Bacterial cellulose doped with P and Cu was used as a catalyst for a microbial fuel cell(MFC) cathode,which was then used to treat ethanol fermentation stillage from food waste.Corresponding output power,coulombic eff...Bacterial cellulose doped with P and Cu was used as a catalyst for a microbial fuel cell(MFC) cathode,which was then used to treat ethanol fermentation stillage from food waste.Corresponding output power,coulombic efficiency(CE),and biological toxicity were detected.Through a series of characterization experiments,the addition of the cathode catalyst was found to improve catalytic activity and accelerate the consumption of the substrate.The resulting maximum output power was 572.16 mW·m^(-2).CE and the removal rate of chemical oxygen demand(COD) in the fermentation stillage by P-Cu-BC reached 26% and 64.5%,respectively.The rate of biotoxicity removal by MFC treatment reached 84.7%.The aim of this study was apply a novel catalyst for MFC and optimize the treatment efficiency of fermentation stillage.展开更多
Antibiotic wastewater contains a variety of pollutant stressors that can induce and promote antibiotic resistance(AR)when released into the environment.Although these substances are mostly in concentrations lower than...Antibiotic wastewater contains a variety of pollutant stressors that can induce and promote antibiotic resistance(AR)when released into the environment.Although these substances are mostly in concentrations lower than those known to induce AR individually,it is possible that antibiotic wastewater discharge might still promote the AR transmission risk via additive or synergistic effects.However,the comprehensive effect of antibiotic wastewater on AR development has rarely been evaluated,and its treatment efficiency remains unknown.Here,samples were collected from different stages of a cephalosporin production wastewater treatment plant,and the potential AR induction effect of their chemical mixtures was explored through the exposure of the antibiotic-sensitive Escherichia coli K12 strain.Incubation with raw cephalosporin production wastewater significantly promoted mutation rates(3.6×10^(3)-9.3×10^(3)-fold)and minimum inhibition concentrations(6.0-6.7-fold)of E.coli against ampicillin and chloramphenicol.This may be attributed to the inhibition effect and oxidative stress of cephalosporin wastewater on E.coli.The AR induction effect of cephalosporin wastewater decreased after the coagulation sedimentation treatment and was completely removed after the full treatment process.A Pearson correlation analysis revealed that the reduction in the AR induction effect had a strong positive correlation with the removal of organics and biological toxicity.This indicates that the antibiotic wastewater treatment had a collaborative processing effect of conventional pollutants,toxicity,and the AR induction effect.This study illustrates the potential AR transmission risk of antibiotic wastewater and highlights the need for its adequate treatment.展开更多
Every day,human beings produce excreta all over the world,and the sludge that accumulates in waste disposal systems is referred to as the‘faecal sludge(FS)’.FS can cause serious environmental pollution in urban area...Every day,human beings produce excreta all over the world,and the sludge that accumulates in waste disposal systems is referred to as the‘faecal sludge(FS)’.FS can cause serious environmental pollution in urban areas if it cannot be disposed of properly.A complete FS management system must include onsite sanitation technologies,FS collection and transport,a treatment plant,and resource recovery or disposal of the treatment end-products.Focusing on the treatment and reuse/disposal step of a FS complete service chain,this research presents two cases of FS treatment in Beijing.In Case 1,FS biogas plant adopts anaerobic digestion(AD)to treat FS,and the digestate can be used as biofertilizer in the surrounding greenhouse.In Case 2,several technologies including solid-liquid separation,dewatering,pyrolysis,AD and co-composting are integrated to find innovative solutions for FS treatment.A comprehensive assessment including the aspects of technology,economy and environment is conducted for further SWOT(Strengths,Weaknesses,Opportunities and Threats)analysis.Then,critical strategies are developed,which include(1)selecting project site for optimized transportation,maximum waste reuse,minimum environmental impact and convenient final effluent disposal;(2)planning technical options at a feasible study stage,considering resource recovery,secondary pollution prevention and fire protection;(3)exploring market channels for by-products sale to increase profitability;(4)guaranteeing engineering quality and service life for the purpose of sustainable operation;(5)minimizing health risks to persons exposed to the untreated FS;and(6)providing necessary training for hygiene protection.The cases in Beijing can provide valuable lessons for urban areas in developing countries and the strategies can provide a reference for stakeholders and decision-makers who intend to develop FS treatment projects.展开更多
A novel porous nanocomposite,cross-linked chitosan and polyethylene glycol(PEG) bead-supported MnFe_(2) O_(4) nanoparticles(CPM),was developed as an efficient adsorbent to remove metalloid(As(Ⅲ))and heavy metals(Cd(...A novel porous nanocomposite,cross-linked chitosan and polyethylene glycol(PEG) bead-supported MnFe_(2) O_(4) nanoparticles(CPM),was developed as an efficient adsorbent to remove metalloid(As(Ⅲ))and heavy metals(Cd(Ⅱ),Cu(Ⅱ),and Pb(Ⅱ)).The characteristics of CPM showed a porous structure,well dispersed MnFe_(2) O_(4),and several of hydroxyl and amino groups(-OH,-NH_(2)).Batch experiments demonstrated that the best adsorption property of As(Ⅲ),Cd(Ⅱ),Cu(Ⅱ),and Pb(Ⅱ) was achieved within 8 h with maximum adsorption capacities of 9.90,9.73,43.94,and 11.98 mg/g,respectively.Competitive and synergistic effects(particularly precipitation) were included in the co-adsorption mechanism of As(Ⅲ) and heavy metals.Thereinto,As(Ⅲ) was partly oxidized by MnFe_(2) O_(4) to As(V),and both were coordinated on MnFe_(2) O_(4) nanoparticles.Pb(Ⅱ) could also bind to MnFe_(2) O_(4) by ion exchange and electrostatic attraction.Furthermore,Cd(Ⅱ) and Cu(Ⅱ) tended to be coordinated on chitosan.Therefore,CPM can serve as a remediation material for water and soil co-contaminated with As(Ⅲ) and heavy metals.展开更多
Recovery of alginate extracted from aerobic granular sludge(AGS)has given rise to a novel research direction.However,these extracted alginate solutions have a water content of nearly 100%.Alternately,ultrafiltration(U...Recovery of alginate extracted from aerobic granular sludge(AGS)has given rise to a novel research direction.However,these extracted alginate solutions have a water content of nearly 100%.Alternately,ultrafiltration(UF)is generally used for concentration of polymers.Furthermore,the introduction of multivalent metal ions into alginate may provide a promising method for the development of novel nanomaterials.In this study,membrane fouling mitigation by multivalent metal ions,both individually and in combination,and properties of recycled materials were investigated for UF recovery of sodium alginate(SA).The filtration resistance showed a significantly negative correlation with the concentration of metal ions,arranged in the order of Mg^2+<Ca^2+<Fe^3+<Al^3+(filtration resistance mitigation),and the moisture content of recycled filter cake showed a marked decrease.For Ca^2+,Mg^2+,Fe^3+,and Ca^2++Fe^3+,the filtration resistances were almost the same when the total charge concentration was less than 5 mmol·L^–1.However,when the total charge concentration was greater than 5 mmol·L^–1,membrane fouling mitigation increased significantly in the presence of Ca^2+or Fe^3+and remained constant for Mg^2+with the increase of total charge concentration.The filtration resistance mitigation was arranged in the order of Fe^3+>Fe^3++Ca^2+>Ca^2+>Mg^2+.Three mechanisms were proposed in the presence of Fe^3+,such as the decrease of SA concentration,change in p H,and production of hydroxide iron colloids from hydrolysis.The properties of recycled materials(filter cake)were investigated via optical microscope observation,dynamic light scattering,Fourier transform infrared,X-ray photoelectron spectroscopy(XPS),and scanning electron microscopy.The results provide further insight into UF recoveries of alginate extracted from AGS.展开更多
