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Ammonia adsorption on graphene and graphene oxide: a first-principles study

Yue PENG, Junhua LI

《环境科学与工程前沿(英文)》 2013年 第7卷 第3期   页码 403-411 doi: 10.1007/s11783-013-0491-6

摘要: Motivated by the recent realization of graphene sensor to detect gas molecules that are harmful to the environment, the ammonia adsorption on graphene or graphene oxide (GO) was investigated using first-principles calculation. The optimal adsorption and orientation of the NH molecules on the graphene surfaces were determined, and the adsorption energies ( ) as well as the Mulliken charge transfers of NH were calculated. The for the graphene are small and seem to be independent of the sites and orientations. The surface epoxy or hydroxyl groups can promote the adsorption of NH on the GO; the enhancement of the for the hydroxyl groups is greater than that for the epoxy groups on the surface. The charge transfers from the molecule to the surfaces also exhibit the same trend. The Br?nsted acid sites and Lewis acid sites could stably exist on the GO with surface hydroxyl groups and on the basal, respectively.

关键词: graphene oxide     first-principles calculations     NH3 adsorption    

Integrating of metal-organic framework UiO-66-NH2 and cellulose nanofibers mat for high-performance adsorption

《化学科学与工程前沿(英文)》 2022年 第16卷 第9期   页码 1387-1398 doi: 10.1007/s11705-022-2154-2

摘要: UiO-66-NH2 is an efficient material for removing pollutants from wastewater due to its high specific surface area, high porosity and water stability. However, recycling them from wastewater is difficult. In this study, the cellulose nanofibers mat deacetylated from cellulose acetate nanofibers were used to combine with UiO-66-NH2 by the method of in-situ growth to remove the toxic dye, rose bengal. Compared to previous work, the prepared composite could not only provide ease of separation of UiO-66-NH2 from the water after adsorption but also demonstrate better adsorption capacity (683 mg∙g‒1 (T = 25 °C, pH = 3)) than that of the simple UiO-66-NH2 (309.6 mg∙g‒1 (T = 25 °C, pH = 3)). Through the analysis of adsorption kinetics and isotherms, the adsorption for rose bengal is mainly suitable for the pseudo-second-order kinetic model and Freundlich model. Furthermore, the relevant research revealed that the main adsorption mechanism of the composite was electrostatic interaction, hydrogen bonding and π–π interaction. Overall, the approach depicts an efficient model for integrating metal-organic frameworks on cellulose nanofibers to improve metal-organic framework recovery performance with potentially broad applications.

关键词: UiO-66-NH2     cellulose nanofibers     rose bengal     adsorption     mechanism    

Denitrification performance and sulfur resistance mechanism of Sm–Mn catalyst for low temperature NH-SCR

《化学科学与工程前沿(英文)》 2023年 第17卷 第5期   页码 617-633 doi: 10.1007/s11705-022-2258-8

摘要: MnOx and Sm–Mn catalysts were prepared with the coprecipitation method, and they showed excellent activities and sulfur resistances for the selective catalytic reduction of NOx by NH3 between 50 and 300 °C in the presence of excess oxygen. 0.10Sm–Mn catalyst indicated better catalytic activity and sulfur resistance. Additionally, the Sm doping led to multi-aspect impacts on the phases, morphology structures, gas adsorption, reactions process, and specific surface areas. Therefore, it significantly enhances the NO conversion, N2 selectivity, and sulfur resistance. Based on various experimental characterization results, the reaction mechanism of catalysts and the effect of SO2 on the reaction process about the catalysts were extensively explored. For 0.10Sm–Mn catalyst, manganese sulfate and sulfur ammonium cannot be generated broadly under the influence of SO2 and the amount of surface adsorbed oxygen. The Bronsted acid sites strengthen significantly due to the addition of SO2, enhancing the sulfur resistance of the 0.10Sm–Mn catalyst.

