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Advanced Oxidation Processes and Equipment Based on Zero-valent Iron
XIONG Zhaokun, ZHANG Heng, LIU Yang, ZHOU Peng, HE Chuanshu, HUANG Rongfu, DU Ye, LAI Bo
Materials Reports
2021,35(21 ):21012 -21021. DOI:10.11896/cldb.21080227
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Zero-valent iron (ZVI) has the characteristics of low reduction potential, directional reduction of toxic groups, low price and easy availability, and environmental friendliness. ZVI has been widely used in the pretreatment of general industrial wastewater. However, ZVI also has problems such as narrow pH range, easy formation of passivation film, and low electron utilization. Advanced oxidation processes based on ZVI have gradually become a research hotspot. The combining of ZVI and oxidants not only significantly improves the removal effect of pollutants, but also broadens the applied range of ZVI. The electron transfer mechanisms among ZVI, oxidants and pollutants are very complicated. The analysis of the complex products and mechanisms in the ZVI/oxidant system has been continuously explored and developed. This article reviews the advanced oxidation processes and equipments based on ZVI. The advanced oxidation systems that combining ZVI with oxygen, hydrogen peroxi-de, ozone, persulfate, permanganate and other oxidants are introduced. The interaction mechanism between ZVI and oxidants is described from the perspective of electron migration. The corrosion products of ZVI and their catalytic capacity in the presence of different oxidants are analyzed. Moreover, the synergistic catalytic oxidation technologies based on ZVI are introduced. Furthermore, advanced oxidation treatment equipment and combined processes based on ZVI in practical wastewater treatment are summarized. Finally, the problems existing in the current ZVI/oxidant systems are analyzed and its application prospects are prospected.
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Research Progress of Gaseous Ozone Decomposition Catalysts
ZHANG Ruiyang, WANG Shuyan, LI Bangxin, ZHANG Aili, ZHANG Qian, ZHOU Ying
Materials Reports
2021,35(21 ):21037 -21049. DOI:10.11896/cldb.21060087
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Advanced oxidation technology involving strong oxidizing ozone has been applied in the fields of water treatment, air purification and sterilization. But the excessive discharge of ozone causes substantial air pollution and represents a major hazard to human health. Compared to typical ozone treatment procedures, such as adsorption, thermal decomposition, absorption and so on, catalytic ozone decomposition has garnered a lot of attention since it is very efficient, safe and environmentally benign. Up to now, great progress has been made on catalysts for ozone decomposition. The types of catalysts have become more abundant, including activated carbon, noble metals, transition metal oxides, metal-organic framework materials, etc., and their application forms have evolved from powder-based materials to monolithic materials.
Nevertheless, two major difficulties severely limit the practical application of catalysts: on the one hand, catalyst deactivation is unavoidable due to the accumulation of intermediate oxygen species at surface active sites, which is the rate-limiting phase of the reaction. On the other hand, due to the intense competing adsorption between water molecules and ozone at active sites, catalysts are rapidly poisoned in moist conditions. As a result, catalysts with high catalytic activity and water resistance are highly desirable.
To enhance the catalytic property, some effective strategies, including enlarging the surface area, fabricating oxygen vacancy, regulating lattice plane, doping and surface modification, are used to increase the concentration of active sites and accelerate the electron transfer. While hydrophobic treatment is a common approach to improve water resistance. Furthermore, researchers have shown in recent years that water can ope-rate as a promoter at some specific active sites, which not only boosts catalytic activity but also prevents unstable performance caused by water adsorption competition.
This overview covers the research progress of catalytic ozone decomposition materials, as well as the gas ozone decomposition reaction process and mechanism. Especially, the advantages and challenges of various catalysts are summarized and the strategies for improving the activity and stability are highlighted. This review serves as a good reference for the preparation of stable and efficient catalytic ozone decomposition materials and the large-scale application of ozone oxidation technology in the chemical industry.
