Nitrate renoxification significantly influences atmospheric nitrogen cycling and global OH budgets.Although numerous nitrite acid(HONO)formation pathways from nitrate photolysis have been widely reported,the influence...Nitrate renoxification significantly influences atmospheric nitrogen cycling and global OH budgets.Although numerous nitrite acid(HONO)formation pathways from nitrate photolysis have been widely reported,the influence of various environmental factors and aerosol properties on reactive nitrogen production remains largely unclear.In this work,we employed NaNO_(3)/humic acid(HA)as a model nitrate photosensitization system to investigate the crucial roles of aerosol acidity,organic fraction,and dissolved oxygen in the production of HONO,NO_(2),and NO_(2)^(-).The presence of HA at 10 mg/L resulted in a remarkable increase in HONO production rates by approximately 2–3 times and NO_(2)^(-) concentration by 3–6 times across a pH range of 5.2 to 2.0.Meanwhile,the molar fraction of gaseous HONO in total N(Ⅲ)production increased from4%to 69%as bulk-phase pH decreased from 5.2 to 2.0.The higher organic fraction(i.e.,20 and 50 mg/L HA concentration)instead inhibited HONO and NO_(2) release.The presence of dissolved oxygen was found to be adverse for reactive nitrogen production.This suggests that the HA photosensitizer promoted the secondary conversion of NO_(2) to HONO mainly via reduced ketyl radical intermediates,while superoxide radical formation might exert a negative effect.Our findings provide comprehensive insights into reactive nitrogen production from photosensitized nitrate photolysis mediated by various external and internal factors,potentially accounting for discrepancies between field observations and model simulations.展开更多
Constructing new Brönsted acid sites within zeolitic materials holds paramount importance for the advancement of solid-acid catalysis.Zeo-type germanosilicates,a class of metallosilicates with a neutral framework...Constructing new Brönsted acid sites within zeolitic materials holds paramount importance for the advancement of solid-acid catalysis.Zeo-type germanosilicates,a class of metallosilicates with a neutral framework composed of tetravalent Ge and Si oxygen tetrahedrons,are conventionally considered not to generate Brönsted acid sites.Herein,we disclose an abnormal phenomenon with Ge-rich IWW-type germanosilicate(IWW-A)as an example that Ge-enriched germanosilicates are featured by mild Brönsted acidity.Using the art-of-state density functional theory calculation,19F magic angle spinning nuclear magnetic resonance,microcalorimetric and ammonia infrared mass spectrometry-temperature-programmed desorption characterizations,the nature of germanosilicate's Brönsted acidity has been demonstrated to be closely related to the neighboring framework Ge-hydroxyl pairs.Besides,the contribution of Ge-OH groups to Brönsted acidity and the role of Ge-pair structure for maintaining mild acid strength have been elucidated.In catalytic cracking of n-hexane and methanol-to-olefins reaction,the IWW-A germanosilicate exhibit high light olefins selectivity,good recyclability and low carbon deposition,outperforming the benchmark zeolite catalyst,ZSM-5 aluminosilicate.展开更多
Thermodynamic modeling is still themostwidely usedmethod to characterize aerosol acidity,a critical physicochemical property of atmospheric aerosols.However,it remains unclear whether gas-aerosol partitioning should b...Thermodynamic modeling is still themostwidely usedmethod to characterize aerosol acidity,a critical physicochemical property of atmospheric aerosols.However,it remains unclear whether gas-aerosol partitioning should be incorporated when thermodynamicmodels are employed to estimate the acidity of coarse particles.In this work,field measurements were conducted at a coastal city in northern China across three seasons,and covered wide ranges of temperature,relative humidity and NH_(3) concentrations.We examined the performance of different modes of ISORROPIA-II(a widely used aerosol thermodynamic model)in estimating aerosol acidity of coarse and fine particles.The M0 mode,which incorporates gas-phase data and runs the model in the forward mode,provided reasonable estimation of aerosol acidity for coarse and fine particles.Compared to M0,the M1 mode,which runs the model in the forward mode but does not include gas-phase data,may capture the general trend of aerosol acidity but underestimates pH for both coarse and fine particles;M2,which runs the model in the reverse mode,results in large errors in estimated aerosol pH for both coarse and fine particles and should not be used for aerosol acidity calculations.However,M1 significantly underestimates liquid water contents for both fine and coarse particles,while M2 provides reliable estimation of liquid water contents.In summary,our work highlights the importance of incorporating gas-aerosol partitioning when estimating coarse particle acidity,and thus may help improve our understanding of acidity of coarse particles.展开更多
Due to the presence of nitrogen,nitrogen-containing volatile organic compounds(NVOCs) are more difficult to remove than conventional volatile organic compounds(VOCs).Both catalytic activity and N_(2)selectivity should...Due to the presence of nitrogen,nitrogen-containing volatile organic compounds(NVOCs) are more difficult to remove than conventional volatile organic compounds(VOCs).Both catalytic activity and N_(2)selectivity should be considered in the design of suitable catalysts.A series of Ag/Ce-Zr solid solution(Ag/CZ)catalysts were prepared and applied to the catalytic oxidation of N,N-dimethylformamide(DMF).Redox ability and acidity were regulated by modifying the Zr content.The introduction of Zr promoted the formation of active oxygen species until the molar ratio of Zr reached 0.5,after which the formation decreased.Moreover,adding Zr increased the number of weak and medium acidic sites,which significantly improved DMF adsorption.The improved DMF adsorption hindered the combination of nitrogen and active oxygen,thus reducing the generation of NO_(x)effectively.Therefore,the Ag/CZ(5:5) catalyst,with suitable redox ability and acidity,exhibited the highest activity(T_(90)=176℃),the lowest elimination temperature of organic compounds(T=255℃),satisfactory N_(2)yield(95%-75% in the range of 240-400℃),and outstanding stability under both common and humid conditions(at least50 h).The reaction mechanism was investigated based on the in situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS) results.During the catalytic oxidation of DMF,the surface lattice oxygen directly participated in the dehydrogenation and dissociation of the C(O)-N bonds.The generated dimethylamine(DMA) was then oxidized by active oxygen species to form the final product.展开更多
Based on the criteria for additional surface acidity generation in composite oxides and composite fluorides proposed by Tanabe and Kemnitz et al.A hypothesis for the origin of additional surface acidity in solid compo...Based on the criteria for additional surface acidity generation in composite oxides and composite fluorides proposed by Tanabe and Kemnitz et al.A hypothesis for the origin of additional surface acidity in solid composites with the same metal cations is proposed.The surface acidsites of We analyze three types of solid composite systems,that is,CrF_(3)/Cr_(2)O_(3),MgF_(2)/MgO,and ZnF_(2)/ZnO,is systematically analyzed,which agrees with experimental results.Accordingly,the origin of additional surface acidity in these solid composites is reasonably explained,and the types of acidic sites are also predicted.展开更多