Discharge of metals and their mineral flotation collectors into the soil environment causes severe ecological and health impacts, which is still not fully understood. This is of great concern, particularly with regard...Discharge of metals and their mineral flotation collectors into the soil environment causes severe ecological and health impacts, which is still not fully understood. This is of great concern, particularly with regards to their effect on the soil microorganisms whose functions determine not only the soil quality and function but also influence the air and water quality. This study aimed to analyze and compare, microcalorimetrically, the single chemical toxic effect with the combined effect of copper (Cu) and two of its main flotation collectors, potassium amyl xanthate (PAX) and sodium isoamyl xanthate (SIAX), on soil microbial community. All chemicals, individually and as a binary mixture of copper and each of its flotation collectors, exhibited a significant dose-effect relationship, and the highest and lowest microbial activity inhibition being associated with SIAX and Cu, respectively (e.g. IC 50 of 447.5, 158.3 and 83.9 μg·g?1 soil for copper, PAX and SIAX, respectively). For all cases, the microbial activity was more affected by the mixture than by the individual mixture components. Increasing the xanthates dose (from 25 to 100 μg·g?1 soil) in the mixture with a copper dose of 200 μg·g?1 soil led to the increase of the microbial activity inhibition rate, from 23.08 % to 53.85% in case of PAX and from 26.92% to 57.69% in case of SIAX). Similarly, the toxicity level of the mixture of equitoxic components doses increased with the increased mixture doses. Since the observed activity level can be attributed to the surviving microbes, capable of adapting to both chemical and their mixture, a genetically based analysis should be conducted to allow identifying and characterizing the potentially resistant strains that can be useful for the remediation of the pollution by copper and xanthates and for the sustainability of copper mining and flotation, and for all soil, water, and air quality and function interest.展开更多
Metal-organic frameworks(MOFs)have favorable characteristics such as large specific surface area,high porosity,structural diversity,and pore surface modification,giving them great potential for development and attract...Metal-organic frameworks(MOFs)have favorable characteristics such as large specific surface area,high porosity,structural diversity,and pore surface modification,giving them great potential for development and attractive prospects in the research area of modern materials electrocatalysis.However,unsatisfactory catalytic activity and poor electronic conductivity are the main challenges facing MOFs.This review focuses on MOF-based materials used in electrocatalysis,based on the types of catalytic reactions that have used MOF-based materials in recent years along with their applications,and also looks at some new electrocatalytic materials and their future development prospects.展开更多
The synthesis process of conventional Mn-based denitrification catalysts is relatively complex and expensive.In this paper,a resource application of chlorella was proposed,and a Chlorella@Mn composite denitrification ...The synthesis process of conventional Mn-based denitrification catalysts is relatively complex and expensive.In this paper,a resource application of chlorella was proposed,and a Chlorella@Mn composite denitrification catalyst was innovatively synthesized by electrostatic interaction.The Chlorella@Mn composite denitrification catalyst prepared under the optimal conditions(0.54 g/L Mn^(2+)concentration,20 million chlorellas/mL concentration,450℃ calcination temperature)exhibited a well-developed pore structure and large specific surface area(122 m^(2)/g).Compared with MnOx alone,the Chlorella@Mn composite catalyst achieved superior performance,with~100%NH_(3)selective catalytic reduction(NH_(3)-SCR)denitrification activity at 100-225℃.The results of NH_(3)temperature-programmed desorption(NH_(3)-TPD)and H_(2)temperature-programmed reduction(H_(2)-TPR)showed that the catalyst had strong acid sites and good redox properties.Zeta potential testing showed that the electronegativity of the chlorella cell surface could be used to enrich with Mn^(2+).X-ray photoelectron spectroscopy(XPS)confirmed that Chlorella@Mn had a high content of Mn^(3+)and surface chemisorbed oxygen.In-situ diffuse refectance infrared Fourier transform spectroscopy(in-situ DRIFTS)experimental results showed that both Langmuir-Hinshelwood(L-H)and Eley-Rideal(E-R)mechanisms play a role in the denitrification process on the surface of the Chlorella@Mn catalyst,where the main intermediate nitrate species is monodentate nitrite.The presence of SO_(2)promoted the generation and strengthening of Bronsted acid sites,but also generated more sulfate species on the surface,thereby reducing the denitrification activity of the Chlorella@Mn catalyst.The Chlorella@Mn composite catalyst had the characteristics of short preparation time,simple process and low cost,making it promising for industrial application.展开更多
Microorganisms are crucial in the bioremediation of organophosphorus pesticides. However, most functional microorganisms (> 99%) are yet to be cultivated. This study applied two cultivation-independent approaches, ...Microorganisms are crucial in the bioremediation of organophosphorus pesticides. However, most functional microorganisms (> 99%) are yet to be cultivated. This study applied two cultivation-independent approaches, DNA-SIP and magnetic-nanoparticle mediated isolation (MMI), to identify the functional microorganisms in degrading dimethoate in agricultural soils. MMI identified five dimethoate degraders: Pseudomonas, Bacillus, Ramlibacter, Arthrobacter, and Rhodococcus, whereas DNA-SIP identified three dimethoate degraders: Ramlibacter, Arthrobacter, and Rhodococcus. Also, MMI showed higher resolution than DNA-SIP in identifying functional microorganisms. Two organic phosphohydrolase (OPH) genes: ophC2 and ophB, were involved in dimethoate metabolism, as revealed by DNA-SIP and MMI. The degradation products of dimethoate include omethoate, O,O,S-trimethyl thiophosphorothioate, N-methyl-2-sulfanylacetamide, O,O-diethyl S-hydrogen phosphorodithioate, O,O,O-trimethyl thiophosphate, O,O,S-trimethyl thiophosphorodithioate, and O,O,O-trimethyl phosphoric. This study emphasizes the feasibility of using SIP and MMI to explore the functional dimethoate degraders, expanding our knowledge of microbial resources with cultivation-independent approaches.展开更多
In order to study the degradation process of dioxins in industrial flue gas,the decomposition of o-dichlorobenzene(o-DCB)in a DBD plasma catalytic reactor was investigated.The results showed that an NTP-catalyzed syst...In order to study the degradation process of dioxins in industrial flue gas,the decomposition of o-dichlorobenzene(o-DCB)in a DBD plasma catalytic reactor was investigated.The results showed that an NTP-catalyzed system,especially using the Cu Mn Ti Oxcatalyst,had better o-DCB degradation performance compared to plasma alone.The combination of the Cu Mn Ti Oxcatalyst with NTP can achieve a degradation efficiency of up to 97.2%for o-DCB;the selectivity of CO and CO_(2)and the carbon balance were 40%,45%,and 85%,respectively.The dielectric constant and electrical property results indicated that the surface discharge capacity of the catalysts played a major role in the degradation of o-DCB,and a higher dielectric constant could suppress the plasma expansion and enhance the duration of the plasma discharge per discharge cycle.According to the O1s XPS and O_(2)-TPD results,the conversion of CO to CO_(2)follows the M-v-K mechanism;thus,the active species on the catalyst surface play an important role.Moreover,the Cu Mn Ti Oxand NTP mixed system exhibited excellent stability,which is probably because Cu doping improved the lifetime of the catalyst.This work can provide an experimental and theoretical basis for research in the degradation of o-DCB by plasma catalyst systems.展开更多
