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2023 Vol.40 Issue.6,
Published 2023-11-15
0
2023 Vol. 40 (6): 0-0 [
Abstract
] (
506
) [
HTML
1KB] [
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875KB] (
4096
)
1
Waste adsorbent derived cobalt modified carbon material for bisphenol A degradation by activating peroxymonosulfate
GUO Xu, ZHANG Qicheng, HE Hongwei, ZHANG Fengbao, FAN Xiaobin, LI Yang
Firstly, a carboxymethyl chitosan aerogel (CMCS) adsorbent is synthesized and applied to purify cobalt ion wastewater. Then, the waste adsorbent after adsorption of cobalt ions is modified and calcined to synthesize the nitrogen-doped carbon material loaded with cobalt nanoparticles (Co@NC-800), which is applied to activate peroxymonosulfate (PMS) to degrade bisphenol A (BPA). Combined with kinetic analysis and a variety of characterization methods, it is proved that Co nanoparticles are the main active sites. By regulating the calcination temperature, it is found that graphite nitrogen is beneficial to improve the synergistic effect of Co nanoparticles and carbon substrate, thus promoting the activation of PMS. Radical quenching experiments and electrochemical analysis confirm that sulfate radical (SO
·-
4
) and hydroxyl radical (·OH) are the main functional active species in the Co@NC-800/PMS system. This study provides a new approach for the efficient utilization of wastewater solid waste to prepare catalyst materials.
Guide:
2023 Vol. 40 (6): 1-14 [
Abstract
] (
354
) [
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1KB] [
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6893KB] (
1147
)
15
Preparation of ethylene/ethanol by electrocatalytic reduction of CO
2
with porous Cu
2
O cube
CAO Guangwei, CAO Xuerui, WANG Hua
Cu
2
O catalyst can effectively electrochemically reduce carbon dioxide to multi carbon C
2+
products. The composition and structure of the catalyst are important factors affecting the catalytic activity and selectivity of C
2+
products. The purpose of this study was to investigate the effect of porous structure of Cu
2
O catalyst on the selectivity of C
2
products for electrochemical reduction of CO
2
. Firstly, Cu
2
O cubes with porous structure (P-Cu
2
O) were prepared by acid etching solid Cu
2
O cubes (S-Cu
2
O). SEM, TEM, XRD, XPS, CV and other characterization results show that the composition of S-Cu
2
O and P-Cu
2
O is the same, and they are mixed Cu valence: Cu
0
and Cu
+
. The morphology of both is about 180 nm cube, while P-Cu
2
O has irregular cavity porous structure. The electrochemical characterization results show that the electrochemical active surface area of P-Cu
2
O is about 1.75 times that of S-Cu
2
O, and the interfacial charge transfer resistance is lower than that of S-Cu
2
O. Linear voltammetric scanning (LSV) results in N
2
and CO
2
atmosphere showed that P-Cu
2
O had higher CO
2
catalytic activity. The electrocatalytic reduction of CO
2
was carried out under different potentials in the gas diffusion electrode flow cell system. The effects of porous structure on CO
2
reduction activity and C
2
product selectivity were investigated. The results showed that when the potential was -1.0 V
vs
. RHE and the electrolyte was 2 mol·L
-1
KOH, the CO
2
reduction product selectivity of P-Cu
2
O was 37.7% (C
2
H
4
: 25.6%, C
2
H
5
OH: 12.1%), and the partial current density was 20.9 mA·cm
-2
, which was ~28% higher than that of S-Cu
2
O. The deep conversion of key intermediate
*
CO was calculated by
*
COR/[
*
COR/CO
(g)
]. The results showed that the deep conversion of
*
CO of P-Cu
2
O was significantly higher than that of S-Cu
2
O. In conclusion, the improvement of the selectivity of P-Cu
2
O for C
2
products is attributed to: the porous structure makes P-Cu
2
O have high active surface area, provides more CO
2
reduction active sites and promotes the formation of CO; the structure of the cavity is conducive to increase the local concentration of
*
CO and accelerate the dimerization of
*
CO to produce C
2
product. This study is of great significance for the design and development of Cu
2
O based high-efficiency catalysts for electrocatalytic reduction of carbon dioxide to multi carbon products.
