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Competition between acidic sites and hydrogenation sites in Cu/ZrO_(2) catalysts with different crystal phases for conversion of biomass-derived organics
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作者 Yuewen Shao Tingting Wang +6 位作者 Kai Sun Zhanming Zhang Lijun Zhang Qingyin Li Shu Zhang Guangzhi Hu Xun Hu 《Green Energy & Environment》 SCIE CSCD 2021年第4期557-566,共10页
Oxides with different crystal phases can have important effects on the configuration of surface atoms,which can further affect the distribution of hydrogenation sites and acidic sites as well as the competitions of th... Oxides with different crystal phases can have important effects on the configuration of surface atoms,which can further affect the distribution of hydrogenation sites and acidic sites as well as the competitions of these varied types of catalytic sites.This could be potentially used to tailor the distribution of the products.In this study,zirconium oxides with different crystal phases supported copper catalysts were prepared for the hydrogenation of the biomass-derived furfural,vanillin,etc.The results showed that both calcination temperature and Cu species affected the shift of zirconia from tetragonal phase to the monoclinic phase.Monoclinic zirconia supported copper catalyst can effectively catalyze the hydrogenation of furfural to furfuryl alcohol via hydrogenation route due to its low amount of Brønsted acidic sites,although the surface area and the exposed metallic Cu surface area were much lower than the tetragonal zirconia supported copper catalyst.Zirconia with tetragonal or tetragonal/monoclinic phases supported copper catalysts contain abundant acidic sites and especially the Br?nsted acidic sites,which catalyzed mainly the conversion of furfural via the acid-catalyzed routes such as the acetalization,rather than the hydrogenation.The acidic sites over the Cu/ZrO_(2)catalyst played more predominant roles than the hydrogenation sites in determining the conversion of the organics like furfural and vanillin. 展开更多
关键词 Zirconia supported copper catalyst Crystal phase HYDROGENATION Hydrogenation sites acidic sites
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Understanding the roles of Brønsted/Lewis acid sites on manganese oxide-zeolite hybrid catalysts for low-temperature NH_(3)-SCR
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作者 Hyun Sub Kim Hwangho Lee +2 位作者 Hongbeom Park Inhak Song Do Heui Kim 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第10期79-88,共10页
Although metal oxide-zeolite hybrid materials have long been known to achieve enhanced catalytic activity and selectivity in NO_(x)removal reactions through the inter-particle diffusion of intermediate species,their s... Although metal oxide-zeolite hybrid materials have long been known to achieve enhanced catalytic activity and selectivity in NO_(x)removal reactions through the inter-particle diffusion of intermediate species,their subsequent reaction mechanism on acid sites is still unclear and requires investigation.In this study,the distribution of Brønsted/Lewis acid sites in the hybrid materials was precisely adjusted by introducing potassium ions,which not only selectively bind to Brønsted acid sites but also potentially affect the formation and diffusion of activated NO species.Systematic in situ diffuse reflectance infrared Fourier transform spectroscopy analyses coupled with selective catalytic reduction of NO_(x)with NH_(3)(NH_(3)-SCR)reaction demonstrate that the Lewis acid sites over MnO_(x)are more active for NO reduction but have lower selectivity to N_(2)than Brønsted acids sites.Brønsted acid sites primarily produce N_(2),whereas Lewis acid sites primarily produce N_(2)O,contributing to unfavorable N_(2)selectivity.The Brønsted acid sites present in Y zeolite,which are stronger than those on MnO_(x),accelerate the NH_(3)-SCR reaction in which the nitrite/nitrate species diffused from the MnO_(x)particles rapidly convert into the N_(2).Therefore,it is important to design the catalyst so that the activated NO species formed in MnO_(x)diffuse to and are selectively decomposed on the Brønsted acid sites of H-Y zeolite rather than that of MnO_(x)particle.For the physically mixed H-MnO_(x)+H-Y sample,the abundant Brønsted/Lewis acid sites in H-MnO_(x)give rise to significant consumption of activated NO species before their inter-particle diffusion,thereby hindering the enhancement of the synergistic effects.Furthermore,we found that the intercalated K+in K-MnO_(x)has an unexpected favorable role in the NO reduction rate,probably owing to faster diffusion of the activated NO species on K-MnO_(x)than H-MnO_(x).This study will help to design promising metal oxide-zeolite hybrid catalysts by identifying the role of the acid sites in two different constituents. 展开更多
