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Atomically dispersed cobalt in MFI zeolite framework for sustainable propane dehydrogenation
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作者 Xiang Fu Jun Yu Weili Dai 《Chinese Journal of Structural Chemistry》 2025年第10期9-10,共2页
Propylene,a pivotal chemical feedstock,is extensively used in synthesizing high-value derivatives such as polypropylene and acrylonitrile[1].Although propylene is predominantly produced via naphtha cracking,a persiste... Propylene,a pivotal chemical feedstock,is extensively used in synthesizing high-value derivatives such as polypropylene and acrylonitrile[1].Although propylene is predominantly produced via naphtha cracking,a persistent supply-demand gap exists[2].Non-oil routes,such as propane dehydrogenation(PDH),are increasingly attractive,particularly with the availability of shale gas[3].Modern non-oxidative PDH heavily relies on Pt nanoparticle catalysts promoted with SnOx(e.g.,PtSn/Al2O3 used in Honeywell UOP's Oleflex process)[4].However,these systems suffer from inherent limitations:high Pt costs,coke formation via deep dehydrogenation,and sintering during regeneration-necessitating environmentally detrimental oxychlorination treatments to restore activity[5]. 展开更多
关键词 naphtha crackinga sustainable propane dehydrogenation propane dehydrogenation pdh shale gas modern pt nanoparticle catalysts honeywell uops oleflex atomically dispersed cobalt chemical feedstockis
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Deciphering origins of hydrocarbon deposits by means of intramolecular carbon isotopes of propane adsorbed on sediments 被引量:1
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作者 Peng Liu Xiao-Feng Wang +6 位作者 Jie Wang Juske Horita Zhi-Yong Wang Ying Lin Rui-Liang Guo Fu-Qi Li Wen-Hui Liu 《Petroleum Science》 2025年第2期546-556,共11页
Hydrocarbons are one of the important fluids within the Earth's crust,and different biotic and abitoic processes can generate hydrocarbon during geological periods.Tracing the sources and sinks of hydrocarbons can... Hydrocarbons are one of the important fluids within the Earth's crust,and different biotic and abitoic processes can generate hydrocarbon during geological periods.Tracing the sources and sinks of hydrocarbons can help us better understand the carbon cycle of the earth.In this study,an improved approach of adsorbed hydrocarbons extraction from sediments was established.The improved thermal desorption approach,compound-specific isotope analysis and position-specific isotope analysis were integrated to investigate the molecular and intramolecular isotope fractionation between trace hydrocarbon gases within sediments and geological hydrocarbon deposits.The isotopic compositions of the terminal position carbon of propane(δ^(13)C_(terminal))serves as a correlation indicator between trace hydrocarbon gases within sediments and geological hydrocarbon deposits.The tight sandstone gas from the Turpan-Hami Basin is a first case study for the application of this novel method to trace hydrocarbon origins.The results showed that the hydrocarbons in the tight sandstone gases in the study area most likely originated from humic organic matter(typeⅢkerogen)at an early mature stage.δ^(13)C_(terminal)values of the thermally desorbed propane gases from different source rocks were distinguishable and the values of the tight sandstone gases significantly overlap with those of the Lower Jurassic Sangonghe source rocks,suggesting their genetic relationship.Overall,the results provided novel position-specific carbon isotopic constraints on origins of hydrocarbons. 展开更多
关键词 Hydrocarbon origins Intramolecular isotope distributions Position-specific isotope analysis(PSIA) propane
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A propane‑selective metal‑organic framework for inverse selective adsorption propane/propylene separation
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作者 YANG Shanqing WANG Lulu +3 位作者 ZHANG Qiang LI Jiajia LI Yilong HU Tongliang 《无机化学学报》 北大核心 2025年第10期2138-2148,共11页
We report a robust pillar-layered metal-organic framework,Zn‑tfbdc‑dabco(tfbdc:tetrafluoroterephthal-ate,dabco:1,4-diazabicyclo[2.2.2]octane),featuring the fluorinated pore environment,for the preferential binding of ... We report a robust pillar-layered metal-organic framework,Zn‑tfbdc‑dabco(tfbdc:tetrafluoroterephthal-ate,dabco:1,4-diazabicyclo[2.2.2]octane),featuring the fluorinated pore environment,for the preferential binding of propane over propylene and thus highly inverse selective separation of propane/propylene mixture.The inverse propane-selective performance of Zn‑tfbdc‑dabco for the propane/propylene separation was validated by single-component gas adsorption isotherms,isosteric enthalpy of adsorption calculations,ideal adsorbed solution theory calculations,along with the breakthrough experiment.The customized fluorinated networks served as a propane-trap to form more interactions with the exposed hydrogen atoms of propane,as unveiled by the simulation studies at the molecular level.With the advantage of inverse propane-selective adsorption behavior,high adsorption capacity,good cycling stability,and low isosteric enthalpy of adsorption,Zn‑tfbdc‑dabco can be a promising candidate adsorbent for the challenging propane/propylene separation to realize one-step purification of the target propylene substance. 展开更多