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Research on Advances of Catalytic Cracking Materials for Organochlorosilane High-boiling Residues
WEI Yuechang, LAI Kezhen, XIONG Jing, LI Yuanfeng, WU Tongtong
Materials Reports
2021,35(21 ):21022 -21027. DOI:10.11896/cldb.21060166
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Organosiliconmaterials are widely applied in various fields due to their excellent properties, including moisture-proof, corrosion resistance, high and low temperature resistance, non-toxic and physiological inertia. However, the production process of organosilicon monomers will produce about 7% by-products, and they are mainly composed of organochlorosilane high-boiling residues with complex composition and low commercial value. Inflammable, pungent and strong corrosive organochlorosilane high-boiling residues are greatly harmful to our health and environment. With the increasing productivity of organosilicon monomer, the efficient utilization of organochlorosilane high-boiling residues has become a diffcult problem to be solved urgently. The recycle of organochlorosilane high-boiling residues is mainly achieved through the synthesis of organosilicon downstream products and organosilicon monomers by catalytic cracking method. The catalytic cracking process needs to break the Si-Si bond and Si-C-Si bond in the presence of catalysts and convert high-boiling residues into methylchlorosilane monomers by selecting a suitable blocking reagent. Lewis acids, organic amines, transition metal elements, activated carbon and molecular sieves are main catalysts for catalytic cracking, and their operating conditions and catalytic performance are different. The cracking ratio of organochlorosilane high-boiling residues can reach more than 99%. Nevertheless, the high operation cost and complex production technology limit the further industrial application and popularization. This review article offers a retrospection of research works with respect to the catalytic cracking materials for organochlorosilane high-boi-ling residues, and the materials include aluminum-based compounds, organic amines or quaternary ammonium salts, transition metals, molecular sieves or activated carbon and metallic phosphate catalysts. We have summarized the research status and problems of the above catalysts and analyzed the development prospects. It is expected to provide an available summary for development prospect of catalytic cracking industrialization.
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Photocatalytic Degradation for Benzene Series in Wide-band Gap Metal Oxide: Reaction Mechanism and Modification Strategies
CHEN Lyucun, CUI Wen, CHEN Peng, LI Kanglu, DONG Fan, WANG Fali
Materials Reports
2021,35(21 ):21001 -21011. DOI:10.11896/cldb.21090250
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Benzene compounds are widely present in water bodies and atmospheric environments, and their refractory and highly toxic characteristics pose a serious threat to human health and the ecological environment. Photocatalytic technology has attracted much attention in pollutant degradation and energy conversion because of mild reaction conditions, strong redox ability, and green and no secondary pollution, especially for the treatment of refractory benzene series.
The advantages of positive valence band position, strong oxidation ability, high photochemistry stability and lower cost on wide-band gap photocatalysts play important role in benzene series degradation. However, wide band gap photocatalysts have limited photo-response range, higher surface potential and difficult separation of photo-generated electron-hole pairs, which limit their application in actual treatment processes. In addition, the effects of wide variety of benzene series, complex structure, and the current in-situ characterization technology limited the understanding of the conversion and ring opening mechanism of benzene series. That restricts the design and preparation for efficient photocatalysts and photocatalytic technology for the practical application in benzene treatment.
This review focuses on the important progress about wide-band gap photocatalytic oxidation technology in the degradation of benzene series, and introduces the latest developments about the reaction mechanism of photocatalytic benzene series degradation, the performance influencing factors of wide-band gap semiconductors, and the modification strategies on wide-band gap semiconductors. Finally, the prospects in reaction mechanism research, degradation efficiency enhancement and practical application are put forward.
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Recent Advances in In
2
O
3
-based Catalysts for CO
2
Hydrogenation
LI Longtai, ZHANG Chunjie, LUO Xuebin, YANG Bin, GUO Limin
Materials Reports
2021,35(21 ):21071 -21078. DOI:10.11896/cldb.21050185
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Alarge amount of carbon dioxide (CO
2
) emitted by humans into the atmosphere has caused many environmental problems and dramatically threatens humankind’s survival. CO
2
catalytic hydrogenation has unique advantages among many CO
2
reduction strategies. The conversion of CO
2
and hydrogen (H
2
) into high value-added chemicals has good prospects for application, both in reducing atmospheric CO
2
concentrations and producing economically valuable commodities.