关键词 Hybrid metal oxide-zeolite The role of acid sites Manganese oxides Physical mixing Selective catalytic reduction of NOx with NH3
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Ni/ZSM-5 Catalysts for Light Olefin Oligomerization:Effects of Supports and Ni Sites on Activity and Selectivity
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作者 Zuo Qi Liang Ke +5 位作者 Ma Yirong Jia Yangxiao Liao Mingjie Zheng Jiajun Li Ruifeng Li Wenlin 《China Petroleum Processing & Petrochemical Technology》 SCIE CAS CSCD 2024年第3期15-23,共9页
A series of Ni/ZSM-5 containing a small amount of Ni was prepared by an ion exchanged method.The impact of the n(SiO_(2))/n(Al_(2)O_(3))ratio on the catalytic activity was studied using the samples 0.09Ni/ZSM-5(60)and... A series of Ni/ZSM-5 containing a small amount of Ni was prepared by an ion exchanged method.The impact of the n(SiO_(2))/n(Al_(2)O_(3))ratio on the catalytic activity was studied using the samples 0.09Ni/ZSM-5(60)and 0.09Ni/ZSM-5(130).To determine the interaction between the Ni species and acid sites on the surface of the catalyst,the catalysts were characterized by N2 adsorption-desorption,X-ray diffraction(XRD),scanning electron microscopy(SEM),and UV-vis spectroscopy.The performance of the catalysts for the catalytic oligomerization of 1-hexene was investigated in detail.The nickel species were found to be uniformly distributed in all the catalysts.It was discovered that the oligomerization activity of the catalyst can be improved using Ni species;however,the contribution of Brønsted acids in oligomerization reactions is greater than that of Ni sites and Lewis acids. 展开更多
关键词 nickel ZEOLITE acid sites OLIGOMERIZATION catalyst
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Influences of Brnsted Acidic Sites in HZSM-5 on Polarization and Electronegativity of Ethene Studied by Molecular Dynamics 被引量:1
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作者 樊建芬 肖鹤鸣 +1 位作者 王秋霞 夏其英 《Chinese Journal of Chemistry》 SCIE CAS CSCD 2002年第7期638-643,共6页
Molecular dynamics simulation has been performed for studying thepolarization and electronegativity of ethene molecules near Broensted acidic sites in H[Al] ZSM-5.The result shows that the molecules are polarized most... Molecular dynamics simulation has been performed for studying thepolarization and electronegativity of ethene molecules near Broensted acidic sites in H[Al] ZSM-5.The result shows that the molecules are polarized most at the edges of intersections and least atthe segments of channels. On the contrary, the highest global molecular electronegativity is foundat the centers of channel segments. Al substitution slightly increases the molecular dipole moment,but hardly affects the molecular electronegativity. Broensted acidic proton decreases the dipolemoment of guest molecule, but increases the molecular elec-tronegativity. 展开更多
关键词 molecular dynamics simulation ETHENE POLARIZATION ELECTRONEGATIVITY H[Al]ZSM-5 broensted acidic sites
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Deactivation mechanism of acetone to isobutene conversion over Y/Beta catalyst
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作者 Chang Wang Tingting Yan Weili Dai 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第9期133-142,共10页
The conversion of acetone derived from biomass to isobutene has attracted extensive attentions.In comparison with Brønsted acidic catalyst,Lewis acidic catalyst could exhibit a better catalytic performance with a... The conversion of acetone derived from biomass to isobutene has attracted extensive attentions.In comparison with Brønsted acidic catalyst,Lewis acidic catalyst could exhibit a better catalytic performance with a higher isobutene selectivity.However,the catalyst stability remains a key problem for the long-running acetone conversion and the reasons for catalyst deactivation are poorly understood up to now.Herein,the deactivation mechanism of Lewis acidic Y/Beta catalyst during the acetone to isobutene conversion was investigated by various characterization techniques,including acetone-temperature-programmed surface reaction,gas chromatography-mass spectrometry,in situ ultraviolet-visible,and ^(13)C cross polarization magic angle spinning nuclear magnetic resonance spectroscopy.A successive aldol condensation and cyclization were observed as the main side-reactions during the acetone conversion at Lewis acidic Y sites.In comparison with the low reaction temperature,a rapid formation and accumulation of the larger cyclic unsaturated aldehydes/ketones and aromatics could be observed,and which could strongly adsorb on the Lewis acidic sites,and thus cause the catalyst deactivation eventually.After a simple calcination,the coke deposits could be easily removed and the catalytic activity could be well restored. 展开更多