关键词 metal-organic framework propane/propylene separation inverse selective adsorption separation
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Unsaturated cobalt single-atoms stabilized by silanol nests of zeolites for efficient propane dehydrogenation
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作者 Liwen Guo Dao Shi +4 位作者 Tianjun Zhang Yanhang Ma Guodong Qi Jun Xu Qiming Sun 《Chinese Journal of Catalysis》 2025年第5期323-333,共11页
Propane dehydrogenation(PDH)has emerged as a key on-purpose technology for the production of propylene,but it often depends on toxic chromium and expensive platinum catalysts,highlighting the need for environmentally ... Propane dehydrogenation(PDH)has emerged as a key on-purpose technology for the production of propylene,but it often depends on toxic chromium and expensive platinum catalysts,highlighting the need for environmentally friendly and cost-effective alternatives.In this study,we developed a facile impregnation method to fabricate unsaturated Co single-atoms with a tricoordinated Co_(1)O_(3)H_(x) structure by regulating silanol nests in purely siliceous Beta zeolites.Detailed PDH catalytic tests and characterizations revealed a positive correlation between the presence of silanol nests and enhanced catalytic activity.Additionally,the unsaturated Co single-atoms exhibited a carbon deposition rate more than an order of magnitude slower than that of Co nanoparticles.Notably,the optimized Co_(0.3%)/deAl-meso-Beta catalyst achieved a record-high propylene formation rate of 21.2 mmol_(C3H6) g_(cat)^(-1) h^(-1),with an exceptional propylene selectivity of 99.1%at 550℃.Moreover,the Co_(0.3%)/deAl-meso-Beta catalyst demonstrated excellent stability,with negligible deactivation after 5 consecutive regeneration cycles.This study emphasizes the pivotal role of silanol nests of zeolites in stabilizing and modulating the coordination environment of metallic active sites,providing valuable insights for the design of high-activity,high-stability,and low-cost PDH catalysts. 展开更多
关键词 propane dehydrogenation Unsaturated cobalt Single-atoms Silanol nest Zeolite
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Understanding the reaction-induced restructuring of CoO_(x) species in silicalite-1 to control selectivity in non-oxidative dehydrogenation of propane
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作者 Qiyang Zhang Vita AKondratenko +8 位作者 Xiangnong Ding Jana Weiss Stephan Bartling Elizaveta Fedorova Dan Zhao Dmitry E.Doronkin Dongxu Wang Christoph Kubis Evgenii V.Kondratenko 《Chinese Journal of Catalysis》 2025年第7期108-119,共12页
Non-oxidative dehydrogenation of propane(PDH)is an important route for large-scale on purpose propene production.Although cobalt-based catalysts are promising alternatives to currently used platinum-or chromium oxide-... Non-oxidative dehydrogenation of propane(PDH)is an important route for large-scale on purpose propene production.Although cobalt-based catalysts are promising alternatives to currently used platinum-or chromium oxide-based catalysts,their further developments are hindered by the uncertainties related to the kind of the active sites involved in the desired and side reactions.To contribute to closing such a gap,we systematically investigate the role of oxidized CoO_(x) and metallic Co0 species in the PDH reaction over catalysts based in Silicalite-1 with supported CoO_(x) species differing in their redox properties.C_(3)H_(8) pulse experiments with sub-millisecond and second resolution at pulse sizes of about 13 and 2200 nmol,respectively,combined with in-depth catalyst characterization and PDH tests at different propane conversions enabled us to understand how the reaction-induced reduction of CoO_(x) affects product selectivity.Propane readily reacts with CoO_(x) to yield propene,carbon oxides and water.The formed Co0 species show high activity to coking and cracking reactions.However,if the size of such species is below 2 nm,these undesired reactions are significantly hindered due to the coverage of the active sites by carbon-containing species.The remaining uncovered surface Co0 sites selectively dehydrogenate propane to propene.The best-performing catalyst showed higher activity than a commercial-like K-CrOx/Al_(2)O_(3) and operated durable in a series of 10 dehydrogenation/regeneration cycles under industrial relevant conditions.The space time yield of propene formation of 0.97 kg·h^(-1)·kgcat^(-1) was achieved at 550℃,52%equilibrium propane conversion and 95% propene selectivity. 展开更多
关键词 propane DEHYDROGENATION PROPENE Cobalt Mechanism
