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2024 Vol.41 Issue.4,
Published 2024-07-15
0
2024 Vol. 41 (4): 0-0 [
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] (
203
) [
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1141
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1
Research progress of synthesis and applications of silica nanosheets
WU Caijun, WANG Junzheng
Silica nanosheet as a type of two-dimensional material, especially mesoporous silica nanosheet possessing the characteristics of mesoporous, they have wide applications in the fields of biological medicine, catalysis and adsorption, separation and purification, etc. Lack of layered precursors of silica in nature and the high surface energy of two-dimensional structure lead to the formation of nanosheets with irregular shape, complicated steps, and small mesopore size. Based on the above problems, this review focuses on the domestic and international research literature about the preparation of silica nanosheets, and briefly illustrates the principles, the advantages, and shortages of different preparation methods. Furthermore, the applications of silica nanosheets in the fields of environment, biology, and energy are summarized, and the prospect of the direction of application research in future is made. This review can provide reference for the further study of silica nanosheets.
2024 Vol. 41 (4): 1-12 [
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187
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2958KB] (
477
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13
Synthesis of 2,6-difluorobenzoyl isocyanate by triphosgene method
ZHANG Tianyong, JU Wenchao, JIANG Shuang, LI Bin, LIU Yufeng, ZHANG Pengfei
2,6-Difluorobenzoyl isocyanate (DFBI) is an important intermediate for the synthesis of benzoyl urea pesticides. The synthetic process of DFBI with phosgene is very dangerous, and the cost of preparation of DFBI using oxalyl chloride is high. Bis(trichloromethyl) carbonate (BTC) is a green substitute for the highly toxic phosgene and diphosgene. It not only is low in toxicity, safe and convenient to use, but also has mild reaction conditions, accurate measurement and low price. The DFBI was synthesized by the reaction of BTC with 2,6-difluorobenzamide (FBA), and the effect of single factor on the synthesis of DFBI was studied. The experimental results show that the optimal conditions are as follows: Chlorobenzene is used as the solvent, the molar ratio of feeding is
n
(BTC)∶
n
(FBA)=1.0∶1.5, BTC is equally fed in two times, and the first stage of cold-phosgenation is reacted at -5 ℃ for 1 h, the second stage of thermal-phosgenation is reacted at 126—128 ℃ for 4 h, and the product yield could reach 86.4%. BTC can be used stably and safely, and the process is easy to industrialize.
2024 Vol. 41 (4): 13-19 [
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184
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512
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20
Wavelength-dependent photoaging mechanism of organic thermochromic materials
LI Ruizhen, ZHAO Zhen, LOU Hongfei, LI Wei, LIU Dongzhi, ZHOU Xueqin
Two three-component reversible thermochromic materials, with phenyl benzoate and 1-octadecanol as the solvent respectively, were employed to study the photoaging mechanism of electron-transfer-based organic thermochromic materials. Five light sources with different wavelengths were exerted to illuminate the thermochromic materials. UV light sources have a center wavelength of 254 nm, 302 nm, 365 nm and 395 nm respectively, and the visible light source is a xenon lamp with a wavelength range of 400—1000 nm. The aging progress together with the phenomenon of thermochromic materials were showed and the
1
H NMR spectra of each irradiated-component were analyzed to investigate their changes by the irradiation of different light sources. The retention content of each component was evaluated to discover the different changes of thermochromic materials with the various wavelength of light sources. Our results suggest that UV-light-induced photoaging of thermochromic materials is mainly caused by the photodegradation of components, and visible-light-induced photoaging of thermochromic materials is primarily due to the loss of solvent component. As the wavelength of UV lights reduces, the photodegradation rate of phenyl benzoate and thermosensitive green dye increases, resulting in the accelerated photoaging rate of corresponding thermochromic materials; whereas the negligible degradation effect of 1-octadecanol by UV lights leads to little degradation of corresponding thermochromic material. Under the visible light, the fact that the loss of phenyl benzoate is much greater than that of 1-octadecanol shows the faster photoaging of phenyl benzoate-based thermochromic material in comparison with 1-octadecanol-based thermochromic material. In conclusion, a wavelength-dependent photoaging mechanism has been discovered for three-components thermochromic materials and this sheds a new light on the anti-photoaging strategy of organic reversible thermochromic materials.
