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Product distributions of Fischer-Tropsch synthesis over Co/AC catalyst 被引量:3
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作者 Weixin Qian Haitao Zhang Weiyong Ying Dingye Fang 《Journal of Natural Gas Chemistry》 EI CAS CSCD 2011年第4期389-396,共8页
The product distributions of Fischer-Tropsch synthesis over Co/AC catalyst are investigated under different reaction conditions in an integral fixed bed reactor.It is found that the product distributions deviate from ... The product distributions of Fischer-Tropsch synthesis over Co/AC catalyst are investigated under different reaction conditions in an integral fixed bed reactor.It is found that the product distributions deviate from the ASF distribution.The deviation from ASF distribution is analyzed by taking the readsorption of alkenes and the following secondary reaction into consideration.It is noted that the contents of alcohol,alkene and alkane decline with the increasing carbon number,showing a slighter declining tendency of alkanes than those of alkenes and alcohols.It is also found that high temperature,space velocity,H2/CO in feed gas and low pressure are preferential for light hydrocarbons and alcohols while against the chain propagation.The effect of space velocity on the product distributions especially on the light products is not obvious.It is noticed that low temperature,space velocity,H2/CO and high pressure lead to high contents of alcohols;high temperature,H2/CO and low space velocity lead to high contents of alkanes.The effect of pressure on the amounts of alkanes is not significant;high space velocity and low temperature,pressure,H2/CO are preferential for alkenes. 展开更多
关键词 Fischer-Tropsch synthesis product distribution co/ac catalyst
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Research progress on catalysts for organic sulfur hydrolysis: Review of activity and stability
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作者 Bingning Wang Xianzhe Wang +3 位作者 Song Yang Chao Yang Huiling Fan Ju Shangguan 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第7期203-216,共14页
The removal of organic sulfur through catalytic hydrolysis is a significant area of research in the field of desulfurization.This review provides an overview of recent advancements in catalytic hydrolysis technology o... The removal of organic sulfur through catalytic hydrolysis is a significant area of research in the field of desulfurization.This review provides an overview of recent advancements in catalytic hydrolysis technology of organic sulfur,including the activity,stability,and atmosphere effects of hydrolysis catalysts.The emphasis is on strategies for enhancing hydrolysis activity and anti-oxygen poisoning property of catalysts.Surface modification,metal doping and nitrogen doping have been found to improve the activity of catalysts.Alkaline components modification is the most commonly used method,the formation of oxygen vacancies through metal doping and creation of nitrogen basic sites through nitrogen doping also contribute to the hydrolysis of organic sulfur.The strategies for anti-oxygen poisoning are discussed in a systematic manner.The structural regulation of catalysts is beneficial for the desorption and diffusion of hydrogen sulfide(H_(2)S),thereby effectively inhibiting its oxidation.Nitrogen doping and the addition of electronic promoters such as transition metals can protect active sites and decrease the number of active oxygen species.These methods have been proven to enhance the anti-poisoning performance of catalysts.Additionally,this article summarizes how different atmospheres affect the activity of hydrolysis catalysts.The objective of this review is to pave the way for the development of efficient,stable and widely used catalysts for organic sulfur hydrolysis. 展开更多
关键词 Organic sulfur HYDROLYSIS catalystS acTIVITY STABILITY
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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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Hydrodechlorination of trifluoro-trichloroethane to chlorotrifluoroethylene:Revealing the deactivation mechanism and regeneration strategy of Pd-Cu/AC catalyst