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Revisiting the origin of the superior performance of defective zirconium oxide catalysts in propane dehydrogenation:Double-edged oxygen vacancy
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作者 Yuqing Tang Yanjun Chen +4 位作者 Aqsa Abid Zichun Meng Xiaoying Sun Bo Li Zhen Zhao 《Chinese Journal of Catalysis》 2025年第1期272-281,共10页
Recent studies have revealed the extraordinary performance of zirconium oxide in propane dehydrogenation,which is attributed to the excellent reactivity of the coordinatively unsaturated zirconium sites(Zr_(cus))aroun... Recent studies have revealed the extraordinary performance of zirconium oxide in propane dehydrogenation,which is attributed to the excellent reactivity of the coordinatively unsaturated zirconium sites(Zr_(cus))around the oxygen vacancies.The origin of the enhanced catalytic activity of ZrO_(2)with defective tetrahedral Zr sites was examined by direct comparison with its pristine counterpart in the current study.Electronic-structure analysis revealed that electrons from oxygen removal were localized within vacancies on the defective surface,which directly attacked the C-H bond in propane.The involvement of localized electrons activates the C-H bond via back-donation to the antibonding orbital on the defective surface;conversely,charge is transferred from propane to the pristine surfaces.The barrier for the first C-H bond activation is clearly significantly reduced on the defective surfaces compared to that on the pristine surfaces,which verifies the superior activity of Zr_(cus).Notably,however,the desorption of both propene and hydrogen molecules from Zr_(cus)is more difficult due to strong binding.The calculated turnover frequency(TOF)for propene formation demonstrates that the pristine surfaces exhibit better catalytic performance at lower temperatures,whereas the defective surfaces have a larger TOF at high temperatures.However,the rate-determining step and reaction order on the defective surface differ from those on the pristine surface,which corroborates that the catalysts follow different mechanisms.A further optimization strategy was proposed to address the remaining bottlenecks in propane dehydrogenation on zirconium oxide. 展开更多
关键词 propane dehydrogenation Zirconium oxide Oxygenvacancy Densityfunctional theory Microkinetic
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Hierarchical zeolites stabilized cobalt(II)as propane dehydrogenation catalyst:Enhanced activity and coke tolerance via alkaline post-treatment
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作者 Kun Yang Anhui Li +7 位作者 Peng Zhang Guilin Liu Liusai Huang Yumeng Fo Luyuan Yang Xiangyang Ji Jian Liu Weiyu Song 《Chinese Chemical Letters》 2025年第5期348-353,共6页
Transition metal cobalt exhibits strong activation capabilities for alkanes,however,the instability of Co sites leads to sintering and coke deposition,resulting in rapid deactivation.Hierarchical zeolites,with their d... Transition metal cobalt exhibits strong activation capabilities for alkanes,however,the instability of Co sites leads to sintering and coke deposition,resulting in rapid deactivation.Hierarchical zeolites,with their diverse pore structures and high surface areas,are used to effectively anchor metals and enhance coke tolerance.Herein,a post-treatment method using an alkaline solution was employed to synthesize meso-microporous zeolite supports,which were subsequently loaded with Co species for propane dehydrogenation catalyst.The results indicate that the application of NaOH,an inorganic base,produces supports with a larger mesopore volume and more abundant hydroxyl nests compared to TPAOH,an organic base.UV-vis,Raman,and XPS analyses reveal that Co in the 0.5Co/SN-1-0.05 catalyst is mainly in the form of tetrahedral Co^(2+),which effectively activates C-H bonds.In contrast,the 0.5Co/S-1 catalyst contains mainly Co_(3)O_(4)species.Co^(2+)supported on hierarchical zeolites shows better propane conversion(58.6%)and propylene selectivity(>96%)compared to pure silica zeolites.Coke characterization indicates that hierarchical zeolites accumulate more coke,but it is mostly in the form of easily removable disordered carbon.The mesopores in the microporous zeolite support help disperse the active Co metal and facilitate coke removal during dehydrogenation,effectively preventing deactivation from sintering and coke coverage. 展开更多
关键词 propane dehydrogenation Hierarchical zeolites Different alkaline treatment Cobalt catalyst Coke tolerance
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Engineering the electronic structure of Pt-KOx cluster catalyst via alkali metal for efficient oxidative dehydrogenation of propane using CO_(2)
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作者 Wanting Li Xinxin Cao +6 位作者 Meiying Dai Tianchang Wang Nannan Sun Jiong Li Wei Han Wei Wei Xinqing Chen 《Journal of Energy Chemistry》 2025年第11期301-310,I0009,共11页
