One-step preparation of a novel graphitic biochar/Cu0/Fe3O4 composite using CO2-ambiance pyrolysis to activate peroxydisulfate for dye degradation

Herein,a one-step co-pyrolysis protocol was adopted for the first time to prepare a novel pyrogenic carbon-Cu⁰/Fe₃O₄ heteroatoms (FCBC) in CO₂ ambiance to discern the roles of each component in PDS activation.During co-pyrolysis,CO₂ catalyzed formation of reducing gases by biomass which facilitated reductive transformation of Fe³⁺ and Cu²⁺ to Cu⁰ and Fe₃O₄,respectively.According to the a...     

载体结构对Co/MgO-Al2O3催化剂催化C2H6/CO2反应性能的影响

采用共沉淀-浸渍法制备了不同载体结构的Co/Al₂O₃、Co/MgO_（25）-Al₂O_3（75） （Co/M₁A₃-Spinel）、Co/MgO_（75）-Al₂O_3（25） （Co/M₃A₁-Solid）和Co/MgO催化剂,用于CO₂氧化乙烷脱氢（ODEC）和乙烷干重整（DRE）反应.XRD、Raman、H₂-TPR、XPS表征结果表明,载体结构显著影响催化剂上Co物种的落位、结构和还原性能.Co³⁺和Co²⁺在C₂H₆/CO₂反应气氛中可相互转化,促进C₂H₆和CO₂活化;尖晶石结构中的Co物种比固溶体中的Co物种可还原性强,在高温ODEC反应条件下,催化剂表面的Co物种会被还原成Co⁰,协同Co³⁺/Co²⁺导致C—C键和/或CC键断裂,使得反应路径向DRE转变.MgO基固溶体结构中Co物种与载体相互作用更强,在高温ODEC反应中避免了被大量还原为低价态的Co⁰,ODEC反应可稳定进行.     

Nano-sized Fe2O3/Fe3O4 facilitate anaerobic transformation of hexavalent chromium in soil–water systems

The purpose of this study is to investigate the effects of nano-sized or submicro Fe_2O_3/Fe_3O_4 on the bioreduction of hexavalent chromium(Cr(VI)) and to evaluate the effects of nano-sized Fe_2O_3/Fe_3O_4 on the microbial communities from the anaerobic flooding soil.The results indicated that the net decreases upon Cr(VI) concentration from biotic soil samples amended with nano-sized Fe_2O_3(317.1 ± 2.1 mg/L) and Fe_3O_4(324.0 ± 22.2 mg/L) within21 days,which were approximately 2-fold of Cr(VI) concentration released from blank control assays(117.1 ± 5.6 mg/L).Furthermore,the results of denaturing gradient gel electrophoresis(DGGE) and high-throughput sequencing indicated a greater variety of microbes within the microbial community in amendments with nano-sized Fe_2O_3/Fe_3O_4 than the control assays.Especially,Proteobacteria occupied a predominant status on the phylum level within the indigenous microbial communities from chromium-contaminated soils.Besides,some partial decrease of soluble Cr(VI) in abiotic nano-sized Fe_2O_3/Fe_3O_4 amendments was responsible for the adsorption of nano-sized Fe_2O_3/Fe_3O_4 to soluble Cr(VI).Hence,the presence of nano-sized Fe_2O_3/Fe_3O_4 could largely facilitate the mobilization and biotransformation of Cr(VI) from flooding soils by adsorption and bio-mediated processes.     

Kinetics of photoelectrocatalytic degradation of humic acid using B2O3·TiO2/Ti photoelectrode

An innovative photoelectrode, B₂O₃·TiO₂/Ti electrode, was prepared by galvanostaticanodisation. The morphology and crystalline texture of the B₂O₃·TiO₂ film on electrode were examined by acomic force microscopy (AFM) and X-ray diffraction respectively. The examination results indicated that the anatase was the dominant component. The kinetics of photoelectrocatalytic(PEC) degradation of humic acid(HA) was investigated; the results demonstrated that effects from strongness to weakness on the photoelectrocatalytic degraded rate of humic acid: power of UV-lamp, area of TiO₂ film, bias, original concentration of humic acid solution. The optimum conditions were power of UV-lamp 125 W, area of TiO2 film 42.0 cm² , bias 1.4 V, original concentration of humic acid solution 5 mg/L in this PEC reaction system.     