2024 Vol. 41 (4): 20-27 [
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155
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28
Preparation and adsorption properties of series of cross-linked graphene sponge
LIN Yanxin, WANG Xin, SHI Ruijie, JIANG Xu, WANG Ning, WANG Ping, FENG Yaqing, MENG Shuxian
In order to explore the preparation and adsorption properties of small molecules and graphene crosslinking materials, graphene hydrogels were prepared by hydrothermal method, and three cross-linked graphene sponge materials were synthesized from ethylenediamine, 1,3-Diaminopropane and Diethylenetriamine, respectively. The structure was characterized by SEM, FTIR and BET, and the difference of liquid adsorption capacity of three cross-linked graphene sponge materials before and after expansion was investigated. Methylene blue was further used as organics in sewage for adsorption simulation experiment. The results show that these series of graphene material have excellent adsorption properties, and the adsorption process conforms to the pseudo-second-order kinetic equation. With the increase of the number of carbons in cross-linked small molecular, the adsorption capacity increases by 26% and the adsorption rate increases to a certain extent. The adsorption performance after expansion is obviously better than that before expansion, which is raised by 1.37 times than before.
2024 Vol. 41 (4): 28-37 [
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194
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339
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38
Synthesis of [RuCl
2
＝CH(
o
-C
6
H
4
X)(PCy
3
)
2
](X=F, Cl, Br) andits applications in olefin metathesis reactions
WU Xiaqian, YANG Xianfeng, BI Shumeng, MA Peng, WANG Jianhui
A series of ruthenium carbene olefin metathesis catalysts [RuCl
2
＝CH(
o
-C
6
H
4
X)(PCy
3
)
2
] (X=F (
10
), Cl (
11
), Br (
12
)) were synthesized and characterized by means of nuclear magnetic resonance spectrometry. The catalysts showed relatively high stability. Kinetic studies on the ring-closing metathesis (RCM) of diethyl diallylmalonate showed that high initiation rate and high final conversion were obtained by using catalyst
10
. These catalysts were found to be effective in ring-closing metathesis and cross metathesis and exhibited remarkable functional group tolerance.
2024 Vol. 41 (4): 38-44 [
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] (
161
) [
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3457KB] (
342
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45
Synthesis of dipropylene glycol and tripropylene glycol over solid acid catalyst
WANG Baohe, DUAN Chenfei, ZHANG Zhaobang, MA Jing, ZHU Jing
The synthesis of dipropylene glycol (DPG) and tripropylene glycol (TPG) from propylene oxide (PO) and propylene glycol (PG) under the catalysis of solid acid was studied in a stainless steel high-pressure batch reactor. The study showed that the catalytic activity of H-ZSM-5 molecular sieve was significantly higher than that of H-13X molecular sieve. After eliminating the influence of internal and external diffusion, the kinetic model of H-ZSM-5 molecular sieve catalyzed reaction was established and the reaction kinetic constants were determined by numerical analysis. The experimental results show that the calculated values agree well with the experimental ones. The reaction conditions were optimized by the mathematical model of reaction dynamics, which provided basic physical data for the industrial production of dipropylene glycol and tripropylene glycol. The fresh and used catalysts were characterized by X-ray diffraction, N
2
adsorption and desorption measurement, Pyridine asorption FTIR, and the cause of deactivation was preliminarily explored.
