From Figure 3.38, it can be seen that the durability of the catalyst
is relatively good, this is proved by three tests of photocatalytic
activity durability of 98%, 92.39% and 91%, respectively. The
decrease in decomposition efficiency may be due to the increase in
the coverage of catalysts by RR-195 as well as by-products, in
addition to the reduction of Fe concentration in the catalyst. Due to
the filtration process is also the cause of reduced catalytic activity.
The results in Figure 3.38 show that the oxidation efficiency of
the Fe-MIL-88B/GO catalyst remained almost unchanged after three
reuse to deplete RR-195, showing that the Fe- MIL-88B/GO is very
stable and can be used for repeated decomposition of RR-195 dyes
27 trang |
Chia sẻ: honganh20 | Ngày: 05/03/2022 | Lượt xem: 285 | Lượt tải: 0
Bạn đang xem trước 20 trang tài liệu Research on synthesizing new composite materials system based on mofs containing fe and graphene oxide as photocatalysts in decomposing dyes in water environment, để xem tài liệu hoàn chỉnh bạn click vào nút DOWNLOAD ở trên
trend of metallic
mechanical frame materials, in this thesis, we focus on synthesizing
3
MOFs materials without using organic, nano-structured solvents
(nano Fe-BTC/GO) and Fenton photocatalyst application for the
treatment of organic pigments (reactive dyes RR-195 and RY-145) in
aqueous environment. The thesis title is “Research on synthesizing
new composite materials system based on MOFs containing Fe and
graphene oxide as photocatalysts in decomposing dyes in water
environment”
* Main research contents of the thesis:
- Research on synthesizing some new nano composite materials,
based on nano Fe-MIL-53, Fe-MIL-88B, Fe-BTC and GO (graphene
oxide) by different methods such as solvent heat, hydrothermal ,
micro-hydropower and mechanical grinding.
- Study the structural, morphological and physicochemical
properties of synthetic materials by modern physical and chemical
methods such as XRD, FTIR, SEM, TEM, XPS, EDX, BET, TG-DTA,
UV -Vis.
- Evaluation of photochemical catalyst using visible light in the
decomposition of dyes RR-195, RY-145 on synthetic materials.
- Comparison of the above catalytic systems to find the most
effective catalyst in decomposition of RR-195 and RY-145 dyes.
- Study the main influencing factors such as pH, H2O2
concentration, initial color concentration to decomposition efficiency
of organic pigments.
- Study on catalytic durability as well as regeneration and reuse
potential of catalysts.
- Proposing the path to decomposition of organic color through
intermediate products formed during the decomposition process.
* Thesis structure
The thesis consists of 146 pages, 99 figures, 15 tables and 142
references. The thesis layout consists of the following sections:
introduction, 3 chapters of content and conclusions. The new
4
contributions of the thesis are published in 05 specialized scientific
journals, including 02 international scientific journals and 02 national
scientific journals.
Chapter 1. Literature review
Chapter 1 is presented in 38 pages, including general introduction
of MOFs, methods of synthesizing MOFs, and application of MOFs.
In MOFs applications, catalyst applications are quite new and have
not been studied much in Vietnam. MOFs act as catalysts in the
decomposition reactions of toxic organic substances, pigments, dyes.
In order to enhance the functionality and applicability, new
composite materials based on the mechanical metal frame material
are of special interest. Recently, a number of composite materials
based on nano MOFs and nano carbon such as nano MIL53/rGO,
MIL88/GO, MIL101/rGO as well as MIL53, MIL88 and MIL101
containing Fe/CNT have been synthesized and evaluated with optical
activity. High catalyst in the decomposition reaction of organic
substances, organic pigments in water environment [9-11]. Therefore,
the use of MOFs/GO nanocomposite photocatalytic materials to treat
dyes is practical and of high scientific significance. From the
overview of the research situation on MOFs materials at home and
abroad, we can see that nanostructured MOFs are a new generation of
MOFs material superior to conventional MOFs because of special
features. such as small particle size (nm), large capillary size (nm),
large surface area, large porous volume increases heat transfer, mass
transfer, speed diffusion of reaction substances to centers operating
with high dispersion. The process of micro-hydrothermal
crystallization creates particles of small size, acting as a catalyst with
redox potential. Studies aimed at reducing the time to germinate and
5
develop MOFs are also a solution to synthesize nanoparticle-sized
MOFs.