Role of NO in Hg oxidation over a commercial selective catalytic reduction catalyst V2O5–WO3/TiO2

Experiments were conducted in a fixed-bed reactor that contained a commercial catalyst, V₂O₅–WO₃/TiO₂, to investigate mercury oxidation in the presence of NO and O₂. Mercury oxidation was improved by NO, and the efficiency was increased by simultaneously adding NO and O₂. With NO and O₂ pretreatment at 350°C, the catalyst exhibited higher catalytic activity for Hg⁰ oxidation, whereas NO pretreatment did not exert a noticeable effect. Decreasing the reaction temperature boosted the performance of the catalyst treated with NO and O₂. Although NO promoted Hg⁰ oxidation at the very beginning, excessive NO counteracted this effect. The results show that NO plays different roles in Hg⁰ oxidation; NO in the gaseous phase may directly react with the adsorbed Hg⁰, but excessive NO hinders Hg⁰ adsorption. The adsorbed NO was converted into active nitrogen species (e.g., NO₂) with oxygen, which facilitated the adsorption and oxidation of Hg⁰. Hg⁰ was oxidized by NO mainly by the Eley–Rideal mechanism. The Hg⁰ temperature-programmed desorption experiment showed that weakly adsorbed mercury species were converted to strongly bound ones in the presence of NO and O₂.     

Newly developed Fe3O4–Cr2O3 magnetic nanocomposite for photocatalytic decomposition of 4-chlorophenol in water

Chlorophenols, typically 4-chlorophenols are highly toxic and non-biodegradable organic contaminants which pose serious threat to the environment, particularly when released into aqueous medium. The removal of these pollutants by efficient method has received worldwide concern in recent past. A new Fe_3O_4–Cr_2O_3 magnetic nanocomposite was synthesized by wet chemical method under ultrasonic irradiation. Microstructure and morphology of the nanocomposite were characterized by powder X-ray diffraction(XRD),Fourier transform infrared(FT-IR), and a transmission electron microscope(TEM). Magnetic and optical properties were studied by a vibrating sample magnetometer(VSM) and an ultraviolet–visible(UV–Vis) spectrophotometer respectively. The magnetic nanocomposite(MNC) was used as photocatalyst for effective decomposition of 4-chlorophenol in water under ultraviolet(UV) irradiation.     

Fe3O4/TiO2-H2O2非均相类Fenton体系对3，4-二氯三氟甲苯的降解

用Fe_3O_4/Ti O_2-H_2O_2体系对3,4-二氯三氟甲苯(3,4-DCBTE)进行降解反应研究,同时考察了pH值、催化剂投加量、H_2O_2投加量、温度等因素对3,4-DCBTE降解效率的影响.实验结果表明,Fe_3O_4/Ti O_2-H_2O_2非均相类Fenton体系对3,4-二氯三氟甲苯的处理效果极佳;并且在H_2O_2投加量为45.0 mg·L~(-1)、Fe_3O_4/TiO_2的物质的量比为1∶1、pH=3.0、温度为40.0℃的条件下反应效果最佳,去除率高达99.1%.同时从实验结果可以看出,pH在2.0~7.0范围内该体系对3,4-二氯三氟甲苯均有降解效果,说明该体系相比于传统的Fenton体系有较宽的pH适用范围.目标污染物的降解符合一级反应动力学,其发生反应所需的活化能为36.9 k J·mol~(-1).     

Mechanism of Hg oxidation in the presence of HCl over a commercial V2O5–WO3/TiO2 SCR catalyst

Experiments were conducted in a fixed-bed reactor containing a commercial V₂O₅/WO₃/TiO₂ catalyst to investigate mercury oxidation in the presence of HCl and O₂. Mercury oxidation was improved significantly in the presence of HCl and O₂, and the Hg⁰ oxidation efficiencies decreased slowly as the temperature increased from 200 to 400°C. Upon pretreatment with HCl and O₂ at 350°C, the catalyst demonstrated higher catalytic activity for Hg⁰ oxidation. Notably, the effect of pretreatment with HCl alone was not obvious. For the catalyst treated with HCl and O₂, better performance was observed with lower reaction temperatures. The results showed that both HCl and Hg⁰ were first adsorbed onto the catalyst and then reacted with O₂ following its adsorption, which indicates that the oxidation of Hg⁰ over the commercial catalyst followed the Langmuir–Hinshelwood mechanism. Several characterization techniques, including Hg⁰ temperature-programmed desorption (Hg-TPD) and X-ray photoelectron spectroscopy (XPS), were employed in this work. Hg-TPD profiles showed that weakly adsorbed mercury species were converted to strongly bound species in the presence of HCl and O₂. XPS patterns indicated that new chemisorbed oxygen species were formed by the adsorption of HCl, which consequently facilitated the oxidation of mercury.     