关键词 Deactivation mechanism Acetone to isobutene Lewis acid sites Y/Beta Spectroscopy
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FCF-LDH/BiVO_(4)with synergistic effect of physical enrichment and chemical adsorption for efficient reduction of nitrate
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作者 Yajie Bai Zhenyuan Fang +5 位作者 Yong Lei Lijing Liu Huaiquan Zhao Hongye Bai Weiqiang Fan Weidong Shi 《Green Energy & Environment》 SCIE EI CAS CSCD 2024年第7期1112-1121,共10页
Photoelectrochemical NO_(3)^(-)reduction(PEC NITRR)not only provides a promising solution for promoting the global nitrogen cycle,but also converts NO_(3)^(-)to the important chemicals(NH_(3)).However,it is still a gr... Photoelectrochemical NO_(3)^(-)reduction(PEC NITRR)not only provides a promising solution for promoting the global nitrogen cycle,but also converts NO_(3)^(-)to the important chemicals(NH_(3)).However,it is still a great challenge to prepare catalysts with excellent NO_(3)^(-)adsorption/activation capacity to achieve high NITRR.Herein,we designed a novel Fe^(2+)~Cu^(2+)Fe^(3+)LDH/BiVO_(4)(FCF-LDH/BVO)catalyst with synergistic effect of chemical adsorption and physical enrichment.Fe^(2+)in FCF-LDH/BVO provides the rich Lewis acid sites for the adsorption of NO_(3)^(-),and the appropriate layer spacing of FCF-LDH further promotes the physical enrichment of NO_(3)^(-)in its interior,thus realizing the effective contact between NO_(3)^(-)and active sites(Fe^(2+)).FCF-LDH/BVO showed excellent NH_(3)production performance(FE_(NH_(3))=66.1%,r_(NH_(3))=13.8μg h^(-1)cm^(-2))and selectivity(FE_(NO_(2)^(-))=2.5%,r_(NO_(2)^(-))=4.9μg h^(-1)cm^(-2))in 0.5 mol L^(-1)Na_(2)SO_(4)electrolyte.In addition,FCF-LDH/BVO maintains the desirable PEC stability for six cycle experiments,showing great potential for practical application.The^(14)NO_(3)^(-)and^(15)NO_(3)^(-)isotope test provides strong evidence for further verification of the origin of N in the generated NH_(3).This LDH catalyst has a great potential in PEC removal of NO_(3)^(-)from groundwater. 展开更多
关键词 LDH Lewis acid sites Physical enrichment Photoelectrochemical NO_(3)^(-)Reduction Ammonia
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Catalytic roles of the acid sites in different pore channels of H‐ZSM‐5 zeolite for methanol‐to‐olefins conversion 被引量:10
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作者 Sen Wang Zhikai Li +4 位作者 Zhangfeng Qin Mei Dong Junfen Li Weibin Fan Jianguo Wang 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2021年第7期1126-1136,共11页
H‐ZSM‐5 zeolite is a typical catalyst for methanol‐to‐olefins(MTO)conversion.Although the performance of zeolite catalysts for MTO conversion is related to the actual location of acid sites in the zeolite framewor... H‐ZSM‐5 zeolite is a typical catalyst for methanol‐to‐olefins(MTO)conversion.Although the performance of zeolite catalysts for MTO conversion is related to the actual location of acid sites in the zeolite framework,the catalytic roles of the acid sites in different pore channels of the H‐ZSM‐5 zeolite are not well understood.In this study,the MTO reaction network,involving the aromatic cycle,alkene cycle,and aromatization process,and also the diffusion behavior of methanol feedstock and olefin and aromatic products at different acid sites in the straight channel,sinusoidal channel,and intersection cavity of H‐ZSM‐5 zeolite was comparatively investigated using density functional theory calculations and molecular dynamic simulations.The results indicated that the aromatic cycle and aromatization process occurred preferentially at the acid sites in the intersection cavities with a much lower energy barrier than that at the acid sites in the straight and sinusoidal channels.In contrast,the formation of polymethylbenzenes was significantly suppressed at the acid sites in the sinusoidal and straight channels,whereas the alkene cycle can occur at all three types of acid sites with similar energy barriers and probabilities.Consequently,the catalytic performance of H‐ZSM‐5 zeolite for MTO conversion,including activity and product selectivity,can be regulated properly through the purposive alteration of the acid site distribution,viz.,the location of Al in the zeolite framework.This study helps to elucidate the relation between the catalytic performance of different acid sites in the H‐ZSM‐5 zeolite framework for MTO conversion,which should greatly benefit the design of efficient catalyst for methanol conversion. 展开更多
