Enhanced remediation of Cr（Ⅵ）-contaminated groundwater by coupling electrokinetics with ZVI/Fe3O4/AC-based permeable reactive barrier

Although widely used in permeation reaction barrier（PRB） for strengthening the removal of various heavy metals, zero-valent iron（ZVI） is limited by various inherent drawbacks, such as easy passivation and poor electron transfer. As a solution, a synergistic system with PRB and electrokinetics（PRB-EK） was established and applied for the efficient removal of Cr（Ⅵ）-contaminated groundwater. As the filling material of PRB, ZVI/Fe₃O₄/activated carbon（ZVI/Fe₃O₄     

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...     

Effect of reduction pretreatment on the structure and catalytic performance of Ir-In2O3 catalysts for CO2 hydrogenation to methanol

In₂O₃has been found a promising application in CO₂hydrogenation to methanol,which is beneficial to the utilization of CO₂.The oxygen vacancy (O_v) site is identified as the catalytic active center of this reaction.However,there remains a great challenge to understand the relations between the state of oxygen species in In₂O₃and the catalytic performance for CO₂hydrogenation to methanol.In the present work,we c...     

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...     

Simultaneous removal of NO and dichloromethane（CH2Cl2） over Nb-loaded cerium nanotubes catalyst

Herein, a series of niobium oxide supported cerium nanotubes（Ce NTs） catalysts with different loading amount of Nb₂O₅（0–10 wt.%） were prepared and used for selective catalytic reduction of NOxwith NH₃（NH₃-SCR） in the presence of CH₂Cl₂. Commercial V₂O₅-WO₃-TiO₂ catalyst was also prepared for comparison. The physcial properties and chemical properties of the Nb₂O₅ lo...     

Insights into the interface of NiCo2O4 spinel/LaCoO3 perovskite nano-composite for CO and soot oxidation

In the quest for the development of thermally stable, highly active and low-cost catalysts for use in catalyzed diesel particulate filter, nano-composites are new areas of research. Therefore, we reported the easy synthesis of spinel NiCo₂O₄/perovskite LaCoO₃ nano-composite,and its individual oxides NiCo₂O₄and LaCoO₃ for comparison. The detailed insights into the physio-chemical characteristics of formed NiCo₂O₄     

Spatial distribution of fossil fuel derived CO2 over India using radiocarbon measurements in crop plants

Examining the contribution of fossil fuel CO₂to the total CO₂changes in the atmosphere is of primary concern due to its alarming levels of fossil fuel emissions over the globe,specifi cally developing countries.Atmospheric radiocarbon represents an important observationa constraint and utilized to trace fossil fuel derived CO₂(CO_2ff) in the atmosphere.For the firs time,we have presented a detailed analysis on the spatial distribution of fossil fuel der...     

Boosting oxygen vacancies by modulating the morphology of Au decorated In2O3 with enhanced CO2 hydrogenation activity to CH3OH

CO₂ hydrogenation to methanol has become one of the most promising ways for CO₂ utilization,however,the CO₂ conversion rate and methanol selectivity of this reaction still need to be improved for industrial application.Here we investigated the structure-activity relationship for CO₂ conversion to methanol of In₂O₃-based catalysts by modulating morphology and decorating Au.Three different Au/In₂O₃catalysts wer...     

Modeling of acute cadmium toxicity in solution to barley root elongation using biotic ligand model theory

Protons（H⁺）as well as different major and trace elements may inhibit cadmium（Cd）uptake in aquatic organisms and thus alleviate Cd toxicity.However,little is known about such interactions in soil organisms.In this study,the independent effects of the cations calcium(Ca²⁺),magnesium(Mg²⁺),potassium（K⁺）,H+and zinc(Zn²⁺)on Cd toxicity were investigated with 5-day long barley root elongation tests in nutrient solutions.The tested concentrations of selected cations and trace metal ions were based on the ranges that occur naturally in soil pore water.The toxicity of Cd decreased with increasing activity of Ca²⁺,Mg²⁺,H⁺and Zn²⁺,but not K⁺.Accordingly,conditional binding constants were obtained for the binding of Cd²⁺,Ca²⁺,Mg²⁺,H⁺,and Zn²⁺ with the binding ligand:log K_CdBL5.19,logK_CaBL2.87,logK_MgBL2.98,logK_HBL5.13 and logK_ZnBL5.42,respectively.Furthermore,it was calculated that on average 29% of the biotic ligand sites needed to be occupied by Cd to induce a 50% decrease in root elongation.Using the estimated constants,a biotic ligand model was successfully developed to predict the Cd toxicity to barley root elongation as a function of solution characteristics.The feasibility and accuracy of its application for predicting Cd toxicity in soils were discussed.     

