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    1. 硅钨酸酸化的新型MIL-101(Cr)催化剂及其对正庚烷异构化反应的催化性能
    张微 刘荣江 马守涛 Dimitriy Kuvshinov 所艳华 汪颖军
    中国炼油与石油化工    2022, 24 (1): 68-80.  
    摘要434)      PDF(pc) (1596KB)(63)    收藏
    0.4%Pt/xSTA-MIL-101(Cr) metal-acid bifunctional catalysts were prepared by impregnation using STA-MIL-101(Cr) as the support. The synthesized samples were verified to exhibit a typical octahedral structure of MIL-101(Cr) and the pore structure were arranged orderly. The specific surface area of the samples was extremely high and the samples were micro-mesoporous composite materials. Silicotungstic acid could retain its Keggin structure in the 0.4%Pt/xSTA-MIL-101(Cr) samples and the catalyst possessed moderately strong Br?nsted acid sites. Besides, the dispersion of Pt particles in MIL-101(Cr) was relatively high. n-Heptane isomerization was first used as a probe to test the novel 0.4%Pt/xSTA-MIL-10(Cr) catalyst. Compared with the conventional silicate catalysts, the catalytic performance of 0.4%Pt/30wt%STA-MIL-101(Cr) was significantly improved with n-heptane conversion of 58.93% and iso-heptane selectivity of 95.68%, respectively, when the reaction time was 2 h at the reaction temperature of 260 oC. The catalyst could still maintain a relatively high catalytic performance during the reaction time of 5 h. Compared with the non-noble metal catalysts, the catalytic efficiency is relatively high. The mechanism model of n-heptane isomerization over 0.4%Pt/xSTA-MIL-101(Cr) catalyst was established.
    参考文献 | 相关文章 | 多维度评价
    2. 碳包覆镍纳米复合材料在锂硫电池正极中的应用
    杨宇翔 谢婧新 吴耿煌 朱娜 李欢 荣峻峰
    中国炼油与石油化工    2021, 23 (4): 1-6.  
    摘要179)      PDF(pc) (882KB)(200)    收藏
    锂硫电池有望成为下一代高能量密度储能设备。近年来,“电催化”的概念被引入锂硫电池领域中,一些过渡金属被证明可以催化含硫物质的电化学转化反应。本工作中,比表面积为146 m2/g的碳包覆镍纳米材料对于硫正极的电化学反应具有电催化作用。加入碳包覆镍材料后,Ni@C/G-S电池获得了比G-S电池更好的电化学性能。在此基础上,通过对碳包覆镍的碳壳表面进行化学改性,进一步提高了锂硫电池的可逆比容量和循环稳定性。此外,本文详细研究了碳壳不同元素掺杂对锂硫电池性能的影响。N-Ni@C-G/S电池在0.2 C、0.5 C和1.0 C倍率下实现了更高的比容量,分别为1229 mAh/g、927 mAh/g和830 mAh/g;而B-Ni@C-G/S电池具有最好的循环稳定性。
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    3. 催化油浆基杂原子掺杂碳球在锂离子电池阳极材料中的应用
    杨光 Dengke Wang Song Chen 张玥 符子剑 Wei Liu
    中国炼油与石油化工    2022, 24 (1): 1-10.  
    摘要144)      PDF(pc) (1988KB)(130)    收藏
    本研究以催化油浆为碳源,采用注入热解法在700-1000℃条件下制备具有良好导电性的杂原子掺杂碳球(CSs)。利用扫描电子显微镜(SEM)、透射电子显微镜(TEM)、X射线衍射(XRD)、拉曼光谱、红外光谱(FT-IR)和X射线光电子能谱(XPS)对材料的结构进行表征。探讨了反应条件对CSs形貌的影响并研究了其作为锂离子电池(LIBs)阳极材料的电化学性能。研究结果表明,杂原子掺杂碳球主要含有C、N、O、S四种元素。随着热解温度的升高,CSs粒径减小但石墨化程度提高。作为锂离子电池阳极材料,在50 mA·g-1的电流密度下,CSs具有365 mAh·g-1的比容量及73.8%的初始库仑效率。在50 mA·g-1到 2 A·g-1的电流范围内CSs具有良好的性能,当电流循环回50 mA·g-1时,CSs仍保持347 mAh·g-1的稳定可逆容量。这主要归因于CSs具有合适的杂原子含量和独特的球形结构。这种杂原子掺杂CSs为制备高效锂离子电池阳极材料提供了一种新的选择。
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    4. Dechlorination of Crude Oil by Phase Transfer Catalyst in Nucleophilic Substitution Reaction
    顾晋 韩鑫 刘纪昌 黄自豪 邢彪
    中国炼油与石油化工    2021, 23 (4): 18-28.  