关键词 Methanol‐to‐olefins H‐ZSM‐5 zeolite Acid site distribution Density functional theory calculation Molecular dynamic simulation
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A high-surface-area silicoaluminophosphate material rich in Brnsted acid sites as a matrix in catalytic cracking 被引量:8
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作者 Shaoiun Xu Qiang Zhang +5 位作者 Zhaoxuan Feng Xiaojing Meng Tongyu Zhao Chunyi Li Chaohe Yang Honghong Shan 《Journal of Natural Gas Chemistry》 EI CAS CSCD 2012年第6期685-693,共9页
A transparent gel-like mesoporous silicoaluminophosphate material (SAP) with molar ratio of Si/Al = 20 was synthesized by hydrothermal method. The physicochemical features of SAP were characterized by XRD, XRF, BET,... A transparent gel-like mesoporous silicoaluminophosphate material (SAP) with molar ratio of Si/Al = 20 was synthesized by hydrothermal method. The physicochemical features of SAP were characterized by XRD, XRF, BET, SEM and FT-IR spectroscopy of pyridine adsorption techniques. The results indicated that incorporation of phosphorus (P) into aluminasilica system altered the basic textural characteristics of aluminasilica. Especially after hydrothermal treatment, the material with large special surface area (up to 492 m2/g) exhibited a good performance on hydrothermal stability. Moreover, the phosphorus modifier can not only increase the amount of Br/"{o}nsted acidic sites (up to 48.44 μmol/g) and the percentage of weak acidic sites in total acidic sites, but also regulate the acid type, such as the ratio of B/L (Lewis acid/Br?nsted acid) increased to 1.15. The performances of samples as matrices for the catalytic cracking of heavy VGO were investigated. At 520 ℃, the catalysts showed much higher gasoline and diesel oil yields achieving to 45.59 wt% and 19.20 wt%, respectively, and lower coke selectivity (2.86%) than conventional FCC matrices, such as kaolin and amorphous silica-alumina. 展开更多
关键词 SILICOALUMINOPHOSPHATE hydrothermal stability Br nsted acid sites MESOPOROUS hydrothermal synthesis
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The effect of FER zeolite acid sites in methanol-to-dimethyl-ether catalytic dehydration 被引量:5
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作者 Enrico Catizzone Alfredo Aloise +1 位作者 Massimo Migliori Girolamo Giordano 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2017年第3期406-415,共10页
In this paper, the effect of acidity of zeolites with FER framework was studied in the methanol dehydration to dimethyl ether reaction, by comparing catalysts with different Si/Al ratios(namely 8, 30 and60). The aim o... In this paper, the effect of acidity of zeolites with FER framework was studied in the methanol dehydration to dimethyl ether reaction, by comparing catalysts with different Si/Al ratios(namely 8, 30 and60). The aim of this work was to investigate how the acid sites concentration, strength, distribution and typology(Br?nsted and Lewis) affect methanol conversion, DME selectivity and coke formation. It was found that the aluminium content affects slightly acid sites strength whilst a relevant effect on acid sites concentration and distribution(Br?nsted/Lewis) was observed as 24% of Lewis sites were found on Alrichest samples, whilst less than 10% of Lewis acid sites were observed on FER at higher Si/Al ratio. All the investigated catalyst samples showed a selectivity toward DME always greater than 0.9 and samples with the lowest Si/Al ratio exhibit the best performances in terms of methanol conversion, approaching the theoretical equilibrium value(around 0.85) at temperatures below 200 °C. Turnover-frequency analysis suggests that this result seems to be related not only to the higher amount of acid sites but also that the presence of Lewis acid sites may play a significant role in converting methanol. On the other hand, the presence of Lewis acid sites, combined with a high acidity, promote the formation of by-products(mainly methane) and coke deposition during the reaction. As final evidence, all the investigated catalysts exhibit very high resistance to deactivation by coke deposition, over 60 h continuous test, and a GC–MS analysis of the coke deposited on the catalyst surface reveals tetra-methyl benzene as main component. 展开更多
关键词 Methanol dehydration Dimethyl ether Lewis acid sites FER zeolite Coke formation
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Evolution mechanism of active sites for selective catalytic reduction of NO_(x) with NH_(3) over Fe-ZSM-5 catalysts doped by Ce/Cu 被引量:2