The necessity to saline and sodic waters is sometimes used for irrigating agricultural activities under certain circumstances, but it is important to note that the use of these waters comes with specific consideration...The necessity to saline and sodic waters is sometimes used for irrigating agricultural activities under certain circumstances, but it is important to note that the use of these waters comes with specific considerations and limitations. One way to decrease undesirable effects of sodic waters on the physical and chemical properties of soils is to apply organic and chemical amendments within the soil. This study aimed to assess the effectiveness of saline water on soil acidity, alkalinity and nutrients leaching in sandy loamy soil at Bella flower farm, in Rwamagana District, Rwanda. The water used was from the Muhazi Lake which is classified as Class I (Saline water quality). Column leaching experiments using treated soils were then conducted under saturated conditions. The soil under experimental was first analyzed for its textural classification, soil properties and is classified as sandy loamy soil. The t-test was taken at 1%, 5% and 10% levels of statistical significance compared to control soil. The results indicated that the application of saline water to soils caused an increase in some soil nutrients like increase of Phosphorus (P), Potassium (K<sup>+</sup>), Magnesium (Mg2<sup>+</sup>), Sulphur (S), CN ratio and Sodium (Na<sup>+</sup>) and decreased soil texture, physical and chemical properties and remained soil nutrients. Consequently, the intensive addition of saline water leachates to soil in PVC pipes led to decreased of soil EC through leaching and a raiser Soluble Sodium Percentage (SSP). The rate of saline water application affected the increase accumulation of SAR and Na% in the top soil layers. The study indicated that saline water is an inefficient amendment for sandy soil with saline water irrigation. The study recommends further studies with similar topic with saline water irrigation, as it accentuated the alkalinity levels.展开更多
Gas adsorption remains an attractive area of research.The hierarchical structure can reduce diffusion limitations and facilitate molecular transport,while acid sites can be used as adsorption sites.These make zeolites...Gas adsorption remains an attractive area of research.The hierarchical structure can reduce diffusion limitations and facilitate molecular transport,while acid sites can be used as adsorption sites.These make zeolites widely used in the field of gas adsorption.How to obtain zeolite adsorbents with better adsorption properties by modulating the hierarchical structure and acid sites is a pressing issue nowadays.This review highlights the strategies to modulate the hierarchical structure as well as the acid sites;and then explains how these strategies are achieved.The mechanism of zeolite adsorption on gases is then described in terms of these two properties.Lastly,the adsorption properties of zeolites for certain gases under specific conditions are summarised.An outlook of zeolite hierarchical structures and acid site modulation strategies is given.展开更多
Pt-HSiW/CeO_(2) catalysts were prepared for chlorobenzene(CB) catalytic combustion by hydrothermal method at different calcination temperatures,and the effects of the surface acidity and chemical valence on the cataly...Pt-HSiW/CeO_(2) catalysts were prepared for chlorobenzene(CB) catalytic combustion by hydrothermal method at different calcination temperatures,and the effects of the surface acidity and chemical valence on the catalytic activity were investigated.The results show that the catalyst calcined at 450℃(Cat-B)exhibits the outstanding catalytic performance,and the Cat-B catalyst possesses 90% conversion of CB at148℃.The excellent catalytic activity of Cat-B is attributed to more Ce^(3+)/(Ce^(3+)+Ce^(4+)),Pt~0/(Pt^(0)+Pt^(2+)),O_(ads)/(O_(latt)+O_(ads)) and Lewis acid sites.The degradation mechanism is proposed based on the analysis of the intermediates with the following reaction pathway:chlorobenzene→phenates/benzoquinone→acetate→maleate→CO_(2)+H_(2)O.展开更多
The acidity characteristics of acid sulphate soils of Kuttanad, Kerala, were studied in detail by collecting surface, profile and subsurface soil samples from 20 locations of six soil series viz., Ambalapuzha, Purakka...The acidity characteristics of acid sulphate soils of Kuttanad, Kerala, were studied in detail by collecting surface, profile and subsurface soil samples from 20 locations of six soil series viz., Ambalapuzha, Purakkad, Thotapally, Thuravur, Kallara and - Thakazhi that belonged to acid sulphate soils. The soils were extremely acidic showing a range of pH （H：O） varying from 2.5 to 5.2. Lowest pH was recorded by Thakazhi series and the highest by Thotapally. The potential acidity of soils ranged from 14.71 cmol.kg-1 to 110.5 cmol-kg1 with Thakazhi series showing the highest value. The contribution of hydrolytic acidity to potential acidity ranged from 70.2% to 97.2%. In all soil series, exchangeable A13＋ was greater than exchangeable H~. A significant correlation was observed among pH （KCI）, pH （H20） and pH （CaCI2） in all series.展开更多
An extremely acidified acid sulfate soil (ASS) was investigated to characterize its soluble and exchangeableacidity. The results showed that soluble acidity of a sample determined by titration with a KOH solutionwas m...An extremely acidified acid sulfate soil (ASS) was investigated to characterize its soluble and exchangeableacidity. The results showed that soluble acidity of a sample determined by titration with a KOH solutionwas much significantly greater than that indicated by pH measured using a PH meter, particularly for theextremely acidic soil samples. This is because the total soluble acidity of the extremely acidic soil sampleswas mainly composed of various soluble Al and Fe species, possibly in forms of Al sulfate complexes (e.g.,AISO4) and ferrous Fe (Fe2+). It is therefore suggested not to use pH alone as an indicator of soluble acidityin ASS, particularly for extremely acidic ASS. It is also likely that AISO4+ actively pericipated in cationexchange reactions. It appears that the possible involvement of this Al sulfate canon in the canon adsorptionhas significant effect on increasing the amount of acidity being adsorbed by the soils.展开更多
Extensive acidic soils,which suffer from accelerated soil acidification,are found in southern China.Soil acidity,aluminum toxicity,and nutrient deficiencies severely limited crop productivity in acidic soils.It has be...Extensive acidic soils,which suffer from accelerated soil acidification,are found in southern China.Soil acidity,aluminum toxicity,and nutrient deficiencies severely limited crop productivity in acidic soils.It has been widely reported that crop residue biochars can ameliorate acidic soils and increase crop productivity.Here,we summarized the positive effects and mechanisms involved in the correction of soil acidity,the alleviation of aluminum toxicity and the increase of soil pH buffering capacity by crop residue biochars.The carbonate,oxygen-containing functional groups and silicates in biochars are the major components responsible for their efficacy in amending acidic soils and resisting soil re-acidification.We conclude that application of crop residue biochars may be a better option than traditional liming to ameliorate acidic soils.Nonetheless,further researches into soil acidification are still required to address some issues that are controversial and poorly understood.展开更多