The oxidative dehydrogenation of propane to propylene using CO_(2)(CO_(2)-ODH)offers a promising route for both propylene production and CO_(2)utilization.In this study,we investigate the effect of alkali metal doping... The oxidative dehydrogenation of propane to propylene using CO_(2)(CO_(2)-ODH)offers a promising route for both propylene production and CO_(2)utilization.In this study,we investigate the effect of alkali metal doping on Pt-based catalysts in CO_(2)-ODH reactions.The optimized 0.1 KPt/S-1 catalyst achieved a high propane conversion of 48.3%,propylene selectivity of 85.5%,and CO_(2)conversion of 19.1%at a low temperature of 500℃with the Pt loading of 0.2 wt%and K loading of 0.1 wt%respectively.Characterization techniques,including high-resolution transmission electron microscope(HR-TEM),CO-diffuse reflectance infrared Fourier transform spectroscopy(CO-DRIFTS),X-ray absorption fine structure(XAFS),and X-ray Photoelectron Spectroscopy(XPS),revealed that the doping of K with Pt led to a strong interaction between potassium and platinum(Pt-KO_(x)cluster).This interaction resulted in a reduction of Pt particle size and a local enrichment of electron density around Pt atoms.These structural modifications improved the anchoring of Pt nanoparticles and enhanced Pt atom dispersion,thereby enhancing the activity of the catalyst and minimizing side reactions.Additionally,pyridine infrared(Py-IR)and temperature-programmed desorption(TPD)studies demonstrated that the prepared0.1 KPt/S-1 catalyst exhibited optimal acidity,which promoted C–H activation and facilitated the efficient adsorption and activation of CO_(2).These dual effects significantly lowered the activation energy for CO_(2)-ODH,enabling efficient dehydrogenation to propylene at a lower temperature of 500℃.This work highlights the critical role of alkali metal doping in modifying the electronic properties of Pt and optimizing catalyst acidity,which collectively contribute to the enhanced performance of the 0.1 KPt/S-1 catalyst.These findings offer valuable insights into the mechanistic pathway of CO_(2)-ODH and provide a foundation for the rational design of high-performance dehydrogenation catalysts. 展开更多
关键词 CATALYSIS ZEOLITE propane dehydrogenation CO_(2)-utilization Alkali metal
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Platinum clusters stabilized by zincosilicate zeolite for efficient propane dehydrogenation
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作者 Hao Liu Ying Zhang +11 位作者 Liyang Liu Tianxiang Chen Xingcong Zhang Peng Hu Chao Xiong Jie Zhou Hao Zhang Lihui Dong Tsz Woon Benedict Lo Bing Nan Xiaohui He Hongbing Ji 《Chinese Journal of Catalysis》 2025年第4期208-219,共12页
Dispersing metals from nanoparticles to clusters is often achieved using ligand protection methods,which exhibit unique properties such as suppressing structure-sensitive side reactions.However,this method is limited ... Dispersing metals from nanoparticles to clusters is often achieved using ligand protection methods,which exhibit unique properties such as suppressing structure-sensitive side reactions.However,this method is limited by the use of different metal precursor salts corresponding to different ligands.An alternative approach,the ion exchange(IE)method,can overcome this limitation to some extent.Nevertheless,there is still an urgent need to address the stabilization of metals(especially precious metals)by using IE method.Here,we reported a Pt cluster catalyst prepared mainly by anchoring Pt atoms via O located near the framework Zn in zincosilicate zeolites and riveted by zeolite surface rings after reduction(reduced Pt/Zn-3-IE).The catalyst can achieve an initial propane conversion of 26%in a pure propane atmosphere at 550℃and shows little deactivation even after 7.5 d of operation.Moreover,the alteration of catalyst by the introduction of framework Zn was also highlighted and interpreted. 展开更多
关键词 Zincosilicate zeolite Acid-site identification Rivet effect Pt clusters propane dehydrogenation
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Efficient carbon integration of CO_(2)in propane aromatization over acidic zeolites
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作者 Cheng Li Xudong Fang +7 位作者 Bin Li Siyang Yan Zhiyang Chen Leilei Yang Shaowen Hao Hongchao Liu Jiaxu Liu Wenliang Zhu 《Chinese Journal of Catalysis》 2025年第5期314-322,共9页
Direct converting carbon dioxide(CO_(2))and propane(C_(3)H_(8))into aromatics with high carbon utilization offers a desirable opportunity to simultaneously mitigate CO_(2)emission and adequately utilize C_(3)H_(8) in ... Direct converting carbon dioxide(CO_(2))and propane(C_(3)H_(8))into aromatics with high carbon utilization offers a desirable opportunity to simultaneously mitigate CO_(2)emission and adequately utilize C_(3)H_(8) in shale gas.Owing to their thermodynamic resistance,converting CO_(2)and C_(3)H_(8) respectively remains difficult.Here,we achieve 60.2%aromatics selectivity and 48.8%propane conversion over H-ZSM-5-25 via a zeolite-catalyzing the coupling of CO_(2)and C_(3)H_(8).Operando dual-beam FTIR spectroscopy combined with ^(13)C-labeled CO_(2)tracing experiments revealed that CO_(2)is directly involved in the generation of aromatics,with its carbon atoms selectively embedded into the aromatic ring,bypassing the reverse water-gas shift pathway.Accordingly,a cooperative aromatization mechanism is proposed.Thereinto,lactones,produced from CO_(2)and olefins,are proven to be the key intermediate.This work not only provides an opportunity for simultaneous conversion of CO_(2)and C_(3)H_(8),but also expends coupling strategy designing of CO_(2)and alkanes over acidic zeolites. 展开更多