Guide:
2023 Vol. 40 (6): 15-27 [
Abstract
] (
293
) [
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1KB] [
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5957KB] (
1272
)
28
Pd/Al-Al
2
O
3
catalyst for anthraquinone hydrogenation to hydrogen peroxide
YUAN Qinqin, LIANG Jingyue, LI Wei, ZHANG Jinli, GUO Cuili
Hydrogenation of anthraquinone to produce H
2
O
2
is a great important industrial reaction. Here, a series of Pd/
x
Al-Al
2
O
3
catalysts with different AlCl
3
contents were prepared by step impregnation method. The catalysts were characterized and analyzed based on XRD, TEM, NH
3
-TPD, XPS and N
2
adsorption and desorption. The Pd/1.0Al-Al
2
O
3
catalyst with 1% AlCl
3
content exhibits excellent hydrogenation efficiency of 8.3 g·L
-1
and selectivity of 99.5% toward anthraquinone hydrogenation, obviously superior to Pd/Al
2
O
3
catalyst (5.2 g·L
-1
and 97.2%). The characterization results show that the catalysts modified by AlCl
3
have abundant surface weak acids, which provide more adsorption sites for anthraquinone molecules. At the same time, the introduction of AlCl
3
could improve the dispersion of metal and increase the interaction between the metal particles and the support, which inhibits the agglomeration and loss of metal particles.
Guide:
2023 Vol. 40 (6): 28-36 [
Abstract
] (
330
) [
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1KB] [
PDF
4864KB] (
755
)
37
Synthesis of GaN-ZnO/MCM-41 for catalyzing CO
2
-based oxidative dehydrogenation of propane to propene
LIU Haiwei, SONG Chengxuan, YU Fang, SONG Jian, WANG Zhipeng, WANG Liyan, LI Yu, WANG Pengfei, CUI Jian
The oxidative dehydrogenation of propane to propene in the presence of CO
2
(CO
2
-OPDH) is considered as a desirable route for propene production, and the development of catalyst with high performance is the key to get a breakthrough in this process. Here, the GaN-ZnO/MCM-41 catalysts with dual-function active sites were constructed via a solid-state nitridation method with GaN-ZnO solid solution as the active component supporting on mesoporous MCM-41. Their catalytic performances for CO
2
-OPDH reaction were further evaluated. The physicochemical properties of obtained catalysts were characterized by a series of techniques such as X-ray diffraction spectroscopy (XRD), N
2
adsorption-desorption measurements, field-emission scanning electron microscopy equipped with an energy dispersive X-ray instrument (SEM-EDX), transmission electron microscopy (TEM),thermogravimetric-mass spectra (TG-MS) and Raman spectra. It is found that the solid solution catalyst can be successfully prepared in a solid-state nitridation method, the propane dehydrogenation activity of which is superior to that of the supported single-component GaN or ZnO catalysts under the same testing conditions. Among them, the Ga
0.5
-Zn
0.5
/MCM-41 catalyst delivers a propane conversion of 22% with the selectivity of 92% towards propene at 600 ℃ in the CO
2
atmosphere. This excellent catalytic performance could be attributed to the formation of solid solution structure, which was beneficial to the dispersion of active components and the generation of more active sites. The calcination temperature influenced the structure of solid solution and thus affected its catalytic activity. In addition, CO
2
can not only increase the activity of the catalyst, but also improve its stability by declining the coke formation in PDH reaction.