    摘要128)      PDF(pc) (836KB)(145)    收藏
    Dechlorination of crude oil is an effective way to alleviate corrosion in refinery units, and the critical process is the removal of organochlorine which can be efficiently removed through nucleophilic substitution reaction catalyzed by phase transfer. Herein, seven typical chlorinated alkanes were selected as model compounds to study the mechanism of dechlorination of crude oil by phase transfer catalyst in the nucleophilic substitution method, and a new dechlorination reagent using hexamethyl quaternary ammonium hydroxide with two quaternary ammonium groups as phase transfer catalyst, ethylenediamine as nucleophile and ethanol as solvent was developed. The results show that the dechlorinating performances of the dechlorination reagent on the model compounds are as follows: epichlorohydrin > 1,2-dichlorobutane > 1,2-dichloroethane > 1,3-dichloropropane > 2-chloropropane > 1-chlorobutane > chloroisobutane, and the results of the reaction kinetics show that epichlorohydrin with epoxy structure has the lowest activation energy in the process of nucleophilic substitution reaction by the phase transfer catalyst which makes it easier to be removed by the dechlorination reagent. The removal rate of epichlorohydrin can reach up to 99.4%. The optimal dechlorination reagent used ethylenediamine as nucleophile, ethanol as solvent and hexamethyl quaternary ammonium hydroxide as phase transfer catalyst. The dechlorinating rate of the Iranian crude oil reached 71.6 % at the reaction temperature of 95°C, the reaction time of 90 minutes, the dechlorination reagent dosage of 1000 mg/kg and the 6:1 molar ratio of phase transfer reagent and nucleophile. In addition, the mechanism of phase transfer in nucleophilic substitution reaction of chloroalkanes is investigated in the paper.
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    5. 增强甲苯燃烧催化活性的MnxCo3-xO4微管:氧化还原性能的影响 氧和氧物种
    张晗禹 胡悦 张潇寒 孙梦瑶 刘蕊 金泉 齐健
    中国炼油与石油化工    2021, 23 (4): 7-17.  
    摘要117)      PDF(pc) (1344KB)(120)    收藏
    Redox property and oxygen species play important role in the catalytic oxidation of volatile organic compounds (VOCs). In this paper, a series of MnxCo3-xO4 catalysts with tubular structure were synthesized and applied for the catalytic combustion of toluene. Various characterization technologies were employed to reveal the relationship between the catalytic performance of the MnxCo3-xO4 catalysts and Mn doping. The results of XRD, SEM and N2 adsorption-desorption showed that the Mn doping had significant effects on the structure and morphology of the MnxCo3-xO4 catalysts. The H2-TPR, O2-TPD and XPS results proved that the strong interaction between Co and Mn resulted in the enhanced Olatt mobility, richer active oxygen species, and enhanced redox property in comparison with the pure Co3O4 sample, which were crucial to the improvement of the catalytic activity of Co-Mn catalysts. The best catalyst, Co5-Mn5 sample, exhibited a good and stable activity to catalytically oxidize toluene at low temperatures even in the presence of water vapor, indicating that it is a potential material for the practically catalytic industrialization for the abatement of toluene.
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    6. Photocatalysts for photocatalytic CO2 reduction:A review
    张力中
    中国炼油与石油化工    2022, 24 (1): 149-160.  
    摘要101)      PDF(pc) (328KB)(96)    收藏
    Energy crisis and environmental pollution have become vitally severe challenges for the current society. During the circumstances of pursuing carbon peak and carbon neutrality, photocatalytic CO2 reduction will be an essential, necessary and even inevitable development requirement and trend. However, there are some bottlenecks that need to be addressed immediately, such as low quantum efficiency and narrow light absorption range for single photocatalysts. Therefore, efficient and stable visible light driving materials are the core challenge in the field of photocatalytic CO2 conversion. This paper reviewed the photocatalysts used for CO2 reduction classified as metal photocatalysts, non-metal photocatalysts, and MOFs photocatalysts, and the CO2 reduction capacity and mechanism of different photocatalysts were described. In the end, the problems to be solved and the future development of photocatalytic CO2 reduction were summarized.