关键词: MnOx     Sm–Mn     catalyst     NH3-SCR     sulfur resistance    

NH3OH+/NH2NH3+作为B位阳离子的无金属六方钙钛矿含能材料 Article

尚宇, 余志鸿, 黄瑞康, 陈劭力, 刘德轩, 陈晓娴, 张伟雄, 陈小明

《工程(英文)》 2020年 第6卷 第9期   页码 1013-1018 doi: 10.1016/j.eng.2020.05.018

摘要: 文中通过合理地选择分子组分,经由易于规模放大的简单合成路线,以NH3OH+NH2NH3+分别作为B位点阳离子构筑了两例无金属六方钙钛矿含能材料(H2dabco)B(ClO4)3(分别命名为DAP-6和DAP-7,其中H2<与基于NH4+阳离子构筑的立方钙钛矿类似物(H2dabco)(NH4)(ClO4)3相比,DAP-6和DAP-7有较高的晶体堆积密度和生成焓,从而具有更高的爆轰性能。

关键词: 含能材料     单质炸药     固体推进剂     无金属六方钙钛矿    

different acid anions on highly efficient Ce-based catalysts for selective catalytic reduction of NO with NH3

《化学科学与工程前沿(英文)》 2023年 第17卷 第10期   页码 1399-1411 doi: 10.1007/s11705-023-2345-5

摘要: Three kinds of Ce-based catalysts (CePO4, CeVO4, Ce2(SO4)3) were synthesized and used for the selective catalytic reduction (SCR) of NO by NH3. NH3-SCR performances were conducted in the temperature range of 80 to 400 °C. The catalytic efficiencies of the three catalysts are as follow: CePO4 > CeVO4 > Ce2(SO4)3, which is in agreement with their abilities of NH3 adsorption capacities. The highest NO conversion rate of CePO4 could reach about 95%, and the catalyst had more than 90% NO conversion rate between 260 and 320 °C. The effect of PO43–, VO43– and SO42– on NH3-SCR performances of Ce-based catalysts was systematically investigated by the X-ray photoelectron spectroscopy analysis, NH3 temperature programmed desorption, H2 temperature programmed reduction and field emission scanning electron microscopy tests. The key factors that can enhance the SCR are the existence of Ce4+, large NH3 adsorption capacity, high and early H2 consumptions, and suitable microstructures for gas adsorption. Finally, CePO4 and CeVO4 catalysts also exhibited relatively strong tolerance of SO2, and the upward trend about 8% was detected due to the sulfation enhancement by SO2 for Ce2(SO4)3.

关键词: CePO4     CeVO4     Ce2(SO4)3     selective catalytic reduction     NO removal    

CeO doping boosted low-temperature NH-SCR activity of FeTiO catalyst: A microstructure analysis and reaction

《环境科学与工程前沿(英文)》 2022年 第16卷 第5期 doi: 10.1007/s11783-022-1539-2

摘要:

• CeO2 doping significantly improved low-temperature NH3-SCR activity on FeTiOx.

关键词: NH3-SCR     CeO2 doping     Low-temperature NOx removal     Improved redox property     In situ XAFS analysis    

Separation of gibberellic acid (GA3) by macroporous adsorption resins

WANG Ruifang, YANG Jialing, SHI Zuoqing, OU Lailiang

《化学科学与工程前沿(英文)》 2008年 第2卷 第2期   页码 171-175 doi: 10.1007/s11705-008-0025-0

摘要: The adsorption effects of several macroporous adsorption resins for gibberellic acid (GA3) were investigated. The dynamic adsorption capacity is 58.38 mg/g dry beads for resin R4 and 96.46 mg/g dry beads for resin R5 which is consistent with the surface area. Aqueous methanol (50%, V/V) is a good eluent and the yield of GA3 is above 95%. The concentration of GA3 could increase five-fold after an adsorption-elution cycle and this is important when considering further crystallization of GA3 in an industrial process.