2024 Vol. 41 (4): 45-54 [
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209
) [
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3098KB] (
385
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55
The doping mechanism of Zn
2+
promoting the polymorphic transition of TiO
2
during calcination
WANG Wei, LU Ruifang, WANG Chenguang, DANG Leping, HAO Lin, WEI Hongyuan
High temperature calcination is an important stage in the production of titanium dioxide by sulfuric acid method. Zinc salt treatment can reduce the temperature of polymorphic transition. But the internal mechanism is still unclear. Using metatitanic acid and zinc sulfate as raw materials and salt treatment agents, the calcination is performed in a muffle furnace at 600 to 900 ℃. The effect of Zn
2+
on polymorphic transition and doping mechanism were discussed by XRD, HRTEM and XPS. The results show that the concentration of Zn
2+
and the calcination temperature significantly affect the doping mechanism and existence state of Zn
2+
in the polymorphic transition. When the concentration of Zn
2+
is less than 1%, Zn
2+
is incorporated into the TiO
2
lattice in substitution mode, replacing Ti
4+
, increasing the cell parameters and forming oxygen vacancies. And with the increase of Zn
2+
concentration, excessive Zn
2+
forms ZnTiO
3
on the surface of TiO
2
. Substitutional doping and ZnTiO
3
can reduce the phase transition temperature and promote polymorphic transition from anatase to rutile through different doping mechanisms.
2024 Vol. 41 (4): 55-64 [
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150
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333
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65
Preparation of highly dispersed and large pore size iron sulfide/SiO
2
catalyst by precipitation deposition method and its efficient conversion of vacuum residue
LIN Congfu, BAI Yang, TIAN Lei, GUO Qiang, YANG Yong, FENG Fuxiang, LIU Yuan
Aiming at the problem of low activity and high reaction pressure of heavy oil slurry bed iron-based catalysts, the precursor was prepared by the precipitated sol-gel method, and the highly dispersed iron sulfide catalyst supported by SiO
2
was obtained by pre-sulfidation. The catalytic performance of the catalyst at a low pressure (5 MPa) on the model compounds naphthalene and Merey vacuum residue was investigated, and the catalyst and precursor were characterized by nitrogen adsorption-desorption, ICP, XRD, Mössbauer (MES), SEM-EDS, TEM and other methods. At the low iron content of the catalyst (Fe
2
O
3
in Fe
2
O
3
/SiO
2
is 20%), the yield of light oil can reach 54.9%, and the coke yield can be as low as 1.6%. The good performance of the catalyst is attributed to the high dispersion of Fe
2
O
3
in the catalyst precursor and iron sulfide in the catalyst and the large pore size with an average pore size of about 20 nm. The catalyst is prepared by a simple and easy method: by adjusting the pH value of the sol, the iron hydroxide colloids are positively charged and the silica particles are negatively charged, and the electrostatic attraction is used to achieve high dispersion and "confinement" of iron hydroxide (to inhibit its agglomeration), and the large pore size is obtained by particle packing.
2024 Vol. 41 (4): 65-75 [
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180
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6590KB] (
387
)
76
Pollution analysis and pollution control research in onshore natural gas production process
ZHAO Wei, FENG Xiaobo, SHEN Dajun, YU Lu, GUO Jinsong, YANG Wenhao, GAO Junmin
As a clean energy, natural gas is of great significance in the energy transition. However, it has a negative impact on the environment because it generates waste gas, waste water, and waste residues, etc. during the production process. To systematically understand the potential environmental impacts of onshore natural gas production and to promote green development of onshore natural gas, this paper analyzes the causes and characteristics of pollutants and the impact of major characteristic pollutants on the environment based on the production process of onshore natural gas from three major links: extraction, gathering and purification, then put forward corresponding pollution prevention and control suggestions from the perspectives of waste water, waste gas, waste residue, and noise. The results of the paper contribute to a comprehensive and systematic understanding of the pollution production characteristics of the onshore natural gas production, provide a reference for pollution prevention and control in the onshore natural gas production process, and an assistance for the realization of the "double carbon" goal.