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    7. 生物炭负载纳米零价铁去除水中石油污染物
    覃菲菲 徐文斐 郝博宇 尹凌皓 宋佳宇 张秀霞
    中国炼油与石油化工    2021, 23 (4): 47-57.  
    摘要96)      PDF(pc) (873KB)(82)    收藏
    在油田开采过程中,化学药剂的大量使用导致原油乳化严重,使得产出液中含有大量难以去除的原油。为了高效、快速且不产生二次污染地处理含油污水,本研究将纳米零价铁负载在菌糠生物炭上,制备了一种新型的铁炭复合材料(SMS-nZVI),并全面评估了其处理高浓度石油污水的的能力。室内模拟除油实验,结果表明,与单独的菌糠生物炭和纳米零价铁相比,SMS-nZVI除油速度快、效果显著。采用SEM,TEM,BET和FTIR对材料的形貌,结构和性能进行了表征,结果表明,采用生物炭做基底材料可以有效地防止纳米零价铁的团聚,增加材料整体比表面积,增强材料吸附能力。将菌糠生物炭基底与其他生物炭基底进行对比发现,菌糠生物炭制备的铁炭复合材料除油效果优于传统的小麦秸秆生物炭。通过对实验条件的优化,得到了具有最佳除油效果的操作工艺:当纳米零价铁与生物炭的质量比为1:5,pH值为4,原油的初始浓度为1000mg·L-1时,水中石油的去除率在5h时可达到95%。将SMS-nZVI暴露在空气中30天进行自然老化处理后,材料仍能保持62%以上的石油去除率,这说明该材料具有良好的稳定性。
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    8. Cu-Zr复合氧化物负载PdO催化氯丙烯醚化合成烯丙基醚
    袁恩先 桑瑞士 菅盘铭
    中国炼油与石油化工    2021, 23 (4): 65-74.  
    摘要96)      PDF(pc) (1778KB)(97)    收藏
    本文采用共沉淀法制备了一系列Cu/Zr比从2/8至9/1的铜-锆复合氧化物,再负载PdO用于氯丙烯与醇醚化反应合成烯丙基醚。PdO/CumZrn催化剂的表征结果证实ZrO2相的存在不仅有益于Pd2+的高分散,同时也能与CuO作用有利于Cu+的生成。PdO/CumZrn催化性能随着Cu/Zr比的增加呈现先增强后减弱的趋势,具有高Cu+含量的PdO/Cu7Zr3催化剂显示出最优性能,反应转化率和选择性分别为53.2%和60.3%。这是因为相比于Cu2+-O2-对,Cu+-Oα-对能够增强醇中-O-H键的解离活化,从而提升了醚化反应。
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    9. 硫掺杂g-C3N4多孔纳米片的制备及其光催化降解性能研究
    刘源 赵华 李会鹏 蔡天凤
    中国炼油与石油化工    2022, 24 (1): 81-89.  
    摘要91)      PDF(pc) (1616KB)(78)    收藏
    Abstract: In this study, sulfur-doped porous g-C3N4 nanosheets (CN-T-U 1.75) have been synthesized successfully by one-step calcination using urea and thiourea as the precursors. CN-T-U 1.75 exhibited excellent photocatalytic performance for Rhodamine B (RhB) degradation under visible light irradiation, with the kinetic reaction rate constant of 0.01838 min-1. Analysis of the characterization results showed that CN-T-U 1.75 had a larger specific surface area, and the doping caused a change in the energy band structure. Moreover, the catalytic mechanism analysis shows it could produce two oxidation groups of ?O2- and ?OH to degrade pollutants synergistically.
    参考文献 | 相关文章 | 多维度评价
    10. 润滑油基础油氧化链引发反应机理的分子模拟
    夏垒 李岩 张红梅 姜正义 龙军
    中国炼油与石油化工    2021, 23 (4): 105-112.  