Direct catalytic propane dehydrogenation(PDH)to obtain propylene is a more economical and environmentally friendly route for propylene production.In particular,alumina-supported Cr2O3 catalysts can have better potenti...Direct catalytic propane dehydrogenation(PDH)to obtain propylene is a more economical and environmentally friendly route for propylene production.In particular,alumina-supported Cr2O3 catalysts can have better potential applications if the acidic properties could be tuned.Herein,a series of rod-shaped porous alumina were prepared through a hydrothermal route,followed by calcination.It was found that the acidity of the synthesized alumina was generally lower than that of the commercial alumina and could be adjusted well by varying the calcination temperature.Such alumina materials were used as supports for active Cr2O3,and the obtained catalysts could enhance the resistance to coke formation associated with similar activity in PDH reaction compared to the commercial alumina.The amount of coke deposited on a self-made catalyst(Cr-Al-800)was 3.6%,which was much lower than that deposited on the reference catalyst(15.7%).The lower acidity of the catalyst inhibited the side reactions and coke formation during the PDH process,which was beneficial for its high activity and superior anti-coking properties.展开更多
The effects of rare earth（RE）on the structure,acidity,and catalytic performance of HZSM-5 zeolite were investigated.A series of RE/HZSM-5 catalysts,containing 7.54% RE（RE=La,Ce,Pr,Nd,Sm,Eu or Gd）,were prepared by ...The effects of rare earth（RE）on the structure,acidity,and catalytic performance of HZSM-5 zeolite were investigated.A series of RE/HZSM-5 catalysts,containing 7.54% RE（RE=La,Ce,Pr,Nd,Sm,Eu or Gd）,were prepared by the impregnation of the ZSM-5 type zeolites（Si/Al=64：1）with the corresponding RE nitrate aqueous solutions.The catalysts were characterized by means of FT-IR,UV-Vis,NH3-TPD,and IR spectroscopy of adsorbed pyridine.The catalytic performances of the RE/HZSM-5 for the catalytic cracking of mixed butane to light olefins were also measured with a fixed bed microreactor.The results revealed that the addition of light rare earth metal on the HZSM-5 catalyst greatly enhanced the selectivity to olefins,especially to propylene,thus increasing the total yield of olefins in the catalytic cracking of butane.Among the RE-modified HZSM-5 samples,Ce/HZSM-5 gave the highest yield of total olefins,and Nd/HZSM-5 gave the highest yield of propene at a reaction temperature of 600℃.The presence of rare earth metal on the HZSM-5 sample,not only modified the acidic properties of HZSM-5 including the amount of acid sites and acid type,that is,the ratio of L/B（Lewis acid/Brnsted acid）,but also altered the basic properties of it,which in turn promoted the catalytic performance of HZSM-5 for the catalytic cracking of butane.展开更多
The coking kinetics and reaction-regeneration on Zn/HZSM-5 （Zn/HZ） catalyst in the conversion of methanol to aromatics were investigated. The highest initial benzene, toluene and xylene （BTX） yield of ca. 67.7% wa...The coking kinetics and reaction-regeneration on Zn/HZSM-5 （Zn/HZ） catalyst in the conversion of methanol to aromatics were investigated. The highest initial benzene, toluene and xylene （BTX） yield of ca. 67.7% was obtained on fresh Zn/HZ catalyst, which showed the worst catalytic stability. The cycle of reaction-regeneration significantly modified the texture and acidity of Zn/HZ catalyst, which in turn affected its catalytic performance and coking behavior in methanol conversion to BTX. The residual carbon located on the surface of Zn/HZ catalyst led to the decrease of acid sites and the change on the acid sites distribution, which played an important roles on its activity and deactivation. It was found that the high B/L ratio and the low total acid sites concentration of the Zn/HZ catalyst favored to the high BTX yield and good catalytic stability in methanol conversion.展开更多
Among the reactions catalyzed by zeolites there are some that exhibit high selectivity due to the spatial confinement effect of the zeolite framework.Tailoring the acidity,particularly the distribution and location of...Among the reactions catalyzed by zeolites there are some that exhibit high selectivity due to the spatial confinement effect of the zeolite framework.Tailoring the acidity,particularly the distribution and location of the Bronsted acid sites in the zeolite is effective for making it a better catalyst for these reactions.We prepared a series of H-mordenite（H-MOR） samples by varying the composition of the sol-gel,using different structure directing agents and post-treatment.NH3-TPD and IR characterization of adsorbed pyridine were employed to determine the amount of Bronsted acid sites in the 8-membered ring and 12-membered ring channels.It was shown that controlled synthesis was a promising approach to improve the concentration of Bronsted acid sites in MOR,even with a low Al content.Using an appropriate composition of Si and Al in the sol-gel favored a higher proportion of Bronsted acid sites in the 8-membered ring channels.HMI as a structure-direct agent gave an obvious enrichment of Bronsted acid sites in the 8-membered ring.Carbonylation of dimethyl ether was used as a probe reaction to examine the modification of the acid properties,especially the Bronsted acid sites in the 8-membered ring channels.There was a linear relationship between methyl acetate formation and the number of Bronsted acid sites in the 8-membered ring channels,demonstrating the successful modification of acid properties.Our results provide information for the rational design and modification of zeolites with spatial constraints.展开更多
A 45-day greenhouse experiment was carried out to determine effect of vesicular-arbuscular (VA) mycorrhizal fungi on colonization rate, plant height, plant growth, hyphae length, total Al in the plants, exchangeable A...A 45-day greenhouse experiment was carried out to determine effect of vesicular-arbuscular (VA) mycorrhizal fungi on colonization rate, plant height, plant growth, hyphae length, total Al in the plants, exchangeable Al in the soil and soil pH by comparison at soil pH 3.5, 4.5 and 6.0. Plant mung bean (Phaseolus radiatus L.) and crotalaria (Crotalaria mucronata Desv.) were grown with and without VA mycorrhizal fungi in pots with red soil. Ten VA mycorrhizal fungi strains were tested, including Glomus epigaeum (No. 90001), Glomus caledonium (No. 90036), Glomus mosseae (No. 90107), Acaulospora spp. (No. 34), Scutellospora heterogama (No. 36), Scutellospora calospora (No. 37), Glomus manihotis (No. 38), Gigaspora spp. (No. 47), Glomus manihotis (No. 49), and Acaulospora spp. (No. 53). Being the most tolerant to acidity, strain 34 and strain 38 showed quicker and higher-rated colonization without lagging, three to four times more in number of nodules, two to four times more in plant dry weight, 30% to 60% more in hyphae length, lower soil exchangeable Al, and higher soil pH than without VA mycorrhizal fungi (CK). Other strains also could improve plant growth and enhance plant tolerance to acidity, but their effects were not marked. This indicated that VA mycorrhizal fungi differed in the tolerance to soil acidity and so did their inoculation effects. In the experiment, acidic soil could be remedied by inoculation of promising VA mycorrhizal fungi tolerant of acidity.展开更多