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作者 Song Tian Yicheng Chen +7 位作者 Xiaoyu Wen Bingcheng Li Jian Lu Zile Li Feng Feng Qingtao Wang Qunfeng Zhang Xiaonian Li 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第6期261-268,共8页
Chlorotrifluoroethylene(CTFE)is a vital fluorinated olefinic monomer produced through the catalytic hydrodechlorination of trichlorotrifluoroethane(CFC-113),an eco-friendly process.However,hydrodechlorination catalyst... Chlorotrifluoroethylene(CTFE)is a vital fluorinated olefinic monomer produced through the catalytic hydrodechlorination of trichlorotrifluoroethane(CFC-113),an eco-friendly process.However,hydrodechlorination catalysts for olefin production often suffer from poor stability.The Pd/AC catalyst and Pd-Cu/AC catalyst prepared by co-impregnation method exhibited poor stability,Pd-Cu/AC catalyst with CFC-113 conversion dropping to around 37%after 50 h of hydrodechlorination reaction.Brunauer-Emmett-Teller,transmission electron microscopy,X-ray photoelectron spectroscopy,and X-ray diffraction of fresh and deactivated Pd/AC catalysts indicate that the deactivation of Pd/AC catalysts is due to high-temperature agglomeration of Pd.Comparative analysis of fresh and deactivated Pd-Cu/AC catalysts using Brunauer-Emmett-Teller,transmission electron microscopy,and thermogravimetric analysis techniques revealed decreased dispersion of active sites,reduced surface area,catalyst aggregation deactivation,and a significant decrease in Cu content.Furthermore,the results of NH3-TPD revealed that the acid sites of the catalyst increased significantly.X-ray diffraction spectra indicated the formation of new species,basic copper chloride(Cu_(2)(OH)_(3)Cl),during the reaction.As the reaction progressed,these new species agglomerated,leading to a gradual loss of catalyst activity.Moreover,the deactivated catalyst was successfully reactivated using a simple alkaline washing method. 展开更多
关键词 CFC-113 HYDRODECHLORINATION CHLOROTRIFLUOROETHYLENE catalyst deactivation
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Porous silica nano-flowers stabilized Pt-Pd bimetallic nanoparticles as heterogeneous catalyst for efficiently synthesizing guaiacol from 2-methoxycyclohexanol
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作者 Junbo Feng Junyan Wu +1 位作者 Dongdong Yan Yadong Zhang 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第6期222-233,共12页
Porous silica nano-flowers(KCC-1)immobilized Pt-Pd alloy NPs(Pt-Pd/KCC-1)with different mass ratios of Pd and Pt were successfully prepared by a facile in situ one-step reduction,using hydrazinium hydroxide as a reduc... Porous silica nano-flowers(KCC-1)immobilized Pt-Pd alloy NPs(Pt-Pd/KCC-1)with different mass ratios of Pd and Pt were successfully prepared by a facile in situ one-step reduction,using hydrazinium hydroxide as a reducing agent.The as-synthesized silica nanospheres possess radial fibers with a distance of 15 nm,exhibiting a high specific surface area(443.56 m^(2)·g^(-1)).Meanwhile,the obtained Pt-Pd alloy NPs are uniformly dispersed on the silica surface with a metallic particle size of 4-6 nm,which exist as metallic Pd and Pt on the surface of monodisperse KCC-1,showing the transfer of electrons from Pd to Pt.The as-synthesized 2.5%Pt-2.5%Pd/KCC-1 exhibited excellent catalytic activity and stability for the continuous dehydrogenation of 2-methoxycyclohexanol to prepare guaiacol.Compared with Pt or Pd single metal supported catalysts,the obtained 2.5%Pt-2.5%Pd/KCC-1 shows 97.2%conversion rate of 2-methoxycyclohexanol and 76.8%selectivity for guaiacol,which attributed to the significant synergistic effect of bimetallic Pt-Pd alloy NPs.Furthermore,turn over frequency value of the obtained 2.5%Pt-2.5%Pd/KCC-1 NPs achieved 4.36 s^(-1),showing higher catalytic efficiency than other two monometallic catalysts.Reaction pathways of dehydro-aromatization of 2-methoxycyclohexanol over the obtained catalyst are proposed.Consequently,the obtained 2.5%Pt-2.5%Pd/KCC-1 NPs prove their potential in the dehydrogenation of 2-methoxycyclohexanol,while the kinetics and mechanistic study of the dehydrogenation reaction over the catalyst in a continuous fixed-bed reactor may provide valuable information for the development of green,outstanding and powerful synthetic pathway of guaiacol. 展开更多
关键词 Supported catalyst Nanoparticles Dehydrogenation 2-Methoxycyclohexanol GUAIacOL