Chapter 2. Experimental
Chapter 2 is presented in 20 pages including:
2.1. Chemistry
2.2. Process of synthesizing materials
- Synthesis of some Fe-BDC/GO composite materials (Fe-MIL-
53/GO, Fe-MIL-88B/GO) by solvent thermal method.
- Synthesis of Fe-BTC/GO composite nanocomposite materials by
solvent thermal method, hydrothermal (at 60oC, 90oC, 120oC),
hydrothermal - microwave (at 90oC with periods of 10, 20, 30, 40)
minute).
- Synthesis of Fe-BTC material (at 20, 40, 60, 80 minutes) and Fe-
BTC/GO composite material (60 minutes) by mechanical mechanical
crushing.
- Research photocatalytic process in the reaction of reactive dye
decomposition of synthesized catalysts.
- Studying RR-195 dye decomposition pathway on Fe-MIL-88B/GO
catalyst through intermediate products determined by liquid-mass
chromatography (LC-MS).
2.3. Characterisation Techniques
- Material characteristics by modern physical methods, using
equipment in Vietnam and Korea: XRD, XPS, EDX, SEM, TEM,
BET, FT-IR, TGA, UV-Vis.
2.4. Method to assess photocatalytic ability of materials in
photocatalytic process in decomposition of dyes
- Develop a model to evaluate photocatalytic activity of materials in
the decomposition reaction RR-195 and RY-145.
6
- Analysis and evaluation of intermediate products formed during the
RR-195 decomposition process on Fe-Mil-88B/GO excavator.
Calculate the efficiency of the decomposition process.
Chapter 3. Results and Discussions
Chapter 3 is presented in 80 pages including:
3.1. Characteristics of structure and morphology of catalytic
systems
3.1.1. X-ray diffraction (XRD)
5 10 15 20 25 30
0
500
1000
1500
2000
2500
3000
3500
C
ư
ờ
n
g
đ
ộ
(
a
.u
)
Góc 2 độ
Fe-MIL-88/GO
Fe-MIL-88
Fe-MIL-53/GO
Fe-MIL-53
Fig. 3.2. XRD patterns of Fe-MIL-53, Fe-MIL-88B, Fe-MIL-53/GO and
Fe-MIL-88B/GO
The XRD patterns of Fe-MIL-53/GO, Fe-MIL-88B/GO materials
appear all the same pic as those of Fe-MIL-53, Fe-MIL-88B
materials. However, the peak intensity at 2θ~11o characteristic of GO
structure sharply decreased and almost no appearance was observed.
This can be explained by the fine dispersion of Fe-MIL-53, Fe-MIL-
88B crystals on the surface of GO layers. The XRD patterns of Fe-
BTC/GO materials synthesized by different methods appears peaks
with the intensity at 2θ ~ 5.8o; 7,8o; 12o; 13.7o; 17,6o and 22,1o are
corresponding to the diffraction planes (012); (104); (110)
characteristic of Fe-BTC structure [125]. However, the 2θ~11o peak
that characterizes GO structure plummeted and almost no occurrence.
2θ (degree)
In
te
n
si
ty
(
a
.u
)
7
This is explained by the dispersion, and alternation of Fe-BTC
material on the surface of GO layers.
Fig.3.6. XRD patterns of Fe-BTC NDM, Fe-BTC/GO were
synthesized by different methods
In the sample Fe-BTC/GO-30 synthesized by hydrothermal-
microwave (30 minutes) has a peak intensity at 2θ ~12o, more
2θ (degree) 2θ (degree)
2θ (degree)
2θ (degree)
2θ (degree)
I
n
te
n
si
ty
(
a
.u
)
In
te
n
si
ty
(
a
.u
)
I
n
te
n
si
ty
(
a
.u
)
8
balanced than Fe-BTC/GO samples synthesized by solvent thermal,
hydrothermal, and mechanical mechanical methods. The XRD pattern
show that Fe-BTC/GO materials synthesized by hydrothermal -
microwave (30 minutes) have a stable crystal phase structure, high
crystallinity.