2024 Vol. 41 (4): 76-87 [
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202
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2605KB] (
365
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88
Bicarbonate promotes the oxidation of As(III) by S(IV)-Mn(II) system
CAO Min, MENG Zihe, SONG Baodong, WU Songhai, HAN Xu
Advanced oxidation processes based on sulfite [S(IV)] have attracted more and more attention due to their low-cost advantages. In this study, we investigated the oxidation effect and mechanism of As(III) in high-arsenic groundwater in the presence of bicarbonate (HCO
-
3
) by the Mn(II)-activated S(IV) system. The results showed that HCO
-
3
significantly promoted the oxidation of As(III) in the S(IV)-Mn(II) system. Kinetic experiments showed that increasing concentrations of S(IV) and Mn(II) promoted the oxidation of As(III), but too high concentrations inhibited the oxidation process. The effect of pH on the oxidation of As(III) due to the species changes of S(IV) and Mn(II) in the reaction solution. The promotion effect of HCO
-
3
on the oxidation of As(III) may due to two aspects: (1) it formed weak coordination with Mn(II), which was helpful for the combination of S(IV) and Mn(II); (2) it promoted the oxidation of Mn(II) to Mn(III), which was favorable for the formation of SO
·-
4
. Quenching experiments revealed that SO
·-
4
was the primarily reactive oxygen species in the oxidation of As(III). This study enhances the understanding of the S(IV)-HCO
-
3
-Mn(II) system and provides a new solution for the treatment of high arsenic water.
2024 Vol. 41 (4): 88-96 [
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] (
195
) [
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1KB] [
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3088KB] (
349
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97
Adsorption properties of UiO-66-NH
2
functionalized cotton fiber prepared by cross-linking for Reactive Blue 4
DUAN Xingyu, QU Hongmei, DONG Min, ZHANG Jiacai, SUN Yiping, LI Xiaolong
A novel amino-rich metal-organic frameworks (MOFs) functionalized cotton fiber-based composite (UCF) was prepared conveniently by cross-linking cotton fiber (CF) and UiO-66-NH
2
with epichlorohydrin (ECH) as the cross-linking agent, and was applied to the high-capacity adsorption of Reactive Blue 4 (RB4) in aqueous solution. Compared with the method of growing MOFs on substrates via hydrothermal synthesis, cross-linking is faster and easier. Scanning electron microscopy (SEM), X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FT-IR) and thermogravimetric analysis (TGA) demonstrated the successful synthesis of UCF. In addition, the effects of adsorbent dosage, pH, temperature, dye concentration and contact time on the adsorption performance were further investigated, the adsorption isotherm, kinetic and thermodynamic properties were explored, and the adsorption mechanism was analyzed and summarized. The results showed that the maximum adsorption capacity of UCF was 539.2 mg·g
-1
under the optimum conditions, which was 785.39% higher than that of raw cotton fiber; The adsorption process followed Freundlich isotherm model and pseudo-second-order kinetic model; The adsorption process was spontaneous and exothermic; Electrostatic interaction was the main driving force of the process. This study provides a simpler strategy for the preparation of biomass-MOFs composites, and shows the application potential of this composite in the field of dye wastewater treatment.
2024 Vol. 41 (4): 97-108 [
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] (
154
) [
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5122KB] (
431
)
109
Experimental investigation of hydroxyl radicals in high concentration for killing biological aerosol pathogens in indoor air
WANG Shuai, KUANG Xinyi, ZHAO Ziqin, LIAO Hongguo, CUI Zhengwei
Environmental safety issues such as air disinfection and sterilization caused by COVID-19 have become hot spots that need to be solved urgently. In this study, a spiral cutter was used to nanoscale bubble and prepare a high-concentration ozone water in a circulation device. Then combined it with a counterflow packing filter, the novel air sterilization rig was set up for killing biological aerosol pathogens in air. The effects of different pH values and temperatures on ozone water concentration and hydroxyl radical concentration were then investigated. The experimental results show that the concentration of ozone water after equilibrium can reach 11.65 m·L
-1
and the concentration of hydroxyl radical reaches 95.84 μmol·L
-1
under the condition of pH=7 and temperature of 25 ℃. The effects of different pH, temperature, spray flow and wind speed on the sterilization rate were further explored. The experimental results show that the sterilization rates of 20, 40 and 60 min are 77.3%, 87.6% and 96.7%, respectively under the conditions of pH=7, temperature 25 ℃, spray flow rate 500 L·h
-1
and wind speed of 2.5 m·s
-1
. Therefore, the current high-concentration ozone water circulation device combined with the packing filter has a good sterilization effect for air sterilization.