Study on the mechanism and reaction characteristics of metal-supported phosphogypsum as oxygen carrier in a chemical looping gasification application

This study aimed to explore the chemical looping gasification (CLG) reaction characteristics of the metal-supported composite phosphogypsum (PG) oxygen carriers (OCs) and the thermodynamic mechanism.The FactSage 7.1 thermodynamic simulation was used to explore the oxygen release and H₂S removal mechanisms.The experimental results showed that the syngas yield of CLG with PG-CuFe₂O₄was more than that with PG–Fe₂O₃20/CuO40or PG–Fe₂O<...     

UV/PMS降解水中罗丹明B的动力学及反应机理

采用紫外(UV)活化过硫酸氢钾(PMS)产生强氧化性硫酸根自由基(SO_4~·-)降解人工染料罗丹明B(RhB).考察了溶液初始p H、氧化剂剂量、RhB初始浓度、天然有机物(NOM)、Fe~(2+)浓度、自由基淬灭剂(甲醇和叔丁醇)及水体中常见阴离子对降解效果的影响,并探测反应体系中生成的无机阳离子及小分子有机酸的种类和浓度.结果表明,降解反应遵循准一级反应动力学,其降解速率受到溶液初始pH的显著影响,当溶液酸性越强或碱性越强时,RhB的降解效果越好,且酸性条件下降解效果优于碱性条件.同时,加大氧化剂剂量及降低底物浓度也会对RhB的降解起促进作用.体系中投加过渡金属Fe~(2+)可显著促进RhB的降解效果,当Fe~(2+)与PMS的浓度比为1∶1时,降解效果最佳.水体中的NO_3~-对RhB的降解有着显著的促进作用,而H_2PO_4~-、C_2O_4~(2-)、Cl~-和NOM则对RhB的降解有抑制作用.采用离子色谱分析了UV/PMS体系降解RhB所产生的NH_4~+,以及甲酸、乳酸、乙酸和草酸,推测RhB在UV/PMS体系中的降解主要是通过共轭结构的破坏、N-位脱乙基并伴有苯环结构的破坏进行的.综合分析表明,UV/PMS工艺可有效运用于罗丹明B污染水体的修复处理过程.     

Cu-Al2O3中骨架铜类芬顿催化去除水中有机污染物

为解决传统铁基芬顿催化剂在水体通常酸碱(pH6)条件下活性低的问题,采用简单共沉淀法制备了Cu掺杂的Al_2O_3类芬顿催化剂.通过X射线衍射(XRD)、X射线光电子能谱(XPS)和紫外可见(UV-vis)吸收光谱分析表明,Cu-Al_2O_3中铜掺杂的质量分数低于4.77%时,催化剂中铜主要以Cu~(2+)和Cu~+的形式共存于Al_2O_3的骨架结构中,形成Al—O—Cu键;过量的铜掺杂会导致外骨架铜物种如铜氧化物团簇的存在.以难降解有机污染物2-氯苯酚(2-chlorophenol,2-CP)和染料罗丹明B(Rhodamine B,Rh B)为目标污染物,对Cu-Al_2O_3的类芬顿催化性能进行了详细地研究.结果表明,骨架铜物种在中性温和条件下对2-CP和Rh B显示出很高的催化去除效率和稳定性,反应2 h,Cu-Al_2O_3(Cu质量分数4.77%)对2-CP的去除率达到54%,相应的TOC去除率达到49%,而铜离子溶出浓度仅为0.025 5 mg·L-1,而Cu-Al_2O_3(Cu质量分数7.58%)由于外骨架铜的存在导致催化活性增加缓慢和稳定性下降.ESR测试结果表明,·OH和HO_2~-/O_2~-·是反应中主要的活性物种.     