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作者 ZHANG Yu-bo WANG Pan +3 位作者 YU Dan ZHAO Hong-yu LYU Xing-lei LEI Li-li 《Journal of Central South University》 SCIE EI CAS CSCD 2022年第7期2239-2252,共14页
Fe-ZSM-5 catalysts modified by Cu and Ce by aqueous solution ion-exchange and incipient wetness impregnation methods were tested in the selective catalytic reduction of NO_(x) with NH_(3).A variety of characterization... Fe-ZSM-5 catalysts modified by Cu and Ce by aqueous solution ion-exchange and incipient wetness impregnation methods were tested in the selective catalytic reduction of NO_(x) with NH_(3).A variety of characterization techniques(NH_(3)-SCO,BET,XRD,XPS,UV-Vis,NH_(3)-TPD,H_(2)-TPR)were used to explore the changes of the active sites,acid sites and pore structure of the catalyst.It was found that the dispersion of active Cu species and Fe species had great influences on the catalytic activity in the whole catalytic process.The Cu doping into the Fe-ZSM-5 catalyst produced new active species,isolated Cu ions and CuO particles,resulting in the improved low-temperature catalytic activity.However,the NH_(3) oxidation was enhanced,and part of the Fe^(3+)active sites and more Brønsted acidic sites in the catalyst were occupied by Cu species,which causes the decrease of the high-temperature activity.The recovery of hightemperature activity could be attributed to the recovery of active Cu species and Fe species promoted by Ce and the promotion of active species dispersion.The results provide theoretical support for adjusting the active window of Febased SCR catalyst by multi-metal doping. 展开更多
关键词 Fe-based zeolite nitric oxide removal Cu/Ce modification active sites acid sites
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Zr(Ⅳ) surface sites determine CH3OH formation rate on Cu/ZrO2/SiO2-CO2 hydrogenation catalysts 被引量:2
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作者 Erwin Lam Kim Larmier +3 位作者 Shohei Tada Patrick Wolf Olga V. Safonova Christophe Copéret 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2019年第11期1741-1748,共8页
Cu/ZrO2/SiO2 are efficient catalysts for the selective hydrogenation of CO2 to CH3OH. In order to understand the role of ZrO2 in these mixed-oxides based catalysts, in situ X-ray absorption spectroscopy has been carri... Cu/ZrO2/SiO2 are efficient catalysts for the selective hydrogenation of CO2 to CH3OH. In order to understand the role of ZrO2 in these mixed-oxides based catalysts, in situ X-ray absorption spectroscopy has been carried out on the Cu and Zr K-edge. Under reaction conditions, Cu remains metallic, while Zr is present in three types of coordination environment associated with 1) bulk ZrO2, 2) coordinatively saturated and 3) unsaturated Zr(Ⅳ) surface sites. The amount of coordinatively unsaturated Zr surface sites can be quantified by linear combination fit of reference X-Ray absorption near edge structure (XANES) spectra and its amount correlates with CH3OH formation rates, thus indicating the importance of Zr(Ⅳ) Lewis acid surface sites in driving the selectivity toward CH3OH. This finding is consistent with the proposed mechanism, where CO2 is hydrogenated at the interface between the Cu nanoparticles that split H2 and Zr(Ⅳ) surface sites that stabilizes reaction intermediates. 展开更多
关键词 CO2 hydrogenation ZrO2/SiO2 supported Cu nanoparticles Lewis acidic surface sites In situ X-ray absorption spectroscopy
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Constrained Al sites in FER-type zeolites 被引量:1
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作者 Weifeng Chu Xiaona Liu +7 位作者 Zhiqiang Yang Hiroya Nakata Xingzhi Tan Xuebin Liu Longya Xu Peng Guo Xiujie Li Xiangxue Zhu 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2021年第11期2078-2087,共10页
Crystallographic sites of Brönsted acids(Si-OH-Al)in zeolites,which are closely associated with the Al sites,play a significant and unique role in the catalytic application,especially when they are distributed in... Crystallographic sites of Brönsted acids(Si-OH-Al)in zeolites,which are closely associated with the Al sites,play a significant and unique role in the catalytic application,especially when they are distributed in open channel systems or confined in cavities with small pore openings.In this article,we unraveled constrained Al crystallographic sites in FER-type zeolites containing the distinct local environments(10-ring channels and ferrierite cavities)by Rietveld refinement against the powder X-ray diffraction data.Final refinement demonstrates that regardless of the types of structure-directing agents and synthetic medium utilized,T1 and/or T3 are Al-rich positions,which are further confirmed by theoretical calculations.This new finding of constrained Al sites in the FER-type zeolite can well explain its limited catalytic activity in the DME carbonylation reaction. 展开更多
