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Facile molybdenum and aluminum recovery from spent hydrogenation catalyst
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作者 Zhenhui Lv Jianan Li +3 位作者 Dong Xue Tao Yang Gang Wang Chong Peng 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第5期72-78,共7页
Industrial catalyst waste has emerged as a hazardous pollutant that requires safe and proper disposal after the unloading process.Finding a valuable and sustainable strategy for its treatment is a significant challeng... Industrial catalyst waste has emerged as a hazardous pollutant that requires safe and proper disposal after the unloading process.Finding a valuable and sustainable strategy for its treatment is a significant challenge compared to traditional methods.In this study,we present a facile method for the recovery of molybdenum and aluminum contents from spent Mo-Ni/Al_(2)O_(3) hydrogenation catalysts through crystallization separation and coprecipitation.Furthermore,the recovered molybdenum and aluminum are utilized as active metals and carriers for the preparation of new catalysts.Their properties were thoroughly analyzed and investigated using various characterization techniques.The hydrogenation activity of these newly prepared catalysts was evaluated on a fixed-bed small-scale device and compared with a reference catalyst synthesized from commercial raw reagents.Finally,the hydrogenation activity of the catalysts was further assessed by using the entire distillate oil of coal liquefaction as the raw oil,specifically focusing on denitrogenation and aromatic saturation.This work not only offers an effective solution for recycling catalysts but also promotes sustainable development. 展开更多
关键词 Waste treatment ALUMINA hydrogenation Catalyst CRYSTALLIZATION Precipitation
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Towards the insights into the deactivation behavior of acetylene hydrogenation catalyst
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作者 Hai-Xia Su Yang Jiao +8 位作者 Jian-Gong Shi Zhi-Wei Yuan Di Zhang Xu-Peng Wang Jing Ren Dan Liu Jian-Zhou Gui Hai-Yang Gao Xiao-Li Xu 《Petroleum Science》 SCIE EI CAS CSCD 2024年第2期1405-1414,共10页
A series of model catalysts were obtained by treating commercial fresh and spent catalysts unloaded from the factory with different methods, including green oil dipping, extraction and high-temperature regeneration;fi... A series of model catalysts were obtained by treating commercial fresh and spent catalysts unloaded from the factory with different methods, including green oil dipping, extraction and high-temperature regeneration;finally, the deactivation behavior of the commercial catalyst for acetylene hydrogenation were studied. The influence of various possible deactivation factors on the catalytic performance was elucidated via detailed structural characterization, surface composition analysis, and activity evaluation.The results showed that green oil, carbon deposit and sintering of active metal were the main reasons for deactivation, among which green oil and carbon deposit led to rapid deactivation, while the activity could be recovered after regeneration by high-temperature calcination. The sintering of active metal components was attributed to the high-temperature regeneration in hydrothermal conditions, which was slow but irreversible and accounted for permanent deactivation. Thus, optimizing the regeneration is expected to extend the service life of the commercial catalyst. 展开更多
关键词 ACETYLENE hydrogenation Green oil Carbon deposit SINTERING Catalyst deactivation
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Relationship between hydrogenation degree and pyrolysis performance of jet fuel
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作者 Qing Liu Tinghao Jia +2 位作者 Lun Pan Jijun Zou Xiangwen Zhang 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第4期35-42,共8页
Understanding the relationship between the chemical composition and pyrolysis performance of endothermic hydrocarbon fuel(EHF) is of great significance for the design and optimization of advanced EHFs. In this work, t... Understanding the relationship between the chemical composition and pyrolysis performance of endothermic hydrocarbon fuel(EHF) is of great significance for the design and optimization of advanced EHFs. In this work, the effect of deep hydrogenation on the pyrolysis of commercial RP-3 is investigated.Fuels with different hydrogenation degrees were obtained by the partially and completely catalytic hydrogenation and their pyrolysis performances were investigated using an apparatus equipped with an electrically heated tubular reactor. The results show that with the increase of hydrogenation degree, fuel conversion almost remains constant during the pyrolysis process(500-650°C, 4 MPa);however, the heat sink increases slightly, and the anti-coking performance significantly improves, which are highly related to their H/C ratios. Detailed characterisations reveal that the difference of the pyrolysis performance can be ascribed to the content of aromatics and cycloalkanes: the former are prone to initiate secondary reactions to form coking precursors, while the latter could act as the hydrogen donor and release hydrogen, which will terminate the radical propagation reactions and suppress the coke deposition. This work should provide the guidance for upgrading EHFs by modulating the composition of EHFs. 展开更多
