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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    

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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    

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Characterization and performance of V

Caiting LI, Qun LI, Pei LU, Huafei CUI, Guangming ZENG

《环境科学与工程前沿（英文）》 2012年 第6卷 第2期   页码 156-161 doi: 10.1007/s11783-010-0295-x

摘要： A series of CeO supported V O catalysts with various loadings were prepared with different calcination temperatures by the incipient impregnation. The catalysts were evaluated for low temperature selective catalytic reduction (SCR) of NO with ammonia (NH ). The effects of O and SO on catalytic activity were also studied. The catalysts were characterized by specific surface areas (S ) and X–ray diffraction (XRD) methods. The experimental results showed that NO conversion changed significantly with the different V O loading and calcination temperature. With the V O loading increasing from 0 to 10 wt%, NO conversion increased significantly, but decreased at higher loading. The optimum calcination temperature was 400°C. The best catalyst yielded above 80% NO conversion in the reaction temperature range of 160°C–300°C. The formation of CeVO on the surface of catalysts caused the decrease of redox ability.

关键词： V2O5/CeO2 catalysts     NH3-SCR (selective catalytic reduction)     the incipient impregnation     low temperatures    

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On the monolayer dispersion behavior of Co<sub>3sub>O<sub>4sub> 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    

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NiBO (B = Mn or Co) catalysts for NH-SCR of NO at low-temperature in microwave field

《环境科学与工程前沿（英文）》 2023年 第17卷 第8期 doi: 10.1007/s11783-023-1696-y

摘要：

● Microwave-assisted catalytic NH3-SCR reaction over spinel oxides is carried out.

关键词： Microwave field     Spinel oxides     NOx     Selective catalytic reduction    

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different acid anions on highly efficient Ce-based catalysts for selective catalytic reduction of NO with NH<sub>3sub>

《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    

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以NH<sub>3sub>OH+/NH<sub>2sub>NH<sub>3sub>+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NH<sub>3sub>OH+和NH<sub>2sub>NH<sub>3sub>+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(H<sub>2sub>dabco)B(ClO<sub>4sub>)<sub>3sub>（分别命名为DAP-6和DAP-7，其中H<sub>2<与基于NH<sub>4sub>+阳离子构筑的立方钙钛矿类似物(H<sub>2sub>dabco)(NH<sub>4sub>)(ClO<sub>4sub>)<sub>3sub>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。特别地，DAP-7具有超高热稳定性（起始分解温度T<sub>dsub> = 375.3 °C）、高爆速（D = 8.883 km·s

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

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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    

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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    

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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    

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Effective regeneration of thermally deactivated commercial V-W-Ti catalysts

Xuesong SHANG, Jianrong LI, Xiaowei YU, Jinsheng CHEN, Chi HE

《化学科学与工程前沿（英文）》 2012年 第6卷 第1期   页码 38-46 doi: 10.1007/s11705-011-1167-z

摘要： An effective method for the regeneration of thermally deactivated commercial monolith SCR catalysts was investigated. Two types of regenerated solutions, namely NH Cl (1 mol/L) and dilute H SO (0.5 mol/L), were employed to treat the used catalyst. The effects of temperature and the regeneration process on the structural and textural properties of the catalysts were determined by X-ray diffraction, scanning electron microscopy, N adsorption/desorption, elemental analysis and Fourier transform infrared spectroscopy. The results suggest that the anatase phase of the used catalyst is maintained after exposure to high temperatures. Some of the catalytic activity was restored after regeneration. The catalyst regenerated by aqueous NH Cl had a higher activity than that of the catalyst treated by dilute H SO . The main reason is that the NH generated from the decomposition of NH Cl at high temperatures can be adsorbed onto the catalyst which promotes the reaction. The aggregated V O were partially re-dispersed during the regeneration process, and the intrinsic oxidation of ammonia with high concentrations of O is a factor that suppresses the catalytic activity.

关键词： V2O5-WO3/TiO2 catalysts     thermal deactivation     regeneration     NH4Cl     dilute H2SO4 solution    

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Chemical poison and regeneration of SCR catalysts for NO<sub>xsub>

Junhua LI,Yue PENG,Huazhen CHANG,Xiang LI,John C. CRITTENDEN,Jiming HAO

《环境科学与工程前沿（英文）》 2016年 第10卷 第3期   页码 413-427 doi: 10.1007/s11783-016-0832-3

摘要： Selective catalytic reduction (SCR) of NO with NH is an effective technique to remove NO from stationary sources, such as coal-fired power plant and industrial boilers. Some of elements in the fly ash deactivate the catalyst due to strong chemisorptions on the active sites. The poisons may act by simply blocking active sites or alter the adsorption behaviors of reactants and products by an electronic interaction. This review is mainly focused on the chemical poisoning on V O -based catalysts, environmental-benign catalysts and low temperature catalysts. Several common poisons including alkali/alkaline earth metals, SO and heavy metals etc. are referred and their poisoning mechanisms on catalysts are discussed. The regeneration methods of poisoned catalysts and the development of poison-resistance catalysts are also compared and analyzed. Finally, future research directions in developing poisoning resistance catalysts and facile efficient regeneration methods for SCR catalysts are proposed.