关键词 CO_(2)utilization propane aromatization Coupling effect Acidic zeolites LACTONE
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Efficient propane dehydrogenation catalyzed by Ru nanoparticles anchored on a porous nitrogen-doped carbon matrix
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作者 Tianyi Yang Fangxi Su +4 位作者 Dehuan Shi Shenghong Zhong Yalin Guo Zhaohui Liu Jianfeng Huang 《Chinese Chemical Letters》 2025年第2期202-205,共4页
Propane dehydrogenation(PDH)is a vital industrial process for producing propene,utilizing primarily Cr-based or Pt-based catalysts.These catalysts often suffer from challenges such as the toxicity of Cr,the high costs... Propane dehydrogenation(PDH)is a vital industrial process for producing propene,utilizing primarily Cr-based or Pt-based catalysts.These catalysts often suffer from challenges such as the toxicity of Cr,the high costs of noble metals like Pt,and deactivation issues due to sintering or coke formation at elevated temperatures.We introduce an exceptional Ru-based catalyst,Ru nanoparticles anchored on a nitrogendoped carbon matrix(Ru@NC),which achieves a propane conversion rate of 32.2%and a propene selectivity of 93.1%at 550°C,with minimal coke deposition and a low deactivation rate of 0.0065 h^(-1).Characterizations using techniques like TEM and XPS,along with carefully-designed controlled experiments,reveal that the notable performance of Ru@NC stems from the modified electronic state of Ru by nitrogen dopant and the microporous nature of the matrix,positioning it as a top contender among state-of-the-art PDH catalysts. 展开更多
关键词 propane dehydrogenation Ru nanoparticles Porous carbon matrix Ru@NC Electronic interaction
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Boosting the first C-H bond activation of propane on rod-like V/CeO_(2)catalyst by photo-assisted thermal catalysis
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作者 Xiangyang Ji Yishuang Chen +3 位作者 Peng Zhang Shaojia Song Jian Liu Weiyu Song 《Chinese Chemical Letters》 2025年第5期320-324,共5页
Crystalized CeO_(2)structures were typically considered potential photocatalysts due to their great capacity to alter the active sites’size and ability to absorb light.However,the controllable fabrication of well-def... Crystalized CeO_(2)structures were typically considered potential photocatalysts due to their great capacity to alter the active sites’size and ability to absorb light.However,the controllable fabrication of well-defined hierarchical structures of CeO_(2)with high reactive facets is significant and challenging.Herein,a series of CeO_(2)supports including hierarchical flower-like(F-CeO_(2)),ball-like(B-CeO_(2)),cube-like(C-CeO_(2)),and rod-like CeO_(2)(R-CeO_(2))supports were prepared by hydrothermal method(BCeO_(2),R-CeO_(2)and C-CeO_(2))or ice-bath method(F-CeO_(2))respectively.V atoms were selected as the active atoms and loaded on these supports.Their structure-activity relationship in photo-assisted thermal propane dehydrogenation(PTPDH)was investigated systematically.The samples were characterized by Xray diffraction,scanning electron microscopy,transmission electron microscopy,N2 adsorption-desorption isotherms,and Fourier transform infrared spectrum.Results show that R-CeO_(2)support exhibits the biggest surface area thus achieving the best dispersion of VOx species.UV-vis spectrum and photoluminescence spectrum indicate that V/F-CeO_(2)has the best light adsorption property and V/R-CeO_(2)has the best carrier migration capacity.The activity tests demonstrate that the V/R-CeO_(2)has the largest net growth rate and the V/F-CeO_(2)has the biggest relative growth ratio.Furthermore,the non-thermal effect was confirmed by the kinetic method,which lowers the propane reaction orders,selectively promoting the first C-H bond activation.The light radiation TPSR experiment confirmed this point.DFT calculations show a good linear relationship between the energy barrier and the exchanged electron number.It inspires the design of high-reactive facets for boosting the intrinsic activity of the C-H bond in photoassisted thermal chemical processes. 展开更多
关键词 propane dehydrogenation Facet engineering Photothermal effect Electrons transfer Reaction kinetics
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Inhibitory Effect of Water on Propane Dehydrogenation over Metal Oxides via Dissociative Adsorption
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作者 Ziyi Li Pengli Yang +4 位作者 Zelin Wu Donglong Fu Zhi-Jian Zhao Sai Chen Chunlei Pei 《Transactions of Tianjin University》 2025年第6期579-589,共11页