Sulfamethoxazole(SMX)is commonly detected in wastewater and cannot be completely decomposed during conventional treatment processes.Ozone(O_(3))is often used in water treatment.This study explored the influence of nat...Sulfamethoxazole(SMX)is commonly detected in wastewater and cannot be completely decomposed during conventional treatment processes.Ozone(O_(3))is often used in water treatment.This study explored the influence of natural organic matters(NOM)in secondary effluent of a sewage treatment plant on the ozonation pathways of SMX.The changes in NOM components during ozonation were also analyzed.SMX was primarily degraded by hydrolysis,isoxazole-ring opening,and double-bond addition,whereas hydroxylation was not the principal route given the low maximum abundances of the hydroxylated products,with m/z of 269 and 287.The hydroxylation process occurred mainly through indirect oxidation because the maximum abundances of the products reduced by about 70%after the radical quencher was added,whereas isoxazole-ring opening and double-bond addition processes mainly depended on direct oxidation,which was unaffected by the quencher.NOM mainly affected the degradation of micropollutants by consuming•OH rather than O_(3)molecules,resulting in the 63%–85%decrease in indirect oxidation products.The NOM in the effluent were also degraded simultaneously during ozonation,and the components with larger aromaticity were more likely degraded through direct oxidation.The dependences of the three main components of NOM in the effluent on indirect oxidation followed the sequence:humic-like substances>fluvic-like substance-s>protein-like substances.This study reveals the ozonation mechanism of SMX in secondary effluent and provides a theoretical basis for the control of SMX and its degradation products in actual water treatment.展开更多
As the main contributor of the formation of particulate matter as well as ozone, volatile organic compounds(VOCs) greatly affect human health and the environmental quality. Catalytic combustion/oxidation has been view...As the main contributor of the formation of particulate matter as well as ozone, volatile organic compounds(VOCs) greatly affect human health and the environmental quality. Catalytic combustion/oxidation has been viewed as an efficient, economically feasible and environmentally friendly way for the elimination of VOCs. Supported metal catalyst is the preferred type of catalysts applied for VOCs catalytic combustion because of the synergy between active components and support as well as its flexibility in the composition. The presence of support not only plays the role of keeping the catalyst with good stability and mechanical strength, but also provides a large specific surface for the good dispersion of active components, which could effectively improve the performance of catalyst as well as decrease the usage of active components, especially the noble metal amount. Mesoporous molecular sieves, owing to their large surface area, unique porous structures, large pore size as well as uniform pore-size distribution, were viewed as superior support for dispersing active components. This review focuses on the recent development of mesoporous molecular sieve supported metal catalysts and their application in catalytic oxidation of VOCs. The effect of active component types, support structure, preparation method, precursors, etc. on the valence state, dispersion as well as the loading of active species were also discussed and summarized. Moreover, the corresponding conversion route of VOCs was also addressed.This review aims to provide some enlightment for designing the supported metal catalysts with superior activity and stability for VOCs removal.展开更多
Ce1-xZrxO_(2) composite oxides(molar,x=0-1.0,interval of 0.2)were prepared by a cetyltrimethylammonium bromide-assisted precipitation method.The enhancement of silver-species modification and catalytic mechanism of ad...Ce1-xZrxO_(2) composite oxides(molar,x=0-1.0,interval of 0.2)were prepared by a cetyltrimethylammonium bromide-assisted precipitation method.The enhancement of silver-species modification and catalytic mechanism of adsorption-transformationdesorption process were investigated over the Ag-impregnated catalysts for lowtemperature selective catalytic oxidation of ammonia(NH_(3)-SCO).The optimal 5 wt.%Ag/Ce_(0.6)Zr_(0.4)O_(2) catalyst presented good NH_(3)-SCO performancewith>90% NH_(3) conversion at temperature(T)≥250°C and 89% N_(2) selectivity.Despite the irregular block shape and underdeveloped specific surface area(∼60m2/g),the naked and Ag-modified Ce_(0.6)Zr_(0.4)O_(2) solid solution still obtained highly dispersed distribution of surface elements analyzed by scanning electron microscope-energy dispersive spectrometer(SEM-EDS)(mapping),N_(2) adsorptiondesorption test and X-ray diffraction(XRD).H2 temperature programmed reduction(H2-TPR)and X-ray photoelectron spectroscopy(XPS)results indicated that Ag-modification enhanced the mobility and activation of oxygen-species leading to a promotion on CeO_(2) reducibility and synergistic Ag0/Ag+and Ce^(4+)/Ce^(3+)redox cycles.Besides,Ag+/Ag_(2)O clusters could facilitate the formation of surface oxygen vacancies that was beneficial to the adsorption and activation of ammonia.NH3-temperature programmed desorption(NH_(3)-TPD)showed more adsorption-desorption capacity to ammoniawere provided by physical,weakandmedium-strong acid sites.Diffused reflectance infrared Fourier transform spectroscopy(DRIFTS)experiments revealed the activation of ammonia might be the control step of NH3-SCO procedure,during which NH3 dehydrogenation derived from NHx-species and also internal selective catalytic reduction(i-SCR)reactions were proposed.展开更多
Energy-saving and efficient monolithic catalysts are hotspots of catalytic purification of industrial gaseous pollutants.Here,we have developed an electrothermal catalytic mode,in which the ignition temperature requir...Energy-saving and efficient monolithic catalysts are hotspots of catalytic purification of industrial gaseous pollutants.Here,we have developed an electrothermal catalytic mode,in which the ignition temperature required for the reaction is provided by Joule heat generated when the current flows through the catalyst.In this paper,Mn/NiAl/NF,Mn/NiFe/NF and Mn/NF metal-based monolithic catalysts were prepared using nickel foam (NF) as the carrier for thermal and electrothermal catalysis of n-heptane.The results indicated that Mn-based monolithic catalysts exhibit high activity in thermal and electrothermal catalysis.Mn/NiFe/NF achieve conversion of n-heptane more than 99%in electrothermal catalysis under a direct-current (DC) power of 6 W,and energy-saving is 54% compared with thermal catalysis.In addition,the results indicated that the introduction of NiAl (or NiFe) greatly enhanced the catalytic activity of Mn/NF,which attributed to the higher specific surface area,Mn3+/Mn4+,Ni3+/Ni^(2+),adsorbed oxygen species (Oads)/lattice oxygen species (Olatt),redox performance of the catalyst.Electrothermal catalytic activity was significantly higher than thermal catalytic activity before complete conversion,which may be related to electronic effects.Besides,Mn/NiFe/NF has good cyclic and long-term stability in electrothermal catalysis.This paper provided a theoretical basis for applying electrothermal catalysis in the field of VOCs elimination.展开更多
This work was undertaken to investigate the behaviors and kinetics of toluene adsorption and desorption on activated carbons with varying pore structure. Five kinds of activated carbon from different raw materials wer...This work was undertaken to investigate the behaviors and kinetics of toluene adsorption and desorption on activated carbons with varying pore structure. Five kinds of activated carbon from different raw materials were selected. Adsorption isotherms and breakthrough curves for toluene were measured. Langmuir and Freundlich equations were fitted to the equilibrium data, and the Freundlich equation was more suitable for simulating toluene adsorption. The process consisted of monolayer, multilayer and partial active site adsorption types. The effect of the pore structure of the activated carbons on toluene adsorption capacity was investigated. The quasi-first-order model was more suitable for describing the process than the quasi-second-order model. The adsorption data was also modeled by the internal particle diffusion model and it was found that the adsorption process could be divided into three stages. In the external surface adsorption process, the rate depended on the specific surface area. During the particle diffusion stage, pore structure and volume were the main factors affecting adsorption rate. In the final equilibrium stage, the rate was determined by the ratio of meso-and macro-pores to total pore volume. The rate over the whole adsorption process was dominated by the toluene concentration. The desorption behavior of toluene on activated carbons was investigated,and the process was divided into heat and mass transfer parts corresponding to emission and diffusion mechanisms, respectively. Physical adsorption played the main role during the adsorption process.展开更多