Guide:
2023 Vol. 40 (6): 37-44 [
Abstract
] (
308
) [
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1KB] [
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4248KB] (
737
)
45
Hydrogenation of chlorinated nitrobenzene by Pd supported on monodispersed nitrogen-doped carbon nanospheres
YU Fang, ZU Rongyan, LYU Yunpeng, HAN Xinghua, WANG Zhipeng, LI Yu, SONG Jian
The preparation of efficient Pd/C catalysts for selective hydrogenation of halogenated nitrobenzene to halogenated aniline is the key to get a breakthrough in this process. Here, supported Pd/CN-
x
(
x
represents the carbonization temperature of carbon-based support) catalysts were prepared via an impregnation method with monodispersed nitrogen-doped carbon nanospheres as the support and metallic palladium as the active component, and their catalytic performances for the hydrogenation of chlorinated nitrobenzene to chlorinated aniline were studied. The morphology, structure and surface chemical properties of obtained catalysts were characterized by Fourier transform-infrared spectroscopy (FT-IR), X-ray diffraction spectroscopy (XRD), transmission electron microscopy (TEM), field emission scanning electron microscopy (SEM) and X-ray photoelectron spectroscopy (XPS). The effect of nitrogen-doped carbon support prepared at different temperatures on the activity and selectivity of selective hydrogenation of chloronitrobenzene for supported palladium catalysts were investigated. Experimental results revealed that the monodispersed nitrogen-doped carbon nanospheres as support could achieve uniform dispersion of Pd nanoparticles, and endow the obtained samples with excellent catalytic properties. In particular, the Pd/CN-600 catalyst exhibits 100% conversion of 3-chloronitrobenzene with a selectivity of 76.9% for 3-chloroaniline. In addition, it was indicated that the nitrogen-containing functional groups on the surface of the carbon nanospheres could influence the effective dispersion of the active Pd component and thus the selectivity of 3-chloroaniline.
Guide:
2023 Vol. 40 (6): 45-52 [
Abstract
] (
290
) [
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1KB] [
PDF
5771KB] (
823
)
53
Effect of calcination temperature on CuO/CeO
2
-ZrO
2
/SiC monolithic catalyst for hydrogen production by methanol steam reforming
AN Guochao, SUN Shu, JIAO Tong, GAO Wenyi, WENG Youyun, WENG Yubing, ZHANG Lei, GAO Zhixian
CuO/CeO
2
-ZrO
2
/SiC monolithic catalyst was prepared by sol-gel method and applied to the hydrogen production reaction of methanol steam reforming. The effect of calcination temperature on CuO/CeO
2
-ZrO
2
/SiC monolithic catalyst was investigated by XRD, BET, H
2
-TPR, N
2
O titration and other characterization methods. The results showed that calcination temperature had a great influence on the catalytic activity of CuO/CeO
2
-ZrO
2
/SiC monolithic catalyst. Combined with the characterization analysis, the catalyst calcined at 500 ℃ had better Cu dispersion and larger Cu specific surface area. Under the conditions of 360 ℃ reaction temperature, 1.2 molar ratio of water to methanol and 4 840 h
-1
space velocity of methanol vapor gas, the conversion of methanol was 77.3%. This paper provides basic data for the development of monolithic catalysts.
Guide:
2023 Vol. 40 (6): 53-58 [
Abstract
] (
244
) [
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1KB] [
PDF
2534KB] (
690
)
59
The study of Pd-based acetylene hydrochlorination catalyst modified by nitrogen-containing ligand
WANG Xingtao, WANG Fumin, ZHANG Xubin
To improve the stability of Pd-based acetylene hydrochloride catalyst, a novel Pd-based catalyst modified with nitrogen ligand was prepared by simple wet impregnation method. The activity of the catalyst with the dosage of 10% nitrogen ligand reaches 99% and only decreases 5% after 20 h under the conditions of 170 ℃, GHSV (C
2
H
2
)=720 h
-1
, and
V
(HCl)/
V
(C
2
H
2
)=1.2. The results of TEM show that the Pd species is highly dispersed. XPS results prove that nitrogen ligands can reduce the reduction of high palladium species during the reaction. Furthermore, the data of the TG, ICP-OES, and BET certify that the nitrogen ligand significantly reduces the carbon deposition and inhibits the loss of Pd species. Besides, the theoretical calculations show that the ligand enhances the adsorption and activation of HCl, and reduces the energy difference in the process of electron transfer from Pd to HCl, which effectively promotes the reaction of hydrochlorination of acetylene.
