Herein,we prepa red novel three-dimensional(3D)gear-s haped Co3O4@C(Co3O4 modified by amorphous carbon)and sheet-like SnO2/CC(SnO2 grow on the carbon cloth)as anode and cathode to achieve efficient removal of 4-nitrop...Herein,we prepa red novel three-dimensional(3D)gear-s haped Co3O4@C(Co3O4 modified by amorphous carbon)and sheet-like SnO2/CC(SnO2 grow on the carbon cloth)as anode and cathode to achieve efficient removal of 4-nitrophenol(4-NP)in the presence of peroxymonosulfate(PMS)and simultaneous electrocatalytic reduction of CO2,respectively.In this process,4-NP was mineralized into CO2 by the Co3O4@C,and the generated CO2 was reduced into HCOOH by the sheet-like SnO2/CC cathode.Compared with the pure Co0.5(Co3O4 was prepared using 0.5 g urea)with PMS(30 mg,0.5 g/L),the degradation efficiency of 4-NP(60 mL,10 mg/L)increased from 74.5%-85.1%in 60 min using the Co0.5 modified by amorphous carbon(Co0.5@C).Furthermore,when the voltage of 1.0 V was added in the anodic system of Co0.5@C with PMS(30 mg,0.5 g/L),the degradation efficiency of 4-NP increased from 85.1%-99.1%when Pt was used as cathode.In the experiments of 4-NP degradation coupled with simultaneous electrocatalytic CO2 reduction,the degradation efficiency of 4-NP was 99.0%in the anodic system of Co0.5@C with addition of PMS(30 mg,0.5 g/L),while the Faraday efficiency(FE)of HCOOH was 24.1%at voltage of-1.3 V using the SnO2/CC as cathode.The results showed that the anode of Co3O4 modified by amorphous carbon can markedly improve the degradation efficiency of 4-NP,while the cathode of SnO2/CC can greatly improve the FE and selectivity of CO2 reduction to HCOOH and the stability of cathode.Finally,the promotion mechanism was proposed to explain the degradation of organic pollutants and reduction of CO2 into HCOOH in the process of electrocatalysis coupled with advanced oxidation processes(AOPs)and simultaneous CO2 reduction.展开更多
As important emerging contaminants, antibiotics have caused potential hazards to the ecological environment and human health due to their extensive production and consumption. Among various techniques for removing ant...As important emerging contaminants, antibiotics have caused potential hazards to the ecological environment and human health due to their extensive production and consumption. Among various techniques for removing antibiotics from wastewater, H_(2)O_(2)-based advanced oxidation processes(AOPs) have received increasing attention due to their fast reaction rate and strong oxidation capability. Hence this review critically discusses:(i) Recent research progress of AOPs with the addition of H_(2)O_(2) for antibiotics removal through different methods of H_(2)O_(2) activation;(ii) recent advances in AOPs that can in-situ generate and activate H_(2)O_(2) for antibiotics removal;(iii) H_(2)O_(2)-based AOPs as a combination with other techniques for the degradation and mineralization of antibiotics in wastewater. Future perspectives about H_(2)O_(2)-based AOPs are also presented to grasp the future research trend in the area.展开更多
Direct propylene epoxidation with H2 and O2,an attractive process to produce propylene oxide(PO),has a potential explosion danger due to the coexistence of flammable gases(i.e.,C3 H6 and H2)and oxidizer(i.e.,O2).The u...Direct propylene epoxidation with H2 and O2,an attractive process to produce propylene oxide(PO),has a potential explosion danger due to the coexistence of flammable gases(i.e.,C3 H6 and H2)and oxidizer(i.e.,O2).The unknown explosion limits of the multi-component feed gas mixture make it difficult to optimize the reaction process under safe operation conditions.In this work,a distribution method is proposed and verified to be effective by comparing estimated and experimental explosion limits of more than 200 kinds of flammable gas mixture.Then,it is employed to estimate the explosion limits of the feed gas mixture,some results of which are also validated by the classic Le Chatelier’s Rule and flammable resistance method.Based on the estimated explosion limits,process optimization is carried out using commercially high and inherently safe reactant concentrations to enhance reaction performance.The promising results are directly obtained through the interface called gOPT in gPROMS only by using a simple,easy-constructed and mature packed-bed reactor,such as the PO yield of 13.3%,PO selectivity of 85.1%and outlet PO fraction of 1.8%.These results can be rationalized by indepth analyses and discussion about the effects of the decision variables on the operation safety and reaction performance.The insights revealed here could shed new light on the process development of the PO production based on the estimation of the explosion limits of the multi-component feed gas mixture containing flammable gase s,inert gas and O2,followed by process optimization.展开更多
Nitric oxide(NO) from flue gas is hard to remove because of low solubility and reactivity. A new technology for photocatalytic oxidation of NO using ultraviolet(UV)/TiO2/H2O2 process is studied in an efficient laborat...Nitric oxide(NO) from flue gas is hard to remove because of low solubility and reactivity. A new technology for photocatalytic oxidation of NO using ultraviolet(UV)/TiO2/H2O2 process is studied in an efficient laboratory-scale reactor. Effects of several key operational parameters on NO removal efficiency are studied, including TiO2 content, H2O2 initial concentration, UV lamp power, NO initial content, oxygen volume fraction and TiO2/H2O2 solution volume. The results illustrate that the NO removal efficiency increases with the increasing of H2O2 initial concentration or UV lamp power. Meanwhile, a lower NO initial content or a higher TiO2/H2O2 solution volume will result in higher NO removal efficiency. In addition, oxygen volume fraction has a little effect.The highest NO removal efficiency is achieved at the TiO2 content of 0.75 g/L, H2O2 initial concentration of 2.5 mol/L, UV lamp power of 36 W, NO initial content of 206×10-6 and TiO2/H2O2 solution volume of 600 m L. It is beneficial for the development and application of NO removal from coal-fired flue gas with UV/TiO2/H2O2 process.展开更多