Rapid degradation of dyes in water by magnetic Fe/Fe3O4/graphene composites

Magnetic Fe⁰/Fe₃O₄/graphene has been successfully synthesized by a one-step reduction method and investigated in rapid degradation of dyes in this work. The material was characterized by N₂ sorption–desorption, scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FT-IR), vibrating-sample magnetometer (VSM) measurements and X-ray photoelectron spectroscopy (XPS). The results indicated that Fe⁰/Fe₃O₄/graphene had a layered structure with Fe crystals highly dispersed in the interlayers of graphene, which could enhance the mass transfer process between Fe⁰/Fe₃O₄/graphene and pollutants. Fe⁰/Fe₃O₄/graphene exhibited ferromagnetism and could be easily separated and re-dispersed for reuse in water. Typical dyes, such as Methyl Orange, Methylene Blue and Crystal Violet, could be decolorized by Fe⁰/Fe₃O₄/graphene rapidly. After 20 min, the decolorization efficiencies of methyl orange, methylene blue and crystal violet were 94.78%, 91.60% and 89.07%, respectively. The reaction mechanism of Fe⁰/Fe₃O₄/graphene with dyes mainly included adsorption and enhanced reduction by the composite. Thus, Fe⁰/Fe₃O₄/graphene prepared by the one-step reduction method has excellent performance in removal of dyes in water.     

Fe2O3/TiO2负载膨胀珍珠岩光催化降解罗丹明B

为获得高效催化活性的光催化材料,研究不同煅烧氛围对材料在可见光下催化性能的影响,以膨胀珍珠岩（EP）为载体,采用溶胶-凝胶法,在不同煅烧氛围（O₂和/或NH₃）下制备Fe₂O₃/TiO₂负载EP的光催化复合材料〔Fe₂O₃-TEP（O₂）、Fe₂O₃-TEP（NH₃）、Fe₂O₃-TEP（O₂,NH₃）、Fe₂O₃-TEP（NH₃,O₂）〕,采用EDS（X-射线色散能谱）、BET（比表面积及孔径分析）、XRD（X射线衍射）、SEM（扫描电子显微镜）、XPS（X射线光电子能谱）等对复合材料进行表征,并研究了其在可见光下对罗丹明B的光催化降解效果.结果表明:①复合材料成功负载了Ti、Fe元素,负载的TiO₂以锐钛矿型存在,Fe₂O₃的掺杂增强了TiO₂对可见光的响应能力;②不同的煅烧氛围明显影响复合材料的晶粒尺寸、比表面积和光催化性能,其中,Fe₂O₃-TEP（O₂,NH₃）的光催化性能最好,4 h后罗丹明B降解率达到87.59%,Fe₂O₃-TEP（NH₃,O₂）、Fe₂O₃-TEP（O₂）和Fe₂O₃-TEP（NH₃）4 h后对罗丹明B的降解率则分别为65.02%、62.48%和47.48%;③在试验条件下,复合材料的光催化反应符合一阶反应动力学方程,Fe₂O₃-TEP（O₂,NH₃）、Fe₂O₃-TEP（NH₃,O₂）、Fe₂O₃-TEP（O₂）和Fe₂O₃-TEP（NH₃）相应的降解速率常数分别为0.008 3、0.004 3、0.004 3和0.002 7 min-1.研究显示,通过溶胶-凝胶法所制备的复合材料（Fe₂O₃-TEP）经煅烧后所得矿相均一;Fe₂O₃掺杂TiO₂可形成Ti—O—Fe键,减小TiO₂固有的禁带宽度;复合材料光催化性能也受到煅烧氛围的影响,先O₂后NH₃煅烧条件下所得材料的光催化性能最佳.      