2024 Vol. 41 (4): 109-116 [
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] (
180
) [
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2890KB] (
351
)
117
Research progress of air classification technology and equipment
FU Min, CAO Zhong, CHEN Xiaoqing, GAO Zefei, ZHAN Mingyu
An air classifier is an equipment used for separating particles of different sizes through an air flow field. It is widely used in mineral processing, food processing, fine chemical industry, biopharmaceuticals, solid waste recovery, and other fields. It plays an important role in controlling the quality of powdered raw materials. This work summarizes the research progress of static and dynamic air classifiers, including the classification of vertical and horizontal flow type gravity classifiers, centrifugal classifiers, and dynamic classifiers. It also covers the research status of key components such as rotary cages, air vanes, material dispersion mechanisms, process parameters, and internal flow fields. The analysis proposes existing problems and prospects the future development direction to provide a reference for the research of air classification technology and equipment. In the future, the research of air classifiers can focus on the kinematics and dynamics analysis of particles in the classifier, the quantitative characterization of the flow field in the classifier, and the optimization of the overall structure and process parameters.
2024 Vol. 41 (4): 117-130 [
Abstract
] (
161
) [
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2698KB] (
335
)
131
Ultrasonic assisted removal of micro-bubbles in water
MA Yongli, SHEN Shilong, CHEN Jilei, XU Yunlong, WANG Tongxin, WEI Xinyu, WANG Qianqian, LIU Mingyan
The bubble generator was used to generate microbubble water to simulate the reinjection water containing micro-bubbles. The microbubble contents of tap water, the prepared micro-bubble-containing water and ultrasonically treated water with micro-bubbles were explored through measurements and characterization of turbidity, electrical conductivity and dissolved oxygen. The effect of ultrasonic treatment on the contents of microbubbles in the sample water was studied through the characterization and analysis of the microbubbles in the liquid samples before and after the elimination of micro-bubbles by ultrasound. The results show that the ultrasonic cavitation helps to accelerate the growth and coalescence of microbubbles. There is an energy transfer process during ultrasonication, which reduces the gas content in the treated water by providing energy and promotes the elimination of microbubbles. The present research lay a foundation for the ultrasonic microbubble removal technology to be used in the efficient reinjection of geothermal water.
2024 Vol. 41 (4): 131-137 [
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] (
153
) [
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1KB] [
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2789KB] (
424
)
138
Preparation and physicochemical properties of low-density spherical ZrO
2
/SiO
2
/Al
2
O
3
ceramic composites particles used for fluidized bed heat transfer
YU Luqi, MA Hongqin, LUO Xinyue, GAO Junyu, GU Xingpeng, LIU Jiahao
In view of the shortcomings of the existing solid particles used in fluidized bed heat exchangers, such as high density, low strength and low wear resistance, low-density spherical ZrO
2
/SiO
2
/Al
2
O
3
composite ceramic particles were prepared by sol-gel and hot oil column curing methods, and the effects of ZrOCl
2
solution and silica sol addition sequence and Zr/Si/Al molar ratio on the microstructure and physicochemical properties of the prepared composite ceramic particles were studied, and the feasibility of the application of the prepared particles in fluidized bed heat transfer was evaluated. The results show that the as-prepared particles with a Zr/Si/Al molar ratio of 1:1:60 have a dry granule density of 1 740 kg·m
-3
and wet granule density of 2 170 kg·m
-3
, much lower than that of the normal ceramic (2 400~2 900 kg·m
-3
). The lower density is beneficial to their uniform fluidization and distribution in the heat exchange tube bundle, and hence ensures the effectiveness of preventing/removing scale and enhancing heat transfer. Besides, the particles with a mean diameter of 1.55 mm present good wear and corrosion resistances, and dry and wet single particle compressive strengths of 116.0 N and 115.7 N, respectively, which are high enough for the fluidized bed. Comprehensive consideration of size, density, mechanical strength, and wear and corrosion resistances, the as-prepared spherical composite ceramic particles are suitable for fluidized bed, especially in a tube heat exchanger for preventing/removing scale and enhancing heat transfer.