The comparison of degradation of Acid Yellow 61 as a model dye compound in both oxidation processes of H 2O 2/UV and O 3 has been studied. When the decolorization rate of Acid Yellow 61 in both reactions presented ...The comparison of degradation of Acid Yellow 61 as a model dye compound in both oxidation processes of H 2O 2/UV and O 3 has been studied. When the decolorization rate of Acid Yellow 61 in both reactions presented similar, it was found there are some differences from the results of AOX removal and production of inorganic ions and organic acids. The results reveal that the H 2O 2/UV has beneficial effect on mineralization than O 3 only for degradation of Acid Yellow 61 solution and it is possible for enhancement of method efficiency by taking longer reaction time and addition of high concentration of oxidants.展开更多
By means of scanning electron microscope(SEM)and high voltage electron microscope(HVEM)we have observed and analysed morphology and micro-structure of silicon oxide film with different thickness formed on(111)silicon ...By means of scanning electron microscope(SEM)and high voltage electron microscope(HVEM)we have observed and analysed morphology and micro-structure of silicon oxide film with different thickness formed on(111)silicon monocrystal under dry oxygen atmosphere at 1100℃.Compared with their oxidation kinetic curves consisted of three stages,we suggested a mechanism on forming silicon oxide film.According to electron and X-ray diffraction analyses the silicon oxide films consisted of silica with different crystal structure.We also have discussed a stacking fault and a dislocation formed in the Si-Sio_2 interface region simulaneously forming silicon oxide film.展开更多
Nanometer SnO2 particles were synthesized by sol-gel dialytic processes and used as a support to prepare CuO supported catalysts via a deposition-precipitation method. The samples were characterized by means of TG-DTA...Nanometer SnO2 particles were synthesized by sol-gel dialytic processes and used as a support to prepare CuO supported catalysts via a deposition-precipitation method. The samples were characterized by means of TG-DTA, XRD, H2-TPR and XPS. The catalytic activity of the CuO/TiO2-SnO2 catalysts was markedly depended on the loading of CuO, and the optimum CuO loading was 8 wt.% （Tloo = 80 ℃）. The CuO/TiO2-SnO2 catalysts exhibited much higher catalytic activity than the CuO/TiO2 and CuO/SnO2 catalysts. H2-TPR result indicated that a large amount of CuO formed the active site for CO oxidation in 8 wt.% CuO/TiO2-SnO2 catalyst.展开更多
The UV/Ag-TiO2/O3 process was investigated for ballast water treatment using Dunaliella salina as an indicator. Inactivation curves were obtained, and the toxicity of effluent was determined. Compared with individual ...The UV/Ag-TiO2/O3 process was investigated for ballast water treatment using Dunaliella salina as an indicator. Inactivation curves were obtained, and the toxicity of effluent was determined. Compared with individual unit processes using ozone or UV/Ag-TiO2, the inactivation efficiency ofD. salina by the combined UV/Ag-TiO2/O3 process was enhanced. The presence of ozone caused an immediate decrease in chlorophyll a （chl-a） concentration. Inactivation efficiency and chl-a removal efficiency were positively correlated with ozone dose and ultraviolet intensity. The initial total residual oxidant （TRO） concentration of effluent increased with increasing ozone dose, and persistence of TRO resulted in an extended period of toxicity. The results suggest that UV/Ag-TiO2/O3 has potential for ballast water treatment.展开更多
This work proposed a strategy of indirectly inducing uniform microarc discharge by controlling the content and distribution ofβ-Mg_(17)Al_(12)phase in AZ91D Mg alloy.Two kinds of nano-particles(ZrO_(2)and TiO_(2))wer...This work proposed a strategy of indirectly inducing uniform microarc discharge by controlling the content and distribution ofβ-Mg_(17)Al_(12)phase in AZ91D Mg alloy.Two kinds of nano-particles(ZrO_(2)and TiO_(2))were designed to be added into the substrate of Mg alloy by friction stir processing(FSP).Then,Mg alloy sample designed with different precipitated morphology ofβ-Mg_(17)Al_(12)phase was treated by microarc oxidation(MAO)in Na_(3)PO_(4)/Na2SiO3electrolyte.The characteristics and performance of the MAO coating was analyzed using scanning electron microscopy(SEM),energy dispersive spectrometer(EDS),X-ray diffraction(XRD),X-ray photoelectron spectroscopy(XPS),contact angle meter,and potentiodynamic polarization.It was found that the coarseα-Mg grains in extruded AZ91D Mg alloy were refined by FSP,and theβ-Mg_(17)Al_(12)phase with reticular structure was broken and dispersed.The nano-ZrO_(2)particles were pinned at the grain boundary by FSP,which refined theα-Mg grain and promoted the precipitation ofβ-Mg_(17)Al_(12)phase in grains.It effectively inhibited the“cascade”phenomenon of microarcs,which induced the uniform distribution of discharge pores.The MAO coating on Zr-FSP sample had good wettability and corrosion resistance.However,TiO_(2)particles were hardly detected in the coating on TiFSP sample.展开更多