AIM: To search the independent factors determining gastric juice acidity and to investigate the acidity of gastric juices in various benign and malignant upper gastrointestinal diseases. METHODS: Fasting gastric juice...AIM: To search the independent factors determining gastric juice acidity and to investigate the acidity of gastric juices in various benign and malignant upper gastrointestinal diseases. METHODS: Fasting gastric juice acidity of 165 healthysubjects and 346 patients with esophageal ulcer (n = 21), gastric ulcer (n = 136), duodenal ulcer (n = 100) or gastric cancer (n = 89) were measured and compared. Additionally, gastric specimens were taken from the antrum and body for rapid urease test and histological examination. RESULTS: Multivariate analysis revealed that bile stain of gastric juice, high acute inflammatory score of the corpus, and atrophy of the corpus were independent risk factors for the development of gastric hypoacidity with odds ratios of 3.1 (95% CI: 1.3-7.3), 3.1 (95% CI: 1.2-7.9) and 3.5 (95% CI: 1.3-9.2). Esophageal ulcer and duodenal ulcer patients had a lower pH level (1.9 and 2.1 vs 2.9, both P < 0.05) of gastric juices than healthy subjects. In contrast, gastric ulcer and gastric cancer patients had a higher pH level (3.4 and 6.6 vs 2.9, both P < 0.001) than healthy controls. Hypoacidity existed in 22%, 5%, 29%, 5% and 88% of healthy subjects, esophageal ulcer, gastric ulcer, duodenal ulcer and gastric cancer patients, respectively. CONCLUSION: Bile reflux, atrophy and dense neutrophil infiltrate of the corpus are three independent factors determining the acidity of gastric juice.展开更多
Strongly acidic soils （pH 〈 5.0） are detrimental to tea （Camellia sinensis） production and quality. Little information exists on the ability of surface amendments to ameliorate subsoil acidity in the tea garden s...Strongly acidic soils （pH 〈 5.0） are detrimental to tea （Camellia sinensis） production and quality. Little information exists on the ability of surface amendments to ameliorate subsoil acidity in the tea garden soils. A 120-d glasshouse column leaching experiment was conducted using commonly available soil ameliorants. Alkaline slag （AS） and organic residues, pig manure （PM） and rapeseed cake （RC） differing in ash alkalinity and C/N ratio were incorporated alone and in combination into the surface （0-15 cm） of soil columns （10 cm internal diameter x 50 cm long） packed with soil from the acidic soil layer （15-30 cm） of an Ultisol （initial pH -- 4.4）. During the 120-d experiment, the soil columns were watered （about 127 mm over 9 applications） according to the long-term mean annual rainfall （1 143 mm） and the leachates were collected and analyzed. At the end of the experiment, soil columns were partitioned into various depths and the chemical properties of soil were measured. The PM with a higher C/N ratio increased subsoil pH, whereas the RC with a lower C/N ratio decreased subsoil pH. However, combined amendments had a greater ability to reduce subsoil acidity than either of the amendments alone. The increases in pH of the subsoil were mainly ascribed to decreased base cation concentrations and the decomposition of organic anions present in dissolved organic carbon （DOC） and immobilization of nitrate that had been leached down from the amended layer. A significant （P 〈 0.05） correlation between alkalinity production （reduced exchangeable acidity - N-cycle alkalinity） and alkalinity balance （net alkalinity production - N-cycle alkalinity） was observed at the end of the experiment. Additionally, combined amendments significantly increased （P ~ 0.05） subsoil cation concentrations and decreased subsoil A1 saturation （P 〈 0.05）. Combined applications of AS with organic amendments to surface soils are effective in reducing subsoil acidity in high-rainfall areas. Further investigations under field conditions and over longer timeframes are needed to fully understand their practical effectiveness in ameliorating acidity of deeper soil layers under naturally occurring leaching regimes.展开更多
The surface acidity of synthetic amorphous AI hydroxide was determined by acid/base titration with several complementary methods including solution analyses of the reacted solutions and XRD characterization of the rea...The surface acidity of synthetic amorphous AI hydroxide was determined by acid/base titration with several complementary methods including solution analyses of the reacted solutions and XRD characterization of the reacted solids. The synthetic specimen was characterized to be the amorphous material showing four broad peaks in XRD pattern. XRD analyses of reacted solids after the titration experiments showed that amorphous AI hydroxide rapidly transformed to crystalline bayerite at the alkaline condition （pH〉10）. The solution analyses after and during the titration Ksp=^aAl^3＋/aH^＋^3 ,was 10^10.3. The amount of consumption of added acid or base during the titration experiment was attributed to both the protonation/deprotonation of dissolved AI species and surface hydroxyl group. The surface acidity constants, surface hydroxyl density and specific surface area were estimated by FITEQL 4.0.展开更多
The effect of acidity and redox capability over sulfuric acid-modified CeO_2 catalysts were studied for the selective catalytic reduction of NO_x with NH_3(NH_3-SCR). The deposition of sulfate significantly enhanced t...The effect of acidity and redox capability over sulfuric acid-modified CeO_2 catalysts were studied for the selective catalytic reduction of NO_x with NH_3(NH_3-SCR). The deposition of sulfate significantly enhanced the catalytic performance over CeO_2. NO_x conversion over4H_2SO_4/CeO_2 at 230–440 °C was higher than 90%. The strong redox capability of CeO_2 could result in unselective NH_3 oxidation and decrease high temperatures catalytic activity and N_2 selectivity. The deposition of sulfate increased the acidity and weakened the redox capability, and then increased the high temperature NO_x conversion and N_2 selectivity. An appropriate level of acidity also promoted the activity at 190–250 °C over ceria-based catalysts, and with further increase in the acidity, the SCR activity decreased slightly. Weak redox capability lowered the low-temperature catalytic activity. Excellent SCR activity requires a balance of acidity and redox capability on the catalysts.展开更多
基金supported by the National Key R&D Program of China(No.2022YFC3701102)the National Natural Science Foundation of China(Nos.22376029,22176038,91744205 and 21777025)the Natural Science Foundation of Shanghai City(No.22ZR1404700).