Catalytic oxidation of toluene over noble metal catalysts is a representative reaction for elimination of volatile organic compounds(VOCs).However,to fully understand the activation of molecular oxygen and the role of...Catalytic oxidation of toluene over noble metal catalysts is a representative reaction for elimination of volatile organic compounds(VOCs).However,to fully understand the activation of molecular oxygen and the role of active oxygen species generated in this reaction is still a challenging target.Herein,MgO nanosheets and single-atom Pt loaded MgO(Pt SA/MgO)nanosheets were synthesized and used as catalysts in toluene oxidation.The activation process of molecular oxygen and oxidation performance on the two catalysts were contrastively investigated.The Pt SA/MgO exhibited significantly enhanced catalytic activity compared to MgO.The oxygen vacancies can be easily generated on the Pt SA/MgO surface,which facilitate the activation of molecular oxygen and the formation of active oxygen species.Based on the experimental data and theoretical calculations,an active oxygen species promoted oxidation mechanism for toluene was proposed.In the presence of H2O,the molecular oxygen is more favorable to be dissociated to generate•OH on the oxygen vacancies of the Pt SA/MgO surface,which is the dominant active oxygen species.We anticipate that this work may shed light on further investigation of t10.1007/s12274-020-2765-1he oxidation mechanism of toluene and other VOCs over noble metal catalysts.展开更多
Mn-Ni oxides with different compositions were prepared using standard co-precipitation(CP) and urea hydrolysis-precipitation(UH) methods and optimized for the selective catalytic reduction of nitrogen oxides(NOx) by N...Mn-Ni oxides with different compositions were prepared using standard co-precipitation(CP) and urea hydrolysis-precipitation(UH) methods and optimized for the selective catalytic reduction of nitrogen oxides(NOx) by NH3 at low temperature.Mn((2))Ni(1)Ox-CP and Mn(2)Ni(1)Ox-UH(with Mn:Ni molar ratio of 2:1) catalysts showed almost identical selective catalytic reduction(SCR) catalytic activity,with about 96% NOx conversion at 750 C and-99%in the temperature range from 100 to 250℃.X-ray diffraction(XRD) results showed that Mn(2)Ni(1)Ox-CP and Mn(2)Ni(1)Ox-UH catalysts crystallized in the form of Mn2NiO4 and MnO2-Mn2NiO4 spinel,respectively.The latter gave relatively good selectivity to N2,which might be due to the presence of the MnO2 phase and high metal-O binding energy,resulting in low dehydrogenation ability.According to the results of various characterization methods,it was found that a high density of surface chemisorbed oxygen species and efficient electron transfer between Mn and Ni in the crystal structure of Mn2NiO4 spinel played important roles in the high-efficiency SCR activity of these catalysts.Mn(2)Ni(1)Ox catalysts presented good resistance to H2O or/and SO2 with stable activity,which benefited from the Mn2NiO4 spinel structure and Eley-Rideal mechanism,with only slight effects from SO2.展开更多
NH_(3)-SCR performances were explored to the relationship between structure morphology and physio-chemical properties over low-dimensional ternary Mn-based catalysts prepared by one-step synthesis method.Due to its st...NH_(3)-SCR performances were explored to the relationship between structure morphology and physio-chemical properties over low-dimensional ternary Mn-based catalysts prepared by one-step synthesis method.Due to its strong oxidation performance,Sn-MnO_(x) was prone to side reactions between NO,NH_(3)and O_(2),resulting in the generation of more NO_(2)and N_(2)O,here most of N_(2)O was driven from the non-selective oxidation of NH_(3),while a small part generated from the side reaction between NH_(3)and NO_(2).Co or Ni doping into Sn-MnO_(x) as solid solution components obviously stronged the electronic interaction for actively mobilization and weakened the oxidation performance for signally reducing the selective tendency of side reactions to N_(2)O.The optimal modification resulted in improving the surface area and enhancing the strong interaction between polyvalent cations in Co/Ni-Mn-SnO_(2)to provide more surface adsorbed oxygen,active sites of Mn^(3+) and Mn^(4+),high-content Sn^(4+) and plentiful Lewis-acidity for more active intermediates,which significantly broadened the activity window of Sn-MnOx,improved the N^(2) selectivity by inhibiting N_(2)O formation,and also contributed to an acceptable resistances to water and sulfur.At low reaction temperatures,the SCR reactions over three catalysts mainly obeyed the typical Elye-rideal(E-R)routs via the reactions of adsorbed L-NH_(x)(x=3,2,1)and B-NH_(4)^(+) with the gaseous NO to generate N_(2) but also N_(2)O by-products.Except for the above basic E-R reactions,as increasing the reaction temperature,the main adsorbed NO_(x)-species were bidentate nitrates that were also active in the Langmuir-Hinshelwood reactions with adsorbed L-NH_(x) species over Co/Ni modified Mn-SnO_(2) catalyst.展开更多
This study explored the superior citrate method(CM)to synthesize Mn-Ce bi-oxides on 3 D monolithic Ni-foam(NF)catalysts for the selective catalytic reduction of NO by NH_(3)(NH_(3)-SCR).The 17 wt%Mn(7)Ce(3)O_(x)/NF(CM...This study explored the superior citrate method(CM)to synthesize Mn-Ce bi-oxides on 3 D monolithic Ni-foam(NF)catalysts for the selective catalytic reduction of NO by NH_(3)(NH_(3)-SCR).The 17 wt%Mn(7)Ce(3)O_(x)/NF(CM-17)catalyst shows the NO_(x)conversion of 98.7%at 175℃and 90%in the presence of 10 vol%H2 O.It is revealed that the combination of surface-active oxygen(formed by high-level oxygen vacancies)and strongly oxidized Mn4+species promots the Fast-SCR reactions,in which Mn4+species play a leading role in NH_(3)-SCR reaction,and the unsaturated Ni atoms and also Ce3+species promote electron exchange and thus improve the redox performance.The coexistence mechanisms of Fast-SCR reactions and E-R pathways are observed over Mn-CeO_(x)/NF catalyst,which may be promoted by the Br?nsted sites at low temperature.In addition,the heat resistance,stability,3 D monolithic porous structure and excellent physical properties of foam nickel provide a unique growth substrates for catalysts preparation and reaction sites for NO_(x)purification.Therefore,industrial application of Mn-Ce bioxides loaded on 3 D monolithic is proposed to be achieved through reasonable preparation methods.展开更多
Cu-Co multiple-oxides modified on HNO_3-pretreated activated coke(AC_(N))were optimized for the simultaneous removal of gaseous CO and elemental mercury(Hg^(0))at low temperature(<200℃).It was found that 2%CuOx-10...Cu-Co multiple-oxides modified on HNO_3-pretreated activated coke(AC_(N))were optimized for the simultaneous removal of gaseous CO and elemental mercury(Hg^(0))at low temperature(<200℃).It was found that 2%CuOx-10%CoOx/AC_(N)catalyst calcined at 400℃resulted in the coexistence of complex oxides including CuO,Cu_2 O,Co_(3)O_(4,Co_(2)O_(3)and CoO phases,which might be good for the simultaneous catalytic oxidation of CO by Co-species and removal of Hg^(0)by Cu-species,benefiting from the synergistic catalysis during the electrointeraction between Go and Cu cations(CoO■Co_(3)O_(4)and Cu_(2)O■CuO).The catalysis removal of CO oxidation was obviously depended on the reaction temperature obtaining94.7%at 200℃,while no obvious promoting effect on the Hg^(0)removal(68.3%-78.7%).These materials were very substitute for the removal of CO and Hg^(0)from the flue gas with the conditions of 8-20 vol.%O_(2)and flue-gas temperature below 200℃.The removal of Hg^(0)followed the combination processes of adsorption and catalytic oxidation reaction via LangmuirHinshelwood mechanism,while the catalysis of CO abided by the Mars-van Krevelen mechanism with lattice oxygen species.展开更多
基金supported by the Open Research Fund Program of Key Laboratory of Cleaner Production and Integrated Resource Utilization of China National Light Industry (CP-2019-YB7)support by Fundamental Research Funds for the Central Universities (TW2019014)support from Sino-US-Japan Joint Laboratory on Organic Solid Waste Resource and Energy Technology of USTB。
文摘Bacterial cellulose doped with P and Cu was used as a catalyst for a microbial fuel cell(MFC) cathode,which was then used to treat ethanol fermentation stillage from food waste.Corresponding output power,coulombic efficiency(CE),and biological toxicity were detected.Through a series of characterization experiments,the addition of the cathode catalyst was found to improve catalytic activity and accelerate the consumption of the substrate.The resulting maximum output power was 572.16 mW·m^(-2).CE and the removal rate of chemical oxygen demand(COD) in the fermentation stillage by P-Cu-BC reached 26% and 64.5%,respectively.The rate of biotoxicity removal by MFC treatment reached 84.7%.The aim of this study was apply a novel catalyst for MFC and optimize the treatment efficiency of fermentation stillage.