(γ’+β)two-phase Ni-Al is a promising high-temperature protective coating material used on Ni-base superalloys since it has good interfacial compatibility with superalloys due to the low Al content compared to singl...(γ’+β)two-phase Ni-Al is a promising high-temperature protective coating material used on Ni-base superalloys since it has good interfacial compatibility with superalloys due to the low Al content compared to single-phaseβ-NiA l.In this paper,we aim to improve the oxidation resistance,whereby Ni-34Al-0.1Dy,a(γ’+β)two-phase Ni-Al alloy,was treated by laser shock processing(LSP)and the oxidation behavior at 1150℃ was investigated.The results showed that after oxidation,Al_(2)O_(3)scale formed on the originalβphase of the untreated alloy with a small grain size(200-800 nm),while for the LSP-treated samples,the scale grown on the originalβphase was dominantly composed of larger Al_(2)O_(3)grains with a size of 2-3μm.The distinction was attributed to the promotion ofθ-Al_(2)O_(3)toα-Al_(2)O_(3)transformation induced by the LSP,because the dislocation density,as well as surface roughness,were increased during LSP treatment which can provide heterogeneous nucleation sites forα-Al_(2)O_(3).In addition,the larger-size Al_(2)O_(3)particles,derived from the direct conversion of needle-likeθ-Al_(2)O_(3)in the initial oxidation stage,could rapidly overspread the wholeβphase surface thus reducing the scale growth rate.展开更多
TiO_(2)has demonstrated outstanding performance in electrochemical advanced oxidation processes(EAOPs)due to its structural stability and high oxygen overpotential.However,there is still much room for improving its el...TiO_(2)has demonstrated outstanding performance in electrochemical advanced oxidation processes(EAOPs)due to its structural stability and high oxygen overpotential.However,there is still much room for improving its electrochemical activity.Herein,narrow bandgap manganese oxide(MnO_(x))was composited with TiO_(2)nanotube arrays(TiO_(2)NTAs)that in-situ oxidized on porous Ti sponge,forming the MnO_(x)-TiO_(2)NTAs anode.XANES and XPS analysis further proved that the composition of MnO_(x)is Mn2O3.Electrochemical characterizations revealed that increasing the composited concentration of MnO_(x)can improve the conductivity and reduce oxygen evolution potential so as to improve the electrochemical activity of the composited MnO_(x)-TiO_(2)NTAs anode.Meanwhile,the optimal degradation rate of benzoic acid(BA)was achieved using MnO_(x)-TiO_(2)NTAs with a MnO_(x)concentration of 0.1 mmol L^(-1),and the role of MnO_(x)was proposed based on DFT calculation.Additionally,the required electrical energy(EE/O)to destroy BA was optimized by varying the composited concentration of MnO_(x)and the degradation voltage.These quantitative results are of great significance for the design and application of high-performance materials for EAOPs.展开更多
We describes a controllable synthesis procedure for growing a-Ee2O3 and Ee3O4 nanowires. High magnetic hematite a-Fe2O3 nanowires are successfully grown on Fe0.5Ni0.5 alloy substrates via an oxide assisted vapor-solid...We describes a controllable synthesis procedure for growing a-Ee2O3 and Ee3O4 nanowires. High magnetic hematite a-Fe2O3 nanowires are successfully grown on Fe0.5Ni0.5 alloy substrates via an oxide assisted vapor-solid process. Experimental results also indicate that previous immersion of the substrates in a solution of oxalic acid causes the grown nanowires to convert gradually into magnetite （Fe3O4） nanowires. Additionally, the saturated state of Fe3O4 nanowires is achieved as the oxalic acid concentration reaches 0.75 mol/L. The average diameter and length of nanowires expands with an increasing operation temperature and the growth density of nanowires accumulates with an increasing gas flux in the vapor-solid process. The growth mechanism of a-Fe2O3 and Fe3O4 nanowires is also discussed. The results demonstrate that the entire synthesis of nanowires can be completed within 2 h.展开更多
Because of the highly toxic cyanide in the gold cyanide residues,cyanide must be removed for environmental protection.The process mineralogy of residues was studied firstly,and then cyanide removal was carried out by ...Because of the highly toxic cyanide in the gold cyanide residues,cyanide must be removed for environmental protection.The process mineralogy of residues was studied firstly,and then cyanide removal was carried out by three chemical methods.The results showed that the residue mainly contained Si,S and Fe.Pyrite was the main metallic mineral,and the iron-complex cyanides make cyanide removal difficult.The minerals in residues were in ultrafine particle size with high monomer dissociation degrees.In H_(2)O_(2)oxidation process,the self-decomposition and side reactions resulted in high consumption of H_(2)O_(2).In Na_(2)S_(2)O_(5)-air oxidation process,the time for complete process was long because of the reactions between Na_(2)S_(2)O_(5)and O_(2).Na_(2)SO_(3)oxidation method was found to be a new method for cyanide removal without air inflation device.The cyanide content was reduced to the national standard level in 90 min at pH 9.0 with optimum Na_(2)SO_(3)dose of 2.0 g/L.展开更多