文摘Nitrate renoxification significantly influences atmospheric nitrogen cycling and global OH budgets.Although numerous nitrite acid(HONO)formation pathways from nitrate photolysis have been widely reported,the influence of various environmental factors and aerosol properties on reactive nitrogen production remains largely unclear.In this work,we employed NaNO_(3)/humic acid(HA)as a model nitrate photosensitization system to investigate the crucial roles of aerosol acidity,organic fraction,and dissolved oxygen in the production of HONO,NO_(2),and NO_(2)^(-).The presence of HA at 10 mg/L resulted in a remarkable increase in HONO production rates by approximately 2–3 times and NO_(2)^(-) concentration by 3–6 times across a pH range of 5.2 to 2.0.Meanwhile,the molar fraction of gaseous HONO in total N(Ⅲ)production increased from4%to 69%as bulk-phase pH decreased from 5.2 to 2.0.The higher organic fraction(i.e.,20 and 50 mg/L HA concentration)instead inhibited HONO and NO_(2) release.The presence of dissolved oxygen was found to be adverse for reactive nitrogen production.This suggests that the HA photosensitizer promoted the secondary conversion of NO_(2) to HONO mainly via reduced ketyl radical intermediates,while superoxide radical formation might exert a negative effect.Our findings provide comprehensive insights into reactive nitrogen production from photosensitized nitrate photolysis mediated by various external and internal factors,potentially accounting for discrepancies between field observations and model simulations.
文摘Constructing new Brönsted acid sites within zeolitic materials holds paramount importance for the advancement of solid-acid catalysis.Zeo-type germanosilicates,a class of metallosilicates with a neutral framework composed of tetravalent Ge and Si oxygen tetrahedrons,are conventionally considered not to generate Brönsted acid sites.Herein,we disclose an abnormal phenomenon with Ge-rich IWW-type germanosilicate(IWW-A)as an example that Ge-enriched germanosilicates are featured by mild Brönsted acidity.Using the art-of-state density functional theory calculation,19F magic angle spinning nuclear magnetic resonance,microcalorimetric and ammonia infrared mass spectrometry-temperature-programmed desorption characterizations,the nature of germanosilicate's Brönsted acidity has been demonstrated to be closely related to the neighboring framework Ge-hydroxyl pairs.Besides,the contribution of Ge-OH groups to Brönsted acidity and the role of Ge-pair structure for maintaining mild acid strength have been elucidated.In catalytic cracking of n-hexane and methanol-to-olefins reaction,the IWW-A germanosilicate exhibit high light olefins selectivity,good recyclability and low carbon deposition,outperforming the benchmark zeolite catalyst,ZSM-5 aluminosilicate.
基金supported by the National Natural Science Foundation of China (Nos.42022050 and 42277088)the Guangdong Basic and Applied Basic Research Fund Committee (Nos.2021A1515011248 and 2023A1515012010)the Guangdong Foundation for the Program of Science and Technology Research (No.2020B1212060053).
文摘Thermodynamic modeling is still themostwidely usedmethod to characterize aerosol acidity,a critical physicochemical property of atmospheric aerosols.However,it remains unclear whether gas-aerosol partitioning should be incorporated when thermodynamicmodels are employed to estimate the acidity of coarse particles.In this work,field measurements were conducted at a coastal city in northern China across three seasons,and covered wide ranges of temperature,relative humidity and NH_(3) concentrations.We examined the performance of different modes of ISORROPIA-II(a widely used aerosol thermodynamic model)in estimating aerosol acidity of coarse and fine particles.The M0 mode,which incorporates gas-phase data and runs the model in the forward mode,provided reasonable estimation of aerosol acidity for coarse and fine particles.Compared to M0,the M1 mode,which runs the model in the forward mode but does not include gas-phase data,may capture the general trend of aerosol acidity but underestimates pH for both coarse and fine particles;M2,which runs the model in the reverse mode,results in large errors in estimated aerosol pH for both coarse and fine particles and should not be used for aerosol acidity calculations.However,M1 significantly underestimates liquid water contents for both fine and coarse particles,while M2 provides reliable estimation of liquid water contents.In summary,our work highlights the importance of incorporating gas-aerosol partitioning when estimating coarse particle acidity,and thus may help improve our understanding of acidity of coarse particles.
基金financially supported by the Fundamental Research Funds for the Central UniversitiesNational Key Research and Development Program of China (Nos.2023YFA1508500,2023YFC3707500 and 2022YFB3504200)the National Natural Science Foundation of China (Nos.22106101 and U21A20326)。
文摘Due to the presence of nitrogen,nitrogen-containing volatile organic compounds(NVOCs) are more difficult to remove than conventional volatile organic compounds(VOCs).Both catalytic activity and N_(2)selectivity should be considered in the design of suitable catalysts.A series of Ag/Ce-Zr solid solution(Ag/CZ)catalysts were prepared and applied to the catalytic oxidation of N,N-dimethylformamide(DMF).Redox ability and acidity were regulated by modifying the Zr content.The introduction of Zr promoted the formation of active oxygen species until the molar ratio of Zr reached 0.5,after which the formation decreased.Moreover,adding Zr increased the number of weak and medium acidic sites,which significantly improved DMF adsorption.The improved DMF adsorption hindered the combination of nitrogen and active oxygen,thus reducing the generation of NO_(x)effectively.Therefore,the Ag/CZ(5:5) catalyst,with suitable redox ability and acidity,exhibited the highest activity(T_(90)=176℃),the lowest elimination temperature of organic compounds(T=255℃),satisfactory N_(2)yield(95%-75% in the range of 240-400℃),and outstanding stability under both common and humid conditions(at least50 h).The reaction mechanism was investigated based on the in situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS) results.During the catalytic oxidation of DMF,the surface lattice oxygen directly participated in the dehydrogenation and dissociation of the C(O)-N bonds.The generated dimethylamine(DMA) was then oxidized by active oxygen species to form the final product.