关键词: industrial     gibberellic     adsorption capacity     crystallization     consistent    

Kinetics and thermodynamics of the phosphine adsorption on the modified activated carbon

Bingnan REN

《化学科学与工程前沿(英文)》 2011年 第5卷 第2期   页码 203-208 doi: 10.1007/s11705-010-0571-0

摘要: The kinetics and the thermodynamics of phosphine (PH ) adsorption on the modified activated carbon have been explained for the adsorption process of PH . This study investigated the kinetic and thermodynamic properties of PH adsorption on the activated carbon impregnated with 5% HCl solution. The thermodynamic properties including PH adsorption isotherm and adsorption heat were separately investigated at 20°C, 70°C, 90°C. The results showed that the Freundlich-type isotherm equation described the isotherms well. The adsorption capacity increased with increasing temperature between 20°C and 70°C. Between 70°C and 90°C, the adsorption capacity decreased obviously with increasing temperature. The adsorption capacity reached the maximum at 70°C. By analyzing the results of the kinetics and the thermodynamics, we found that the adsorption of PH was dominated by physical adsorption at the lower temperature (20°C). Then with increasing temperature, chemical adsorption gradually dominated in the adsorption process. The adsorption capacity decreased at above 70°C is due to the exothermic effects in the process of adsorption.

关键词: adsorption     PH3     activated carbon     kinetics     thermodynamics    

Removal of ammonium and nitrate through Anammox and FeS-driven autotrophic denitrification

《环境科学与工程前沿(英文)》 2023年 第17卷 第6期 doi: 10.1007/s11783-023-1674-4

摘要:

● Simultaneous NH4+/NO3 removal was achieved in the FeS denitrification system

关键词: Anammox     Denitrification     FeS     NH4+/NO3     Sulfammox    

On the monolayer dispersion behavior of Co3O4 on HZSM-5 support: designing applicable

《化学科学与工程前沿(英文)》 2023年 第17卷 第11期   页码 1741-1754 doi: 10.1007/s11705-023-2332-x

摘要: Based on monolayer dispersion theory, Co3O4/ZSM-5 catalysts with different loadings have been prepared for selective catalytic reduction of nitrogen oxides by ammonia. Co3O4 can spontaneously disperse on HZSM-5 support with a monolayer dispersion threshold of 0.061 mmol 100 m–2, equaling to a weight percentage around 4.5%. It has been revealed that the quantities of surface active oxygen (O2) and acid sites are crucial for the reaction, which can adsorb and activate NOx and NH3 reactants effectively. Below the monolayer dispersion threshold, Co3O4 is finely dispersed as sub-monolayers or monolayers and in an amorphous state, which is favorable to generate the two kinds of active sites, hence promoting the performance of ammonia selective catalytic reduction of nitrogen oxide. However, the formation of crystalline Co3O4 above the capacity is harmful to the reaction performance. 4% Co3O4/ZSM-5, the catalyst close to the monolayer dispersion capacity, possesses the most abundant active O2 species and acidic sites, thereby demonstrating the best reaction performance in all the samples. It is proposed the optimal Co3O4/ZSM-5 catalyst can be prepared by loading the capacity amount of Co3O4 onto HZSM-5 support.

关键词: Co3O4/ZSM-5     NOx-SCR by NH3     monolayer dispersion threshold effect     surface acid sites     surface active O2 anions    

Promotion of transition metal oxides on the NH

Weiman Li, Haidi Liu, Yunfa Chen

《环境科学与工程前沿(英文)》 2017年 第11卷 第2期 doi: 10.1007/s11783-017-0914-x

摘要: Manganese and chromium oxides promote the NH -SCR activity of Zr-Ce mixed oxide. Cr-Zr-Ce mixed oxide exhibited>80% NO conversion at a wide temperature window. More acid sites and higher reducibility may responsible for the high SCR ability. Chromium oxide and manganese oxide promoted ZrO -CeO catalysts were prepared by a homogeneous precipitation method for the selective catalytic reduction of NO with NH . A series of characterization including X-ray diffraction (XRD), high-resolution transmission electron microscope (HR-TEM), Brunauer–Emmett–Teller (BET) surface area analysis, H temperature-programmed reduction (H -TPR), and X-ray photoelectron spectroscopy (XPS) were used to evaluate the influence of the physicochemical properties on NH -SCR activity. Cr-Zr-Ce and Mn-Zr-Ce catalysts are much more active than ZrO -CeO binary oxide for the low temperature NH -SCR, mainly because of the high specific surface area, more surface oxygen species, improved reducibility derived from synergistic effect among different elements. Mn-Zr-Ce catalyst exhibited high tolerance to SO and H O. Cr-Zr-Ce mixed oxide exhibited>80% NO conversion at a wide temperature window of 100°C–300°C. DRIFT studies showed that the addition of Cr is beneficial to the formation of Bronsted acid sites and prevents the formation of stable nitrate species because of the presence of Cr . The present mixed oxide can be a candidate for the low temperature abatement of NO .