Up to 9% of the global CO_(2) emissions come from the iron and steel industry. Here, a combined chemical looping process to produce CO, a building block for the chemical industry, from the CO_(2) -rich blast furnace g...Up to 9% of the global CO_(2) emissions come from the iron and steel industry. Here, a combined chemical looping process to produce CO, a building block for the chemical industry, from the CO_(2) -rich blast furnace gas of a steel mill is proposed. This cyclic process can make use of abundant Fe_(3)O_(4) and CaO as solid oxygen and CO_(2) carriers at atmospheric pressure. A proof of concept was obtained in a laboratory-scale fixed bed reactor with synthetic blast furnace gas and Fe_(3)O_(4) /CaO = 0.6 kg/kg. CO production from the proposed process was investigated at both isothermal conditions(1023 K) and upon imposing a temperature program from 1023 to 1148 K. The experimental results were compared using performance indicators such as CO yield, CO space time yield, carbon recovery of the process, fuel utilisation, and solids’ utilisation.The temperature-programmed CO production resulted in a CO yield of 0.056 ± 0.002 mol per mol of synthetic blast furnace gas at an average CO space time yield of 7.6 mmol kgFe^(-1) s^(-1) over 10 cycles, carbon recovery of 48% ± 1%, fuel utilisation of 23% ± 2%, and an average calcium oxide and iron oxide utilisation of 22% ± 1% and 11% ± 1%. These experimental performance indicators for the temperature-programmed CO production were consistently better than those of the isothermal implementation mode by 20% to 35%. Over 10 consecutive process cycles, no significant losses in CO yield were observed in either implementation mode. Process simulation was carried out for 1 million metric tonnes per year of equivalent CO_(2) emissions from the blast furnace gas of a steel mill to analyse the exergy losses in both modes of operation. Comparison of the exergy efficiency of the temperature-programmed process to the isothermal process showed that the former is more efficient because of the higher CO concentration achievable,despite 20% higher exergy losses caused by heat transfer required to change temperature.展开更多
Undoped nickel-based catalysts supported on depleted uranium oxide allow one to carry out CO_(2)methanation process under extremely low reaction temperature under atmospheric pressure and powered by a contactless indu...Undoped nickel-based catalysts supported on depleted uranium oxide allow one to carry out CO_(2)methanation process under extremely low reaction temperature under atmospheric pressure and powered by a contactless induction heating.By adjusting the reaction conditions,the catalyst is able to perform CO_(2)methanation reaction under autothermal process operated inside a non-adiabatic reactor,without any external energy supply.Such autothermal process is possible thanks to the high apparent density of the UO_x which allows one to confine the reaction heat in a small catalyst volume in order to confine the exothermicity of the reaction inside the catalyst and to operate the reaction at equilibrium heat in-heat out.Such autothermal operation mode allows one to significantly reduce the complexity of the process compared to that operated using adiabatic reactor,where complete insulation is required to prevent heat disequilibrium,in order to reduce as much as possible,the heat exchange with the external medium.The catalyst displays an extremely high stability as a function of time on stream as no apparent deactivation.It is expected that such new catalyst with unprecedented catalytic performance could open new era in the field of heterogeneous catalysis where traditional supports show their limitations to operate catalytic processes under severe reaction conditions.展开更多
The electrochemical carbon dioxide reduction reaction(CO_(2)RR),which can produce value-added chemical feedstocks,is a proton-coupled-electron process with sluggish kinetics.Thus,highly efficient,cheap catalysts are u...The electrochemical carbon dioxide reduction reaction(CO_(2)RR),which can produce value-added chemical feedstocks,is a proton-coupled-electron process with sluggish kinetics.Thus,highly efficient,cheap catalysts are urgently required.Transition metal oxides such as CoO_(x),FeO_(x),and NiO_(x)are low-cost,low toxicity,and abundant materials for a wide range of electrochemical reactions,but are almost inert for CO_(2)RR.Here,we report for the first time that nitrogen doped carbon nanotubes(N-CNT)have a surprising activation effect on the activity and selectivity of transition metal-oxide(MO_(x)where M=Fe,Ni,and Co)nanoclusters for CO_(2)RR.MO_(x)supported on N-CNT,MO_(x)/N-CNT,achieves a CO yield of 2.6–2.8 mmol cm−2 min−1 at an overpotential of−0.55 V,which is two orders of magnitude higher than MO_(x)supported on acid treated CNTs(MO_(x)/O-CNT)and four times higher than pristine N-CNT.The faraday efficiency for electrochemical CO_(2)-to-CO conversion is as high as 90.3%at overpotential of 0.44 V.Both in-situ XAS measurements and DFT calculations disclose that MO_(x)nanoclusters can be hydrated in CO_(2)saturated KHCO_(3),and the N defects of N-CNT effectively stabilize these metal hydroxyl species under carbon dioxide reduction reaction conditions,which can split the water molecules and provide local protons to inhibit the poisoning of active sites under carbon dioxide reduction reaction conditions.展开更多
A comparative study of catalytic CO oxidation and selective CO oxidation over Pt/Al2O3 and CeO2-promoted Pt/Al2O3 catalysts has been investigated for the removal of a trace amount of CO from the reformed gas. The cata...A comparative study of catalytic CO oxidation and selective CO oxidation over Pt/Al2O3 and CeO2-promoted Pt/Al2O3 catalysts has been investigated for the removal of a trace amount of CO from the reformed gas. The catalysts were prepared by sol gel and incipient wetness impregnation. CO oxidation and selective CO oxidation were carried out with a 5%Pt/Al2O3 and a 5%Pt/15%CeO2/Al2O3. The presence of 15%CeO2 inthe 5%Pt/Al2O3 dramatically improves the activities to CO oxidation and selective CO oxidation at low temperature (0℃). FTIR results indicate that CO could react with lattice oxygen from ceria and release CO2 as a product. Low space velocity would obtain high CO conversion at low temperatures while high space velocity would obtain high CO conversion at high temperatures. The results also show that a 5%Pt/15%CeO2/Al2O3 can completely oxidize 1% CO at180℃with selectivity of 52% and space velocity of70,000 cm3·g-1·h-1. Under the realistic gas feed with 1%O2, this catalyst is very stable and retains its activity and selectivity at180℃during 72 h.展开更多