基金supported by the National Key Research and Development Program of China(No.2017ZX07103-007)。
文摘Antibiotic wastewater contains a variety of pollutant stressors that can induce and promote antibiotic resistance(AR)when released into the environment.Although these substances are mostly in concentrations lower than those known to induce AR individually,it is possible that antibiotic wastewater discharge might still promote the AR transmission risk via additive or synergistic effects.However,the comprehensive effect of antibiotic wastewater on AR development has rarely been evaluated,and its treatment efficiency remains unknown.Here,samples were collected from different stages of a cephalosporin production wastewater treatment plant,and the potential AR induction effect of their chemical mixtures was explored through the exposure of the antibiotic-sensitive Escherichia coli K12 strain.Incubation with raw cephalosporin production wastewater significantly promoted mutation rates(3.6×10^(3)-9.3×10^(3)-fold)and minimum inhibition concentrations(6.0-6.7-fold)of E.coli against ampicillin and chloramphenicol.This may be attributed to the inhibition effect and oxidative stress of cephalosporin wastewater on E.coli.The AR induction effect of cephalosporin wastewater decreased after the coagulation sedimentation treatment and was completely removed after the full treatment process.A Pearson correlation analysis revealed that the reduction in the AR induction effect had a strong positive correlation with the removal of organics and biological toxicity.This indicates that the antibiotic wastewater treatment had a collaborative processing effect of conventional pollutants,toxicity,and the AR induction effect.This study illustrates the potential AR transmission risk of antibiotic wastewater and highlights the need for its adequate treatment.
基金National Key Research and Development Plan(2016YFE0115600)Fundamental Research Funds for the Central Universities(TW201704)The authors would like to take this opportunity to express our sincere appreciation for the support of National Environment and Energy International Science and Technology Cooperation Base and Reinvent the Toilet Challenge-China Regional Program(Global Development Grant Number OPP1051913).
文摘Every day,human beings produce excreta all over the world,and the sludge that accumulates in waste disposal systems is referred to as the‘faecal sludge(FS)’.FS can cause serious environmental pollution in urban areas if it cannot be disposed of properly.A complete FS management system must include onsite sanitation technologies,FS collection and transport,a treatment plant,and resource recovery or disposal of the treatment end-products.Focusing on the treatment and reuse/disposal step of a FS complete service chain,this research presents two cases of FS treatment in Beijing.In Case 1,FS biogas plant adopts anaerobic digestion(AD)to treat FS,and the digestate can be used as biofertilizer in the surrounding greenhouse.In Case 2,several technologies including solid-liquid separation,dewatering,pyrolysis,AD and co-composting are integrated to find innovative solutions for FS treatment.A comprehensive assessment including the aspects of technology,economy and environment is conducted for further SWOT(Strengths,Weaknesses,Opportunities and Threats)analysis.Then,critical strategies are developed,which include(1)selecting project site for optimized transportation,maximum waste reuse,minimum environmental impact and convenient final effluent disposal;(2)planning technical options at a feasible study stage,considering resource recovery,secondary pollution prevention and fire protection;(3)exploring market channels for by-products sale to increase profitability;(4)guaranteeing engineering quality and service life for the purpose of sustainable operation;(5)minimizing health risks to persons exposed to the untreated FS;and(6)providing necessary training for hygiene protection.The cases in Beijing can provide valuable lessons for urban areas in developing countries and the strategies can provide a reference for stakeholders and decision-makers who intend to develop FS treatment projects.
基金funded by the National Key Research and Development Project (No. 2020YFC1807700)the National Key Research and Development Project (No. 2019YFC1805900)+4 种基金the Youth Fund Project of GRINM (No. 12008)the Youth Fund Project of GRINM (No. 12119)the Open Foundation of State Key Laboratory of Mineral Processing (No. BGRIMM-KJSKL-2020-07)the Open Foundation of State Key Laboratory of Vanadium and Titanium Resources Comprehensive Utilization (No. 2021P4FZG13A)the National Natural Science Foundation of China (No. 51704028)。
文摘A novel porous nanocomposite,cross-linked chitosan and polyethylene glycol(PEG) bead-supported MnFe_(2) O_(4) nanoparticles(CPM),was developed as an efficient adsorbent to remove metalloid(As(Ⅲ))and heavy metals(Cd(Ⅱ),Cu(Ⅱ),and Pb(Ⅱ)).The characteristics of CPM showed a porous structure,well dispersed MnFe_(2) O_(4),and several of hydroxyl and amino groups(-OH,-NH_(2)).Batch experiments demonstrated that the best adsorption property of As(Ⅲ),Cd(Ⅱ),Cu(Ⅱ),and Pb(Ⅱ) was achieved within 8 h with maximum adsorption capacities of 9.90,9.73,43.94,and 11.98 mg/g,respectively.Competitive and synergistic effects(particularly precipitation) were included in the co-adsorption mechanism of As(Ⅲ) and heavy metals.Thereinto,As(Ⅲ) was partly oxidized by MnFe_(2) O_(4) to As(V),and both were coordinated on MnFe_(2) O_(4) nanoparticles.Pb(Ⅱ) could also bind to MnFe_(2) O_(4) by ion exchange and electrostatic attraction.Furthermore,Cd(Ⅱ) and Cu(Ⅱ) tended to be coordinated on chitosan.Therefore,CPM can serve as a remediation material for water and soil co-contaminated with As(Ⅲ) and heavy metals.
基金partially supported by the Beijing Outstanding Talents TrainingScience and Technology Programs of the Beijing Municipal Education Commission(SQKM201710016001)+1 种基金the BUCEA Post Graduate Innovation Projectthe Beijing Advanced Innovation Center for Future Urban Design。
文摘Recovery of alginate extracted from aerobic granular sludge(AGS)has given rise to a novel research direction.However,these extracted alginate solutions have a water content of nearly 100%.Alternately,ultrafiltration(UF)is generally used for concentration of polymers.Furthermore,the introduction of multivalent metal ions into alginate may provide a promising method for the development of novel nanomaterials.In this study,membrane fouling mitigation by multivalent metal ions,both individually and in combination,and properties of recycled materials were investigated for UF recovery of sodium alginate(SA).The filtration resistance showed a significantly negative correlation with the concentration of metal ions,arranged in the order of Mg^2+<Ca^2+<Fe^3+<Al^3+(filtration resistance mitigation),and the moisture content of recycled filter cake showed a marked decrease.For Ca^2+,Mg^2+,Fe^3+,and Ca^2++Fe^3+,the filtration resistances were almost the same when the total charge concentration was less than 5 mmol·L^–1.However,when the total charge concentration was greater than 5 mmol·L^–1,membrane fouling mitigation increased significantly in the presence of Ca^2+or Fe^3+and remained constant for Mg^2+with the increase of total charge concentration.The filtration resistance mitigation was arranged in the order of Fe^3+>Fe^3++Ca^2+>Ca^2+>Mg^2+.Three mechanisms were proposed in the presence of Fe^3+,such as the decrease of SA concentration,change in p H,and production of hydroxide iron colloids from hydrolysis.The properties of recycled materials(filter cake)were investigated via optical microscope observation,dynamic light scattering,Fourier transform infrared,X-ray photoelectron spectroscopy(XPS),and scanning electron microscopy.The results provide further insight into UF recoveries of alginate extracted from AGS.