3.1.2. Scanning electron microscopy (SEM) and Transmission
electron microscopy (TEM)
In Figure 3.10, TEM image of Fe-MIL-88B material shows small
pseudo-Fe nanoparticles of size 5-8 nm, fastened on the surface of
Fe-MIL-88B crystals. On the TEM image of Fe-MIL-88B/GO
composite material, Fe nanoparticles tend to cluster to form larger
particles (the size increases from 5-8 nm to 10-20 nm. ). This may be
due to the interaction between Fe ions with hydroxyl and carboxylic
groups in GO to form Fe complex.
Fig.3.10. TEM image of GO (A), Fe-MIL-88B(B) and Fe-MIL-
88B/GO(C)
9
Fig. 3.14. SEM image of Fe-BTC/GO tổng hợp bằng các phương pháp khác
nhau (a) Fe-BTC/GO –NDM; (b) Fe-BTC/GO-90oC; (c) Fe-BTC/GO VS-
30; (d) Fe-BTC/GO NC-60
As shown in Figure 3.14 (a), the material Fe-BTC/GO-NDM has
Fe-BTC nanoparticles unevenly dispersed on the surface layers of
GO, the particles are uneven in size and tend to contract. Clustered
together to form large crystals of about 120-150 nm. Figure 3.14 (b)
of Fe-BTC/GO-90oC material found that Fe-BTC particles are
dispersed evenly on the surface layer of GO, Fe-BTC nanoparticle
size is in the range of 60 - 80 nm. Some Fe-BTC particles tend to
cluster in sizes between 80 and 100 nm. Fe-BTC/GOVS-30 material
(Figure 3.14 c) has Fe-BTC particles of uniform size and evenly
distributed over the surface of GO, the particle size is about 40-50
nm. Fe-BTC/GO materials synthesized by mechanical grinding
(Figure 3.14d) have a particle size of 100-150 nm and Fe-BTC
particles are unevenly dispersed on the GO layers. Thus, SEM image
of Fe-BTC/GO materials synthesized by different methods show that
Fe-BTC/GOVS-30 materials (synthesized by hydrothermal-
microwave) have Fe- BTC is evenly dispersed on GO carriers and
has a nanoparticle size of about 40 -50 nm. This is explained by the
rapid germination and development of Fe-BTC crystals, so the
crystallization process takes place quickly to help control the size of
the crystal particle.
3.1.3. Energy-dispersive X-ray spectroscopy (EDX)
Table 3.1. Composition of elements in materials Fe-MIL-53/GO and
Fe-MIL-88B/GO
Materials Fe-MIL-53/GO Fe-MIL-88B/GO
Element % wt % atomic % wt % atomic
C 64.54 73.60 63.93 73.52
O 28.95 24.76 28.56 24.63
Fe 6.51 1.64 7.51 1.85
Table 3.1 shows that the Fe content in Fe-MIL-53/GO and Fe-MIL-
88B/GO materials accounts for 6.51% and 10.02%, respectively
(according to Fe theory, 10.02%, 7.51% by weight, respectively).
10
This is explained by the amount of Fe does not react with H2BDC
ligand so the washing process is washed out into the environment.
Table 3.4. Composition of elements in Fe-BTC/GO materials
synthesized by different methods
Samples Element C O Fe Cl Total
Fe-BTC-NDM % wt 62.99 30.69 6.20 0.12 100
% atomic 72.07 26.36 1.53 0.04 100
Fe-BTC/GO
NDM
% wt 66.76 28.91 4.21 0.12 100
% wt 74.66 24.29 1.01 0.04 100
Fe-BTC/GO 90oC % wt 62.48 30.42 7.02 0.08 100
% atomic 71.94 26.29 1.74 0.03 100
Fe-BTC/GO-30 %wt 61.75 31.25 6.93 0.07 100
% atomic 71.09 27.17 1.71 0.03 100
Fe-BTC/GO-NC %wt 68.74 27.66 3.49 0.11 100
% atomic 76.13 23.00 0.83 0.04 100
Table 3.4 shows the main components of Fe-BTC/GO materials
including C, O Fe, Cl. However, Fe content depends on different
synthesis methods. By various synthetic methods such as solvent
heat, hydrothermal, microwave, and mechanical grinding, the
percentage of iron mass 4.21%, 7.02%, 6.93%, 3.49%, respectively.