基金The Key Research and Development Program of Zhejiang Province(2021C01003)National Natural Science Foundation of China(52025011,51971202,51872260 and 52171019)The Zhejiang Provincial Natural Science Foundation of China(LD19B030001,Z4080070 and LR23B030004)。
文摘Based on the criteria for additional surface acidity generation in composite oxides and composite fluorides proposed by Tanabe and Kemnitz et al.A hypothesis for the origin of additional surface acidity in solid composites with the same metal cations is proposed.The surface acidsites of We analyze three types of solid composite systems,that is,CrF_(3)/Cr_(2)O_(3),MgF_(2)/MgO,and ZnF_(2)/ZnO,is systematically analyzed,which agrees with experimental results.Accordingly,the origin of additional surface acidity in these solid composites is reasonably explained,and the types of acidic sites are also predicted.
文摘The necessity to saline and sodic waters is sometimes used for irrigating agricultural activities under certain circumstances, but it is important to note that the use of these waters comes with specific considerations and limitations. One way to decrease undesirable effects of sodic waters on the physical and chemical properties of soils is to apply organic and chemical amendments within the soil. This study aimed to assess the effectiveness of saline water on soil acidity, alkalinity and nutrients leaching in sandy loamy soil at Bella flower farm, in Rwamagana District, Rwanda. The water used was from the Muhazi Lake which is classified as Class I (Saline water quality). Column leaching experiments using treated soils were then conducted under saturated conditions. The soil under experimental was first analyzed for its textural classification, soil properties and is classified as sandy loamy soil. The t-test was taken at 1%, 5% and 10% levels of statistical significance compared to control soil. The results indicated that the application of saline water to soils caused an increase in some soil nutrients like increase of Phosphorus (P), Potassium (K<sup>+</sup>), Magnesium (Mg2<sup>+</sup>), Sulphur (S), CN ratio and Sodium (Na<sup>+</sup>) and decreased soil texture, physical and chemical properties and remained soil nutrients. Consequently, the intensive addition of saline water leachates to soil in PVC pipes led to decreased of soil EC through leaching and a raiser Soluble Sodium Percentage (SSP). The rate of saline water application affected the increase accumulation of SAR and Na% in the top soil layers. The study indicated that saline water is an inefficient amendment for sandy soil with saline water irrigation. The study recommends further studies with similar topic with saline water irrigation, as it accentuated the alkalinity levels.
基金supported by“Shanghai Science and Technology Innovation Action Plan”-Baoshan Transformation Development Science and Technology Special Project (No.21SQBS01100)the National Natural Science Foundation of China (Nos.22276137 and52170087)。
文摘Gas adsorption remains an attractive area of research.The hierarchical structure can reduce diffusion limitations and facilitate molecular transport,while acid sites can be used as adsorption sites.These make zeolites widely used in the field of gas adsorption.How to obtain zeolite adsorbents with better adsorption properties by modulating the hierarchical structure and acid sites is a pressing issue nowadays.This review highlights the strategies to modulate the hierarchical structure as well as the acid sites;and then explains how these strategies are achieved.The mechanism of zeolite adsorption on gases is then described in terms of these two properties.Lastly,the adsorption properties of zeolites for certain gases under specific conditions are summarised.An outlook of zeolite hierarchical structures and acid site modulation strategies is given.
基金Project supported by the National Natural Science Foundation of China (21872096)Key Research and Development Project of Henan Province (231111320400)+3 种基金Zhongyuan Yingcai Jihua (ZYYCYU202012183)Academic Leader of Henan Institute of Urban Construction (YCJXSJSDTR202204)College Students'Innovation and Entrepreneurship Training Program of Henan Province(202211765053)Doctoral Research Start-up Project of Henan University of Urban Construction (990/Q2017011)。
文摘Pt-HSiW/CeO_(2) catalysts were prepared for chlorobenzene(CB) catalytic combustion by hydrothermal method at different calcination temperatures,and the effects of the surface acidity and chemical valence on the catalytic activity were investigated.The results show that the catalyst calcined at 450℃(Cat-B)exhibits the outstanding catalytic performance,and the Cat-B catalyst possesses 90% conversion of CB at148℃.The excellent catalytic activity of Cat-B is attributed to more Ce^(3+)/(Ce^(3+)+Ce^(4+)),Pt~0/(Pt^(0)+Pt^(2+)),O_(ads)/(O_(latt)+O_(ads)) and Lewis acid sites.The degradation mechanism is proposed based on the analysis of the intermediates with the following reaction pathway:chlorobenzene→phenates/benzoquinone→acetate→maleate→CO_(2)+H_(2)O.
文摘The acidity characteristics of acid sulphate soils of Kuttanad, Kerala, were studied in detail by collecting surface, profile and subsurface soil samples from 20 locations of six soil series viz., Ambalapuzha, Purakkad, Thotapally, Thuravur, Kallara and - Thakazhi that belonged to acid sulphate soils. The soils were extremely acidic showing a range of pH （H：O） varying from 2.5 to 5.2. Lowest pH was recorded by Thakazhi series and the highest by Thotapally. The potential acidity of soils ranged from 14.71 cmol.kg-1 to 110.5 cmol-kg1 with Thakazhi series showing the highest value. The contribution of hydrolytic acidity to potential acidity ranged from 70.2% to 97.2%. In all soil series, exchangeable A13＋ was greater than exchangeable H~. A significant correlation was observed among pH （KCI）, pH （H20） and pH （CaCI2） in all series.
文摘An extremely acidified acid sulfate soil (ASS) was investigated to characterize its soluble and exchangeableacidity. The results showed that soluble acidity of a sample determined by titration with a KOH solutionwas much significantly greater than that indicated by pH measured using a PH meter, particularly for theextremely acidic soil samples. This is because the total soluble acidity of the extremely acidic soil sampleswas mainly composed of various soluble Al and Fe species, possibly in forms of Al sulfate complexes (e.g.,AISO4) and ferrous Fe (Fe2+). It is therefore suggested not to use pH alone as an indicator of soluble acidityin ASS, particularly for extremely acidic ASS. It is also likely that AISO4+ actively pericipated in cationexchange reactions. It appears that the possible involvement of this Al sulfate canon in the canon adsorptionhas significant effect on increasing the amount of acidity being adsorbed by the soils.