    摘要85)      PDF(pc) (345KB)(117)    收藏
    Chain initiation reactions in the oxidation process of lubricant base stock molecules were studied by molecular simulations. Two ways to initiate lubricant oxidation were investigated. They were the dissociation of chemical bonds in base stock molecules and the reaction between base stock molecules and oxygen (O2), respectively. Reaction activation energies of above methods were calculated. The results show that C—C bonds are more likely to break than C—H bonds to generate free radicals by the pyrolysis of chemical bonds. The C—C bonds with tertiary carbon atoms are preferential positions to crack. However, bond dissociation energies of them are above 360 kJ/mol, which are difficult to occur under lubricant working conditions. The chain initiation is more likely to occur by the way that O2 attacks the two atoms in C—H bonds at the same time, and embeds into the C—H bond to produce hydrocarbon peroxides. And then, the O—O bond is cracked to form hydroxyl radicals and alkoxy radicals. The C—H bonds with tertiary carbon atoms are the preferential reaction sites, whose reaction activation energy is about 190.11 kJ/mol.
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    11. Study on viscosity reducing and oil displacement agent for water-flooding heavy oil reservoir
    秦冰 赵琳 江建林
    中国炼油与石油化工    2022, 24 (1): 11-18.  
    摘要83)      PDF(pc) (1282KB)(119)    收藏
    In the process of water-flooding development of heavy oil reservoir, due to the high viscosity and oil-water mobility ratio of heavy oil, there are some problems such as poor fluidity, high residual oil saturation and low recovery efficiency, which seriously restrict the efficient development of heavy oil. The molecular structure characteristics of asphaltene and resin in heavy oil were analyzed. Based on the three most concerned properties of chemical agents, including emulsification performance, interface performance and oil washing performance, three chemical oil displacement agents for heavy oil reservoirs were developed, and the structure of the chemical agents were characterized by high resolution mass spectrometry. The performance evaluation of chemical agent and core displacement experiment show that there is no obvious correlation between the properties of chemical agents, including interfacial tension, emulsifying ability and oil washing ability. For heavy oil reservoirs, the emulsification and viscosity reduction performance of chemical agents was more important than oil washing capacity, and oil washing capacity was more important than interface performance. Viscosity reduction performance was the key parameter of oil displacement agent suitable for heavy oil reservoir. The composite binary system of viscosity reducer and polymer had better oil recovery than using viscosity reducer alone.
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    12. 碳微球负载镍催化顺酐选择性加氢制备丁二酸酐
    周娅芬 陈其嶙 王清 宋宇 周丽梅
    中国炼油与石油化工    2021, 23 (4): 75-82.  
    摘要81)      PDF(pc) (818KB)(141)    收藏
    采用水热法制备了胶态碳微球(CMS),进一步制备了碳微球负载镍催化剂(Ni/CMS), 并进行了FTIR、XRD、SEM、TEM和N2吸附表征。对Ni/CMS催化顺酐(MA) 选择性加氢制备丁二酸酐(SA) 进行了考察,结果表明,以葡萄糖为碳源,经过500 ○C焙烧制备的Ni/CMS催化剂表现最佳的性能,氢气压力、反应温度和反应时间对加氢反应中顺酐转化率有很大影响。以乙酸酐作溶剂,在90 ○C、1.0 MPa H2压力、反应3小时的温和条件下,顺酐在Ni/CMS催化剂上转化率达到98.4%,丁二酸酐选择性为100%。
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    13. Study on Spray Characteristics of Dimethyl carbonate Blended Fuel in IC Engines
    付炜 周坤 刘俊亚 谢鸿玺 李亚运 陆磊 包继虎 程云朗
    中国炼油与石油化工    2021, 23 (4): 29-36.  
    摘要80)      PDF(pc) (1542KB)(121)    收藏
    In this study, the spray characteristics of the blended fuel of biodiesel and Dimethyl carbonate were compared with those of biodiesel and diesel. The macroscopic spray characteristics parameters including spray tip penetration, maximum spray width, average spray cone angle and peak tip velocity were used to evaluate the spray characteristics of the blended fuel. The results showed that the spray tip penetration of blended fuel was lower than that of biodiesel, while the spray cone angle and maximum spray width of blended fuel were both larger than that of biodiesel. On the basis of Hiroyasu and Arai mathematical model, combined with the actual working conditions of this experiment, including the viscosity and density of the fuel physical parameters, a correct model of spray penetration was established, and the experimental results were compared.