关键词 RP-3 FUEL PYROLYSIS hydrogenation DEPOSITION
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P-induced electron transfer interaction for enhanced selective hydrogenation rearrangement of furfural to cyclopentanone
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作者 Weichen Wang Hongke Zhang +4 位作者 Yidan Wang Fangyuan Zhou Zhiyu Xiang Wanbin Zhu Hongliang Wang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第5期43-51,共9页
Optimizing the intrinsic activity of non-noble metal by precisely tailoring electronic structure offers an appealing way to construct cost-effective catalysts for selective biomass valorization.Herein,we reported a P-... Optimizing the intrinsic activity of non-noble metal by precisely tailoring electronic structure offers an appealing way to construct cost-effective catalysts for selective biomass valorization.Herein,we reported a P-doping bifunctional catalyst(Ni-P/mSiO_(2))that achieved 96.6%yield for the hydrogenation rearrangement of furfural to cyclopentanone at mild conditions(1 MPaH_(2),150°C).The turnover frequency of Ni-P/mSiO_(2)was 411.9 h^(-1),which was 3.2-fold than that of Ni/mSiO_(2)(127.2 h^(-1)).Detailed characterizations and differential charge density calculations revealed that the electron-deficient Niδ+species were generated by the electron transfer from Ni to P,which promoted the ring rearrangement reaction.Density functional theory calculations illustrated that the presence of P atoms endowed furfural tilted adsorb on the Ni surface by the C=O group and facilitated the desorption of cyclopentanone.This work unraveled the connection between the localized electronic structures and the catalytic properties,so as to provide a promising reference for designing advanced catalysts for biomass valorization. 展开更多
关键词 FURFURAL hydrogenation rearrangement P-DOPING Electron transfer Biomass valorization
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Silica-modified Pt/TiO_(2) catalysts with tunable suppression of strong metal-support interaction for cinnamaldehyde hydrogenation
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作者 Zhengjian Hou Yuanyuan Zhu +6 位作者 Hua Chi Li Zhao Huijie Wei Yanyan Xi Lishuang Ma Xiang Feng Xufeng Lin 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第6期189-198,共10页
Tuning Strong Metal-support Interactions(SMSI)is a key strategy to obtain highly active catalysts,but conventional methods usually enable TiO_(x) encapsulation of noble metal components to minimize the exposure of nob... Tuning Strong Metal-support Interactions(SMSI)is a key strategy to obtain highly active catalysts,but conventional methods usually enable TiO_(x) encapsulation of noble metal components to minimize the exposure of noble metals.This study demonstrates a catalyst preparation method to modulate a weak encapsulation of Pt metal nanoparticles(NPs)with the supported TiO_(2),achieving the moderate suppression of SMSI effects.The introduction of silica inhibits this encapsulation,as reflected in the characterization results such as XPS and HRTEM,while the Ti^(4+) to Ti^(3+) conversion due to SMSI can still be found on the support surface.Furthermore,the hydrogenation of cinnamaldehyde(CAL)as a probe reaction revealed that once this encapsulation behavior was suppressed,the adsorption capacity of the catalyst for small molecules like H_(2) and CO was enhanced,which thereby improved the catalytic activity and facilitated the hydrogenation of CAL.Meanwhile,the introduction of SiO_(2) also changed the surface structure of the catalyst,which inhibited the occurrence of the acetal reaction and improved the conversion efficiency of C=O and C=C hydrogenation.Systematic manipulation of SMSI formation and its consequence on the performance in catalytic hydrogenation reactions are discussed. 展开更多
关键词 Pt catalyst Silica modification hydrogenation CINNAMALDEHYDE Strong metal-support interaction
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Microenvironment and electronic state modulation of Pd nanoparticles within MOFs for enhancing low-temperature activity towards DCPD hydrogenation