基金funded by the National Key Research and Development of China(2016YFD0200302)the National Key Basic Research Program of China(2014CB441003)
文摘Extensive acidic soils,which suffer from accelerated soil acidification,are found in southern China.Soil acidity,aluminum toxicity,and nutrient deficiencies severely limited crop productivity in acidic soils.It has been widely reported that crop residue biochars can ameliorate acidic soils and increase crop productivity.Here,we summarized the positive effects and mechanisms involved in the correction of soil acidity,the alleviation of aluminum toxicity and the increase of soil pH buffering capacity by crop residue biochars.The carbonate,oxygen-containing functional groups and silicates in biochars are the major components responsible for their efficacy in amending acidic soils and resisting soil re-acidification.We conclude that application of crop residue biochars may be a better option than traditional liming to ameliorate acidic soils.Nonetheless,further researches into soil acidification are still required to address some issues that are controversial and poorly understood.
基金supported by the National Natural Science Foundation of China(21733002)Joint Sino-German Research Project(2161101168)Cheung Kong Scholars Program of China(T2015036)~~
文摘Direct catalytic propane dehydrogenation(PDH)to obtain propylene is a more economical and environmentally friendly route for propylene production.In particular,alumina-supported Cr2O3 catalysts can have better potential applications if the acidic properties could be tuned.Herein,a series of rod-shaped porous alumina were prepared through a hydrothermal route,followed by calcination.It was found that the acidity of the synthesized alumina was generally lower than that of the commercial alumina and could be adjusted well by varying the calcination temperature.Such alumina materials were used as supports for active Cr2O3,and the obtained catalysts could enhance the resistance to coke formation associated with similar activity in PDH reaction compared to the commercial alumina.The amount of coke deposited on a self-made catalyst(Cr-Al-800)was 3.6%,which was much lower than that deposited on the reference catalyst(15.7%).The lower acidity of the catalyst inhibited the side reactions and coke formation during the PDH process,which was beneficial for its high activity and superior anti-coking properties.
基金Project supported by the National Basic Research Program of China(2004CB2178062005CB221402)+1 种基金the National NaturalScience Foundation of China(20373043)Young Scientists Innovation Foundation of CNPC(04E7025)
文摘The effects of rare earth（RE）on the structure,acidity,and catalytic performance of HZSM-5 zeolite were investigated.A series of RE/HZSM-5 catalysts,containing 7.54% RE（RE=La,Ce,Pr,Nd,Sm,Eu or Gd）,were prepared by the impregnation of the ZSM-5 type zeolites（Si/Al=64：1）with the corresponding RE nitrate aqueous solutions.The catalysts were characterized by means of FT-IR,UV-Vis,NH3-TPD,and IR spectroscopy of adsorbed pyridine.The catalytic performances of the RE/HZSM-5 for the catalytic cracking of mixed butane to light olefins were also measured with a fixed bed microreactor.The results revealed that the addition of light rare earth metal on the HZSM-5 catalyst greatly enhanced the selectivity to olefins,especially to propylene,thus increasing the total yield of olefins in the catalytic cracking of butane.Among the RE-modified HZSM-5 samples,Ce/HZSM-5 gave the highest yield of total olefins,and Nd/HZSM-5 gave the highest yield of propene at a reaction temperature of 600℃.The presence of rare earth metal on the HZSM-5 sample,not only modified the acidic properties of HZSM-5 including the amount of acid sites and acid type,that is,the ratio of L/B（Lewis acid/Brnsted acid）,but also altered the basic properties of it,which in turn promoted the catalytic performance of HZSM-5 for the catalytic cracking of butane.
基金supported by the National Ministry of Education(NCET-10-878)Shaanxi"13115"Innovation Project(2009ZDKJ-70)Shaanxi Key Innovation Project(2011ZKC4-08)
文摘The coking kinetics and reaction-regeneration on Zn/HZSM-5 （Zn/HZ） catalyst in the conversion of methanol to aromatics were investigated. The highest initial benzene, toluene and xylene （BTX） yield of ca. 67.7% was obtained on fresh Zn/HZ catalyst, which showed the worst catalytic stability. The cycle of reaction-regeneration significantly modified the texture and acidity of Zn/HZ catalyst, which in turn affected its catalytic performance and coking behavior in methanol conversion to BTX. The residual carbon located on the surface of Zn/HZ catalyst led to the decrease of acid sites and the change on the acid sites distribution, which played an important roles on its activity and deactivation. It was found that the high B/L ratio and the low total acid sites concentration of the Zn/HZ catalyst favored to the high BTX yield and good catalytic stability in methanol conversion.
基金supported by the National Natural Science Foundation of China(21325626,21406120)the Postdoctoral Science Foundation of China(2014M560181,2015T80214)~~
文摘Among the reactions catalyzed by zeolites there are some that exhibit high selectivity due to the spatial confinement effect of the zeolite framework.Tailoring the acidity,particularly the distribution and location of the Bronsted acid sites in the zeolite is effective for making it a better catalyst for these reactions.We prepared a series of H-mordenite（H-MOR） samples by varying the composition of the sol-gel,using different structure directing agents and post-treatment.NH3-TPD and IR characterization of adsorbed pyridine were employed to determine the amount of Bronsted acid sites in the 8-membered ring and 12-membered ring channels.It was shown that controlled synthesis was a promising approach to improve the concentration of Bronsted acid sites in MOR,even with a low Al content.Using an appropriate composition of Si and Al in the sol-gel favored a higher proportion of Bronsted acid sites in the 8-membered ring channels.HMI as a structure-direct agent gave an obvious enrichment of Bronsted acid sites in the 8-membered ring.Carbonylation of dimethyl ether was used as a probe reaction to examine the modification of the acid properties,especially the Bronsted acid sites in the 8-membered ring channels.There was a linear relationship between methyl acetate formation and the number of Bronsted acid sites in the 8-membered ring channels,demonstrating the successful modification of acid properties.Our results provide information for the rational design and modification of zeolites with spatial constraints.
基金Project (No. G1999011807) supported by the National Key Basic Research and Development Programme of China
文摘A 45-day greenhouse experiment was carried out to determine effect of vesicular-arbuscular (VA) mycorrhizal fungi on colonization rate, plant height, plant growth, hyphae length, total Al in the plants, exchangeable Al in the soil and soil pH by comparison at soil pH 3.5, 4.5 and 6.0. Plant mung bean (Phaseolus radiatus L.) and crotalaria (Crotalaria mucronata Desv.) were grown with and without VA mycorrhizal fungi in pots with red soil. Ten VA mycorrhizal fungi strains were tested, including Glomus epigaeum (No. 90001), Glomus caledonium (No. 90036), Glomus mosseae (No. 90107), Acaulospora spp. (No. 34), Scutellospora heterogama (No. 36), Scutellospora calospora (No. 37), Glomus manihotis (No. 38), Gigaspora spp. (No. 47), Glomus manihotis (No. 49), and Acaulospora spp. (No. 53). Being the most tolerant to acidity, strain 34 and strain 38 showed quicker and higher-rated colonization without lagging, three to four times more in number of nodules, two to four times more in plant dry weight, 30% to 60% more in hyphae length, lower soil exchangeable Al, and higher soil pH than without VA mycorrhizal fungi (CK). Other strains also could improve plant growth and enhance plant tolerance to acidity, but their effects were not marked. This indicated that VA mycorrhizal fungi differed in the tolerance to soil acidity and so did their inoculation effects. In the experiment, acidic soil could be remedied by inoculation of promising VA mycorrhizal fungi tolerant of acidity.