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    14. 钠离子交换型层状磷酸锆的合成与摩擦学性能
    田成光 张效胜 徐红 董晋湘
    中国炼油与石油化工    2021, 23 (4): 83-94.  
    摘要75)      PDF(pc) (1911KB)(95)    收藏
    本文以磷酸氢二钠为钠源合成了钠离子交换型层状磷酸锆材料(Na-α-ZrP),该方法是一种高效的离子交换方法。分别采用四球摩擦试验机和SRV试验机研究了Na-α-ZrP作为锂基润滑脂添加剂的摩擦学性能,此外,还研究了Na-α-ZrP与ZDDP的协同效果。结果表明,Na-α-ZrP能有效提高锂基脂的减摩抗磨性能,与ZDDP复配后,在高载荷下表现出优异的抗磨性能。使用3D光学轮廓仪、扫描电子显微镜(SEM)、能谱仪(EDS)和X射线光电子能谱(XPS)观察了磨损表面,提出了其中可能存在的润滑机理。简单高效的合成方法和优越的摩擦学性能使Na-α-ZrP具备成为润滑添加剂的潜在可能。
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    15. Investigation of nitrite production pathway in integrated partial denitrification/anammox process via isotope labelling technique and the relevant microbial communities
    李妍喆 盖佳柠 张晓飞 赵东风 国亚东 余庚星 赵朝成 刘芳 赵瑞玉 刘春爽
    中国炼油与石油化工    2022, 24 (1): 129-134.  
    摘要75)      PDF(pc) (795KB)(52)    收藏
    本文采用UASB反应器研究了短程反硝化/厌氧氨氧化(PDA)工艺的脱氮性能。在氮负荷率为0.64kg/(m3?d)实现了较高的总氮(TN)去除率(91.97%)。15N同位素标记实验结果显示,厌氧氨氧化菌确实在PDA中执行了将硝酸盐转化为亚硝酸盐的功能,贡献率约为36.3%。Candidatus_Brocadia, Candidatus_Kuenenia 和Thauera分别是厌氧氨氧化和反硝化过程的功能菌株。Thauera 和Candidatus_Brocadia 在高负荷下(0.64kg/(m3?d))对TN去除非常重要。实验结果为PDA工艺的应用提供了理论和技术基础。
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    16. 一种防卡咬螺纹润滑剂的理化和摩擦学性能研究
    王志民 向硕 刘晓强 鲍一晨 石秀强 何燕
    中国炼油与石油化工    2021, 23 (4): 95-104.  
    摘要72)      PDF(pc) (2918KB)(89)    收藏
    Di-aromatics base oil and graphite powder, adding with viscosity index improver and anti-oxidant and rheological additive, were used to prepare a kind of anti-seize thread lubricant. Its physical chemistry properties, such as water resistance, thermal oxidation and aging properties, tribological performance were evaluated and compared with those of some commercial product. The results show that the overall the overall performance of the anti-seize thread lubricant met the level of some commercial product, and some properties such as thermal stability, anti-wear and anti-friction properties were better. It is more suitable for high temperature conditions.
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    17. Reaction Process of Heavy Hydrocarbon in Ebullated Bed Hydrogenation
    王建军 仝玉军 杨涛 葛海龙 孟兆会
    中国炼油与石油化工    2021, 23 (4): 113-120.  
    摘要71)      PDF(pc) (453KB)(111)    收藏
    The properties and structural changes of unconverted oil (UCO) in ebullated bed residue hydrogenation at different conversion rates were analyzed to clarify the reaction process of heavy components. Meanwhile, the processing routes of UCO, delay coking and solvent deasphalting, were investigated. The results showed that with the increase of conversion, the impurity removal rate increased; meanwhile the contents of sulfur and metal in UCO decreased, while the contents of nitrogen and residual carbon increased, and the colloidal stability of UCO became worse. The structural parameters of UCO indicated that the change of heavy oil molecular structure was mainly opening of cycloalkanes ring, hydrogenation saturation of aromatic rings and dealkylation reaction during the ebullated bed hydrogenation; the aromatic structure was basically unchanged at high conversion, mainly due to the ring opening of cycloalkanes and the fracture reaction of alkyl side chains. The coking route of UCO showed that low sulfur petroleum coke with different grades could be prepared by adjusting ebullated bed conversion to produce UCOs with different properties. The coke generating coefficient and sulfur transfer coefficient in UCO coking process were higher than those in residue coking. The properties of deasphalt oil (DAO) of UCO was significantly improved and could be used as FCC or hydrocracking feedstock. The DAO yield of UCO feedstock at high conversion was higher, and its sulfur content was lower and residual carbon value was higher.