3.1.4. N2 adsorption–desorption isotherms (BET)
Table 3.5 shows the surface area and total capillary volume, the
average capillary width of materials Fe-MIL-53/GO, Fe-MIL-
88B/GO increases compared to Fe-MIL-53, Fe -MIL-88B. This is
explained by the uniform distribution of Fe-MIL-53, Fe-MIL-88B on
the GO layers to help improve the porosity and size of Fe-MIL-53,
Fe-MIL-88B crystals [117]. Moreover, the crystals of Fe-MIL-53,
Fe-MIL-88B are dispersed on GO layers smaller than the original Fe-
MIL-53, Fe-MIL-88B crystals, this is explained. by the epoxy groups
on the GO layers preventing the clumping and agglomeration of the
crystals Fe-MIL-53, Fe-MIL-88B, resulting in the formation of Fe-
11
MIL-53, Fe-MIL-88B nanoparticles on the GO carrier. This also
contributes to the specific surface of the material. In Table 3.5 Fe-
MIL-88B/GO materials have the largest surface area (99 m2/g).
Table 3.5. Textual characteristics of Fe-MIL-53, Fe-MIL-88B, Fe-
MIL-53/GO and Fe-MIL-88B/GO
Samples SBET (m
2/g) Vpore (cm
3/g) DBJH (nm)
Fe-MIL-53 62 0.14 4.1 – 7.2
Fe-MIL-53/GO 80 0.21 10.2 – 20.3
Fe-MIL-88B 89 0.15 3.2 – 7.4
Fe-MIL-88B/GO 99 0.23 12.2 – 21.3
Table 3.9. Textual characteristics of Fe-BTC and Fe-BTC/GO
synthesized by different methods
Samples SBET (m
2/g) Vpore (cm
3/g) DBJH (nm)
Fe-BTC-NDM 349 0.55 2.2 – 3.2
Fe-BTC/GO-NDM 376 1.33 12.5 – 23.7
Fe-BTC/GO-90oC 786 0.82 5.9 -7.2
Fe-BTC/GO-30 1015 1.13 6.5-8.2
Fe-BTC/GO-NC 60 849 0.65 7.4-18.4
Table 3.9 shows that Fe-BTC/GO material has a high specific
surface area (376 - 1015 m2/g) and a large total capillary volume
(0.82-1.33 cm3/g) compared to the material. Fe-BTC. Fe-BTC/GO
materials have an average increase in capillary width compared to
Fe-BTC samples, which is favorable for adsorption and diffusion
processes. This is explained by the dispersion of Fe-BTC crystals on
the GO carrier (GO has a layered structure). Fe-BTC/GO-30 material
(synthesized by microwave hydrothermal method for 30 minutes) has
the largest surface area and a large total capillary volume. This is
explained by the fact that Fe-BTC/GO is synthesized by micro-
hydrothermal method with small particle size of about 40-50 nm,
12
uniformly distributed on the GO carrier layer and stable phase
structure, high crystallinity (Figure 3.6).
3.1.5. Fourier transform infrared spectroscopy (FTIR)
Fig. 3.24. FTIR spectra of Fe-MIL-53, Fe-MIL-88B, Fe-MIL-53/GO
and Fe-MIL-88B/GO
FTIR spectrum of Fe-MIL-53/GO and Fe-MIL-88B/GO is almost
identical to Fe-MIL-53 and Fe-MIL-88 except for two low-intensity
oscillations occurring at 2339-2360 cm-1 relates to the saturated and
unsaturated CH oscillations, showing the interaction between MIL53,
MIL-88B and GO. The absorption band at the top of 759-711 cm-1 is
characteristic related to the oscillation of the BTC ligands. The peaks
at 750 cm-1 correspond to the C-H strain variation of benzene. High
strength peaks of 624 cm-1 characterize the oscillation of the Fe - O
bond [140].