基金the National Natural Science Foundation of China(Nos.51878325,51868050,51622806,51378246 and 51720105001)the Natural Science Foundation of Jiangxi Province(Nos.20162BCB22017,20165BCB18008,20171ACB20017,20133ACB21001 and 20171BAB206049)the Graduate Innovation Fund of Jiangxi Province(No.YC2018-S360)。
文摘Herein,we prepa red novel three-dimensional(3D)gear-s haped Co3O4@C(Co3O4 modified by amorphous carbon)and sheet-like SnO2/CC(SnO2 grow on the carbon cloth)as anode and cathode to achieve efficient removal of 4-nitrophenol(4-NP)in the presence of peroxymonosulfate(PMS)and simultaneous electrocatalytic reduction of CO2,respectively.In this process,4-NP was mineralized into CO2 by the Co3O4@C,and the generated CO2 was reduced into HCOOH by the sheet-like SnO2/CC cathode.Compared with the pure Co0.5(Co3O4 was prepared using 0.5 g urea)with PMS(30 mg,0.5 g/L),the degradation efficiency of 4-NP(60 mL,10 mg/L)increased from 74.5%-85.1%in 60 min using the Co0.5 modified by amorphous carbon(Co0.5@C).Furthermore,when the voltage of 1.0 V was added in the anodic system of Co0.5@C with PMS(30 mg,0.5 g/L),the degradation efficiency of 4-NP increased from 85.1%-99.1%when Pt was used as cathode.In the experiments of 4-NP degradation coupled with simultaneous electrocatalytic CO2 reduction,the degradation efficiency of 4-NP was 99.0%in the anodic system of Co0.5@C with addition of PMS(30 mg,0.5 g/L),while the Faraday efficiency(FE)of HCOOH was 24.1%at voltage of-1.3 V using the SnO2/CC as cathode.The results showed that the anode of Co3O4 modified by amorphous carbon can markedly improve the degradation efficiency of 4-NP,while the cathode of SnO2/CC can greatly improve the FE and selectivity of CO2 reduction to HCOOH and the stability of cathode.Finally,the promotion mechanism was proposed to explain the degradation of organic pollutants and reduction of CO2 into HCOOH in the process of electrocatalysis coupled with advanced oxidation processes(AOPs)and simultaneous CO2 reduction.
基金financially supported by National Natural Science Foundation of China(Nos.21976096,52170085 and 21773129)Tianjin Development Program for Innovation and Entrepreneurship+2 种基金Key Project of Natural Science Foundation of Tianjin(No.21JCZDJC00320)Tianjin Post-graduate Students Research and Innovation Project(No.2021YJSB013)Fundamental Research Funds for the Central Universities,Nankai University。
文摘As important emerging contaminants, antibiotics have caused potential hazards to the ecological environment and human health due to their extensive production and consumption. Among various techniques for removing antibiotics from wastewater, H_(2)O_(2)-based advanced oxidation processes(AOPs) have received increasing attention due to their fast reaction rate and strong oxidation capability. Hence this review critically discusses:(i) Recent research progress of AOPs with the addition of H_(2)O_(2) for antibiotics removal through different methods of H_(2)O_(2) activation;(ii) recent advances in AOPs that can in-situ generate and activate H_(2)O_(2) for antibiotics removal;(iii) H_(2)O_(2)-based AOPs as a combination with other techniques for the degradation and mineralization of antibiotics in wastewater. Future perspectives about H_(2)O_(2)-based AOPs are also presented to grasp the future research trend in the area.
基金Supported by the National Natural Science Foundation of China(91434117,21776077)the Shanghai Rising-Star Program(17QA1401200)+1 种基金the Program for Professor of Special Appointment(Eastern Scholar)at Shanghai Institutions of Higher Learningthe Open Project of State Key Laboratory of Chemical Engineering(SKL-Che-15C03).
文摘Direct propylene epoxidation with H2 and O2,an attractive process to produce propylene oxide(PO),has a potential explosion danger due to the coexistence of flammable gases(i.e.,C3 H6 and H2)and oxidizer(i.e.,O2).The unknown explosion limits of the multi-component feed gas mixture make it difficult to optimize the reaction process under safe operation conditions.In this work,a distribution method is proposed and verified to be effective by comparing estimated and experimental explosion limits of more than 200 kinds of flammable gas mixture.Then,it is employed to estimate the explosion limits of the feed gas mixture,some results of which are also validated by the classic Le Chatelier’s Rule and flammable resistance method.Based on the estimated explosion limits,process optimization is carried out using commercially high and inherently safe reactant concentrations to enhance reaction performance.The promising results are directly obtained through the interface called gOPT in gPROMS only by using a simple,easy-constructed and mature packed-bed reactor,such as the PO yield of 13.3%,PO selectivity of 85.1%and outlet PO fraction of 1.8%.These results can be rationalized by indepth analyses and discussion about the effects of the decision variables on the operation safety and reaction performance.The insights revealed here could shed new light on the process development of the PO production based on the estimation of the explosion limits of the multi-component feed gas mixture containing flammable gase s,inert gas and O2,followed by process optimization.