Guide:
2023 Vol. 40 (6): 59-69 [
Abstract
] (
244
) [
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1KB] [
PDF
4802KB] (
673
)
70
Synthesis of pentaerythritol in microchannel reactor
SUN Yang, XIE Tian, QUAN Hongdong, YANG Xiuguo, LI Hongyan
There are some problems such as low yield of pentaerythritol in domestic industrial production. Using formaldehyde and acetaldehyde as raw materials and sodium hydroxide as catalyst, pentaerythritol was synthesized by microchannel reactor and quantitatively analyzed by liquid chromatography. The effects of reaction temperature, reaction time and raw materials on the yield were investigated. The response surface experiment was designed by Design-Expert 8 software, and the experimental conditions were optimized. The results showed that when the reaction temperature was 44 ℃ and the reaction time was 161 min,
n
(formaldehyde)∶
n
(acetaldehyde)=5∶1, the molar yield of pentaerythritol was 93.17%. Compared with the traditional kettle reaction, the molar yield of pentaerythritol is increased by 25.21%, which has the prospect of industrialization.
Guide:
2023 Vol. 40 (6): 70-77 [
Abstract
] (
256
) [
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1KB] [
PDF
4108KB] (
927
)
78
Thermal performance and pressure drop in a gas-solid circulating fluidized bed spiral plate heat exchanger
JIANG Feng, Sun Xingyi, QI Guopeng, LI Xiulun
In this study, the fluidized bed heat transfer and fouling prevention technology is applied to the gas-phase heat transfer process in spiral plate heat exchanger, and a gas-solid circulating fluidized bed spiral plate heat exchanger is designed and built. The effects of operating parameters such as air flow rate (80—125 m
3
·h
-1
), particle addition (0.5%—2.0%) and particle type on the heat transfer performance and pressure drop of circulating fluidized bed spiral plate heat exchanger using constant temperature water as hot fluid, air as cold fluid and three kinds of solid particles as solid working medium are studied. The experimental results show that the addition of particles can obviously improve the heat transfer performance of the spiral plate heat exchanger, but also increase the pressure drop. Within the range of operating parameters investigated in the experiment, the heat transfer enhancement factor of the best heat transfer enhancement effect can reach 29.28%. At this time, the particles added in the system are polyformaldehyde particles, the air flow rate is 125 m
3
·h
-1
, and the amount of added particles is 2.0%, but the corresponding pressure drop ratio also reaches 20.86%. The three-dimensional diagrams of heat transfer enhancement factor and pressure drop ratio and the comprehensive influence radar diagrams are drawn which can guide the industrial applications.
Guide:
2023 Vol. 40 (6): 78-88 [
Abstract
] (
291
) [
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1KB] [
PDF
7836KB] (
908
)
89
The physicochemical properties of binary mixture of ether functionalized ionic liquid [C
2
2O1IM][NTf
2
]+formamide (FA)/dimethylformamide (DMF)
YANG Jialin, DU Yanping, LIU Bin, CHANG Wei, HOU Haiyun, WANG Ning, XIE Peijing, YANG Simeng
1-(2-methoxyethyl)-3-ethyl imidazole bis (trifluoromethyl) sulfonyl imide salt ([C
2
2O1IM][NTf
2
]) as ether functional ionic liquid has many excellent characteristics such as good thermal stability, low viscosity and high conductivity. In this work, the binary mixture of ([C
2
2O1IM][NTf
2
])+formamide (FA), dimethylformamide (DMF) was studied. The density
ρ
, sound velocity
u
and viscosity
η
of the binary mixture in the whole composition range were measured at the temperature range of 15—50 ℃ and atmospheric pressure. According to the experimental data, excess molar volume
V
E
m
, isentropic compression coefficient deviation Δ
κ
s
and viscosity deviation Δ
η
of the system were calculated. The results can be explained by intermolecular interactions in these mixtures.