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    18. 增容剂对SBS改性沥青相容性和流变特性的影响研究
    董夫强 郝运哲 于新 时敬涛 陈贝 秦成林
    中国炼油与石油化工    2021, 23 (4): 37-46.  
    摘要68)      PDF(pc) (1027KB)(110)    收藏
    Adding compatibilizer to polymer-modified asphalt (PMA) is an effective method to improve material compatibility and performance. However, only a few studies have systematically focused on how compatibilizer can affect the performance of styrene-butadiene-styrene (SBS) polymer-modified asphalt (PMA). In this study, six compatibilizers with different compositions were used to prepare SBS PMA samples. Conventional performance, viscosity-temperature characteristics, viscoelastic behavior, creep properties, and morphology were investigated. The results show that adding compatibilizer to SBS PMA has a great effect on performance. High aromatics content in compatibilizers improve the high-temperature performance of SBS PMA, while a high saturates content increases low-temperature performance. Additionally, a high aromatics compatibilizer increases temperature sensitivity. While the aromatics content improves the compatibility of SBS PMA to some extent, adding compatibilizer to SBS PMA has few effects on microstructure. From our results, we can conclude that the optimum aromatics content for adding compatibilizer to SBS PMA is from 33.21 wt% to 54.22 wt%.
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    19. SA-ZnO@ODA-GO@PU 超疏水涂层的抗菌防腐性能
    刘芳 孔灿 李炜 姜国飞 王雪尧
    中国炼油与石油化工    2022, 24 (1): 117-128.  
    摘要65)      PDF(pc) (1660KB)(65)    收藏
    为了解决循环冷却水系统的腐蚀问题,合成了SA-ZnO@ODA-GO@PU超疏水管道防护涂料。涂料经过疏水改性后,涂层的接触角(CA)在150°以上。涂层的抗菌能力对防腐性能至关重要。SA-ZnO@ODA-GO会严重破坏细胞结构,使细胞内容物外流,增加蛋白质的漏出率,使细菌在24小时内无法达到对数生长期。SA-ZnO@ODA-GO@PU涂层SA的缓蚀机理分析表明,疏水改性涂层形成物理屏障,防止水分子进入碳钢。在试样表面,涂层阻止了电荷转移。
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    20. Fe2O3复合BiOCl的制备及其光催化性能研究
    刘晓庆 王紫莎 胡宇星 王海芳
    中国炼油与石油化工    2022, 24 (1): 59-67.  
    摘要65)      PDF(pc) (1731KB)(74)    收藏
    Fe2O3 was synthesized by the solvothermal method, and the synthesized Fe2O3 was added in the process of preparing BiOCl by hydrolysis, and then Fe2O3/BiOCl photocatalytic materials with different composite ratios were prepared. The optimal Fe2O3/BiOCl (1Fe/50Bi) sample showed a highest photocatalytic efficiency for cationic dyes (Rhodamine B) and anionic dye (methyl orange) degradation irradiated with visible light, as compared with that of a bare BiOCl catalyst. Meanwhile, radical capturing experiments indicated that the photo-induced holes (h+) is the main active species. X-ray powder diffraction and ultraviolet-visible diffuse reflectance spectroscopy were used to characterize the structural and optical properties, which proved that Fe2O3 was successfully composited to the BiOCl surface and effectively reduced the bandgap of BiOCl. More importantly, the optimal 1Fe/50Bi sample shows the highest photocatalytic efficiency for tetracycline (TC) degradation (98%) irradiated with visible light, as compared with that of a bare BiOCl catalyst. Consequently, the Fe2O3/BiOCl photocatalyst have potential applications in environmental purification.
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