Metal oxide catalysts are widely employed in propane dehydrogenation(PDH)for propylene synthesis,requiring sequential reduction-reaction-regeneration cycles.However,the eff ect of water present in the inlet gas or rea... Metal oxide catalysts are widely employed in propane dehydrogenation(PDH)for propylene synthesis,requiring sequential reduction-reaction-regeneration cycles.However,the eff ect of water present in the inlet gas or reactor on the catalytic per-formance of various metal oxides remains insuffi ciently understood.This study examines the infl uence of water on supported metal oxide catalysts,specifi cally CoO x/Al_(2)O_(3),VO x/Al_(2)O_(3),and an industrial analog CrO x/Al_(2)O_(3) catalyst.By combining titration experiments,in situ Fourier transform infrared spectroscopy,kinetic analysis,and isotopic techniques,we demon-strate that even trace amounts of water can markedly suppress PDH performance via dissociative adsorption on the oxide surface.Methanol pretreatment eff ectively scavenges adsorbed water,recovering Lewis acid-base sites and consequently restoring PDH activity.This work underscores the profound inhibitory role of trace water in PDH over metal oxide catalysts and illustrates the potential of methanol pretreatment as an effective strategy to mitigate this limitation. 展开更多
关键词 propane dehydrogenation Metal oxide catalysts Water inhibition Dissociative adsorption Methanol pretreatment
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A hybrid azolate framework for record propylene/propane sieving separation
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作者 Yiwen Yuan Lingyao Wang Yuanbin Zhang 《Chinese Journal of Structural Chemistry》 2025年第5期3-5,共3页
As an important chemical product,propylene(C_(3)H_(6))is widely used in production of many crucial chemical products such as polypropylene.Propane(C_(3)H_(8))is introduced as an inevitable gas impurity during the naph... As an important chemical product,propylene(C_(3)H_(6))is widely used in production of many crucial chemical products such as polypropylene.Propane(C_(3)H_(8))is introduced as an inevitable gas impurity during the naphtha cracking in propylene production.At present,thermal-driven energy-intensive cryogenic distillation is the most common purification method in industry.An energy-efficient,cost-effective and environmental-friendly separation technology is required to get polymer grade C_(3)H_(6)(higher than 99.5%).In face of the increasing demand of propylene,new separation technology based on porous adsorbents is expected to be a promising alternative.In recent years,metal-organic frameworks(MOFs)have obtained attention by their high porosity,regular adjustable pore shape and pore environment and keep making breakthroughs in separation and purification of many industrial gas mixtures,and are thus considered as one of the most potential types of adsorbents.The physical properties of C_(3)H_(6)and C_(3)H_(8),such as boiling point,size and kinetic diameter,are close to each other,making their separation a challenge.Most C_(3)H_(6)/C_(3)H_(8)sieving MOFs based on narrow sieving channels that restrict the access of molecules larger than their confined entrance purify mixtures at the cost of diffusion and capacity.To improve the adsorption of MOFs based on molecular sieving,a novel‘pearl-necklace’strategy was designed,which was named for its connected channel and molecular pocket vividly,but the diffusion limitation remains unsolved. 展开更多
关键词 propylene propane sieving separation naphtha cracking production many crucial chemical products gas impurity hybrid azolate frameworks purification method chemical productpropylene cryogenic distillation
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Vanadium-based catalysts for propane direct dehydrogenation to propylene:Modification strategies and research direction
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作者 Manqi Zhao Heting Hou +5 位作者 Dehua He Huimin Liu Shaoyuan Sun Dezheng Li Chao Wang Yiming Lei 《Chinese Journal of Structural Chemistry》 2025年第11期121-135,共15页
Direct propane dehydrogenation(DPDH)represents a highly attractive route for on-purpose propylene production,a key building block in the petrochemical industry.In particular,among various catalytic platforms,vanadium-... Direct propane dehydrogenation(DPDH)represents a highly attractive route for on-purpose propylene production,a key building block in the petrochemical industry.In particular,among various catalytic platforms,vanadium-based catalysts have emerged as promising candidates due to their tunable properties including redox ability,surface acidity,and resistance to coking.Although the catalytic community has obtained great achievement in this area,how to promote vanadium-based catalysts towards the next step in DPDH applications like industrial-level implementations is still challenging.Moreover,there are still several controversial theories in our community,meaning it is necessary to clarify these indistinct points to pave the way for the next generation of research.Herein,the pivotal modification strategies of vanadium-based catalysts have been summarized via introducing representative works.In addition,the current unclear mechanism and research gaps,especially in the issues of deactivation and selectivity control,are also revealed so that the potential research directions are well-founded proposed.By integrating fundamental understanding and practical considerations,this review aims to inspire the further development of vanadium-based DPDH catalysts for in-depth academic research and next-generation industrial deployment. 展开更多