基金Project(2011CB201505)supported by the National Key Basic Research Program of ChinaProject(BA2011031)supported by the Special Fund of Transformation of Scientific and Technological Achievements of Jiangsu Province,China
文摘Nitric oxide(NO) from flue gas is hard to remove because of low solubility and reactivity. A new technology for photocatalytic oxidation of NO using ultraviolet(UV)/TiO2/H2O2 process is studied in an efficient laboratory-scale reactor. Effects of several key operational parameters on NO removal efficiency are studied, including TiO2 content, H2O2 initial concentration, UV lamp power, NO initial content, oxygen volume fraction and TiO2/H2O2 solution volume. The results illustrate that the NO removal efficiency increases with the increasing of H2O2 initial concentration or UV lamp power. Meanwhile, a lower NO initial content or a higher TiO2/H2O2 solution volume will result in higher NO removal efficiency. In addition, oxygen volume fraction has a little effect.The highest NO removal efficiency is achieved at the TiO2 content of 0.75 g/L, H2O2 initial concentration of 2.5 mol/L, UV lamp power of 36 W, NO initial content of 206×10-6 and TiO2/H2O2 solution volume of 600 m L. It is beneficial for the development and application of NO removal from coal-fired flue gas with UV/TiO2/H2O2 process.
文摘The comparison of degradation of Acid Yellow 61 as a model dye compound in both oxidation processes of H 2O 2/UV and O 3 has been studied. When the decolorization rate of Acid Yellow 61 in both reactions presented similar, it was found there are some differences from the results of AOX removal and production of inorganic ions and organic acids. The results reveal that the H 2O 2/UV has beneficial effect on mineralization than O 3 only for degradation of Acid Yellow 61 solution and it is possible for enhancement of method efficiency by taking longer reaction time and addition of high concentration of oxidants.
文摘By means of scanning electron microscope(SEM)and high voltage electron microscope(HVEM)we have observed and analysed morphology and micro-structure of silicon oxide film with different thickness formed on(111)silicon monocrystal under dry oxygen atmosphere at 1100℃.Compared with their oxidation kinetic curves consisted of three stages,we suggested a mechanism on forming silicon oxide film.According to electron and X-ray diffraction analyses the silicon oxide films consisted of silica with different crystal structure.We also have discussed a stacking fault and a dislocation formed in the Si-Sio_2 interface region simulaneously forming silicon oxide film.
基金supported by the National Natural Science Foundation of China (20771061 and 20871071)the 973 Program (2005CB623607)Science and Technology Commission Foundation of Tianjin (08JCYBJC00100 and 09JCYBJC03600)
文摘Nanometer SnO2 particles were synthesized by sol-gel dialytic processes and used as a support to prepare CuO supported catalysts via a deposition-precipitation method. The samples were characterized by means of TG-DTA, XRD, H2-TPR and XPS. The catalytic activity of the CuO/TiO2-SnO2 catalysts was markedly depended on the loading of CuO, and the optimum CuO loading was 8 wt.% （Tloo = 80 ℃）. The CuO/TiO2-SnO2 catalysts exhibited much higher catalytic activity than the CuO/TiO2 and CuO/SnO2 catalysts. H2-TPR result indicated that a large amount of CuO formed the active site for CO oxidation in 8 wt.% CuO/TiO2-SnO2 catalyst.
基金supported by the Heilongjiang Provincial Science and Technology Development Program (No.GC06C20503)
文摘The UV/Ag-TiO2/O3 process was investigated for ballast water treatment using Dunaliella salina as an indicator. Inactivation curves were obtained, and the toxicity of effluent was determined. Compared with individual unit processes using ozone or UV/Ag-TiO2, the inactivation efficiency ofD. salina by the combined UV/Ag-TiO2/O3 process was enhanced. The presence of ozone caused an immediate decrease in chlorophyll a （chl-a） concentration. Inactivation efficiency and chl-a removal efficiency were positively correlated with ozone dose and ultraviolet intensity. The initial total residual oxidant （TRO） concentration of effluent increased with increasing ozone dose, and persistence of TRO resulted in an extended period of toxicity. The results suggest that UV/Ag-TiO2/O3 has potential for ballast water treatment.
基金funded by China Postdoctoral Science Foundation(No.2021M700569)Chongqing Postdoctoral Science Foundation(No.7 cstc2021jcyj-bshX0087)。
文摘This work proposed a strategy of indirectly inducing uniform microarc discharge by controlling the content and distribution ofβ-Mg_(17)Al_(12)phase in AZ91D Mg alloy.Two kinds of nano-particles(ZrO_(2)and TiO_(2))were designed to be added into the substrate of Mg alloy by friction stir processing(FSP).Then,Mg alloy sample designed with different precipitated morphology ofβ-Mg_(17)Al_(12)phase was treated by microarc oxidation(MAO)in Na_(3)PO_(4)/Na2SiO3electrolyte.The characteristics and performance of the MAO coating was analyzed using scanning electron microscopy(SEM),energy dispersive spectrometer(EDS),X-ray diffraction(XRD),X-ray photoelectron spectroscopy(XPS),contact angle meter,and potentiodynamic polarization.It was found that the coarseα-Mg grains in extruded AZ91D Mg alloy were refined by FSP,and theβ-Mg_(17)Al_(12)phase with reticular structure was broken and dispersed.The nano-ZrO_(2)particles were pinned at the grain boundary by FSP,which refined theα-Mg grain and promoted the precipitation ofβ-Mg_(17)Al_(12)phase in grains.It effectively inhibited the“cascade”phenomenon of microarcs,which induced the uniform distribution of discharge pores.The MAO coating on Zr-FSP sample had good wettability and corrosion resistance.However,TiO_(2)particles were hardly detected in the coating on TiFSP sample.