In recent years, indium oxide (In
2
O
3
) catalysts have received much attention in the academic community as a new and efficient catalyst for the CO
2
hydrogenation to methanol. After activation, the In
2
O
3
surface generates a large number of oxygen vacancies, which are periodically generated and annihilated, that inhibit the occurrence of side reactions and hydrogenates CO
2
to methanol with high selectivity. It was reported in the literature that In
2
O
3
had a methanol selectivity close to 100% at 200—300 ℃. Especially at higher temperatures, the relatively high methanol selectivity was still maintained. This excellent performance at high temperatures allows In
2
O
3
to be used in coupling with zeolite to design bifunctional catalysts for the CO
2
catalytic hydrogenation directly to hydrocarbons.
The drawback of In
2
O
3
catalysts is that their low CO
2
conversion limits the methanol yield. The academic community has adopted several strategies to optimize the In
2
O
3
-based catalysts. There are two main strategies: (1) loading In
2
O
3
onto other oxide supports and (2) introducing other metal elements into the In
2
O
3
system. Loading In
2
O
3
onto other oxide supports can increase the dispersion of In
2
O
3
species, increase the content of oxygen vacancies, enhance the ability to adsorb CO
2
, and stabilize key intermediate species. Loading In
2
O
3
onto ZrO
2
is a typical example of this strategy, which can significantly enhance the intrinsic activity of the catalyst. The introduction of other metallic elements into the In
2
O
3
can enhance H
2
dissociative adsorption and H
2
spillover. The introduction of metals such as Pd, Pt, Cu, Rh, Au, Co, and Ni into the In
2
O
3
has been reported in the literature with good results.
This review summarized the research advances of In
2
O
3
-based catalysts for CO
2
hydrogenation, reviewed the structure of In
2
O
3
, the current status of In
2
O
3
for CO
2
hydrogenation, and the design and improvement of new In
2
O
3
-based catalysts for CO
2
hydrogenation, and provided an outlook on the research ideas and development prospects of In
2
O
3
-based catalysts for CO
2
hydrogenation, to provide thoughts and references for the future research of In
2
O
3
catalytic systems for CO
2
hydrogenation.
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A Review of Catalysts with Activities for Simultaneous Hydrolyses of Carbonyl Sulfide and Carbon Disulfide at Low Temperatures
LIANG Jianxing, LI Xianwei, LIU Daoqing, GU Jianan, SUN Tonghua, JIA Jinping
Materials Reports
2021,35(21 ):21028 -21036. DOI:10.11896/cldb.20050176
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By-product coal gas from the steel industry is secondary energy produced from the steel enterprise, which is difficult to reuse because it contains COS and CS
2
with the high chemical stability. The by-product coal gas is discharged to the atmospheric environment by some steel enterprises because it is difficult to reuse, which leads to the energy-wasting and environmental pollution. Therefore, many technologies have been developed for the removal of COS and CS
2
, where hydrolysis method is general desulfurization technology for removing COS and CS
2
in the waste gas.
However, the operating temperature for the hydrolysis catalysts is relatively high in the present, meanwhile, by-product coal gas from the steel industry has the characteristics of low temperature, low heating value and high content of carbon dioxide and oxygen. Therefore, various low-temperature hydrolysis catalysts have been developed for the single catalytic hydrolysis of COS and CS
2
, and simultaneously catalytic hydrolysis. The development of these catalysts not only dramatically reduces the operating temperature but remains the excellent hydrolysis efficiency.