基金Supported by Research grant NSC-96-2314-B-075B-009 from the National Science Council, Taiwan
文摘AIM: To search the independent factors determining gastric juice acidity and to investigate the acidity of gastric juices in various benign and malignant upper gastrointestinal diseases. METHODS: Fasting gastric juice acidity of 165 healthysubjects and 346 patients with esophageal ulcer (n = 21), gastric ulcer (n = 136), duodenal ulcer (n = 100) or gastric cancer (n = 89) were measured and compared. Additionally, gastric specimens were taken from the antrum and body for rapid urease test and histological examination. RESULTS: Multivariate analysis revealed that bile stain of gastric juice, high acute inflammatory score of the corpus, and atrophy of the corpus were independent risk factors for the development of gastric hypoacidity with odds ratios of 3.1 (95% CI: 1.3-7.3), 3.1 (95% CI: 1.2-7.9) and 3.5 (95% CI: 1.3-9.2). Esophageal ulcer and duodenal ulcer patients had a lower pH level (1.9 and 2.1 vs 2.9, both P < 0.05) of gastric juices than healthy subjects. In contrast, gastric ulcer and gastric cancer patients had a higher pH level (3.4 and 6.6 vs 2.9, both P < 0.001) than healthy controls. Hypoacidity existed in 22%, 5%, 29%, 5% and 88% of healthy subjects, esophageal ulcer, gastric ulcer, duodenal ulcer and gastric cancer patients, respectively. CONCLUSION: Bile reflux, atrophy and dense neutrophil infiltrate of the corpus are three independent factors determining the acidity of gastric juice.
基金This study was supported by the National Natural Science Foundation of China （No. 41401336）, the Na- tural Science Foundation of Jiangsu Province, China （No. BK20130105）, the State Key Laboratory of Soil and Sustainable Agriculture, Chinese Academy of Sci-ence （No. Y412201452）, and the Environmental Pro- tection Public Benefit Research Foundation of China （No. 201309036）. We thank the three anonymous refe- rees for their helpful comments.
文摘Strongly acidic soils （pH 〈 5.0） are detrimental to tea （Camellia sinensis） production and quality. Little information exists on the ability of surface amendments to ameliorate subsoil acidity in the tea garden soils. A 120-d glasshouse column leaching experiment was conducted using commonly available soil ameliorants. Alkaline slag （AS） and organic residues, pig manure （PM） and rapeseed cake （RC） differing in ash alkalinity and C/N ratio were incorporated alone and in combination into the surface （0-15 cm） of soil columns （10 cm internal diameter x 50 cm long） packed with soil from the acidic soil layer （15-30 cm） of an Ultisol （initial pH -- 4.4）. During the 120-d experiment, the soil columns were watered （about 127 mm over 9 applications） according to the long-term mean annual rainfall （1 143 mm） and the leachates were collected and analyzed. At the end of the experiment, soil columns were partitioned into various depths and the chemical properties of soil were measured. The PM with a higher C/N ratio increased subsoil pH, whereas the RC with a lower C/N ratio decreased subsoil pH. However, combined amendments had a greater ability to reduce subsoil acidity than either of the amendments alone. The increases in pH of the subsoil were mainly ascribed to decreased base cation concentrations and the decomposition of organic anions present in dissolved organic carbon （DOC） and immobilization of nitrate that had been leached down from the amended layer. A significant （P 〈 0.05） correlation between alkalinity production （reduced exchangeable acidity - N-cycle alkalinity） and alkalinity balance （net alkalinity production - N-cycle alkalinity） was observed at the end of the experiment. Additionally, combined amendments significantly increased （P ~ 0.05） subsoil cation concentrations and decreased subsoil A1 saturation （P 〈 0.05）. Combined applications of AS with organic amendments to surface soils are effective in reducing subsoil acidity in high-rainfall areas. Further investigations under field conditions and over longer timeframes are needed to fully understand their practical effectiveness in ameliorating acidity of deeper soil layers under naturally occurring leaching regimes.
文摘The surface acidity of synthetic amorphous AI hydroxide was determined by acid/base titration with several complementary methods including solution analyses of the reacted solutions and XRD characterization of the reacted solids. The synthetic specimen was characterized to be the amorphous material showing four broad peaks in XRD pattern. XRD analyses of reacted solids after the titration experiments showed that amorphous AI hydroxide rapidly transformed to crystalline bayerite at the alkaline condition （pH〉10）. The solution analyses after and during the titration Ksp=^aAl^3＋/aH^＋^3 ,was 10^10.3. The amount of consumption of added acid or base during the titration experiment was attributed to both the protonation/deprotonation of dissolved AI species and surface hydroxyl group. The surface acidity constants, surface hydroxyl density and specific surface area were estimated by FITEQL 4.0.
基金financially supported by National Key R&D Program of China(No.2016YFC0205301)the Key Project of National Natural Science Foundation(No.21637005)+1 种基金the National Natural Science Foundation of China(No.21607149)the Natural Science Foundation of Fujian Province,China(No.2016J05142)
文摘The effect of acidity and redox capability over sulfuric acid-modified CeO_2 catalysts were studied for the selective catalytic reduction of NO_x with NH_3(NH_3-SCR). The deposition of sulfate significantly enhanced the catalytic performance over CeO_2. NO_x conversion over4H_2SO_4/CeO_2 at 230–440 °C was higher than 90%. The strong redox capability of CeO_2 could result in unselective NH_3 oxidation and decrease high temperatures catalytic activity and N_2 selectivity. The deposition of sulfate increased the acidity and weakened the redox capability, and then increased the high temperature NO_x conversion and N_2 selectivity. An appropriate level of acidity also promoted the activity at 190–250 °C over ceria-based catalysts, and with further increase in the acidity, the SCR activity decreased slightly. Weak redox capability lowered the low-temperature catalytic activity. Excellent SCR activity requires a balance of acidity and redox capability on the catalysts.