关键词 Direct propane dehydrogenation Vanadium-based catalysts Modification strategies Catalysis
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A Comprehensive Review of Platinum-Based Catalysts for Propane Dehydrogenation:Strategies and Machine Learning Insights for Performance Optimization
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作者 Bi Wu Sihan Sun +2 位作者 Jimei Zhang Lei Wang Yanchun Shi 《Carbon and Hydrogen》 2025年第2期164-190,共27页
Propane dehydrogenation(PDH)is a key process for increasing the production of propylene,which is an important part of the chemical industry.Platinum-based catalysts have emerged as efficient catalysts for this reactio... Propane dehydrogenation(PDH)is a key process for increasing the production of propylene,which is an important part of the chemical industry.Platinum-based catalysts have emerged as efficient catalysts for this reaction due to their excellent activity and selectivity.However,challenges such as high platinum cost,catalyst deactivation,and side reactions remain significant barriers to their widespread use in industry.This review provides a comprehensive overview of recent advances in platinumbased catalysts for PDH,focusing on strategies to optimize their performance.We discuss the design and synthesis of Pt-based catalysts,emphasizing the role of promoters,such as Sn,Zn,Ga,and other promoters,in improving selectivity and stability.We also explore the effects of support materials and zeolite encapsulated catalysts on dispersion and activity for Pt-based catalysts.In addition,we highlight the use of machine learning to predict catalyst performance and guide the development of nextgeneration Pt-based catalyst materials.This review synthesizes insights from experimental studies and machine learning computational modeling and aims to provide a route for overcoming the limitations of Pt-based catalysts and advancing the PDH process. 展开更多
关键词 machine learning PROMOTION propane dehydrogenation Pt-based catalysts
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Highly dispersed Pt/Co_(3)O_(4)catalyst constructed by vacancy defect inductive effect for enhanced catalytic propane total oxidation
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作者 Chao Feng Gaoyan Xiong +8 位作者 Chong Chen Yan Lin Zhong Wang Yukun Lu Fang Liu Xuebing Li Yunqi Liu Runduo Zhang Yuan Pan 《Chinese Journal of Catalysis》 2025年第8期21-33,共13页
Directional design of efficient catalysts for volatile organic compounds degradation remains a complex,yet effective and challenging process.Herein,oxygen-rich vacancy Co_(3)O_(4)-anchored Pt catalysts were prepared t... Directional design of efficient catalysts for volatile organic compounds degradation remains a complex,yet effective and challenging process.Herein,oxygen-rich vacancy Co_(3)O_(4)-anchored Pt catalysts were prepared through atom-trapping strategy and relevant vacancy defect inductive effect was proposed.The 0.6Pt/VO-Co_(3)O_(4)catalyst presented a reaction rate value of 32.2×10^(-5)mol·g_(cat)^(-1)·s^(-1)at 160℃for catalytic propane total oxidation,which was nearly 5 times the reaction rate of Co_(3)O_(4)(6.7×10^(-5)mol·g_(cat)^(-1)·s^(-1)).Also,it exhibited excellent water-resistance and catalytic stability.The Pt atoms were stabilized on the Co_(3)O_(4)surface by vacancy defects to improve dispersion.Meanwhile,the vacancy defect inductive effect induced stronger electron interaction between Pt and Co_(3)O_(4)on the surface,thus promote the redox ability at low-temperature.The mobility and oxygen-activating ability of surface lattice oxygen were also strengthened by the vacancy defect inductive effect.This facilitated the generation of more surface-active oxygen species for the cleavage of C-H bond and the deep oxidation of intermediate species.Overall,this study proposed a novel concept the fabrication of highly efficient catalysts for the purpose of catalytic oxidation. 展开更多
关键词 propane total oxidation Pt/Co_(3)O_(4) Oxygen vacancy Defect inductive effect Synergetic catalysis
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PtSnNa/SUZ-4:An efficient catalyst for propane dehydrogenation 被引量:9
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作者 周华兰 龚静静 +4 位作者 许波连 邓生财 丁元华 俞磊 范以宁 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2017年第3期529-536,共8页