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作者 Zhiyuan Liu Changan Wang +8 位作者 Ping Yang Wei Wang Hongyi Gao Guoqing An Siqi Liu Juan Chen Tingting Guo Xinmeng Xu Ge Wang 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第9期112-122,共11页
Precise control of the local environment and electronic state of the guest is an important method of controlling catalytic activity and reaction pathways.In this paper,guest Pd NPs were introduced into a series of hos... Precise control of the local environment and electronic state of the guest is an important method of controlling catalytic activity and reaction pathways.In this paper,guest Pd NPs were introduced into a series of host UiO-67 MOFs with different functional ligands and metal nodes,the microenvironment and local electronic structure of Pd is modulated by introducing bipyridine groups and changing metal nodes(Ce_(6)O_(6) or Zr_(6)O_(6)).The bipyridine groups not only promoted the dispersion Pd NPs,but also facilitated electron transfer between Pd and UiO-67 MOFs through the formation of Pd-N bridges.Compared with Zr6 clusters,the tunability and orbital hybridisation of the 4f electronic structure in the Ce_(6) clusters modulate the electronic structure of Pd through the construction of the Ce-O-Pd interfaces.The optimal catalyst Pd/UiO-67(Ce)-bpy presented excellent low-temperature activity towards dicyclopentadiene hydrogenation with a conversion of>99% and a selectivity of>99%(50℃,10 bar).The results show that the synergy of Ce-O-Pd and Pd-N promotes the formation of active Pd^(δ+),which not only enhances the adsorption of H_(2) and electron-rich C=C bonds,but also contributes to the reduction of proton migration distance and improves proton utilization efficiency.These results provide valuable insights for investigating the regulatory role of the host MOFs,the nature of host-guest interactions,and their correlation with catalytic performance. 展开更多
关键词 Interface regulation Pd^(δ+) MICROENVIRONMENT Electronic state hydrogenation
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CO_(2) hydrogenation to methanol over the copper promoted In_(2)O_(3) catalyst
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作者 Rui Zou Chenyang Shen +4 位作者 Kaihang Sun Xinbin Ma Zhuoshi Li Maoshuai Li Chang-Jun Liu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第6期135-145,I0004,共12页
The metal promoted In_(2)O_(3) catalysts for CO_(2) hydrogenation to methanol have attracted wide attention because of their high activity with high methanol selectivity.However,there was still no experimental confirm... The metal promoted In_(2)O_(3) catalysts for CO_(2) hydrogenation to methanol have attracted wide attention because of their high activity with high methanol selectivity.However,there was still no experimental confirmation if copper could be a good promoter for In_(2)O_(3).Herein,the Cu promoted In_(2)O_(3) catalyst was prepared using a deposition-precipitation method.Such prepared Cu/In_(2)O_(3) catalyst shows significantly higher CO_(2) conversion and space time yield(STY)of methanol,compared to the un-promoted In_(2)O_(3) catalyst.The loading of Cu facilitates the activation of both H_(2) and CO_(2) with the interface between the Cu cluster and defective In_(2)O_(3) as the active site.The Cu/In_(2)O_(3) catalyst takes the CO hydrogenation pathway for methanol synthesis from CO_(2) hydrogenation.It exhibits a unique size effect on the CO adsorption.At temperatures below 250℃,CO adsorption on Cu/In_(2)O_(3) is stronger than that on In_(2)O_(3),causing higher methanol selectivity.With increasing temperatu res,the Cu catalyst aggregates,which leads to the formation of weak CO adsorption site and causes a decrease in the methanol selectivity.Compared with other metal promoted In_(2)O_(3) catalysts,it can be concluded that the catalyst with stronger CO adsorption possesses higher methanol selectivity. 展开更多
关键词 CO_(2)hydrogenation METHANOL Cu In_(2)O_(3) CO SELECTIVITY DFT
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Enhanced Ethylene Production from Electrocatalytic Acetylene Semi-hydrogenation Over Porous Carbon-Supported Cu Nanoparticles
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作者 Li Li Fanpeng Chen +1 位作者 Bo-Hang Zhao Yifu Yu 《Transactions of Tianjin University》 EI CAS 2024年第4期297-304,共8页