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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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Screening the optimal Co_(x)/CeO_(2)(110)(x=1–6)catalyst for methane activation in coalbed gas
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作者 Li’nan Huang Danyang Li +3 位作者 Lei Jiang Zhiqiang Li Dong Tian Kongzhai Li 《International Journal of Coal Science & Technology》 EI CAS CSCD 2024年第3期256-271,共16页
The challenges posed by energy and environmental issues have forced mankind to explore and utilize unconventional energy sources.It is imperative to convert the abundant coalbed gas(CBG)into high value-added products,... The challenges posed by energy and environmental issues have forced mankind to explore and utilize unconventional energy sources.It is imperative to convert the abundant coalbed gas(CBG)into high value-added products,i.e.,selective and efficient conversion of methane from CBG.Methane activation,known as the“holy grail”,poses a challenge to the design and development of catalysts.The structural complexity of the active metal on the carrier is of particular concern.In this work,we have studied the nucleation growth of small Co clusters(up to Co_(6))on the surface of CeO_(2)(110)using density functional theory,from which a stable loaded Co/CeO_(2)(110)structure was selected to investigate the methane activation mechanism.Despite the relatively small size of the selected Co clusters,the obtained Co_(x)/CeO_(2)(110)exhibits interesting properties.The optimized Co_(5)/CeO_(2)(110)structure was selected as the optimal structure to study the activation mechanism of methane due to its competitive electronic structure,adsorption energy and binding energy.The energy barriers for the stepwise dissociation of methane to form CH3^(*),CH2^(*),CH^(*),and C^(*)radical fragments are 0.44,0.55,0.31,and 1.20 eV,respectively,indicating that CH^(*)dissociative dehydrogenation is the rate-determining step for the system under investigation here.This fundamental study of metal-support interactions based on Co growth on the CeO_(2)(110)surface contributes to the understanding of the essence of Co/CeO_(2) catalysts with promising catalytic behavior.It provides theoretical guidance for better designing the optimal Co/CeO_(2) catalyst for tailored catalytic reactions. 展开更多
关键词 Co cluster growth Ce-based catalysts Methane activation DFT
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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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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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Effect of samarium doping on the activity and sulfur resistance of Ce/MnFeO_(x) catalyst for low-temperature selective catalytic reduction of NO_(x) by ammonia
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作者 Qiyao Zhang Shuangshuang Zhang +1 位作者 Xu Hu Yongmin Huang 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第7期272-282,共11页
The self-made MnFeO_(x) catalysts doped with cerium and samarium were prepared by impregnation method for low-temperature selective catalytic reduction(SCR)by NH3.In this work,the surface properties of the series of M... The self-made MnFeO_(x) catalysts doped with cerium and samarium were prepared by impregnation method for low-temperature selective catalytic reduction(SCR)by NH3.In this work,the surface properties of the series of MnFe-based catalysts were studied.The results indicate Sm-modified catalyst have superior low-temperature SCR activity;NO_(x) conversion maintained at nearby to 100%at 90℃ to 240℃.In addition,The N_(2) selectivity of Sm doping remains above 80%in the range of 60℃ to 150℃.In SO_(2) poisoning test,the NO_(x) conversion can be remained>90%after 10 h of reaction.The XPS,NH_(3)-TPD and H_(2)-TPR results show the catalyst with Sm doping enhances the acid sites and oxidation catalytic sites of mixed oxides serves for improving oxygen vacancies and transfer electrons.In situ diffuse reflaxions infrared Fourier transformations spectroscopy(DRIFTS)results show that NO_(x) is more easily adsorbed on the surface after Sm doping,which provided favorable conditions for the NH_(3)-SCR reaction to proceed.The reaction at the catalyst surface will follow the L-H reaction mechanism by transient reaction test. 展开更多