The structure and catalytic properties of PtSn catalysts supported on SUZ-4 and ZSM-5 zeolite have been studied by using various experimental techniques including XRD,nitrogen adsorption,NH3-TPD,TG,H2-TPR and TPO tech... The structure and catalytic properties of PtSn catalysts supported on SUZ-4 and ZSM-5 zeolite have been studied by using various experimental techniques including XRD,nitrogen adsorption,NH3-TPD,TG,H2-TPR and TPO techniques combined with propane dehydrogenation tests.It has been shown that SUZ-4-supported PtSnNa(PtSnNa/SUZ-4) was determined to be a better catalyst for propane dehydrogenation than conventional catalysts supported on ZSM-5,owing to its higher catalytic activity and stability.Dibenzothiophene poisoning experiments were performed to investigate the detailed structures of the two supported catalysts.The characterization of the two catalysts indicates that the distribution of Pt on the porous support affects the activity.In contrast to ZSM-5-supported catalysts,Pt particles on the PtSnNa/SUZ-4 are primarily dispersed over the external surface and are not as readily deactivated by carbon deposition.This is because that the strong acid sites of the SUZ-4 zeolite evidently prevented the impregnation of the Pt precursor H_2PtCl_6 into the zeolite.In contrast,the weak acid sites of the ZSM-5 zeolite led to more of the precursor entering the zeolite tunnels,followed by transformation to highly dispersed Pt clusters during calcination.In the case of the PtSnNa/ZSM-5,the interactions between Sn oxides and the support were lessened,owing to the weaker acidity of the ZSM-5 zeolite.The dispersed Sn oxides were therefore easier to reduce to the metallic state,thus decreasing the catalytic activity for hydrocarbon dehydrogenation. 展开更多
关键词 SUZ-4 zeolite PtSnNa catalyst propane dehydrogenation Catalyst stability Pt distribution
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Effect of preparation conditions on selective oxidation of propane to acrylic acid 被引量:1
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作者 YU Zhen-xing ZHENG Wei +3 位作者 XU Wen-long ZHANG Yu-hang FU Hong-ying ZHANG Ping 《Transactions of Nonferrous Metals Society of China》 SCIE EI CAS CSCD 2009年第S02期476-479,共4页
The effects of chemical composition and preparation conditions,especially calcination atmosphere and water content on the catalytic performances of MoVTeNbO mixed oxide catalyst system for the selective oxidation of p... The effects of chemical composition and preparation conditions,especially calcination atmosphere and water content on the catalytic performances of MoVTeNbO mixed oxide catalyst system for the selective oxidation of propane to acrylic acid were investigated.Among the catalysts studied,Mo_(1.0)V_(0.3)Te_(0.23)Nb_(0.12)O_(x) catalyst calcined in inert atmosphere at 600℃shows the best performance in terms of propane conversion and selectivity to acrylic acid.The results reveal that proper chemical composition, calcination atmosphere and water content affect greatly the catalysts in many ways including structure,chemical composition,which are related to their catalytic performances;and 51.0%propane conversion and 30.5%one-pass yield to acrylic acid can be achieved at the same time. 展开更多
关键词 selective oxidation propane oxidation catalysts preparation acrylic acid propane
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The effect of ethanol on the performance of CrO_x/SiO_2 catalysts during propane dehydrogenation 被引量:2
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作者 李利娜 朱文良 +6 位作者 石磊 刘勇 刘红超 倪友明 刘世平 周慧 刘中民 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2016年第3期359-366,共8页
The effects of ethanol vapor pretreatment on the performance of CrOx/SiO2 catalysts during the dehydrogenation of propane to propylene were studied with and without the presence of CO2.The catalyst pretreated with eth... The effects of ethanol vapor pretreatment on the performance of CrOx/SiO2 catalysts during the dehydrogenation of propane to propylene were studied with and without the presence of CO2.The catalyst pretreated with ethanol vapor exhibited better catalytic activity than the pristine CrOx/SiO2,generating 41.4% propane conversion and 84.8% propylene selectivity.The various catalyst samples prepared were characterized by X-ray diffraction,transmission electron microscopy,temperature-programmed reduction,X-ray photoelectron spectroscopy and reflectance UV-Vis spectroscopy.The data show that coordinative Cr^3+ species represent the active sites during the dehydrogenation of propane and that these species serve as precursors for the generation of Cr^3+.Cr^3+ is reduced during the reaction,leading to a decrease in catalytic activity.Following ethanol vapor pretreatment,the reduced CrOx in the catalyst is readily re-oxidized to Cr^6+ by CO2.The pretreated catalyst thus exhibits high activity during the propane dehydrogenation reaction by maintaining the active Cr^3+ states. 展开更多
关键词 propane DEHYDROGENATION CrOx/SiO2 catalyst Ethanol vapor pretreatment Carbon dioxide
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