碳化泡沫负载Co3O4活化过硫酸盐降解罗丹明B

Co₃O₄具有优良的活化过硫酸盐的性能而受到人们的重视,但Co₃O₄粉体易团聚、使用过程中难以分离、易流失和重复利用率差等问题严重制约了其实际应用．通过水热法制备碳化三聚氰胺泡沫负载Co₃O₄非均相催化剂．采用X-射线衍射仪（XRD）和扫描电子显微镜（SEM）对催化剂的结构和表面形貌进行分析．研究不同因素对催化剂活化过硫酸氢钾（PMS）降解罗丹明B（RhB）的性能．其最优催化工艺参数：催化剂投加量为35 mg·L^-1、PMS质量浓度为50 mg·L^-1和pH为7、RhB初始质量浓度为10 mg·L^-1,30 min反应后对RhB降解率为98%．结果表明,增大碳化泡沫负载Co₃O₄非均相催化剂投加量和PMS质量浓度能明显提高对RhB的降解率;而增加RhB初始质量浓度和提高pH值会明显抑制RhB的降解率．催化反应过程符合准一级动力学方程．温度对RhB降...     

Photodegradation of amoxicillin by catalyzed Fe3+/H2O2 process

Three oxidation processes of UV-Fe³⁺(EDTA)/H₂O₂ (UV: ultraviolet light; EDTA: ethylenediaminetetraacetic acid), UV-Fe³⁺/H₂O₂ and Fe³⁺/H₂O₂ were simultaneously investigated for the degradation of amoxicillin at pH 7.0. The results indicated that, 100% amoxicillin degradation and 81.9% chemical oxygen demand (COD_Cr) removal could be achieved in the UV-Fe³⁺ (EDTA)/H₂O₂ process. The treatment efficiency of amoxicillin and COD_Cr removal were found to decrease to 59.0% and 43.0% in the UV-Fe³⁺/H₂O₂ process; 39.6% and 31.3% in the Fe³⁺/H₂O₂ process. Moreover, the results of biodegradability (biological oxygen demand (BOD₅)/COD_Cr ratio) revealed that the UV-Fe³⁺ (EDTA)/H₂O₂ process was a promising strategy to degrade amoxicillin as the biodegradability of the effluent was improved to 0.45, compared with the cases of UV-Fe³⁺/H₂O₂ (0.25) and Fe³⁺/H₂O₂ (0.10) processes. Therefore, it could be deduced that EDTA and UV light performed synergetic catalytic effect on the Fe³⁺/H₂O₂ process, enhancing the treatment efficiency. The degradation mechanisms were also investigated via UV-Vis spectra, and high performance liquid chromatography-mass spectra. The degradation pathway of amoxicillin was further proposed.     

Decontamination of alachlor herbicide wastewater by a continuous dosing mode ultrasound/Fe2+/H2O2 process

We used a ultrasound/Fe2+/H2O2 process in continuous dosing mode to degrade the alachlor.Experimental results indicated that lower pH levels enhanced the degradation and mineralization of alachlor. The maximum alachlor degradation(initial alachlor concentration of 50 mg/L) was as high as 100% at pH 3 with ultrasound of 100 Watts, 20 mg/L of Fe2+, 2 mg/min of H2O2 and 20℃ within60 min reaction combined with 46.8% total organic carbon removal. Higher reaction temperatures inhibited the degradation of alachlor. Adequate dosages of Fe2+and H2O2 in ultrasound/Fe2+/H2O2process not only enhance the degradation efficiency of alachlor but also save the operational cost than the sole ultrasound or Fenton process. A continuous dosing mode ultrasound/Fe2+/H2O2 process was proven as an effective method to degrade the alachlor.     