Electrocatalytic semi-hydrogenation of acetylene(C_(2)H_(2))over copper nanoparticles(Cu NPs)offers a promising non-petroleum alternative for the green production of ethylene(C2H4).However,server hydrogen evolution re... Electrocatalytic semi-hydrogenation of acetylene(C_(2)H_(2))over copper nanoparticles(Cu NPs)offers a promising non-petroleum alternative for the green production of ethylene(C2H4).However,server hydrogen evolution reaction(HER)competition in this process prominently decreases C2H4 selectivity,thereby hindering its practical application.Herein,a Cu-based composite catalyst,wherein porous carbon with nanoscale pores was used as a support,is constructed to gather the C_(2)H_(2) feedstocks for suppressing the undesirable HER.As a result,the as-prepared catalyst exhibited C_(2)H_(2) conversion of 27.1%and C_(2)H_(4) selectivity of 88.4%at a C2H4 partial current density of 0.25 A/cm^(2) under optimal−1.0 V versus reversible hydrogen electrode(RHE)under the simulated coal-derived C_(2)H_(2) atmosphere,significantly outperforming the single Cu NPs counterparts.In addition,a series of in situ and ex situ experimental results show that not only the porous nature of the carbon support but also the stabilized Cu^(0)–Cu^(+) dual active sites through the strong metal–support interactions enhance the adsorption capacity of C_(2)H_(2),leading to high C_(2)H_(2) partial pressure,restraining the HER and thus improving the C2H4 selectivity. 展开更多
关键词 ELECTROCATALYSIS Cu-based catalyst hydrogenation ETHYLENE SELECTIVITY
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Kinetics insights into size effects of carbon nanotubes'growth and their supported platinum catalysts for 4,6-dinitroresorcinol hydrogenation
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作者 Yan Zhang Xiangxue Zhang +6 位作者 Keng Sang Wenyao Chen Gang Qian Jing Zhang Xuezhi Duan Xinggui Zhou Weikang Yuan 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第8期133-140,共8页
Size effects are a well-documented phenomenon in heterogeneous catalysis,typically attributed to alterations in geometric and electronic properties.In this study,we investigate the influence of catalyst size in the pr... Size effects are a well-documented phenomenon in heterogeneous catalysis,typically attributed to alterations in geometric and electronic properties.In this study,we investigate the influence of catalyst size in the preparation of carbon nanotube(CNT)and the hydrogenation of 4,6-dinitroresorcinol(DNR)using Fe_(2)O_(3)and Pt catalysts,respectively.Various Fe_(2)O_(3)/Al_(2)O_(3)catalysts were synthesized for CNT growth through catalytic chemical vapor deposition.Our findings reveal a significant influence of Fe_(2)O_(3)nanoparticle size on the structure and yield of CNT.Specifically,CNT produced with Fe_(2)O_(3)/Al_(2)O_(3)containing 28%(mass)Fe loading exhibits abundant surface defects,an increased area for metal-particle immobilization,and a high carbon yield.This makes it a promising candidate for DNR hydrogenation.Utilizing this catalyst support,we further investigate the size effects of Pt nanoparticles on DNR hydrogenation.Larger Pt catalysts demonstrate a preference for 4,6-diaminoresorcinol generation at(100)sites,whereas smaller Pt catalysts are more susceptible to electronic properties.The kinetics insights obtained from this study have the potential to pave the way for the development of more efficient catalysts for both CNT synthesis and DNR hydrogenation. 展开更多
关键词 KINETICS Size effects Catalytic hydrogenation Active site
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Tuning the product selectivity of dimethyl oxalate hydrogenation over WO_(x) modified Cu/SiO_(2) catalysts
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作者 Zheng Li Zhuo Ma +9 位作者 Yihui Li Ziang Zhao Yuan Tan Ziyin Liu Xingkun Chen Nian Lei Huigang Wang Wei Lu Hejun Zhu Yunjie Ding 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第10期128-138,I0004,共12页
Product selectivity and reaction pathway are highly dependent on surface structure of heterogeneous catalysts.For vapor-phase hydrogenation of dimethyl oxalate(DMO),"EG route"(DMO→methyl glycolate(MG)ethyle... Product selectivity and reaction pathway are highly dependent on surface structure of heterogeneous catalysts.For vapor-phase hydrogenation of dimethyl oxalate(DMO),"EG route"(DMO→methyl glycolate(MG)ethylene glycol(EG)→ethanol(ET))and"MA route"(DMO→MG→methyl acetate(MA))were proposed over traditional Cu based catalysts and Mo-based or Fe-based catalysts,respectively.Herein,tunable yield of ET(93.7%)and MA(72.1%)were obtained through different reaction routes over WO_(x) modified Cu/SiO_(2) catalysts,and the corresponding reaction route was further proved by kinetic study and in-situ DRIFTS technology.Mechanistic studies demonstrated that H_(2) activation ability,acid density and Cu-WO_(x) interaction on the catalysts were tuned by regulating the surface W density,which resulted in the different reaction pathway and product selectivity.What's more,high yield of MA produced from DMO hydrogenation was firstly reported with the H_(2) pressure as low as 0.5 MPa. 展开更多