关键词： flue gas     DeNOx     SCR catalyst     poison and regeneration    

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Investigation of fluorescence characterization and electrochemical behavior on the catalysts of nanosized Pt-Rh/γ-Al

Chang-Mao HUNG, Wen-Liang LAI, Jane-Li LIN

《环境科学与工程前沿（英文）》 2013年 第7卷 第3期   页码 428-434 doi: 10.1007/s11783-013-0517-0

摘要： This work describes the environmentally friendly technology for oxidation of ammonia (NH ) to form nitrogen at temperatures range from 423K to 673K by selective catalytic oxidation (SCO) over a nanosized Pt-Rh/γ-Al O catalyst prepared by the incipient wetness impregnation method of hexachloroplatinic acid (H PtCl ) and rhodium (III) nitrate (Rh(NO ) ) with γ-Al O in a tubular fixed-bed flow quartz reactor (TFBR). The characterization of catalysts were thoroughly measured using transmission electron microscopy (TEM), three-dimensional excitation-emission fluorescent matrix (EEFM) spectroscopy, UV-Vis absorption, dynamic light-scattering (DLS), zeta potential meter, and cyclic voltammetry (CV). The results demonstrated that at a temperature of 673K and an oxygen content of 4%, approximately 99% of the NH was removed by catalytic oxidation over the nanosized Pt-Rh/γ-Al O catalyst. N was the main product in NH -SCO process. Further, it reveals that the oxidation of NH was proceeds by the over-oxidation of NH into NO, which was conversely reacted with the NH to yield N . Therefore, the application of nanosized Pt-Rh/γ-Al O catalyst can significantly enhance the catalytic activity toward NH oxidation. One fluorescent peak for fresh catalyst was different with that of exhausted catalyst. It indicates that EEFM spectroscopy was proven to be an appropriate and effective method to characterize the Pt clusters in intrinsic emission from nanosized Pt-Rh/γ-Al O catalyst. Results obtained from the CV may explain the significant catalytic activity of the catalysts.

关键词： ammonia (NH3)     nanosized Pt-Rh/γ-Al2O3 catalyst     excitation-emission fluorescent matrix (EEFM)     selective catalytic oxidation (SCO)     tubular fixed-bed reactor (TFBR)    

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The effect of preparation conditions of Pt/Al

Lei YUAN, Xiang ZHENG, Kaijiao DUAN, Hao HU, Jinggang WANG, Seong Ihl WOO, Zhiming LIU

《环境科学与工程前沿（英文）》 2013年 第7卷 第3期   页码 457-463 doi: 10.1007/s11783-013-0512-5

摘要： Selective catalytic reduction of NO by H in the presence of oxygen has been investigated over Pt/Al O catalysts pre-treated under different conditions. Catalyst preparation conditions exert significant influence on the catalytic performance, and the catalyst pre-treated by H or H then followed by O is much more active than that pre-treated by air. The higher surface area and the presence of metallic Pt over Pt/Al O pre-treated by H or pretreated by H then followed by O can contribute to the formation of NO , which then promotes the reaction to proceed at low temperatures.

关键词： NOx reduction     Pt/Al2O3     preparation condition     H2-SCR    

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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    

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标题 作者 时间 类型 操作

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

期刊论文

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

期刊论文

Characterization and performance of V

Caiting LI, Qun LI, Pei LU, Huafei CUI, Guangming ZENG

期刊论文

On the monolayer dispersion behavior of Co<sub>3sub>O<sub>4sub> on HZSM-5 support: designing applicable

期刊论文

NiBO (B = Mn or Co) catalysts for NH-SCR of NO at low-temperature in microwave field

期刊论文

different acid anions on highly efficient Ce-based catalysts for selective catalytic reduction of NO with NH<sub>3sub>

期刊论文

以NH<sub>3sub>OH+/NH<sub>2sub>NH<sub>3sub>+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

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

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

期刊论文

Promotion of transition metal oxides on the NH

Weiman Li, Haidi Liu, Yunfa Chen

期刊论文

Effective regeneration of thermally deactivated commercial V-W-Ti catalysts

Xuesong SHANG, Jianrong LI, Xiaowei YU, Jinsheng CHEN, Chi HE

期刊论文

Chemical poison and regeneration of SCR catalysts for NO<sub>xsub>

Junhua LI,Yue PENG,Huazhen CHANG,Xiang LI,John C. CRITTENDEN,Jiming HAO

期刊论文

Investigation of fluorescence characterization and electrochemical behavior on the catalysts of nanosized Pt-Rh/γ-Al

Chang-Mao HUNG, Wen-Liang LAI, Jane-Li LIN

期刊论文

The effect of preparation conditions of Pt/Al

Lei YUAN, Xiang ZHENG, Kaijiao DUAN, Hao HU, Jinggang WANG, Seong Ihl WOO, Zhiming LIU

期刊论文

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

Yue PENG, Junhua LI

期刊论文