文摘Discharge of metals and their mineral flotation collectors into the soil environment causes severe ecological and health impacts, which is still not fully understood. This is of great concern, particularly with regards to their effect on the soil microorganisms whose functions determine not only the soil quality and function but also influence the air and water quality. This study aimed to analyze and compare, microcalorimetrically, the single chemical toxic effect with the combined effect of copper (Cu) and two of its main flotation collectors, potassium amyl xanthate (PAX) and sodium isoamyl xanthate (SIAX), on soil microbial community. All chemicals, individually and as a binary mixture of copper and each of its flotation collectors, exhibited a significant dose-effect relationship, and the highest and lowest microbial activity inhibition being associated with SIAX and Cu, respectively (e.g. IC 50 of 447.5, 158.3 and 83.9 μg·g?1 soil for copper, PAX and SIAX, respectively). For all cases, the microbial activity was more affected by the mixture than by the individual mixture components. Increasing the xanthates dose (from 25 to 100 μg·g?1 soil) in the mixture with a copper dose of 200 μg·g?1 soil led to the increase of the microbial activity inhibition rate, from 23.08 % to 53.85% in case of PAX and from 26.92% to 57.69% in case of SIAX). Similarly, the toxicity level of the mixture of equitoxic components doses increased with the increased mixture doses. Since the observed activity level can be attributed to the surviving microbes, capable of adapting to both chemical and their mixture, a genetically based analysis should be conducted to allow identifying and characterizing the potentially resistant strains that can be useful for the remediation of the pollution by copper and xanthates and for the sustainability of copper mining and flotation, and for all soil, water, and air quality and function interest.
基金financially supported by the National Natural Science Foundation of China(Nos.21677010,51808037)the National Key R&D Program of China(No.2021YFB3500702)the Special Fund of Beijing Key Laboratory of Indoor Air Quality Evaluation and Control(No.BZ0344KF21-04)。
文摘Metal-organic frameworks(MOFs)have favorable characteristics such as large specific surface area,high porosity,structural diversity,and pore surface modification,giving them great potential for development and attractive prospects in the research area of modern materials electrocatalysis.However,unsatisfactory catalytic activity and poor electronic conductivity are the main challenges facing MOFs.This review focuses on MOF-based materials used in electrocatalysis,based on the types of catalytic reactions that have used MOF-based materials in recent years along with their applications,and also looks at some new electrocatalytic materials and their future development prospects.
基金supported by the National Natural Science Foundation of China (No.U20A20130)the Fundamental Research Funds for the Central Universities (No.FRF-TP-20-03B)。
文摘The synthesis process of conventional Mn-based denitrification catalysts is relatively complex and expensive.In this paper,a resource application of chlorella was proposed,and a Chlorella@Mn composite denitrification catalyst was innovatively synthesized by electrostatic interaction.The Chlorella@Mn composite denitrification catalyst prepared under the optimal conditions(0.54 g/L Mn^(2+)concentration,20 million chlorellas/mL concentration,450℃ calcination temperature)exhibited a well-developed pore structure and large specific surface area(122 m^(2)/g).Compared with MnOx alone,the Chlorella@Mn composite catalyst achieved superior performance,with~100%NH_(3)selective catalytic reduction(NH_(3)-SCR)denitrification activity at 100-225℃.The results of NH_(3)temperature-programmed desorption(NH_(3)-TPD)and H_(2)temperature-programmed reduction(H_(2)-TPR)showed that the catalyst had strong acid sites and good redox properties.Zeta potential testing showed that the electronegativity of the chlorella cell surface could be used to enrich with Mn^(2+).X-ray photoelectron spectroscopy(XPS)confirmed that Chlorella@Mn had a high content of Mn^(3+)and surface chemisorbed oxygen.In-situ diffuse refectance infrared Fourier transform spectroscopy(in-situ DRIFTS)experimental results showed that both Langmuir-Hinshelwood(L-H)and Eley-Rideal(E-R)mechanisms play a role in the denitrification process on the surface of the Chlorella@Mn catalyst,where the main intermediate nitrate species is monodentate nitrite.The presence of SO_(2)promoted the generation and strengthening of Bronsted acid sites,but also generated more sulfate species on the surface,thereby reducing the denitrification activity of the Chlorella@Mn catalyst.The Chlorella@Mn composite catalyst had the characteristics of short preparation time,simple process and low cost,making it promising for industrial application.
基金The authors would like to thank the National Natural Science Foundation of China(Nos.42177359 and 41807119)the Natural Science Foundation of Beijing(No.8212030)+1 种基金the Fundamental Research Funds for the Central Universities(Nos.FRF-TP-20-010A3 and FRF-IDRY-22-001)the Open Fund of National Engineering Laboratory for Site Remediation Technologies(No.NEL-SRT201907).
文摘Microorganisms are crucial in the bioremediation of organophosphorus pesticides. However, most functional microorganisms (> 99%) are yet to be cultivated. This study applied two cultivation-independent approaches, DNA-SIP and magnetic-nanoparticle mediated isolation (MMI), to identify the functional microorganisms in degrading dimethoate in agricultural soils. MMI identified five dimethoate degraders: Pseudomonas, Bacillus, Ramlibacter, Arthrobacter, and Rhodococcus, whereas DNA-SIP identified three dimethoate degraders: Ramlibacter, Arthrobacter, and Rhodococcus. Also, MMI showed higher resolution than DNA-SIP in identifying functional microorganisms. Two organic phosphohydrolase (OPH) genes: ophC2 and ophB, were involved in dimethoate metabolism, as revealed by DNA-SIP and MMI. The degradation products of dimethoate include omethoate, O,O,S-trimethyl thiophosphorothioate, N-methyl-2-sulfanylacetamide, O,O-diethyl S-hydrogen phosphorodithioate, O,O,O-trimethyl thiophosphate, O,O,S-trimethyl thiophosphorodithioate, and O,O,O-trimethyl phosphoric. This study emphasizes the feasibility of using SIP and MMI to explore the functional dimethoate degraders, expanding our knowledge of microbial resources with cultivation-independent approaches.
基金supported by the National Key R&D Program of China(No.2022YFE0208100)the Key Science and Technology Planning Project of HBIS Group Co.,Ltd.(No.HG2020204-2)+1 种基金the Hebei Provincial Key R&D Program Project(No.22373805D)the Guangdong Air Pollution Control Engineering Laboratory Open Fund Project(No.20193236-09-06)。
文摘In order to study the degradation process of dioxins in industrial flue gas,the decomposition of o-dichlorobenzene(o-DCB)in a DBD plasma catalytic reactor was investigated.The results showed that an NTP-catalyzed system,especially using the Cu Mn Ti Oxcatalyst,had better o-DCB degradation performance compared to plasma alone.The combination of the Cu Mn Ti Oxcatalyst with NTP can achieve a degradation efficiency of up to 97.2%for o-DCB;the selectivity of CO and CO_(2)and the carbon balance were 40%,45%,and 85%,respectively.The dielectric constant and electrical property results indicated that the surface discharge capacity of the catalysts played a major role in the degradation of o-DCB,and a higher dielectric constant could suppress the plasma expansion and enhance the duration of the plasma discharge per discharge cycle.According to the O1s XPS and O_(2)-TPD results,the conversion of CO to CO_(2)follows the M-v-K mechanism;thus,the active species on the catalyst surface play an important role.Moreover,the Cu Mn Ti Oxand NTP mixed system exhibited excellent stability,which is probably because Cu doping improved the lifetime of the catalyst.This work can provide an experimental and theoretical basis for research in the degradation of o-DCB by plasma catalyst systems.
基金This work was supported by the National Key Research and Development Project(No.2019YFD1100204).The experimental supporting by National Environmental and Energy Base for International Science&Technology Cooperation was greatly appreciated.