基金financially supported by the National Natural Science Foundation of China(Grant No.51901011)the National Science and Technology Major Project(Grant Nos.2017-Ⅵ-0002-0072 and 2017-VII-0007-0100)+1 种基金the Fundamental Research Funds for Central Universities(Grant No.YWF-21-BJ-J-1034)the support from Youth Talent Support Program of Beihang University。
文摘(γ’+β)two-phase Ni-Al is a promising high-temperature protective coating material used on Ni-base superalloys since it has good interfacial compatibility with superalloys due to the low Al content compared to single-phaseβ-NiA l.In this paper,we aim to improve the oxidation resistance,whereby Ni-34Al-0.1Dy,a(γ’+β)two-phase Ni-Al alloy,was treated by laser shock processing(LSP)and the oxidation behavior at 1150℃ was investigated.The results showed that after oxidation,Al_(2)O_(3)scale formed on the originalβphase of the untreated alloy with a small grain size(200-800 nm),while for the LSP-treated samples,the scale grown on the originalβphase was dominantly composed of larger Al_(2)O_(3)grains with a size of 2-3μm.The distinction was attributed to the promotion ofθ-Al_(2)O_(3)toα-Al_(2)O_(3)transformation induced by the LSP,because the dislocation density,as well as surface roughness,were increased during LSP treatment which can provide heterogeneous nucleation sites forα-Al_(2)O_(3).In addition,the larger-size Al_(2)O_(3)particles,derived from the direct conversion of needle-likeθ-Al_(2)O_(3)in the initial oxidation stage,could rapidly overspread the wholeβphase surface thus reducing the scale growth rate.
基金the support from the Brook Byers Institute for Sustainable Systems,Hightower ChairGeorgia Research Alliance at the Georgia Institute of Technology。
文摘TiO_(2)has demonstrated outstanding performance in electrochemical advanced oxidation processes(EAOPs)due to its structural stability and high oxygen overpotential.However,there is still much room for improving its electrochemical activity.Herein,narrow bandgap manganese oxide(MnO_(x))was composited with TiO_(2)nanotube arrays(TiO_(2)NTAs)that in-situ oxidized on porous Ti sponge,forming the MnO_(x)-TiO_(2)NTAs anode.XANES and XPS analysis further proved that the composition of MnO_(x)is Mn2O3.Electrochemical characterizations revealed that increasing the composited concentration of MnO_(x)can improve the conductivity and reduce oxygen evolution potential so as to improve the electrochemical activity of the composited MnO_(x)-TiO_(2)NTAs anode.Meanwhile,the optimal degradation rate of benzoic acid(BA)was achieved using MnO_(x)-TiO_(2)NTAs with a MnO_(x)concentration of 0.1 mmol L^(-1),and the role of MnO_(x)was proposed based on DFT calculation.Additionally,the required electrical energy(EE/O)to destroy BA was optimized by varying the composited concentration of MnO_(x)and the degradation voltage.These quantitative results are of great significance for the design and application of high-performance materials for EAOPs.
文摘We describes a controllable synthesis procedure for growing a-Ee2O3 and Ee3O4 nanowires. High magnetic hematite a-Fe2O3 nanowires are successfully grown on Fe0.5Ni0.5 alloy substrates via an oxide assisted vapor-solid process. Experimental results also indicate that previous immersion of the substrates in a solution of oxalic acid causes the grown nanowires to convert gradually into magnetite （Fe3O4） nanowires. Additionally, the saturated state of Fe3O4 nanowires is achieved as the oxalic acid concentration reaches 0.75 mol/L. The average diameter and length of nanowires expands with an increasing operation temperature and the growth density of nanowires accumulates with an increasing gas flux in the vapor-solid process. The growth mechanism of a-Fe2O3 and Fe3O4 nanowires is also discussed. The results demonstrate that the entire synthesis of nanowires can be completed within 2 h.
基金financially supported by the National Key R&D Program of China(No.2018YFC1902002)the Special Fund for the National Natural Science Foundation of China(No.U1608254)。
文摘Because of the highly toxic cyanide in the gold cyanide residues,cyanide must be removed for environmental protection.The process mineralogy of residues was studied firstly,and then cyanide removal was carried out by three chemical methods.The results showed that the residue mainly contained Si,S and Fe.Pyrite was the main metallic mineral,and the iron-complex cyanides make cyanide removal difficult.The minerals in residues were in ultrafine particle size with high monomer dissociation degrees.In H_(2)O_(2)oxidation process,the self-decomposition and side reactions resulted in high consumption of H_(2)O_(2).In Na_(2)S_(2)O_(5)-air oxidation process,the time for complete process was long because of the reactions between Na_(2)S_(2)O_(5)and O_(2).Na_(2)SO_(3)oxidation method was found to be a new method for cyanide removal without air inflation device.The cyanide content was reduced to the national standard level in 90 min at pH 9.0 with optimum Na_(2)SO_(3)dose of 2.0 g/L.