Bi2O3-TiO2复合光催化剂协同处理铬-邻苯二甲酸酯复合污染

以硝酸铋和钛酸丁酯为前驱体,采用水热法制备了Bi_2O_3-TiO_2复合半导体材料,并利用X射线衍射(XRD)、紫外-可见吸收光谱(UVVis)、能谱分析(EDS)、X射线光电子能谱(XPS)等手段对复合材料的结构进行了表征.同时,考察了Bi_2O_3-TiO_2复合材料对重金属Cr(Ⅵ)和难降解邻苯二甲酸二丁酯(DBP)复合污染的处理性能,并探讨了复合催化剂协同处理复合污染的作用机制.结果表明:该复合催化剂在可见光下能同时降低重金属Cr(Ⅵ)和有机物DBP的浓度,抑制电子和空穴复合,表现出比对单一Cr(Ⅵ)及DBP污染物更高的处理效率.当Bi_2O_3含量为4%时,复合催化剂表现出最佳的光催化活性.     

Highly selective catalytic reduction of NOxby MnOx–CeO2–Al2O3 catalysts prepared by self-propagating high-temperature synthesis

We first present preparation of MnOx–CeO_2–Al_2O_3 catalysts with varying Mn contents through a self-propagating high-temperature synthesis(SHS) method, and studied the application of these catalysts to the selective catalytic reduction of NOxwith NH3(NH_3-SCR).Using the catalyst with 18 wt.% Mn(18 MnCe1Al2), 100% NO conversion was achieved at 200°C and a gas hourly space velocity of 15384 hr-1, and the high-efficiency SCR temperature window, where NO conversion is greater than 90%, was widened to a temperature range of 150–300°C. 18 MnCe1Al2 showed great resistance to SO_2(100 ppm)and H_2O(5%) at 200°C. The catalysts were characterized using X-ray diffraction, X-ray photoelectron spectroscopy, Brunauer–Emmett–Teller(BET) analysis, scanning electron microscopy, Fourier transform infrared spectroscopy, and H_2 temperature programmed reduction. The characterization results showed that the surface atomic concentration of Mn increased with increasing Mn content, which led to synergism between Mn and Ce and improved the activity in the SCR reaction. 18 MnCe1Al2 has an extensive pore structure,with a BET surface area of approximately 135.4 m~2/g, a pore volume of approximately 0.16 cm~3/g, and an average pore diameter of approximately 4.6 nm. The SCR reaction on 18 MnCe1Al2 mainly followed the Eley-Rideal mechanism. The performances of the MnOx–CeO_2–Al_2O_3 catalysts were good, and because of the simplicity of the preparation process,the SHS method is applicable to their industrial-scale manufacture.     

纳米Fe3O4/CeO2-H2O2非均相类Fenton体系对3,4-二氯三氟甲苯的降解

以浸渍法制备的新型纳米Fe3O4/Ce O2为催化剂,3,4-二氯三氟甲苯(3,4-DCBTE)为目标污染物,在Fe3O4/Ce O2-H2O2非均相类Fenton体系中对目标污染物的降解进行研究,考察催化剂的催化效果和温度、p H、H2O2投加量等因素对催化剂催化效果的影响.结果表明,以纳米Fe3O4/Ce O2作为催化剂的非均相类Fenton体系对3,4-二氯三氟甲苯的处理效果极佳;随着温度的升高,纳米Fe3O4/Ce O2的催化效果不断提高;在偏酸性环境中,p H越低催化效果越好,p H=2时反应去除效率可达96.67%;随着H2O2投加量的增加,3,4-二氯三氟甲苯的降解效率先提高后降低,投加量为15 mg·L-1时去除效果最好可达99.47%;随着催化剂投加量的增加,同样出现了处理效果先升高后降低的现象,投加量为0.5 g·L-1时催化效果最好可达99.64%.在以纳米Fe3O4/Ce O2为催化剂的非均相类Fenton体系中,3,4-二氯三氟甲苯的降解符合一级反应动力学,反应所需活化能较低只需30.26 k J·mol-1.     