文摘Sulfamethoxazole(SMX)is commonly detected in wastewater and cannot be completely decomposed during conventional treatment processes.Ozone(O_(3))is often used in water treatment.This study explored the influence of natural organic matters(NOM)in secondary effluent of a sewage treatment plant on the ozonation pathways of SMX.The changes in NOM components during ozonation were also analyzed.SMX was primarily degraded by hydrolysis,isoxazole-ring opening,and double-bond addition,whereas hydroxylation was not the principal route given the low maximum abundances of the hydroxylated products,with m/z of 269 and 287.The hydroxylation process occurred mainly through indirect oxidation because the maximum abundances of the products reduced by about 70%after the radical quencher was added,whereas isoxazole-ring opening and double-bond addition processes mainly depended on direct oxidation,which was unaffected by the quencher.NOM mainly affected the degradation of micropollutants by consuming•OH rather than O_(3)molecules,resulting in the 63%–85%decrease in indirect oxidation products.The NOM in the effluent were also degraded simultaneously during ozonation,and the components with larger aromaticity were more likely degraded through direct oxidation.The dependences of the three main components of NOM in the effluent on indirect oxidation followed the sequence:humic-like substances>fluvic-like substance-s>protein-like substances.This study reveals the ozonation mechanism of SMX in secondary effluent and provides a theoretical basis for the control of SMX and its degradation products in actual water treatment.
基金supported by the Open Research Fund Program of State Environmental Protection Key Laboratory of Food Chain Pollution Control (No. FC_(2)021YB05)the Opening Fund of State Key Laboratory of Heavy Oil Processing (No. SKLOP202002001)+1 种基金Fundamental Research Funds for the Central Universities (No. FRF-IDRY-20-004)National Natural Science Foundation of China (No. U20A20130)。
文摘As the main contributor of the formation of particulate matter as well as ozone, volatile organic compounds(VOCs) greatly affect human health and the environmental quality. Catalytic combustion/oxidation has been viewed as an efficient, economically feasible and environmentally friendly way for the elimination of VOCs. Supported metal catalyst is the preferred type of catalysts applied for VOCs catalytic combustion because of the synergy between active components and support as well as its flexibility in the composition. The presence of support not only plays the role of keeping the catalyst with good stability and mechanical strength, but also provides a large specific surface for the good dispersion of active components, which could effectively improve the performance of catalyst as well as decrease the usage of active components, especially the noble metal amount. Mesoporous molecular sieves, owing to their large surface area, unique porous structures, large pore size as well as uniform pore-size distribution, were viewed as superior support for dispersing active components. This review focuses on the recent development of mesoporous molecular sieve supported metal catalysts and their application in catalytic oxidation of VOCs. The effect of active component types, support structure, preparation method, precursors, etc. on the valence state, dispersion as well as the loading of active species were also discussed and summarized. Moreover, the corresponding conversion route of VOCs was also addressed.This review aims to provide some enlightment for designing the supported metal catalysts with superior activity and stability for VOCs removal.
基金financially supported by National Natural Science Foundation of China (No.U20A20130)Fundamental Research Funds for the Central Universities (No.06500152)
文摘Ce1-xZrxO_(2) composite oxides(molar,x=0-1.0,interval of 0.2)were prepared by a cetyltrimethylammonium bromide-assisted precipitation method.The enhancement of silver-species modification and catalytic mechanism of adsorption-transformationdesorption process were investigated over the Ag-impregnated catalysts for lowtemperature selective catalytic oxidation of ammonia(NH_(3)-SCO).The optimal 5 wt.%Ag/Ce_(0.6)Zr_(0.4)O_(2) catalyst presented good NH_(3)-SCO performancewith>90% NH_(3) conversion at temperature(T)≥250°C and 89% N_(2) selectivity.Despite the irregular block shape and underdeveloped specific surface area(∼60m2/g),the naked and Ag-modified Ce_(0.6)Zr_(0.4)O_(2) solid solution still obtained highly dispersed distribution of surface elements analyzed by scanning electron microscope-energy dispersive spectrometer(SEM-EDS)(mapping),N_(2) adsorptiondesorption test and X-ray diffraction(XRD).H2 temperature programmed reduction(H2-TPR)and X-ray photoelectron spectroscopy(XPS)results indicated that Ag-modification enhanced the mobility and activation of oxygen-species leading to a promotion on CeO_(2) reducibility and synergistic Ag0/Ag+and Ce^(4+)/Ce^(3+)redox cycles.Besides,Ag+/Ag_(2)O clusters could facilitate the formation of surface oxygen vacancies that was beneficial to the adsorption and activation of ammonia.NH3-temperature programmed desorption(NH_(3)-TPD)showed more adsorption-desorption capacity to ammoniawere provided by physical,weakandmedium-strong acid sites.Diffused reflectance infrared Fourier transform spectroscopy(DRIFTS)experiments revealed the activation of ammonia might be the control step of NH3-SCO procedure,during which NH3 dehydrogenation derived from NHx-species and also internal selective catalytic reduction(i-SCR)reactions were proposed.
基金financially supported by National Natural Science Foundation of China (Nos. 51808037 and 21876010)Fundamental Research Funds for the Central Universities, China (No. FRF-IDRY-20–018)+1 种基金China Postdoctoral Science Foundation (No. 2020M680903)Natural Science Foundation of Guangdong Province, China (No. 2020A1515011197)。
文摘Energy-saving and efficient monolithic catalysts are hotspots of catalytic purification of industrial gaseous pollutants.Here,we have developed an electrothermal catalytic mode,in which the ignition temperature required for the reaction is provided by Joule heat generated when the current flows through the catalyst.In this paper,Mn/NiAl/NF,Mn/NiFe/NF and Mn/NF metal-based monolithic catalysts were prepared using nickel foam (NF) as the carrier for thermal and electrothermal catalysis of n-heptane.The results indicated that Mn-based monolithic catalysts exhibit high activity in thermal and electrothermal catalysis.Mn/NiFe/NF achieve conversion of n-heptane more than 99%in electrothermal catalysis under a direct-current (DC) power of 6 W,and energy-saving is 54% compared with thermal catalysis.In addition,the results indicated that the introduction of NiAl (or NiFe) greatly enhanced the catalytic activity of Mn/NF,which attributed to the higher specific surface area,Mn3+/Mn4+,Ni3+/Ni^(2+),adsorbed oxygen species (Oads)/lattice oxygen species (Olatt),redox performance of the catalyst.Electrothermal catalytic activity was significantly higher than thermal catalytic activity before complete conversion,which may be related to electronic effects.Besides,Mn/NiFe/NF has good cyclic and long-term stability in electrothermal catalysis.This paper provided a theoretical basis for applying electrothermal catalysis in the field of VOCs elimination.
基金supported by the Program for New Century Excellent Talents in University(NCET-12-0776)the National Natural Science Foundation of China(21507004)the Fundamental Research Funds for the Central Universities(FRF-TP-15-046A1)
文摘This work was undertaken to investigate the behaviors and kinetics of toluene adsorption and desorption on activated carbons with varying pore structure. Five kinds of activated carbon from different raw materials were selected. Adsorption isotherms and breakthrough curves for toluene were measured. Langmuir and Freundlich equations were fitted to the equilibrium data, and the Freundlich equation was more suitable for simulating toluene adsorption. The process consisted of monolayer, multilayer and partial active site adsorption types. The effect of the pore structure of the activated carbons on toluene adsorption capacity was investigated. The quasi-first-order model was more suitable for describing the process than the quasi-second-order model. The adsorption data was also modeled by the internal particle diffusion model and it was found that the adsorption process could be divided into three stages. In the external surface adsorption process, the rate depended on the specific surface area. During the particle diffusion stage, pore structure and volume were the main factors affecting adsorption rate. In the final equilibrium stage, the rate was determined by the ratio of meso-and macro-pores to total pore volume. The rate over the whole adsorption process was dominated by the toluene concentration. The desorption behavior of toluene on activated carbons was investigated,and the process was divided into heat and mass transfer parts corresponding to emission and diffusion mechanisms, respectively. Physical adsorption played the main role during the adsorption process.
基金This work was financially supported by National Natural Science Foundation of China (Nos. 51808037, 21601136 and 21876010)the Science & Technology Development Fund of Tianjin Education Commission for Higher Education (No. 2018KJ126)the Fundamental Research Funds for the Central Universities (No. FRF-TP-16-060A1).