关键词 ETHANOL Dimethyl oxalate Selective hydrogenation Methyl acetate WCu/SiO_(2)catalyst
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Regulating the oxidation state of Pd to enhance the selective hydrogenation for 5-hydroxymethylfurfural
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作者 Xin Li Yue Ma +3 位作者 Xuning Wang Jianguo Wu Dong Cao Daojian Cheng 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第8期60-68,共9页
The highly selective hydrogenation of 5-hydroxymethylfurfural to 2,5-dihydroxymethylfuran is an important reaction in the field of biomass hydrogenation,because it is a bridge between biomass resources and chemical in... The highly selective hydrogenation of 5-hydroxymethylfurfural to 2,5-dihydroxymethylfuran is an important reaction in the field of biomass hydrogenation,because it is a bridge between biomass resources and chemical industry.Here,we precisely constructed carbon nitride supported Pd-based catalysts by a simple impregnation-reduction method.By changing the reduction temperature,catalysts with different oxidation state could be precisely constructed.Moreover,the important correlation between the ratio of Pd^(0)/Pd^(2+)and catalytic activity is revealed during the selective hydrogenation of HMF.The Pd/g—C_(3)N_(4)—300 catalyst with a Pd^(0)/Pd^(2+)ratio of 3/2 showed the highest catalytic activity,which could get 96.9%5-hydroxymethylfurfural conversion and 90.3%2,5-dihydroxymethylfuran selectivity.Further density functional theory calculation revealed that the synergistic effect between Pd0and Pd2+in Pd/g—C_(3)N_(4)—300 system could boost the adsorption of the substrate and the dissociation of hydrogen.In this work,we highlight the important correlation between metal oxidation state and catalytic activity,which provides valuable insights for the rational design of precious metal catalysts for hydrogenation reactions. 展开更多
关键词 Pd/g-C_(3)N_(4) Selective hydrogenation 5-HYDROXYMETHYLFURFURAL 2 5-dihydroxymethylfuran Oxidation state
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Effect of Different Morphologies Induced by Solvent on ZIF-67 Derived Co@NC for Catalytic Phenol Hydrogenation
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作者 WANG Dong-wei MA Zhan-wei +2 位作者 LI Jing FENG Hu-lin HU Bin 《分子催化(中英文)》 CAS CSCD 北大核心 2024年第5期399-408,I0001,共11页
The Co@NC catalysts with different morphologies were prepared by two step process,solvent control growth and pyrolysis method.The polyhedral Co@NC-67P-450 catalyst has a relatively high CoNx content and exhibits excel... The Co@NC catalysts with different morphologies were prepared by two step process,solvent control growth and pyrolysis method.The polyhedral Co@NC-67P-450 catalyst has a relatively high CoNx content and exhibits excellent phenol hydrogenation activity(conversion 96.9%)at 160℃,3 MPa,which is higher than that of leaf shaped Co@NC-67L-450 catalyst(conversion 75.4%).We demonstrated Co_(3)O_(4)was reduced to the Co^(0)during the reaction.Moreover,CoNx species contribute to the superior hydrogenation activity of phenol.The Co-based catalysts can be easily recovered through the magnetic separation and performed the high stability. 展开更多
关键词 metal organic frameworks Co-based catalyst MORPHOLOGY phenol hydrogenation
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Pd^(0)-O v-Ce^(3+) Interfacial Sites with Charge Redistribution for Enhanced Hydrogenation of Methyl Oleate to Methyl Stearate
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作者 Zhaohui Meng Ying Liao +6 位作者 Ling Liu Yaqian Li Hao Yan Xiang Feng Xiaobo Chen Yibin Liu Chaohe Yang 《Transactions of Tianjin University》 EI CAS 2024年第4期359-368,共10页
Improving the efficiency of metal/reducible metal oxide interfacial sites for hydrogenation reactions of unsaturated groups(e.g.,C=C and C=O)is a promising yet challenging endeavor.In our study,we developed a Pd/CeO_(... Improving the efficiency of metal/reducible metal oxide interfacial sites for hydrogenation reactions of unsaturated groups(e.g.,C=C and C=O)is a promising yet challenging endeavor.In our study,we developed a Pd/CeO_(2) catalyst by enhancing the oxygen vacancy(O V)concentration in CeO_(2) through high-temperature treatment.This process led to the formation of an interface structure ideal for supporting the hydrogenation of methyl oleate to methyl stearate.Specifi cally,metal Pd^(0) atoms bonded to the O V in defective CeO_(2) formed Pd^(0)-O v-Ce^(3+)interfacial sites,enabling strong electron transfer from CeO_(2) to Pd.The interfacial sites exhibit a synergistic adsorption eff ect on the reaction substrate.Pd^(0) sites promote the adsorption and activation of C=C bonds,while O V preferably adsorbs C=O bonds,mitigating competition with C=C bonds for Pd^(0) adsorption sites.This synergy ensures rapid C=C bond activation and accelerates the attack of active H*species on the semi-hydrogenated intermediate.As a result,our Pd/CeO_(2)-500 catalyst,enriched with Pd^(0)-O v-Ce^(3+)interfacial sites,dem-onstrated excellent hydrogenation activity at just 30℃.The catalyst achieved a Cis-C18:1 conversion rate of 99.8% and a methyl stearate formation rate of 5.7 mol/(h·g metal).This work revealed the interfacial sites for enhanced hydrogenation reactions and provided ideas for designing highly active hydrogenation catalysts. 展开更多