核-壳结构的Fe-FeOxH2x-3催化UV/H2O2降解腐殖酸

采用硼氢化钠还原法制备了核-壳结构的Fe-FeOxH2x-3纳米复合材料,在近紫外光和H2O2催化条件下,对饮用水消毒副产物前驱体腐殖酸的去除比纳米零价铁的去除高.说明零价铁表面铁氧化物能加速界面电子转移,提高反应效率.探讨了H2O2浓度、腐殖酸初始浓度和起始溶液pH对反应速率的影响.研究结果表明,H2O2最佳投加量为5 mmol·L-1,在pH为5～9时,催化剂都显示了较高的活性;腐殖酸不但被脱色降解,而且TOC去除率达到60%,并且生成的中间产物降低了三氯甲烷的生成趋势.     

MnO2/Al2O3催化剂-微气泡臭氧体系催化降解喹啉及其机理

制备了纳米MnO₂,并以Al₂O₃为载体制备了掺杂型MnO₂/Al₂O₃颗粒催化剂.催化剂焙烧温度和时间分别为500℃和4 h、MnO₂质量分数为8%时,催化剂具有最高的臭氧催化氧化活性.SEM分析表明,纳米MnO₂均匀分布于Al₂O₃载体表面.MnO₂/Al₂O₃催化剂的比表面积（BET）为183.22 m²·g^-1,平均孔容为0.27 cm³·g^-1,平均孔径为4.87 nm.建立了MnO₂/Al₂O₃催化剂-微气泡臭氧催化反应体系,研究了该体系对喹啉的降解去除效果及其机理.臭氧微气泡的平均粒径为61.7 μm.微气泡臭氧投量为30 mg·L^-1时,反应60 min后喹啉去除率能达到95%以上;反应20 min后,MnO₂/Al₂O₃催化剂-微气泡臭氧体系对实际煤化工废水二级出水的TOC去除率可达到55%以上.以叔丁醇作为分子探针,证明了羟基自由基（·OH）氧化作用在臭氧微气泡催化氧化体系中对喹啉的降解起到主导作用.     

Enhancement of the CO2 adsorption and hydrogenation to CH4 capacity of Ru–Na–Ca/γ–Al2O3 dual function material by controlling the Ru calcination atmosphere

Integrated CO₂capture and utilization (ICCU) technology requires dual functional materials(DFMs) to carry out the process in a single reaction system.The influence of the calcination atmosphere on efficiency of 4%Ru-8%Na₂CO₃-8%CaO/γ-Al₂O₃DFM is studied.The adsorbent precursors are first co-impregnated onto alumina and calcined in air.Then,Ru precursor is impregnated and four aliquotes are subjected to different calcination protocols:static a...     

Enhanced photocatalytic performance of Bi2O2CO3/Bi4O5Br2/reduced graphene oxide Z-schemehe terojunction via a one-pot room-temperature synthesis

Bi₂O₂CO₃(BOC)/Bi₄O₅Br₂(BOB)/reduced graphene oxide (rGO) Z-scheme heterojunction with promising photocatalytic properties was synthesized via a facile one-pot room-temperature method.Ultra-thin nanosheets of BOC and BOB were grown in situ on r GO.The formed 2D/2D direct Z-scheme heterojunction of BOC/BOB with oxygen vacancies (OVs) effectively leads to lower negative electron reduction potential of BOB as well as higher positive h...     

γ-射线辐照-H2O2联合技术降解3-氯酚的研究

利用60Coγ-射线辐照3-氯酚(3-CP)水溶液,研究了其辐射降解特性.通过测量辐射后3-氯酚的去除率、紫外-可见光谱、脱氯率、总有机碳(TOC)去除率等,探讨了吸收剂量、氯酚初始浓度、H2O2加入对氯酚降解效果的影响,并初步探讨了氯酚降解动力学特性.结果表明,当3-氯酚浓度为10 mg.L-1,辐射剂量为2 kGy时,脱氯率可达100%,TOC去除率达53%;当辐射剂量提高到8 kGy时,3-氯酚可完全矿化,TOC去除率达100%.3-氯酚的辐照降解过程可用一级反应动力学方程拟合.氯酚单独γ-辐射以及辐照/H2O2联合处理的一级反应动力学常数k分别为0.279 h-1和0.542 h-1.     