T
ra
n
sm
it
a
n
ce
(
%
T
)
Wavenumber (cm-1)
13
Fig. 3.27. FTIR spectra of Fe-BTC/GO synthesized by different
methods
3.1.6. X-ray Photoelectron Spectroscopy (XPS)
Complete survey of XPS, C1s, O1s and Fe2p spectra for Fe-MIL-
88B, Fe-MIL-88B/GO is shown in Figure 3.30. Figure 3.30a and c
show optoelectronic currents with binding energies of 284 eV, 530
eV, and 711 eV corresponding to C1s, O1s and Fe2p. In Figures
3.30b and d show four vertices at about 284.9; 286.2; 288.1 and
289.5 eV correspond to the C-C, C-O, C=O and O-C=O links [141].
In addition, the shift of the C1s band to higher binding energies
shows the interaction of carbon in H2BDC and carbon in GO.
Moreover, the increase in peak intensity of the C-C group, and the
decrease of the peak intensity of the C-O groups, C=O and O-C=O of
Fe-MIL-88B/GO compared to Fe-MIL-88B, showing the interaction
between Fe-MIL-88B and GO in Fe-MIL-88B/GO materials. In the
Số sóng (cm-1)
T
ra
n
sm
it
a
n
ce
(
%
T
)
(%
T
)
Wavenumber (cm-1)
14
XPS spectrum of O1s (Figure 3.30e), there are 2 peaks at 531.7 and
533.7eV corresponding to Fe-O-C bonds. In Fe2p spectrum of Fe-
MIL-88B/GO (Figure 3.30f), there are two peaks at 711.9 and
725.7eV corresponding to Fe2p3/2 of Fe2O3 and Fe2p1/2 of α-FeOOH
[126-129 ].
Hình 3.30. Phổ XPS của Fe-MIL88B (c, d) và compozit Fe-
MIL88B/GO (a) (b) C1S; (e) O1S; (f) Fe2p
Fig. 3.28. XPS of Fe-MIL88B (c, d) và compozit Fe-MIL88B/GO (a)
(b) C1S; (e) O1S; (f) Fe2p
3.1.7. Results of TGA analysis of Fe-BTC/GO materials
As shown in Figure 3.37, Fe-BTC/GO materials synthesized by
different methods have high thermal stability (300oC). The higher
this temperature, the combustion of thermal decomposition occurs.
a b
c d
e
f
15
Fig. 3.30. TGA of Fe-BTC/GO samples
3.1.8. Results of UV-vis solid analysis of Fe-BTC/GO materials
Fig. 3.31. Energy gap of Fe-BTC/GO materials is synthesized by
different methods
The energy of the Eg region of Fe-BTC/GO material synthesized
by hydrothermal-microwave method (30 minutes) is 2.2eV;
FeBTC/GO synthesized by hydrothermal method is 2.4 eV; Fe-
BTC/GO synthesized by mechanical grinding method is 2.48 eV
which is less than the band gap energy of Fe-BTC material (2.5 -2.7
eV) [132]. The presence of the external GO carrier helps disperse the
Fe-BTC crystals evenly, creating small sized particles, the GO carrier
is very important to receive electrons from the conduction area of
photocatalyst MOFs, minimizing recombination between electrons
(
a
h
v
)1
/2
(e
V
)1
/2
Temperture (oC)
%
w
t
hv (eV)
16
and h+ holes and effectively increasing catalytic activity as well as
catalytic durability [129]. The results of solid UV-Vis analysis
showed that Fe-BTC/GO materials synthesized by hydrothermal-
microwave method (30 minutes) had the smallest value (2.2 eV), so it
had the best catalytic activity.