关键词 hydrogenation Interfacial sites Oxygen vacancy C=C bond
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Triple the steady-state reaction rate by decorating the In_(2)O_(3)surface with SiO_(x)for CO_(2)hydrogenation
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作者 Hao Wang Chun Yang +8 位作者 Xiaoyan Yu Mingrui Wang Runze Yang Xiaowa Nie Ben Hang Yin Alex C.K.Yip Chunshan Song Guanghui Zhang Xinwen Guo 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第8期96-105,I0003,共11页
Indium oxide(In_(2)O_(3)),as a promising candidate for CO_(2)hydrogenation to C_(1) products,often suffers from sintering and activity decline,closely related to the undesirable structural evolution under reaction con... Indium oxide(In_(2)O_(3)),as a promising candidate for CO_(2)hydrogenation to C_(1) products,often suffers from sintering and activity decline,closely related to the undesirable structural evolution under reaction conditions.Based on the comprehension of the dynamic evolution,this study presents an efficient strategy to alleviate the agglomeration of In_(2)O_(3)nanoparticles by the surface decoration with highly dispersed silica species(SiO_(x)).Various structural characterizations combined with density functional theory calculations demonstrated that the sintering resulted from the over-reduction,while the enhanced stability originated from the anchoring effect of highly stable In-OSi bonds,which hinders the substantial formation of metallic In(In^(0))and the subsequent agglomeration.0.6Si/In_(2)O_(3)exhibited CO_(2)conversion rate of10.0 mmol g^(-1)h^(-1)at steady state vs.3.5 mmol g^(-1)h^(-1)on In_(2)O_(3)in CO_(2)hydrogenation.Enhanced steady-state activity was also achieved on Pd-modified catalysts.Compared to the traditional Pd/In_(2)O_(3)catalyst,the methanol production rate of Pd catalyst supported on 0.6Si/In_(2)O_(3)was enhanced by 23%,showing the potential of In_(2)O_(3)modified by SiO_(x)in serving as a platform material.This work provides a promising method to design new In_(2)O_(3)-based catalysts with improved activity and stability in CO_(2)hydrogenation. 展开更多
关键词 CO_(2)hydrogenation In_(2)O_(3)sintering Dynamic structural evolution Surface SiO_(x)modification DFT simulations
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Preparation of palladium-based catalyst by plasma-assisted atomic layer deposition and its applications in CO_(2) hydrogenation reduction
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作者 唐守贤 田地 +4 位作者 李筝 王正铎 刘博文 程久珊 刘忠伟 《Plasma Science and Technology》 SCIE EI CAS CSCD 2024年第6期31-39,共9页
Supported Pd catalyst is an important noble metal material in recent years due to its high catalytic performance in CO_(2)hydrogenation.A fluidized-bed plasma assisted atomic layer deposition(FP-ALD) process is report... Supported Pd catalyst is an important noble metal material in recent years due to its high catalytic performance in CO_(2)hydrogenation.A fluidized-bed plasma assisted atomic layer deposition(FP-ALD) process is reported to fabricate Pd nanoparticle catalyst over γ-Al_(2)O_(3)or Fe_(2)O_(3)/γ-Al_(2)O_(3)support,using palladium hexafluoroacetylacetonate as the Pd precursor and H_(2)plasma as counter-reactant.Scanning transmission electron microscopy exhibits that highdensity Pd nanoparticles are uniformly dispersed over Fe_(2)O_(3)/γ-Al_(2)O_(3)support with an average diameter of 4.4 nm.The deposited Pd-Fe_(2)O_(3)/γ-Al_(2)O_(3)shows excellent catalytic performance for CO_(2)hydrogenation in a dielectric barrier discharge reactor.Under a typical condition of H_(2)to CO_(2)ratio of 4 in the feed gas,the discharge power of 19.6 W,and gas hourly space velocity of10000 h^(-1),the conversion of CO_(2)is as high as 16.3% with CH_(3)OH and CH4selectivities of 26.5%and 3.9%,respectively. 展开更多
关键词 atomic layer deposition CO_(2)hydrogenation palladium based catalyst
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Comparison of Perovskite Systems Based on AFeO_(3)(A=Ce,La,Y)in CO_(2) Hydrogenation to CO
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作者 Anna N.Matveyeva Shamil O.Omarov 《Transactions of Tianjin University》 EI CAS 2024年第4期337-358,共22页