Guide:
2023 Vol. 40 (6): 89-95 [
Abstract
] (
294
) [
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1KB] [
PDF
3987KB] (
754
)
96
Electromagnetic thermal characteristics in a continuous-flow microwave reactor coupled with multilayer flow elements
ZHU Yulian, JIN Guangyuan, ZHUANG Qin, XU Ming, ZHENG Qingyu, SONG Feihu, LI Jing, SONG Chunfang, LI Zhenfeng
Microwave heating is widely used in continuous flow systems because of its unique volume heating, but its obvious disadvantage is that the uneven temperature leads to local thermal runaway and affects the heating efficiency of materials. Therefore, the effects of material volume, material spacing, waveguide position, microwave power and material flow rate on utilization of microwave energy and heating efficiency are discussed through multiphysics coupling calculation. The results show that placing two layers of materials in the microwave continuous flow reactor has the best utilization of microwave energy and heating efficiency; the change of material spacing and waveguide position makes asynchronous difference of the microwave energy utilization and heating effect of the two-layer materials in the reactor; increasing the microwave power increases the difference in the heating effect of the double-layer material in the reactor, while increasing the material flow rate improves this difference.
Guide:
2023 Vol. 40 (6): 96-106 [
Abstract
] (
216
) [
HTML
1KB] [
PDF
8520KB] (
1093
)
107
Advances in process characteristics and mechanisms of ammonia combustion and co-firing
LIU Feng, FENG Shaobo, ZHAO Bingtao, XU Hongtao, LIAO Xiaowei, DOU Wenyu, LI Yazhou
Ammonia combustion and co-firing are of positive significance to replace fossil fuels for carbon-free and carbon-reduced combustion to achieve carbon peaking and carbon neutrality goals. Focusing on the applications of ammonia and blended ammonia as fuels in chemical industry, the present work elaborates on the issues of ammonia combustion and ammonia-based co-firing, including (i) the reaction path, reaction equation, and mechanism model; (ii) the main limiting factors including the effect of equivalent ratio, ammonia ratio, and initial temperature on flame propagation speed and flame temperature; (iii) the mathematical modeling and prediction performances of reactions, fluid flow, and energy transport; (iv) the generation and control of nitrogen oxides during the combustion process; (v) applications of ammonia co-firing technology. Finally, the future outlook is highlighted to advance the fundamentals and technologies of ammonia combustion and co-firing.
Guide:
2023 Vol. 40 (6): 107-118 [
Abstract
] (
306
) [
HTML
1KB] [
PDF
4361KB] (
1208
)
119
Progress in modification of zeolite synthesized from fly ash and its application in water treatment
TANG Xuejing, LUO Jia, HU Zhenzhong
Fly ash is a kind of fine particulate solid waste. Inappropriate disposal of fly ash will damage the environment and affect human health. The production of zeolite from fly ash is a high value utilization way, which not only solved the disposal problem of fly ash, but also provided a new environmental protection material with the concept of "treating waste by waste". In this paper, the characteristics of fly ash and zeolite and the synthetic methods of zeolite from fly ash are briefly reviewed by summarizing the relevant literatures in the recent years. The modification methods of zeolite derived by fly ash, such as cationic surfactant modification, ion exchange modification and magnetic modification have been focused on this review. The application of modified zeolite acting as adsorbent, and catalyst carrier for water treatment is also summarized. Suggestions on modification of zeolite from fly ash and its application in sub-water treatment are put forward.