关键词: NH3-selective catalytic reduction     NOx     Low temperature     Cr-Zr-Ce    

Influence of HS and NH on biogas dry reforming using Ni catalyst: a study on single and synergetic effect

《环境科学与工程前沿(英文)》 2023年 第17卷 第3期 doi: 10.1007/s11783-023-1632-1

摘要:

● NH3 in biogas had a slight inhibitory effect on dry reforming.

关键词: Biogas     Dry reforming     Sulfur poisoning     Ammonia     Synergetic effect     Hydrogen    

Effect of alumina and zirconia as binders on the activity of Fe-BEA for NH

Jin Shi, Zihao Zhang, Mingxia Chen, Zhixiang Zhang, Wenfeng Shangguan, Shunchao Gu, Hirano Shin-ichi

《环境科学与工程前沿(英文)》 2018年 第12卷 第1期 doi: 10.1007/s11783-018-1012-4

摘要: Fe-BEA catalysts are active for the NH -SCR of NO. For industrial application, a binder should be added to the Fe-BEA catalysts to make them tightly adhere to the monoliths. The addition of alumina and zirconia as binders to the Fe-BEA led to a different effect on NO conversion. The catalytic activity of the mixed samples was evaluated by the temperature programmed procedure in a flow-reactor system, and the mechanism was analyzed via SEM, BET, XRD and XPS. It was found that larger iron particles were formed by the migration of parent iron particles in the Fe-BEA catalyst with alumina. This led to the increase of Fe magnitude and iron cluster, enhancing the abilities of NO oxidation and storage. Accordingly, the SCR activity increased slightly in low temperature but decreased sharply in high temperature. For the Fe-BEA with zirconia sample, NO oxidation and storage abilities decreased due to the less iron clusters. The increase of Fe magnitude resulted in higher catalytic oxidation ability, which gave rise to little change in the SCR activity compared with the Fe-BEA.

关键词: NH3-SCR     NO     Fe-BEA     Binder     Alumina     Zirconia    

Utilization of aluminum hydroxide waste generated in fluoride adsorption and coagulation processes for

Jiawei JU,Ruiping LIU,Zan HE,Huijuan LIU,Xiwang ZHANG,Jiuhui QU

《环境科学与工程前沿(英文)》 2016年 第10卷 第3期   页码 467-476 doi: 10.1007/s11783-015-0809-7

摘要: Although Al-based coagulation and adsorption processes have been proved highly efficient for fluoride (F) removal, the two processes both generate large amount of Al(OH) solid waste containing F (Al(OH) -F). This study aimed to investigate the feasibility of utilizing Al(OH) -F generated in Al(OH) adsorption (Al(OH) -F ) and coagulation (Al(OH) -F ) for the adsorption of cadmium ion (Cd(II)). The adsorption capacity of Al(OH) -F and Al(OH) -F for Cd(II) was similar as that of pristine aluminum hydroxide (Al(OH) ), being of 24.39 and 19.90 mg·g , respectively. The adsorption of Cd(II) onto Al(OH) -F and Al(OH) -F was identified to be dominated by ion-exchange with sodium ion (Na ) or hydrogen ion (H ), surface microprecitation, and electrostatic attraction. The maximum concentration of the leached fluoride from Al(OH) -F and Al(OH) -F is below the Chinese Class-I Industrial Wastewater Discharge Standard for fluoride (<10 mg·L ). This study demonstrates that the Al(OH) solid wastes generated in fluoride removal process could be potentially utilized as a adsorbent for Cd(II) removal.