The catalysts for the single catalytic hydrolysis of COS and CS
2
mainly include metal oxide-based catalysts, activated carbon-based catalysts and hydrotalcite-like based catalysts. The metal oxide-based catalysts mainly use
γ
-Al
2
O
3
and TiO
2
as carries, and TiO
2
-based catalysts possess excellent anti-poisoning performance. The activated carbon-based catalysts can enhance its hydrolysis performance at low temperature by adjusting active components and its content, and improving the quality of activated carbon. The hydrotalcite-like based catalysts have excellent hydro-lysis catalytic performance at low temperature through tailoring their metal components in the brucite-like layers, preparing methods and conditions. Besides, catalysts for simultaneous catalytic hydrolysis of COS and CS
2
are mainly the activated carbon-based catalysts, due to activated carbon has special physicochemical characteristics.
This review concludes the development of COS and CS
2
hydrolysis catalysts at low temperature, and introduces the single catalytic hydrolysis, simultaneous catalytic hydrolysis for COS and CS
2
, and its catalytic mechanism. Meanwhile, the current problems for the development of low-temperature hydrolysis catalysts are analyzed, and the feasible research directions in the future for the different kinds of low-temperature hydrolysis catalysts are proposed, on which to develop more low-temperature catalysts for the simultaneous hydrolysis of COS and CS
2
. More importantly, this review provides a reference for the research direction and industrial application of the low-temperature catalysts for the simultaneous hydrolysis of COS and CS
2
in the by-product coal gas from the steel industry in the future.
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Application of Metal-Organic Framework in CO
2
Photocatalytic Reduction
ZHANG Zhongwei, GUO Ruitang, QIN Yang, GUO Deyu, PAN Weiguo
Materials Reports
2021,35(21 ):21058 -21070. DOI:10.11896/cldb.20070204
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Although human beings rely on fossil fuels to accelerate the development of modern society, the over-use of fossil fuels has raised a series of problems such as tough energy crisis and environmental exacerbation. Excessive depletion of fossil fuels leads to the sharp increase of CO
2
content in the atmosphere, which is the main cause of the global greenhouse effect. Among the abundant technologies for reducing CO
2
emissions, the photocatalytic reduction of CO
2
technology not only reduces the CO
2
content in the atmosphere, but also converts CO
2
into valuable chemicals through solar energy, which is considered to be one of the most promising technologies.
Metal-organic frameworks (MOFs), also known as porous coordination polymers, are three-dimensional porous materials with a periodic network structure composed of inorganic metal ions (or metal clusters) and organic ligands. MOFs are particularly promising materials due to large surface area, adjustable structure, unique electronic band structures and abundant catalytic active sites, which make it more and more favored by researchers in the photocatalytic reduction of CO
2
. At present, MOFs used for photocatalytic reduction of CO
2
mainly include single MOFs photocatalyst and composite photocatalyst based on MOFs. The article lists specific examples to illustrate the advantages and uniqueness of MOF-based photocatalytic materials in the reduction of CO
2
and modified methods to improve photocatalytic activity.
This review summarizes recent research progresses in MOF-based photocatalysts for photocatalytic reduction of CO
2
. Besides, it discusses strategies in rational design of MOF-based photocatalysts (MOFs functionalization, semiconductor/MOFs, photosensitizer/MOFs and noble me-tal/MOFs) with enhanced performance on CO
2
reduction. Moreover, challenges and outlook on using MOFs-based photocatalysts for CO
2
reduction are also put forward.