3.2. Evaluation of photocatalytic activity of synthesized materials
3.2.1. Evaluate catalytic activity of dye decomposition RR-195 of
Fe-BDC/GO catalyst
3.2.1.1. Comparison of dye decomposition activity of RR-195 dye
on Fe-BDC and Fe-BDC / GO catalysts
Fig. 3.33. Catalytic activity of Fe-MIL-53, Fe-MIL-88B, Fe-MIL-53/
GO, Fe-MIL-88B/GO in dye decomposition RR-195
To compare the catalytic activity of synthetic catalyst systems
include: Fe-MIL-53, Fe-MIL-53/GO, Fe-MIL-88B, Fe-MIL-88B/GO
during RR-195 was performed under conditions: initial RR-195
concentration was 100 mg/L; the amount of catalyst is 0.3g/L; H2O2
concentration is 136 mg/L; pH = 5.5; temperature T = 25oC and
together lighting.
From the results obtained, we can see that Fe-MIL-53/GO and Fe-
MIL-88B/GO are much more photochemical than Fe-MIL-53 and Fe-
MIL-88B. This proves the synergistic effect of Fe-MIL-53, Fe-MIL-
Time (min)
C
/C
o
17
88B with GO. From Figure 3.33, the catalytic activity of Fe-MIL-
88B/GO is much higher than that of Fe-MIL-53/GO. This can be
explained by the higher surface area of Fe-MIL-88B/GO (99 m2/g)
than that of Fe-MIL-53/GO (80 m2/g).
3.2.1.3. Study on factors affecting RR-195 dye decomposition ability
of Fe-MIL-88B/GO catalyst materials
Effect of pH: To investigate the effect of pH, we performed RR-
195 decomposition reaction on Fe-MIL-88B/GO composite material
at different pH values. The experiments were conducted at three
different pH values: 3.0; 5.5 and 8.0 under the same conditions: H2O2
(30%) 136 mg/L, catalyst content of 0.3g/L, RR-195 concentration of
100 ppm, temperature t = 25oC and lighting for 25 minutes. The
results showed that, with pH = 3.0, the rate of RR-195 decomposition
took place quickly, when increasing pH = 5.5, the rate of RR-195
decomposition was slower but still achieved a conversion efficiency
of 98% after 25. minute (same as at pH = 3). When pH> 6 efficiency
decomposition process sharply reduced. Therefore pH=5.5 is selected
for the next research process.
Effect of H2O2 concentration: Similar experiments were conducted at
different H2O2 concentrations: 68 mg/L; 136 mg/L and 204 mg/L
with the same reaction conditions. Results showed that the
decomposition process RR-195 increased as the concentration of
H2O2 increased. When H2O2 concentration increased from 68 to 136
mg/L after 25 minutes, process efficiency increased sharply and
reached 98%. This is because the •OH radicals from H2O2 are highly
generated which promotes the reaction process leading to increased
speed and degradation efficiency. However, when continuing to
increase the amount of H2O2 (6mL/L) in the solution, this excess
18
H2O2 will work with the •OH radical to form the HOO• reduce the
efficiency of the decomposition process.
3.2.1.3. Evaluate the activity of Fe-MIL-88B/GO catalyst materials
under different conditions
Figure 3.37A shows that under the condition of oxidation reaction
under sunlight and without catalyst, the conversion of RR-195 is
negligible. In Figure 3.37B, the adsorption process takes place
quickly and reaches equilibrium after 25 minutes of reaction. The
adsorption efficiency of RR-195 on catalyst reaches 25%. During
Fenton reaction (in the presence of catalyst, H2O2), after 25 minutes
of reaction, the efficiency reached 75% (Figure 3.37C). However, in
the Photo-Fenton process (in the presence of catalysts, H2O2 and
lighting) the efficiency reached 98% (Figure 3.37D). From these
results, we found that the Fe-MIL-88B/GO composite has a high RR-
195 decomposition efficiency.
Fig. 3.37. Decomposition process RR-195 on Fe-MIL-88B/GO catalyst
under different conditions
Time (min)
19
3.2.1.4. Study on Fe-MIL-88B / GO catalyst durability
Fig. 3.38. Stability of catalytic activity over Fe-MIL-88B/GO
From Figure 3.38, it can be seen that the durability of the catalyst
is relatively good, this is proved by three tests of photocatalytic
activity durability of 98%, 92.39% and 91%, respectively. The
decrease in decomposition efficiency may be due to the increase in
the coverage of catalysts by RR-195 as well as by-products, in
addition to the reduction of Fe concentration in the catalyst. Due to
the filtration process is also the cause of reduced catalytic activity.