CO_(2) is the most cost-eff ective and abundant carbon resource,while the reverse water-gas reaction(rWGS)is one of the most eff ective methods of CO_(2) utilization.This work presents a comparative study of rWGS acti... CO_(2) is the most cost-eff ective and abundant carbon resource,while the reverse water-gas reaction(rWGS)is one of the most eff ective methods of CO_(2) utilization.This work presents a comparative study of rWGS activity for perovskite systems based on AFeO_(3)(where A=Ce,La,Y).These systems were synthesized by solution combustion synthesis(SCS)with diff erent ratios of fuel(glycine)and oxidizer(φ),diff erent amounts of NH 4 NO_(3),and the addition of alumina or silica as supports.Various techniques,including X-ray diff raction analysis,thermogravimetric analysis,Fourier transform infrared spectroscopy(FTIR),scanning electron microscopy,energy-dispersive X-ray spectroscopy,N 2-physisorption,H_(2) temper-ature-programmed reduction,temperature-programmed desorption of H_(2) and CO_(2),Raman spectroscopy,and in situ FTIR,were used to relate the physicochemical properties with the catalytic performance of the obtained composites.Each specifi c perovskite-containing system(either bulk or supported)has its own optimalφand NH_(4) NO_(3) amount to achieve the highest yield and dispersion of the perovskite phase.Among all synthesized systems,bulk SCS-derived La-Fe-O systems showed the highest resistance to reducing environments and the easiest hydrogen desorption,outperforming La-Fe-O produced by solgel combustion(SGC).CO_(2) conversion into CO at 600°C for bulk ferrite systems,depending on the A-cation type and preparation method,follows the order La(SGC)<Y<Ce<La(SCS).The diff erences in properties between La-Fe-O obtained by the SCS and SGC methods can be attributed to diff erent ratios of oxygen and lanthanum vacancy contributions,hydroxyl coverage,morphology,and free iron oxide presence.In situ FTIR data revealed that CO_(2) hydrogenation occurs through formates generated under reaction conditions on the bulk system based on La-Fe-O,obtained by the SCS method.γ-Al_(2)O_(3) improves the dispersion of CeFeO_(3) and LaFeO_(3) phases,the specifi c surface area,and the quantity of adsorbed H_(2) and CO_(2).This led to a signifi cant increase in CO_(2) conversion for supported CeFeO_(3) but not for the La-based system compared to bulk and SiO_(2)-supported perovskite catalysts.However,adding alumina increased the activity per mass for both Ce-and La-based perovskite systems,reducing the amount of rare-earth components in the catalyst and thereby lowering the cost without substantially compromising stability. 展开更多
关键词 Perovskites LaFeO_(3) CeFeO_(3) YFeO_(3) Solution combustion synthesis CO_(2) hydrogenation Reverse water–gas reaction(rWGS)
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Increased Oxygen Vacancies in CuO-ZnO Snowflake-like Composites Drive the Hydrogenation of CO_(2) to Methanol
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作者 San Xiaoguang Wu Wanmeng +4 位作者 Zhang Lei Meng Dan Chang Xiangshuang Tan Jianen Qi Jian 《China Petroleum Processing & Petrochemical Technology》 SCIE CAS CSCD 2024年第2期22-33,共12页
Cu/ZnO is widely used in the hydrogenation of carbon dioxide (CO_(2)) to methanol (CH_(3)OH) to improve the lowconversion rate and selectivity generally observed. In this work, a series of In, Zr, Co, and Ni-doped CuO... Cu/ZnO is widely used in the hydrogenation of carbon dioxide (CO_(2)) to methanol (CH_(3)OH) to improve the lowconversion rate and selectivity generally observed. In this work, a series of In, Zr, Co, and Ni-doped CuO-ZnO catalysts wassynthesized via a hydrothermal method. By introducing a second metal element, the activity and dispersion of the activesites can be adjusted and the synergy between the metal and the carrier can be enhanced, forming an abundance of oxygenvacancies. Oxygen vacancies not only adsorb CO_(2) but also activate the intermediates in methanol synthesis, playing a keyrole in the entire reaction. Co3O4-CuO-ZnO had the best catalytic performance (a CO_(2) conversion rate of 9.17%;a CH_(3)OHselectivity of 92.77%). This study describes a typical strategy for multi-component doping to construct a catalyst with anabundance of oxygen vacancies, allowing more effective catalysis to synthesize CH_(3)OH from CO_(2). 展开更多
关键词 CuO-ZnO catalyst CO_(2)hydrogenation to CH_(3)OH doping oxygen vacancy SYNERGY
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MOF-assisted Synthesis of Dual-atom Palladium Catalysts for Acetylene Semi-hydrogenation
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作者 Chen Jie Xu Yuebing +2 位作者 Qi Jian Liu Bing Liu Xiaohao 《China Petroleum Processing & Petrochemical Technology》 SCIE CAS CSCD 2024年第3期42-52,共11页