关键词 SCR Sm doping catalyst Sulfur resistance In situ DRIFTS SELECTIVITY
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Boric Acid-Assisted Pyrolysis for High-Loading Single-Atom Catalysts to Boost Oxygen Reduction Reaction in Zn-Air Batteries
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作者 Chenxi Xu Jiexing Wu +12 位作者 Liang Chen Yi Gong Boyang Mao Jincan Zhang Jinhai Deng Mingxuan Mao Yan Shi Zhaohui Hou Mengxue Cao Huanxin Li Haihui Zhou Zhongyuan Huang Yafei Kuang 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2024年第2期102-110,共9页
The emerging of single-atom catalysts(SACs)offers a great opportunity for the development of advanced energy storage and conversion devices due to their excellent activity and durability,but the actual mass production... The emerging of single-atom catalysts(SACs)offers a great opportunity for the development of advanced energy storage and conversion devices due to their excellent activity and durability,but the actual mass production of high-loading SACs is still challenging.Herein,a facile and green boron acid(H_(3)BO_(3))-assisted pyrolysis strategy is put forward to synthesize SACs by only using chitosan,cobalt salt and H_(3)BO_(3)as precursor,and the effect of H_(3)BO_(3)is deeply investigated.The results show that molten boron oxide derived from H_(3)BO_(3)as ideal high-temperature carbonization media and blocking media play important role in the synthesis process.As a result,the acquired Co/N/B tri-doped porous carbon framework(Co-N-B-C)not only presents hierarchical porous structure,large specific surface area and abundant carbon edges but also possesses high-loading single Co atom(4.2 wt.%),thus giving rise to outstanding oxygen catalytic performance.When employed as a catalyst for air cathode in Zn-air batteries,the resultant Co-N-B-C catalyst shows remarkable power density and long-term stability.Clearly,our work gains deep insight into the role of H_(3)BO_(3)and provides a new avenue to synthesis of high-performance SACs. 展开更多
关键词 boric acid oxygen reduction reaction single-atom catalysts Zn-air batteries
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Critical role of carbon support in metal nanoaggregate facilitating Fe-N-C catalyst for PEM fuel cell application
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作者 Liming Guo Xin Wan +4 位作者 Qingtao Liu Xiaofang Liu Jiaxiang Shang Ronghai Yu Jianglan Shui 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第10期669-676,I0014,共9页
Metal nanoaggregates can simultaneously enhance the activity and stability of Fe-N-C catalysts in proton-exchange-membrane fuel cells(PEMFC).Previous studies on the relevant mechanism have focused on the direct intera... Metal nanoaggregates can simultaneously enhance the activity and stability of Fe-N-C catalysts in proton-exchange-membrane fuel cells(PEMFC).Previous studies on the relevant mechanism have focused on the direct interaction between FeN_(4)active sites and metal nanoaggregates.However,the role of carbon support that hosts metal nanoaggregates and active sites has been overlooked.Here,a Fe-N-C catalyst encapsulating inactive gold nanoparticles is prepared as a model catalyst to investigate the electronic tuning of Au nanoparticles(NPs)towards the carbon support.Au NPs donate electrons to carbon support,making it rich inπelectrons,which reduces the work function and regulates the electronic configuration of the FeN_(4)sites for an enhanced ORR activity.Meanwhile,the electron-rich carbon support can mitigate the electron depletion of FeN_(4)sites caused by carbon support oxidation,thereby preserving its high activity.The yield and accumulation of H_(2)O_(2)are thus alleviated,which delays the oxidation of the catalyst and benefits the stability.Due to the electron-rich carbon support,the composite catalyst achieves a top-level peak power density of 0.74 W/cm^(2) in a 1.5 bar H_(2)-air PEMFC,as well as the improved stability.This work elucidates the key role of carbon support in the performance enhancement of the FeN-C/metal nanoaggregate composite catalysts for fuel cell application. 展开更多
关键词 Fuel cells Oxygen reduction reaction Fe-N-C Hetero-structure catalyst Carbon support
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Atomically dispersed calcium as solid strong base catalyst with high activity and stability