关键词 FER-type zeolite Aluminum siting Structural characterization Bronsted acid site DME carbonylation
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Surface BrØnsted-Lewis dual acid sites for high-efficiency dinitrogen photofixation in pure water
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作者 Cai Chen Jiewei Chen +8 位作者 Zhiyuan Wang Fei Huang Jian Yang Yunteng Qu Kuang Liang Xiao Ge Yanggang Wang Hui Zhang Yuen Wu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2022年第4期824-830,共7页
As is known to all, nitrogen not only plays an important role in the industrial development of human society but also plays an important part in the proteins that constitute the essence of life[1]. In 1910, the Haber-... As is known to all, nitrogen not only plays an important role in the industrial development of human society but also plays an important part in the proteins that constitute the essence of life[1]. In 1910, the Haber-Bosch process was first used to synthesize ammonia. 展开更多
关键词 Photocatalytic nitrogen fixation Brùnsted-Lewis dual acid sites Surface-modified TiO2 Surface states F and H atoms
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Effect of the Structure and Acidic Property of Activated Bentonite on Removal of Olefin in Aromatics
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作者 Wu Wenjuan Chen Changwei +1 位作者 Wang Xin Shi Li (The State Key Laboratory of Chemical Engineering,East China University of Science and Technology, Shanghai 200237) 《China Petroleum Processing & Petrochemical Technology》 SCIE CAS 2009年第4期23-26,共4页
In this research work,three kinds of activated bentonite used as solid acid catalysts had been synthesized and studied on removal of olefins from the reformate oil.Activated bentonite samples were analyzed using the B... In this research work,three kinds of activated bentonite used as solid acid catalysts had been synthesized and studied on removal of olefins from the reformate oil.Activated bentonite samples were analyzed using the BET and pyridine-FTIR measurements to investigate their physical and chemical properties.The results showed that both textural properties and surface acidity of the bentonite could affect the catalytic activity.Among the catalyst samples,one kind of bentonite purchased from Hubei with high surface area,high pore volume and more acid sites revealed high activity in removing olefins from the reformate. 展开更多
关键词 bentomte N_2 adsorption isotherm pore size distribution acid sites
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Performances of CuSO_4/TiO_2 catalysts in selective catalytic reduction of NO_x by NH_3 被引量:6
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作者 于艳科 陈进生 +1 位作者 王金秀 陈衍婷 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2016年第2期281-287,共7页
A series of CuSO4/TiO2 catalysts were prepared using a wet impregnation method.The activity of each sample in the selective catalytic reduction of NO by NH3(NH3-SCR) was determined.The effects of SO2 and H2O,and the... A series of CuSO4/TiO2 catalysts were prepared using a wet impregnation method.The activity of each sample in the selective catalytic reduction of NO by NH3(NH3-SCR) was determined.The effects of SO2 and H2O,and their combined effect,on the activity were examined at 340 ℃ for 24 h.The catalysts were characterized using N2 adsorption-desorption,X-ray diffraction,X-ray photoelectron spectroscopy,temperature-programmed reduction of H2(H2-TPR),temperature-programmed desorption of NH3(NH3-TPD),and in situ diffuse-reflectance infrared Fourier-transform spectroscopy(DRIFTS).The CuSO4/TiO2 catalysts had good activities,with low production of N2O above 340 ℃.SO2 or a combination of SO2 and H2O had little effect on the activity,and H2O caused only a slight decrease in activity during the experimental period.The NH3-TPD and H2-TPR results showed that CuSO4 increased the amounts of acid sites and adsorbed oxygen on the catalyst.In situ DRIFTS showed that the NH3-SCR reaction on the CuSO4/TiO2 catalysts followed an Eley-Rideal mechanism.The reaction of gaseous NO with NH3 adsorbed on Lewis acid sites to form N2 and H2O could be the main reaction pathway,and oxygen adsorption might favor this process. 展开更多
关键词 Selective catalytic reduction Copper sulfate ACTIVITY Eley-Rideal mechanism Lewis acid sites