2024 Vol. 41 (4): 138-146 [
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] (
194
) [
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3105KB] (
382
)
147
Application of solvent extraction technology in phosphate ore processing technology
PENG Xianglong, LIU Songlin, SUI Yanfeng, LI Baiyu, LI Tianxiang, ZHU Jing
Solvent extraction technology, as one of the most commonly used methods in the separation and purification of industrial substances, is widely applied to many aspects of phosphate rock processing. This paper briefly describes the application of solvent extraction technology in the process of preparing phosphoric acid from phosphate rock, and focuses on the extraction and purification of wet phosphoric acid and raffinate acid in the process of phosphate rock processing, as well as the extraction of associated fluorine, iodine and rare earth resources from phosphate rock. The recovery processes were compared, and the extraction methods were compared with other purification methods. Finally, the application of solvent extraction technology in the processing of phosphate rock was summarized and suggestions for future research were given.
2024 Vol. 41 (4): 147-159 [
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] (
207
) [
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1262KB] (
414
)
160
Study on the rupture of liquid bridges in liquid-liquid two-phase coaxial flow
JIAO Boya, GUO Kai, LIU Hui, LIU Chunjiang, ZHENG Longyun, ZHANG Yanan
Droplet formation is often encountered in many industrial processes and it is widely used in petrochemical, fine chemical, energy, food, biological pharmaceutical, and environmental protection. Compared with the traditional batch production mode, continuous droplet production based on liquid-liquid two-phase flow has simpler operation and higher product benefit, which receives more attentions. In liquid-liquid two-phase flow, a liquid bridge is formed when the dispersed phase forms the main droplet, and the liquid bridge shrinks into satellite droplet after rupture due to the surface tension. The volume of satellite droplet is usually one thousandth of the main droplet, so that the appearance of satellite droplet will lead to poor single dispersion of the droplet. In this paper, the formation and rupture process of the liquid bridge as well as the factors influencing the maximum length of the liquid bridge are studied by experiment and CFD method. A device is built to record the generation of droplets in the liquid-liquid coaxial flow using a high-speed camera. The liquid bridge formation and rupture process is recorded and the maximum liquid bridge length is obtained using the CFD calculation. The results show that the maximum length of the liquid bridge decreases when the capillary number increases. But the capillary number is not the only factor affecting the maximum length of the liquid bridge. It also related to the viscosity ratio of the two phases. When the viscosity ratio of the two phases increases, the shear force of the liquid bridge increases, while the maximum length of the liquid bridge decreases. The rupture process of the liquid bridge is closely related to the variation of velocity around the liquid bridge.
2024 Vol. 41 (4): 160-168 [
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] (
186
) [
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1KB] [
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3442KB] (
366
)
169
Influence of rotating inner zone on the characteristics of flow field and torque simulated by MRF method
ZHANG Wei, CHEN Chen, LIU Panpan
The Multi-Reference Frame (MRF) method is commonly used in the numerical investigation of mixing process, however, the discussion on the size of the rotational domain is not well developed. Numerical simulations of the stirring process in a Rushton impeller mixing tank were carried out. By compared with experimental results, the optimum inner zone size was determined, and discussion on the height of the inner zone was complemented. In addition, the basis for dividing the rotating inner zone applicable to different mixing cylinder structures was proposed. The results show that the influence of the interface position is mainly in the direction of the impeller discharge flow, and the influence of the inner zone on the torque calculation is less than 5%. The proposed definition of inner domain diameter
Z
=(
d
in
-
D
)/(
T
-2
b
-
D
) can be applied to mixing equipment of different structures, the accuracy of numerical simulations is highest when the inner zone is delineated at
Z
=0.29, which can provide a theoretical reference for the selection of the rotating zone size under the MRF method.
2024 Vol. 41 (4): 169-178 [
Abstract
] (
189
) [
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1KB] [
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5708KB] (
439
)
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