Guide:
2023 Vol. 40 (6): 119-129 [
Abstract
] (
298
) [
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1KB] [
PDF
1515KB] (
948
)
130
Epoxy resin composite coating with silane coupling agent modified graphene oxide generating effective corrosion protection
NAN Ding, LI Xin, XU Yu, LIU Qiong, WANG Biao, HUANG Zhenghong
The silane coupling agent functionalized graphene oxide (KGO) was prepared using a simple one-step hydrothermal method and combined it with epoxy resin to synthesize a high-performance anticorrosive coating. KGO was characterized by Fourier transform infrared spectroscopy (FTIR), Raman spectroscopy, scanning electron microscopy (SEM) and X-ray diffraction analysis (XRD). Epoxy resin composite coatings with 0.1%, 0.2%, and 0.3% KGO (KGO/EP) were prepared and their corrosion resistance was characterized by electrochemical impedance spectroscopy (EIS) and salt spray test. The results reveal that the shielding and corrosion resistance of epoxy resin composite coating are improved significantly by KGO. The corrosion current density decreases from 8.8×10
-8
A·cm
-2
to 2.0×10
-8
A·cm
-2
, the impedance modulus (｜
Z
｜
0.01 Hz
) of 0.2 KGO/EP remains at a relatively high value after 72 h of immersion in 3.5% NaCl, which is about two order higher than that of GO/EP. When the mass fraction of KGO in the KGO/EP composite coating is 0.2%, the corrosion resistance of the coating is optimal.
Guide:
2023 Vol. 40 (6): 130-135 [
Abstract
] (
335
) [
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1KB] [
PDF
2939KB] (
1050
)
136
Influence factors and kinetics of higher concentration ozone water on inactivation of algae
ZHAO Ziqin, KUANG Xinyi, WANG Shuai, LIAO Hongguo, CUI Zhengwei
At present, the available advanced oxidation processes for algae removal have problems of low efficiency, secondary pollution, etc. Taking Chlorella as research object, a high concentration ozone water cycle device assisted by a spiral cutter was designed to kill Chlorella. The effects of equilibrium concentration of ozone water, reaction time, initial optical density of algal cells and initial reaction temperature on Chlorella inactivation were investigated and kinetic analysis was conducted. The results show that the algae removal rate of ozone water on Chlorella could be as high as 96.02% when the equilibrium concentration of ozone water was 9 mg·L
-1
, the initial reaction temperature was 25 ℃, the initial optical density of algal cells was 0.4 and the reaction time was 12 min. By comparing the fitting parameters, the results show that the first-order kinetic fitting was appropriate when the equilibrium concentration of ozone water was not lower than 11 mg·L
-1
, the initial optical density of algal cells was not higher than 0.5, and the initial reaction temperature was not lower than 20 ℃, and moreover the second-order kinetic fitting was more appropriate when the equilibrium concentration of ozone water was lower than 11 mg·L
-1
, the initial optical density of algal cells was higher than 0.5, and the initial reaction temperature was lower than 20 ℃.
Guide:
2023 Vol. 40 (6): 136-143 [
Abstract
] (
302
) [
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1KB] [
PDF
2707KB] (
767
)
144
Effect of nanobubbles on the apparent viscosity of organic solutions
GUO Xingfei, CHAO Shulin, HUANG Yaqi
In order to investigate the effect of nanobubbles (NB) on the apparent viscosity of organic liquids, inorganic ceramic membranes were used to generate NB in solutions to monitor the apparent viscosity variations of liquids. CFD was used to simulate the variations of apparent viscosity of solutions with NB verify the experimental results. The experimental results show that the particle size distribution of NB is in the range of 125—425 nm at 0.3 MPa and average surface tension of H
2
O decreases from 72.0 to 68.1 mN·m
-1
in the presence of NB at the liquid surface. In addition, after bubbling time of 30 min the apparent viscosity of H
2
O, BSA solution and SA solution decrease from 1.07, 1.3 and 2.27 to 1.01, 1.24 and 2.27 mPa·s, respectively. The apparent viscosity of the solutions continues to decrease with increasing NB concentration. The simulations by the CFD-PBM coupled model show that the variations of the apparent viscosity of solutions are consistent with the experimental results, confirming the effectiveness of NB in reducing the apparent viscosity of liquids.
Guide:
2023 Vol. 40 (6): 144-150 [
Abstract
] (
305
) [
HTML
1KB] [
PDF
3077KB] (
660
)
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