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Effect of external surface of HZSM-5 zeolite on product distribution in the conversion of methanol to hydrocarbons 被引量:3
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作者 Junhui Li Yanan Wang +4 位作者 Wenzhi Jia Zhiwen Xi Huanhui Chen Zhirong Zhu Zhonghua Hu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2014年第6期771-780,共10页
The external surface of HZSM-5 zeolite was passivated by liquid siliceous deposition and by acidic sites poisoning with lepidine, respectively. Then methanol-to-hydrocarbons (MTH) reaction was investigated over the ... The external surface of HZSM-5 zeolite was passivated by liquid siliceous deposition and by acidic sites poisoning with lepidine, respectively. Then methanol-to-hydrocarbons (MTH) reaction was investigated over the above as-prepared catalysts and the dissoluble coke on these used catalysts was analyzed by GC-MS, to study the role of the external surface of HZSM-5 in the catalytic reaction. Comparison with the experi- mental results based on parent ZSM-5 showed that the product distribution of MTH reaction was obviously influenced by the external surface. Evidences were listed as follows: (1) the final product on parent HZSM-5 showed higher aromatic selectivity, lower olefin selectivity, lower ra- tio of C2/C3+ aliphatics and higher ratio of C3/C4+ aliphatics than the reaction mixture produced by the sole catalysis of acidic sites in HZSM-5 channel; (2) a little of pentamethylbenzene and hexamethylbenzene in the product on parent HZSM-5, was produced via multi-methylation of methylbenzene on the external surface. The above conclusion may also be suitable for MTH reaction over other zeolites with 10-ring channel. 展开更多
关键词 METHANOL-TO-HYDROCARBONS product distribution HZSM-5 external surface acidic sites
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Methane combustion over palladium catalyst within the confined space of MFI zeolite 被引量:10
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作者 Mingyang Gao Zhongmiao Gong +6 位作者 Xuefei Weng Weixiang Shang Yuchao Chai Weili Dai Guangjun Wu Naijia Guan Landong Li 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2021年第10期1689-1699,共11页
Isolated cationic Pd species encapsulated in MFI zeolite,i.e.,Pd@MFI,have been successfully prepared via in situ hydrothermal route followed by oxidative treatment.The as-prepared Pd@MFI samples are investigated as pr... Isolated cationic Pd species encapsulated in MFI zeolite,i.e.,Pd@MFI,have been successfully prepared via in situ hydrothermal route followed by oxidative treatment.The as-prepared Pd@MFI samples are investigated as promising catalysts in the reaction of methane combustion.Typically,Pd@H-ZSM-5 shows remarkable activity in methane catalytic combustion with a low apparent activation energy value of 70.7 kj/mol as well as good catalytic stability even in excess water vapor.Detailed characterization results demonstrate the strong interaction between Pd sites and zeolite framework in Pd@ZSM-5 and the efficient stabilization of isolated Pd sites by zeolite thereof.Spectroscopy analyses reveal that the presence of BrΦnsted acid sites is beneficial to methane adsorption and its subsequent activation on adjacent Pd sites,constructing cooperation between Bronsted acid sites and Pd sites within the confined space of MFI zeolite toward high-efficiency methane catalytic combustion.The reaction mechanism of methane combustion catalyzed by Pd@H-ZSM-5 model catalyst is finally discussed. 展开更多
关键词 Methane combustion Palladium catalyst ZEOLITE ENCAPSULATION BrΦnsted acid sites
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Depolymerization and hydrodeoxygenation of lignin to aromatic hydrocarbons with a Ru catalyst on a variety of Nb-based supports 被引量:8
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作者 Di Ma Shenglu Lu +2 位作者 Xiaohui Liu Yong Guo Yanqin Wang 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2019年第4期609-617,M0006,共10页
Efficient conversion of lignin to aromatic hydrocarbons via depolymerization and subsequent hydrodeoxygenation is important.Previously,we found that NbOx species played a key role in the activation and cleavage of C-O... Efficient conversion of lignin to aromatic hydrocarbons via depolymerization and subsequent hydrodeoxygenation is important.Previously,we found that NbOx species played a key role in the activation and cleavage of C-O bonds in lignin and its model compounds.In this study,commercial niobic acid(HY-340),niobium phosphate(NbPO-CBMM)and lab-made layered niobium oxide(Nb2O5-Layer)were chosen as supports to study the effect of Brosted and Lewis acids on the activation of C-O bonds in lignin conversion.A variety of Ru-loaded,Nb-based