文摘Catalytic oxidation of toluene over noble metal catalysts is a representative reaction for elimination of volatile organic compounds(VOCs).However,to fully understand the activation of molecular oxygen and the role of active oxygen species generated in this reaction is still a challenging target.Herein,MgO nanosheets and single-atom Pt loaded MgO(Pt SA/MgO)nanosheets were synthesized and used as catalysts in toluene oxidation.The activation process of molecular oxygen and oxidation performance on the two catalysts were contrastively investigated.The Pt SA/MgO exhibited significantly enhanced catalytic activity compared to MgO.The oxygen vacancies can be easily generated on the Pt SA/MgO surface,which facilitate the activation of molecular oxygen and the formation of active oxygen species.Based on the experimental data and theoretical calculations,an active oxygen species promoted oxidation mechanism for toluene was proposed.In the presence of H2O,the molecular oxygen is more favorable to be dissociated to generate•OH on the oxygen vacancies of the Pt SA/MgO surface,which is the dominant active oxygen species.We anticipate that this work may shed light on further investigation of t10.1007/s12274-020-2765-1he oxidation mechanism of toluene and other VOCs over noble metal catalysts.
基金financially supported by the National Key R&D Program of China (No.2017YFC0210303)National Natural Science Foundation of China (Nos.21806009 and 21677010)+1 种基金China Postdoctoral Science Foundation (Nos.2019T120049 and 2018M631344)Fundamental Research Funds for the Central Universities (No.FRF-TP-18-019A1).
文摘Mn-Ni oxides with different compositions were prepared using standard co-precipitation(CP) and urea hydrolysis-precipitation(UH) methods and optimized for the selective catalytic reduction of nitrogen oxides(NOx) by NH3 at low temperature.Mn((2))Ni(1)Ox-CP and Mn(2)Ni(1)Ox-UH(with Mn:Ni molar ratio of 2:1) catalysts showed almost identical selective catalytic reduction(SCR) catalytic activity,with about 96% NOx conversion at 750 C and-99%in the temperature range from 100 to 250℃.X-ray diffraction(XRD) results showed that Mn(2)Ni(1)Ox-CP and Mn(2)Ni(1)Ox-UH catalysts crystallized in the form of Mn2NiO4 and MnO2-Mn2NiO4 spinel,respectively.The latter gave relatively good selectivity to N2,which might be due to the presence of the MnO2 phase and high metal-O binding energy,resulting in low dehydrogenation ability.According to the results of various characterization methods,it was found that a high density of surface chemisorbed oxygen species and efficient electron transfer between Mn and Ni in the crystal structure of Mn2NiO4 spinel played important roles in the high-efficiency SCR activity of these catalysts.Mn(2)Ni(1)Ox catalysts presented good resistance to H2O or/and SO2 with stable activity,which benefited from the Mn2NiO4 spinel structure and Eley-Rideal mechanism,with only slight effects from SO2.
基金financially supported by National Natural Science Foundation of China (Nos. U20A20130, 21806009)China Postdoctoral Science Foundation (2019T120049)Fundamental Research Funds for the Central Universities (No. 06500152).
文摘NH_(3)-SCR performances were explored to the relationship between structure morphology and physio-chemical properties over low-dimensional ternary Mn-based catalysts prepared by one-step synthesis method.Due to its strong oxidation performance,Sn-MnO_(x) was prone to side reactions between NO,NH_(3)and O_(2),resulting in the generation of more NO_(2)and N_(2)O,here most of N_(2)O was driven from the non-selective oxidation of NH_(3),while a small part generated from the side reaction between NH_(3)and NO_(2).Co or Ni doping into Sn-MnO_(x) as solid solution components obviously stronged the electronic interaction for actively mobilization and weakened the oxidation performance for signally reducing the selective tendency of side reactions to N_(2)O.The optimal modification resulted in improving the surface area and enhancing the strong interaction between polyvalent cations in Co/Ni-Mn-SnO_(2)to provide more surface adsorbed oxygen,active sites of Mn^(3+) and Mn^(4+),high-content Sn^(4+) and plentiful Lewis-acidity for more active intermediates,which significantly broadened the activity window of Sn-MnOx,improved the N^(2) selectivity by inhibiting N_(2)O formation,and also contributed to an acceptable resistances to water and sulfur.At low reaction temperatures,the SCR reactions over three catalysts mainly obeyed the typical Elye-rideal(E-R)routs via the reactions of adsorbed L-NH_(x)(x=3,2,1)and B-NH_(4)^(+) with the gaseous NO to generate N_(2) but also N_(2)O by-products.Except for the above basic E-R reactions,as increasing the reaction temperature,the main adsorbed NO_(x)-species were bidentate nitrates that were also active in the Langmuir-Hinshelwood reactions with adsorbed L-NH_(x) species over Co/Ni modified Mn-SnO_(2) catalyst.
基金Project supported by the National Key R&D Program of China(2017YFC0210303)National Natural Science Foundation of China(21806009)+1 种基金China Postdoctoral Science Foundation(2019T120049)Fundamental Research Funds for the Central Universities(06500152,FRF-TP-18-019A1)。
文摘This study explored the superior citrate method(CM)to synthesize Mn-Ce bi-oxides on 3 D monolithic Ni-foam(NF)catalysts for the selective catalytic reduction of NO by NH_(3)(NH_(3)-SCR).The 17 wt%Mn(7)Ce(3)O_(x)/NF(CM-17)catalyst shows the NO_(x)conversion of 98.7%at 175℃and 90%in the presence of 10 vol%H2 O.It is revealed that the combination of surface-active oxygen(formed by high-level oxygen vacancies)and strongly oxidized Mn4+species promots the Fast-SCR reactions,in which Mn4+species play a leading role in NH_(3)-SCR reaction,and the unsaturated Ni atoms and also Ce3+species promote electron exchange and thus improve the redox performance.The coexistence mechanisms of Fast-SCR reactions and E-R pathways are observed over Mn-CeO_(x)/NF catalyst,which may be promoted by the Br?nsted sites at low temperature.In addition,the heat resistance,stability,3 D monolithic porous structure and excellent physical properties of foam nickel provide a unique growth substrates for catalysts preparation and reaction sites for NO_(x)purification.Therefore,industrial application of Mn-Ce bioxides loaded on 3 D monolithic is proposed to be achieved through reasonable preparation methods.
基金financially supported by the National Key R&D Program of China(No.2017YFC0210303)the National Natural Science Foundation of China(Nos.21806009,21677010)+1 种基金the China Postdoctoral Science Foundation(No.2018M631344)。
文摘Cu-Co multiple-oxides modified on HNO_3-pretreated activated coke(AC_(N))were optimized for the simultaneous removal of gaseous CO and elemental mercury(Hg^(0))at low temperature(<200℃).It was found that 2%CuOx-10%CoOx/AC_(N)catalyst calcined at 400℃resulted in the coexistence of complex oxides including CuO,Cu_2 O,Co_(3)O_(4,Co_(2)O_(3)and CoO phases,which might be good for the simultaneous catalytic oxidation of CO by Co-species and removal of Hg^(0)by Cu-species,benefiting from the synergistic catalysis during the electrointeraction between Go and Cu cations(CoO■Co_(3)O_(4)and Cu_(2)O■CuO).The catalysis removal of CO oxidation was obviously depended on the reaction temperature obtaining94.7%at 200℃,while no obvious promoting effect on the Hg^(0)removal(68.3%-78.7%).These materials were very substitute for the removal of CO and Hg^(0)from the flue gas with the conditions of 8-20 vol.%O_(2)and flue-gas temperature below 200℃.The removal of Hg^(0)followed the combination processes of adsorption and catalytic oxidation reaction via LangmuirHinshelwood mechanism,while the catalysis of CO abided by the Mars-van Krevelen mechanism with lattice oxygen species.