关键词: Al(OH)3     fluoride     cadmium     adsorption     reclamation     sequential extraction    

Adsorption of 1,3-propanediol from synthetic mixture using polymeric resin as adsorbents

W. LUERRUK, A. SHOTIPRUK, V. TANTAYAKOM, P. PRASITCHOKE, C. MUANGNAPOH

《化学科学与工程前沿(英文)》 2009年 第3卷 第1期   页码 52-57 doi: 10.1007/s11705-009-0087-7

摘要: The aim of this work was to separate 1,3-PDO from a synthetic mixture using polymeric resins, Amberlite XAD-7 and XAD-16 resins. The equilibrium adsorption of 1,3-PDO onto two polymeric resins were investigated in binary and tertiary systems. Experimental results of binary component adsorption equilibrium indicated that the adsorption capacity ( ) of 1,3-PDO at 160 g/L onto XAD-7 and XAD-16 was 835.96 and 584.61 mg 1,3-PDO/g dry resin, respectively. The adsorption isotherms were closely predicted by the Langmuir-Freundlich model among the two isotherm model tested. The value of n of 1,3-PDO adsorbed on XAD-7 are much higher than those on XAD-16. This result suggested that XAD-7 resin has a higher affinity for the 1,3-PDO adsorption than XAD-16 resin. Moreover, the value of adsorption capacity of 1,3-PDO in the binary and tertiary component were compared at the same conditions. In the tertiary system, although the selectivity of 1,3-PDO from XAD-7 was approximately six times higher than XAD-16, the adsorption capacity of 1,3-PDO at 160 g/L onto XAD-16 was higher than XAD-7. Interestingly, the reusability of XAD-7 and XAD-16 resins in the three cycle times shows a slight loss of adsorption capacity. Furthermore, the investigation about desorption by an ethanol/water mixture at 50% ( / ) indicated that the desorption yield of 1,3-PDO from XAD-7 was lower than XAD-16 resin for both the binary and tertiary component. This was due to the more favorable adsorption characteristics of XAD-7 resin than XAD-16 resin.

关键词: adsorption     1     3-propanediol     glycerol     polymeric resin     adsorption isotherm    

标题 作者 时间 类型 操作

Ammonia adsorption on graphene and graphene oxide: a first-principles study

Yue PENG, Junhua LI

期刊论文

Integrating of metal-organic framework UiO-66-NH2 and cellulose nanofibers mat for high-performance adsorption

期刊论文

Denitrification performance and sulfur resistance mechanism of Sm–Mn catalyst for low temperature NH-SCR

期刊论文

NH3OH+/NH2NH3+作为B位阳离子的无金属六方钙钛矿含能材料

尚宇, 余志鸿, 黄瑞康, 陈劭力, 刘德轩, 陈晓娴, 张伟雄, 陈小明

期刊论文

different acid anions on highly efficient Ce-based catalysts for selective catalytic reduction of NO with NH3

期刊论文

CeO doping boosted low-temperature NH-SCR activity of FeTiO catalyst: A microstructure analysis and reaction

期刊论文

Separation of gibberellic acid (GA3) by macroporous adsorption resins

WANG Ruifang, YANG Jialing, SHI Zuoqing, OU Lailiang

期刊论文

Kinetics and thermodynamics of the phosphine adsorption on the modified activated carbon

Bingnan REN

期刊论文

Removal of ammonium and nitrate through Anammox and FeS-driven autotrophic denitrification

期刊论文

On the monolayer dispersion behavior of Co3O4 on HZSM-5 support: designing applicable

期刊论文

Promotion of transition metal oxides on the NH

Weiman Li, Haidi Liu, Yunfa Chen

期刊论文

Influence of HS and NH on biogas dry reforming using Ni catalyst: a study on single and synergetic effect

期刊论文

Effect of alumina and zirconia as binders on the activity of Fe-BEA for NH

Jin Shi, Zihao Zhang, Mingxia Chen, Zhixiang Zhang, Wenfeng Shangguan, Shunchao Gu, Hirano Shin-ichi

期刊论文

Utilization of aluminum hydroxide waste generated in fluoride adsorption and coagulation processes for

Jiawei JU,Ruiping LIU,Zan HE,Huijuan LIU,Xiwang ZHANG,Jiuhui QU

期刊论文

Adsorption of 1,3-propanediol from synthetic mixture using polymeric resin as adsorbents

W. LUERRUK, A. SHOTIPRUK, V. TANTAYAKOM, P. PRASITCHOKE, C. MUANGNAPOH

期刊论文