基金financial support from the project Cabon4PUR which has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No 768919support of Dr. Alessandro Longo for Rietveld refinement of XRDsupport of the Wim Rogiers and Micha?l Lottin at the LCT for the fixed bed reactor setup used for experimental validation of the process concept。
文摘Up to 9% of the global CO_(2) emissions come from the iron and steel industry. Here, a combined chemical looping process to produce CO, a building block for the chemical industry, from the CO_(2) -rich blast furnace gas of a steel mill is proposed. This cyclic process can make use of abundant Fe_(3)O_(4) and CaO as solid oxygen and CO_(2) carriers at atmospheric pressure. A proof of concept was obtained in a laboratory-scale fixed bed reactor with synthetic blast furnace gas and Fe_(3)O_(4) /CaO = 0.6 kg/kg. CO production from the proposed process was investigated at both isothermal conditions(1023 K) and upon imposing a temperature program from 1023 to 1148 K. The experimental results were compared using performance indicators such as CO yield, CO space time yield, carbon recovery of the process, fuel utilisation, and solids’ utilisation.The temperature-programmed CO production resulted in a CO yield of 0.056 ± 0.002 mol per mol of synthetic blast furnace gas at an average CO space time yield of 7.6 mmol kgFe^(-1) s^(-1) over 10 cycles, carbon recovery of 48% ± 1%, fuel utilisation of 23% ± 2%, and an average calcium oxide and iron oxide utilisation of 22% ± 1% and 11% ± 1%. These experimental performance indicators for the temperature-programmed CO production were consistently better than those of the isothermal implementation mode by 20% to 35%. Over 10 consecutive process cycles, no significant losses in CO yield were observed in either implementation mode. Process simulation was carried out for 1 million metric tonnes per year of equivalent CO_(2) emissions from the blast furnace gas of a steel mill to analyse the exergy losses in both modes of operation. Comparison of the exergy efficiency of the temperature-programmed process to the isothermal process showed that the former is more efficient because of the higher CO concentration achievable,despite 20% higher exergy losses caused by heat transfer required to change temperature.
基金ORANO Chimie-Enrichissement Co.for the financial support of this project。
文摘Undoped nickel-based catalysts supported on depleted uranium oxide allow one to carry out CO_(2)methanation process under extremely low reaction temperature under atmospheric pressure and powered by a contactless induction heating.By adjusting the reaction conditions,the catalyst is able to perform CO_(2)methanation reaction under autothermal process operated inside a non-adiabatic reactor,without any external energy supply.Such autothermal process is possible thanks to the high apparent density of the UO_x which allows one to confine the reaction heat in a small catalyst volume in order to confine the exothermicity of the reaction inside the catalyst and to operate the reaction at equilibrium heat in-heat out.Such autothermal operation mode allows one to significantly reduce the complexity of the process compared to that operated using adiabatic reactor,where complete insulation is required to prevent heat disequilibrium,in order to reduce as much as possible,the heat exchange with the external medium.The catalyst displays an extremely high stability as a function of time on stream as no apparent deactivation.It is expected that such new catalyst with unprecedented catalytic performance could open new era in the field of heterogeneous catalysis where traditional supports show their limitations to operate catalytic processes under severe reaction conditions.
基金Y.C.and J.C.are contributed equally to the paper.Project supported by the National Natural Science Foundation of China (U19A2017)the Fundamental Research Funds for the Central South University and the Australian Research Council (DP180100731 and DP180100568)。
文摘The electrochemical carbon dioxide reduction reaction(CO_(2)RR),which can produce value-added chemical feedstocks,is a proton-coupled-electron process with sluggish kinetics.Thus,highly efficient,cheap catalysts are urgently required.Transition metal oxides such as CoO_(x),FeO_(x),and NiO_(x)are low-cost,low toxicity,and abundant materials for a wide range of electrochemical reactions,but are almost inert for CO_(2)RR.Here,we report for the first time that nitrogen doped carbon nanotubes(N-CNT)have a surprising activation effect on the activity and selectivity of transition metal-oxide(MO_(x)where M=Fe,Ni,and Co)nanoclusters for CO_(2)RR.MO_(x)supported on N-CNT,MO_(x)/N-CNT,achieves a CO yield of 2.6–2.8 mmol cm−2 min−1 at an overpotential of−0.55 V,which is two orders of magnitude higher than MO_(x)supported on acid treated CNTs(MO_(x)/O-CNT)and four times higher than pristine N-CNT.The faraday efficiency for electrochemical CO_(2)-to-CO conversion is as high as 90.3%at overpotential of 0.44 V.Both in-situ XAS measurements and DFT calculations disclose that MO_(x)nanoclusters can be hydrated in CO_(2)saturated KHCO_(3),and the N defects of N-CNT effectively stabilize these metal hydroxyl species under carbon dioxide reduction reaction conditions,which can split the water molecules and provide local protons to inhibit the poisoning of active sites under carbon dioxide reduction reaction conditions.
文摘A comparative study of catalytic CO oxidation and selective CO oxidation over Pt/Al2O3 and CeO2-promoted Pt/Al2O3 catalysts has been investigated for the removal of a trace amount of CO from the reformed gas. The catalysts were prepared by sol gel and incipient wetness impregnation. CO oxidation and selective CO oxidation were carried out with a 5%Pt/Al2O3 and a 5%Pt/15%CeO2/Al2O3. The presence of 15%CeO2 inthe 5%Pt/Al2O3 dramatically improves the activities to CO oxidation and selective CO oxidation at low temperature (0℃). FTIR results indicate that CO could react with lattice oxygen from ceria and release CO2 as a product. Low space velocity would obtain high CO conversion at low temperatures while high space velocity would obtain high CO conversion at high temperatures. The results also show that a 5%Pt/15%CeO2/Al2O3 can completely oxidize 1% CO at180℃with selectivity of 52% and space velocity of70,000 cm3·g-1·h-1. Under the realistic gas feed with 1%O2, this catalyst is very stable and retains its activity and selectivity at180℃during 72 h.