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Study on Synthesis and Performance of Melamine Sponge-based High-efficiency Flexible Denitration Catalytic Material
WANG Chengzhi, GAO Fengyu, YU Qingjun, YI Honghong, NI Shuquan, TANG Xiaolong
Materials Reports
2021,35(21 ):21079 -21084. DOI:10.11896/cldb.21010055
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Atwo-step hydrothermal method was applied to synthesize the MnCo nanoarray denitration catalyst on carbon foam substrate (MF) for the selective catalytic reduction of NO
x
by NH
3
. The effect of Co-doping on the low temperature performance of Mn-MF was also studied. The results show that Co-doping can significantly improve the low-temperature activity and selectivity of Mn-MF and the resistance of H
2
O and SO
2
. The Mn
2
Co-MF catalyst has the best low-temperature performance and the denitration efficiency can reach more than 90% at 140—220 ℃. In addition, SEM, XRD, XPS, H
2
-TPR, NH
3
-TPD and other characterization techniques are applied to explore the relationship between the catalytic performance, redox performance and structure of Mn
2
Co-MF catalyst. The results show that the introduction of Co can not only increase the specific surface area and pore volume of the catalyst, but also promote the enrichment of oxygen species on the surface of the Mn
2
Co-MF catalyst, produce more acid sites, and improve the reducibility of the catalyst, thereby improving the low temperature activity.
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Research Progress of Manganese Dioxide Catalyst for Ozone Decomposition
QIU Jing, ZHAO Ming, WANG Jianli, CHEN Yaoqiang
Materials Reports
2021,35(21 ):21050 -21057. DOI:10.11896/cldb.20070148
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Manganese oxides show diversity of properties with the change of structure and show unique advantages in the field of purification of atmospheric pollutants for example ozone decomposition. Ground ozone is a common atmospheric pollutant. Ozone will not only cause photochemical pollution, but also cause serious damage to human health due to its strong oxidation. It is very important to reduce the concentration of ground ozone. Ozone treatment methods include catalytic decomposition, liquid absorption, electromagnetic radiation, thermal decomposition, etc. Catalytic decomposition method is widely used because of low energy consumption and environment-friendly characteristics. Considering the performance, price and application background, manganese oxides is the main stream of ozone catalytic decomposition. The difference in structure can affect ability of catalyze ozone decomposition. The structures of manganese oxides are various, which has profound research significance. However, the performance of manganese oxides is also affected by water vapor during actual use. The higher the relative humidity, the more serious the catalyst deactivation. It is the goal of scholars to prepare manganese-based catalyst with excellent performance at low temperature, high humidity and high space velocity. This review summarizes the progress of manganese oxides in ozone catalytic decomposition in recent years, and focuses on the progress of single component manganese-based catalysts and composite oxide manganese-based catalysts, and briefly describes the effect of basic cations on the activity of manganese-based catalyst, and summarizes water vapor, carrier selection, space velocity can affect catalyst activity. What's more, this review points out existing problems, key points and development trend of catalytic ozone decomposition.
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Effect of Iron Content on the Degradation of Methylene Blue in Fe-P-C Amorphous Alloy
MA Yaya, LI Qiang, MU Baoxia, MA Xu
Materials Reports
2021,35(21 ):21085 -21090. DOI:10.11896/cldb.21060276
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In this work, four kinds of Fe
80+2
x
P
10-
x
C
10-
x
(x=0,1,2,3, at%) amorphous alloy ribbons with different Fe contents were prepared. The catalytic degradation of methylene blue (MB) solution by Fe
80+2
x
P
10-
x
C
10-
x
(x=0,1,2,3, at%) amorphous alloy ribbons was studied by Fenton-like reaction. The results show that Fe-P-C amorphous alloy ribbons exhibit excellent degradation performance of MB solution by Fenton-like reaction, and the higher the iron content, the better the degradation performance. However, when the iron content exceeds 82at%, the effect of iron content on the degradation performance is not obvious.The surface morphology observation showed that with the increase of Fe content, the surface of the Fe-P-C amorphous ribbon after reaction showed a more porous structure, which was beneficial to obtain high degradation efficiency. The cyclic degradation test shows that the four Fe-P-C amorphous alloys with different iron contents have little difference and have long service life, which may be related to the formation of surface morphology with loose lamellar structure and 3D flower-like grid structure during the degradation process. The results of X-ray electron energy spectrum analysis showed that the different Fe content did not affect the degradation reaction mechanism of Fe-P-C amorphous alloy.
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