Done

Two samples which are Run 1 and Run 12 is tested for Fourier Transform Infrared
spectroscopy (FTIR). The frequency range is 4000–400 cm−1. The sample is given to Puan
Aida and the result is given after the experiment done.

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