BiOCl/SiO2/Fe3O4复合材料可见光催化去除水中亚甲基蓝

以FeCl_3·6H_2O、FeCl_2·4H_2O、(C_2H_5)_4SiO_4、Bi(NO_3)_3·5H_2O、KCl为主要原料,采用化学共沉淀法和水热法制备了BiOCl/SiO_2/Fe_3O_4光催化剂,并对其进行EDS、TEM、XRD、FT-IR、UV-Vis表征,最后通过亚甲基蓝降解实验,研究了催化剂在合成过程中pH及催化剂投加量对其光催化性能的影响.结果表明,在pH=6、催化剂初始投加量为0.5 g·L~(-1)时,对亚甲基蓝的可见光催化效果最佳,光照120 min后对10 mg·L~(-1)的亚甲基蓝溶液的脱色率达到93.2%.BiOCl/SiO_2/Fe_3O_4经过简单的无水乙醇和水洗后,可高效重复利用4次.综合表明,BiOCl/SiO_2/Fe_3O_4是一种在处理染料废水中具有应用前景的磁性光催化剂.     

UV强化草酸络合Fe3+活化过硫酸盐氧化降解苯胺

采用UV-草酸络合Fe~(3+)[UV-Fe(C_2O_4)3-3]活化过硫酸钠(PS)氧化降解苯胺,研究了Fe(C_2O_4)3-3浓度,PS浓度,pH对PS活化效率及苯胺氧化降解效果的影响机制.结果表明,Fe(C_2O_4)3-3浓度和pH决定了UV-Fe(C_2O_4)3-3体系中Fe~(3+)向Fe2+的转化过程,并对活化PS氧化降解苯胺产生显著影响.随着Fe(C_2O_4)3-3浓度增加,PS的分解率不断提高,但当浓度高于0.75 mmol·L~(-1)时,草酸根离子(C2O_2-4)对硫酸根自由基(SO·-4)的竞争以及SO·-4之间的相互淬灭作用降低了苯胺的降解效果,降解速率大小顺序为5 mmol·L~(-1)0.25 mmol·L~(-1)0.5 mmol·L~(-1)1 mmol·L~(-1)0.75 mmol·L~(-1);中性和碱性条件不利于Fe(C_2O_4)3-3发生光化学反应生成Fe2+,但当初始pH为7和9时,由于PS活化分解过程降低反应体系pH,反应300min时PS的活化率可分别达到74%和67%,苯胺去除率分别高达91%和97%,均高于初始pH为酸性条件下的结果;苯胺降解率随初始PS浓度增加而增大,当PS浓度大于10 mmol·L~(-1)时,苯胺降解过程由二级反应变为准一级反应,但此时过量的PS因与SO·-4发生反应而显著降低PS用于氧化降解苯胺的利用率.     

Catalytic performance of Fe3O4-CoO/Al2O3 catalyst in ozonation of 2-(2,4-dichlorophenoxy)propionic acid, nitrobenzene and oxalic acid in water

Fe3O4-CoO/Al2O3 catalyst was prepared by incipient wetness impregnation using Fe(NO3) 3·9H2O and Co(NO3) 2·6H2O as the precursors,and its catalytic performance was investigated in ozonation of 2-(2,4-dichlorophenoxy) propionic acid(2,4-DP) ,nitrobenzene and oxalic acid.The experimental results indicated that Fe3O4-CoO/Al2O3 catalyst enabled an interesting improvement of ozonation eciency during the degradation of each organic pollutant,and the Fe3O4-CoO/Al2O3 catalytic ozonation system followed a radical-type mechanism.The kinetics of ozonation alone and Fe3O4-CoO/Al2O3 catalytic ozonation of three organic pollutants in aqueous solution were discussed under the mere consideration of direct ozone reaction and OH radical reaction to well investigate its performance.In the catalytic ozonation of 2,4-DP,the apparent reaction rate constants(k) were determined to be 1.456×10-2 min-1 for ozonation alone and 4.740×10-2 min-1 for O3/Fe3O4-CoO/Al2O3.And O3/Fe3O4-CoO/Al2O3 had a larger Rct(6.614×10-9) calculated by the relative method than O3 did(1.800×10-9) ,showing O3/Fe3O4-CoO/Al2O3 generated more hydroxyl radical.Similar results were also obtained in the catalytic ozonation of nitrobenzene and oxalic acid.The above results demonstrated that the catalytic performance of Fe3O4-CoO/Al2O3 in ozonation of studied organic substance was universal to a certain degree.