catalysts with different Ru particle sizes were prepared and applied to the conversion of p-cresol.The results show that all the Ru/Nb-based catalysts produce high mole yields of C7-C9 hydrocarbons(82.3%-9.1%).What's more,Ru/Nb2O5-Layer affords the best mole yield of C7-C9 hydrocarbons and selectivity for C7-C9 aromatic hydrocarbons,of up to 99.1% and 88.0%,respectively.Moreover,it was found that Lewis acid sites play important roles in the depolymerization of enzymatic lignin into phenolic monomers and the cleavage of the C-O bond of phenols.Additionally,the electronic state and particle size of Ru are significant factors which influence the selectivity for aromatic hydrocarbons.A partial positive charge on the metallic Ru surface and a smaller Ru particle size are beneficial in improving the selectivity for aromatic hydrocarbons. 展开更多
关键词 LIGNIN Aromatic hydrocarbons Nb-based supports Lewis acid sites Ru
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Chemical deactivation of Cu-SAPO-18 deNO_x catalyst caused by basic inorganic contaminants in diesel exhaust 被引量:7
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作者 Shujun Ming Lei Pang +5 位作者 Chi Fan Wen Guo Yahao Dong Peng Liu Zhen Chen Tao Li 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2019年第4期590-599,M0005,共11页
Contaminants(K,Na,Ca,and Mg)were introduced into Cu-SAPO-18 via incipient wetness impregnation to investigate their effect on the selective catalytic reduction of NOx with NH3(NH3-SCR)over Cu-SAPO-18.After the introdu... Contaminants(K,Na,Ca,and Mg)were introduced into Cu-SAPO-18 via incipient wetness impregnation to investigate their effect on the selective catalytic reduction of NOx with NH3(NH3-SCR)over Cu-SAPO-18.After the introduction of contaminants into Cu-SAPO-18,the quantity of acidic sites and Cu^2+ species in catalyst decreases owing to the replacement of H^+ and Cu^2+ by K^+,Na^+,Ca^2+,and Mg^2+.Furthermore,the loss of isolated Cu^2+ induces the generation of CuO and CuAl2O4-like phases,which causes further loss in the Brunauer-Emmett-Teller surface area of the catalyst.Consequently,the deNOx performance of the contaminated Cu-SAPO-18 catalysts drops.Such decline in NH3-SCR performance becomes more pronounced by increasing the contaminant contents from 0.5 to 1.0 mmol/gcatal.In addition,the deactivation influence of the contaminants on Cu-SAPO-18 is presented in the order of K>Na>Ca>Mg,which is consistent with the order of reduction of acidic sites.To a certain degree,the effect of the acidic sites on the deactivation of Cu-SAPO-18 might be more significant than that of isolated Cu2+ and the catalyst framework.Moreover,kinetic analysis of NH3-SCR was conducted,and the results indicate that there is no influence of contaminants on the NH3-SCR mechanism. 展开更多
关键词 Cu-SAPO-18 catalyst Basic inorganic contaminant Selective catalytic reduction of NOx with NH3 acidic site Isolated Cu……2+
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SMFs-supported Pd nanocatalysts in selective acetylene hydrogenation:Pore structure-dependent deactivation mechanism 被引量:5
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作者 Elaheh Esmaeili Ali Morad Rashidi +2 位作者 Yadollah Mortazavi Abbas Ali Khodadadi Mehdi Rashidzadeh 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2013年第5期717-725,共9页
In the present study,CNFs,ZnO and Al2O3 were deposited on the SMFs panels to investigate the deactivation mechanism of Pd-based catalysts in selective acetylene hydrogenation reaction.The examined supports were charac... In the present study,CNFs,ZnO and Al2O3 were deposited on the SMFs panels to investigate the deactivation mechanism of Pd-based catalysts in selective acetylene hydrogenation reaction.The examined supports were characterized by SEM,NH3-TPD and N2adsorption-desorption isotherms to indicate their intrinsic characteristics.Furthermore,in order to understand the mechanism of deactivation,the resulted green oil was characterized using FTIR and SIM DIS.FTIR results confirmed the presence of more unsaturated constituents and then,more branched hydrocarbons formed upon the reaction over alumina-supported catalyst in comparison with the ones supported on CNFs and ZnO,which in turn,could block the pores mouths.Besides the limited hydrogen transfer,N2 adsorption-desorption isotherms results supported that the lowest pore diameters of Al2O3/SMFs close to the surface led to fast deactivation,compared with the other catalysts,especially at higher temperatures. 展开更多
关键词 selective hydrogenation alloy formation acidic site pore structure SMFs-supported Pd nanocatalysts
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