The results in Figure 3.38 show that the oxidation efficiency of
the Fe-MIL-88B/GO catalyst remained almost unchanged after three
reuse to deplete RR-195, showing that the Fe- MIL-88B/GO is very
stable and can be used for repeated decomposition of RR-195 dyes
3.2.1.5.RR-195 decomposition pathway of Fe-MIL-88B/GO catalyst
The intermediate product of the decomposition process RR-195
of Fe-BTC/GO photochemical catalyst was analyzed by liquid
chromatography with mass spectrometry on LC-MS. shown in the
image below:
Figure 3.39. The intermediate product of the RR-195 decomposition
reaction uses Fe-MIL-88B/GO catalyst
20
The decomposition process of RR-195 on Fe-MIL-88B/GO catalyst is
carried out in 3 main steps: cutting S bonding circuit, followed by N cutting
circuit and finally short-circuit hydrocarbons.
3.2.2. Evaluate the catalytic activity of dye decomposition on Fe-BTC/GO
catalytic systems
3.2.2.4. Comparison of Fe-BTC/GO catalytic activity synthesized by
different methods
As shown in Figure 3.45, samples of Fe-BTC / GO materials synthesized
by different methods (solvent heat, hydrothermal, microwave -
hydrothermal, mechanical chemistry) have high catalytic activity in the
reaction. decomposition reaction RY-145.
Fe-BTC/GO materials synthesized by hydrothermal-microwave methods
have the highest catalytic activity. This is explained by the Fe-BTC/GO
material with stable structure, uniformly distributed over the surface of the
GO, the particle size of about 40-50nm, a high surface area (1015 m2/g).
Good for diffusion and adsorption process, so catalytic activity is high. This
helps Fe to combine with carboxyl groups to create Fe(OH)2, FeO makes
strong photochemical center, thereby reacting with H2O2 to create •OH
more, making higher reaction efficiency. Moreover, Fe-BTC/GOVS-30
materials have a lower band energy of 2.2 eV than those of Fe-BTC/GO
90oC (2.4 eV) and Fe-BTC/GONDM (2.48 eV) conducive to absorbing
visible light.
21
Figure 3.44. Evaluation of Fe-BTC/GO catalyst activity
synthesized by different methods (RY-145 concentration is 100 ppm,
catalyst: 0.3g/L, H2O2: 136 mg/L, pH = 6.5 )
3.2.2.5. Study on factors affecting RY-145 decomposition on Fe-
BTC / GO-30 catalyst materials
Influencing factors such as pH, H2O2 concentration and catalytic
stability during dye decomposition were investigated. The results
show that the best condition in the decomposition process RY-145 is
pH=3; H2O2 concentration is 13 mg/L. The durability of Fe-
BTC/GO-30 catalysts is highly durable, almost unchanged after three
uses. This result opens up the possibility of photocatalytic
applications in the treatment of toxic organic substances. From the
table of results comparing the photocatalytic systems on MOFs, we
can see the photocatalytic systems (Fe-MIL-53/GO, Fe-MIL-88B/GO
and Fe-BTC/GO) in The thesis has high activity in decomposition
reaction of organic pigments. Moreover, the synthesized
photocatalysts in the thesis are much more active than the published
results (fewer catalysts, higher concentration of dyes, shorter
processing time to achieve effective results). removal rate of organic
pigments).
Time (min)
C
/C
o
22
CONCLUSION
1. Successfully synthesized Fe-MIL-53/GO, Fe-MIL-88B/GO
materials by solvent thermal method. The results of XRD, FT-IR,
XPS analysis shows that Fe-MIL-53, Fe-MIL-88B crystals can
disperse and lie in the bonds of the GO layers, a new phase appears
α-FeOOH in Fe-MIL-88B/GO. The formation of this phase is due to
the interaction between Fe of MIL-88B and hydroxyl group,
carboxylic group of GO. From the TEM image of the Fe-MIL-53/GO
composite material, Fe-MI
Các file đính kèm theo tài liệu này:
- research_on_synthesizing_new_composite_materials_system_base.pdf