The selective removal of trace acetylene in ethylene feed gas is of great significance in the petrochemicalindustry;however, there are still challenges in designing and developing high-performance catalysts. Here, a M... The selective removal of trace acetylene in ethylene feed gas is of great significance in the petrochemicalindustry;however, there are still challenges in designing and developing high-performance catalysts. Here, a MOFassistedencapsulation strategy was adopted for the precise synthesis of diatomic Pd2 sites on a ZnO support. When usedfor the acetylene semi-hydrogenation reaction, the dual-atom Pd2-ZnO catalyst exhibited improved catalytic performance,achieving complete conversion of acetylene at 125 °C with an 89% selectivity to ethene, as compared to Pd single-atom andnanoparticles. This enhancement was mainly attributed to the catalyst’s ability to dissociate H2 and facilitate the desorptionof intermediate C2H4. Moreover, the strong interaction between the support and the diatomic Pd sites was responsible for thecatalyst’s excellent stability during the long-term reaction. 展开更多
关键词 dual-atom palladium acetylene semi-hydrogenation MOFs hydrogen dissociation intermediate
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Effect of Fe Addition on Dehydrogenation Performance of Methylcyclohexance over Pt/Al_(2)O_(3)
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作者 Tong Fengya Tian Hao +2 位作者 Wang Hao Miao Changxi Song Lei 《China Petroleum Processing & Petrochemical Technology》 SCIE CAS CSCD 2024年第1期12-18,共7页
Catalysts with varying Fe contents were prepared using a sequential impregnation method to investigate the effects of Fe addition on the physicochemical properties of Pt/Al_(2)O_(3) and their performance in methylcycl... Catalysts with varying Fe contents were prepared using a sequential impregnation method to investigate the effects of Fe addition on the physicochemical properties of Pt/Al_(2)O_(3) and their performance in methylcyclohexane(MCH)dehydrogenation.The results demonstrated that the addition of Fe to Pt/Al_(2)O_(3) enhanced the electron density of Pt and improved catalytic activity,while exhibiting negligible influence on the catalytic selectivity for toluene.When the Fe content was 0.057%,the catalyst exhibited the highest MCH consumption rate,which was approximately two times higher than that of the catalyst without Fe.Additionally,the incorporation of Fe inhibited the formation of coke and reduced the quantity of coke deposits on the catalyst,thereby improving its catalytic durability.Overall,Fe shows promise as a prospective secondary element for Pt/Al_(2)O_(3) to enhance the MCH dehydrogenation performance. 展开更多
关键词 methylcyclohexane dehydrogenation hydrogen storage DEACTIVATION Fe addition
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Inclusion of CoTiO_(3) to ameliorate the re/dehydrogenation properties of the Mg–Na–Al system
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作者 N.A.Ali N.Y.Yusnizam +3 位作者 N.A.Sazelee Sami-ullah Rather Haizhen Liu M.Ismail 《Journal of Magnesium and Alloys》 SCIE EI CAS CSCD 2024年第3期1215-1226,共12页
For the first time,the MgH_(2)–NaAlH_(4)(ratio 4:1)destabilized system with CoTiO_(3) addition has been explored.The CoTiO_(3)-doped MgH_(2)–NaAlH_(4) sample begins to dehydrogenate at 130℃,which is declined by 40... For the first time,the MgH_(2)–NaAlH_(4)(ratio 4:1)destabilized system with CoTiO_(3) addition has been explored.The CoTiO_(3)-doped MgH_(2)–NaAlH_(4) sample begins to dehydrogenate at 130℃,which is declined by 40℃ compared to the undoped MgH_(2)–NaAlH_(4).Moreover,the de/rehydrogenation kinetics characteristics of the CoTiO_(3)-doped MgH_(2)–NaAlH_(4) were greatly ameliorated.With the inclusion of CoTiO_(3),the MgH_(2)–NaAlH_(4) composite absorbed 5.2 wt.%H_(2),higher than undoped MgH_(2)–NaAlH_(4).In the context of dehydrogenation,the CoTiO_(3)-doped MgH_(2)–NaAlH_(4) sample desorbed 2.6 wt.%H_(2),almost doubled compared to the amount of hydrogen desorbed from the undoped MgH_(2)–NaAlH_(4) sample.The activation energy obtained by the Kissinger analysis for MgH_(2) decomposition was significantly lower by 35.9 kJ/mol than the undoped MgH_(2)–NaAlH_(4) sample.The reaction mechanism demonstrated that new phases of MgCo and AlTi_(3) were generated in situ during the heating process and are likely to play a substantial catalytic function and be useful in ameliorating the de/rehydrogenation properties of the destabilized MgH_(2)–NaAlH_(4) system with the inclusion of CoTiO_(3). 展开更多
关键词 Destabilize system Magnesium hydride Sodium alanate Hydrogen storage Additive.
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