Mesoporous carbon adsorbents from melamine–formaldehyde resin using nanocasting technique for CO2 adsorption

Mesoporous carbon adsorbents, having high nitrogen content, were synthesized via nanocasting technique with melamine–formaldehyde resin as precursor and mesoporous silica as template. A series of adsorbents were prepared by varying the carbonization temperature from 400 to 700°C. Adsorbents were characterized thoroughly by nitrogen sorption, X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), thermogravimetric analysis (TGA), elemental (CHN) analysis, Fourier transform infrared (FTIR) spectroscopy and Boehm titration. Carbonization temperature controlled the properties of the synthesized adsorbents ranging from surface area to their nitrogen content, which play major role in their application as adsorbents for CO₂ capture. The nanostructure of these materials was confirmed by XRD and TEM. Their nitrogen content decreased with an increase in carbonization temperature while other properties like surface area, pore volume, thermal stability and surface basicity increased with the carbonization temperature. These materials were evaluated for CO₂ adsorption by fixed-bed column adsorption experiments. Adsorbent synthesized at 700°C was found to have the highest surface area and surface basicity along with maximum CO₂ adsorption capacity among the synthesized adsorbents. Breakthrough time and CO₂ equilibrium adsorption capacity were investigated from the breakthrough curves and were found to decrease with increase in adsorption temperature. Adsorption process for carbon adsorbent–CO₂ system was found to be reversible with stable adsorption capacity over four consecutive adsorption–desorption cycles. From three isotherm models used to analyze the equilibrium data, Temkin isotherm model presented a nearly perfect fit implying the heterogeneous adsorbent surface.     

Integrated CO2 capture and reduction catalysis:Role of γ-Al2O3 support,unique state of potassium and synergy with copper

Carbon dioxide capture and reduction (CCR) process emerges as an efficient catalytic strategy for CO₂ capture and conversion to valuable chemicals.K-promoted Cu/Al₂O₃ catalysts exhibited promising CO₂ capture efficiency and highly selective conversion to syngas(CO+H₂).The dynamic nature of the Cu-K system at reaction conditions complicates the identification of the catalytically active phase and surface sites.The present work aims at more pr...     

壳-核结构Fe3O4/MnO2磁性吸附剂的制备、表征及铅吸附去除研究

采用共沉淀法制备了具有壳-核结构的磁性吸附剂Fe₃O₄/MnO₂,对其性质进行了系统表征,并对其铅吸附行为进行了初步研究.透射电镜(TEM)结果表明,Fe₃O₄/MnO₂为大小不规则的纳米级细小颗粒.X-射线衍射仪(XRD)表征结果表明,Fe₃O₄/MnO₂具有尖晶石的结构.振动样品磁强计(VSM)测得比饱和磁化强度为54.7 A·m²·kg^-1, 吸附剂磁性较强,易于磁分离;BET比表面积为76.5 m²·g^-1.吸附试验结果表明,Fe₃O₄/MnO₂对铅具有良好的去除效果(特别是在低平衡浓度情况下),最大吸附量为142.0 mg·g^-1(pH=5.0);Langmuir等温线能更好地拟合Fe₃O₄/MnO₂对溶液中铅的吸附(R²=0.852);吸附速率较快,在初始30 min内可达到平衡吸附量的80%,准二级动力学模型(R²=0.959)能较好地描述吸附过程;溶液pH对Fe₃O₄/MnO₂吸附铅的影响较为明显,随pH升高,吸附量增大,但离子强度变化对吸附影响不大.     

TiO2–PANI/Cork composite: A new floating photocatalyst for the treatment of organic pollutants under sunlight irradiation

A novel photocatalyst based on TiO_2–PANI composite supported on small pieces of cork has been reported. It was prepared by simple impregnation method of the polyaniline(PANI)–modified TiO_2 on cork. The TiO_2–PANI/Cork catalyst shows the unique feature of floating on the water surface. The as-synthesized catalyst was characterized by X-ray diffraction(XRD),scanning electron micrograph(SEM), transmission electron microscopy(TEM), thermogravimetric analysis(TGA), Fourier transform infrared spectroscopy(FT-IR), UV–vis diffuse reflectance spectra(UV–vis DRS) and the Brunauer–Emmett–Teller(BET) surface area analysis. Characterization suggested the formation of anatase highly dispersed on the cork surface. The prepared floating photocatalyst showed high efficiency for the degradation of methyl orange dye and other organic pollutants under solar irradiation and constrained conditions, i.e., no-stirring and no-oxygenation. The TiO_2–PANI/Cork floating photocatalyst can be reused for at least four consecutive times without significant decrease of the degradation efficiency.