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作者 Xiang-Bin Shao Zhi-Wei Xing +5 位作者 Si-Yu Liu Ke-Xin Miao Shi-Chao Qi Song-Song Peng Xiao-Qin Liu Lin-Bing Sun 《Green Energy & Environment》 SCIE EI CAS CSCD 2024年第10期1619-1626,共8页
Solid strong base catalysts are highly attractive for diverse reactions owing to their advantages of neglectable corrosion,facile separation,and environmental friendliness.However,their widespread applications are imp... Solid strong base catalysts are highly attractive for diverse reactions owing to their advantages of neglectable corrosion,facile separation,and environmental friendliness.However,their widespread applications are impeded by basic components aggregation and low stability.In this work,we fabricate single calcium atoms on graphene(denoted as Ca1/G)by use of a redox strategy for the first time,producing solid strong base catalyst with high activity and stability.The precursor Ca(NO_(3))_(2)is first reduced to CaO at 400℃ by the support graphene,forming CaO/G with conventional basic sites,and the subsequent reduction at 850℃results in the generation of Ca1/G with atomically dispersed Ca.Various characterizations reveal that Ca single atoms are anchored on graphene in tetra-coordination(Ca-C_(2)-N_(2))where N is in situ doped from Ca(NO_(3))_(2).The atomically dispersed Ca,along with their anchoring on the support,endow Ca1/G with high activity and stability toward the transesterification reaction of ethylene carbonate with methanol.The turnover frequency value reaches 128.0 h^(-1)on Ca1/G,which is much higher than the traditional counterpart CaO/G and various reported solid strong bases(2.9-46.2 h^(-1)).Moreover,the activity of Ca1/G is well maintained during 5 cycles,while 60%of activity is lost for the conventional analogue CaO/G due to the leaching of Ca. 展开更多
关键词 Solid strong base Single Ca atoms Heterogeneous catalysts TRANSESTERIFICATION REacTION
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Engineering oxygen vacancies on Tb-doped ceria supported Pt catalyst for hydrogen production through steam reforming of long-chain hydrocarbon fuels
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作者 Zhourong Xiao Changxuan Zhang +5 位作者 Peng Li Desong Wang Xiangwen Zhang Li Wang Jijun Zou Guozhu Li 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第4期181-192,共12页
Steam reforming of long-chain hydrocarbon fuels for hydrogen production has received great attention for thermal management of the hypersonic vehicle and fuel-cell application.In this work,Pt catalysts supported on Ce... Steam reforming of long-chain hydrocarbon fuels for hydrogen production has received great attention for thermal management of the hypersonic vehicle and fuel-cell application.In this work,Pt catalysts supported on CeO_(2)and Tb-doped CeO_(2)were prepared by a precipitation method.The physical structure and chemical properties of the as-prepared catalysts were characterized by powder X-ray diffraction,scanning electron microscopy,transmission electron microscopy,Raman spectroscopy,H_(2)temperature programmed reduction,and X-ray photoelectron spectroscopy.The results show that Tb-doped CeO_(2)supported Pt possesses abundant surface oxygen vacancies,good inhibition of ceria sintering,and strong metal-support interaction compared with CeO_(2)supported Pt.The catalytic performance of hydrogen production via steam reforming of long-chain hydrocarbon fuels(n-dodecane)was tested.Compared with 2Pt/CeO_(2),2Pt/Ce_(0.9)Tb_(0.1)O_(2),and 2Pt/Ce_(0.5)Tb_(0.5)O_(2),the 2Pt/Ce_(0.7)Tb_(0.3)O_(2)has higher activity and stability for hydrogen production,on which the conversion of n-dodecane was maintained at about 53.2%after 600 min reaction under 700℃at liquid space velocity of 9 ml·g^(-1)·h^(-1).2Pt/CeO_(2)rapidly deactivated,the conversion of n-dodecane was reduced to only 41.6%after 600 min. 展开更多
关键词 Steam reforming N-DODECANE Hydrogen production Pt-based catalyst Oxygen vacancy CeO_(2)
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Understanding the catalytic performance and deactivation behaviour of second-promoter doped Pt/WO_(χ)/γ-Al_(2)O_(3) catalysts in the glycerol hydrogenolysis for selective and cleaner production of 1,3-propanediol
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作者 Rafik Rajjak Shaikh Sittichai Damruang +2 位作者 Rais Ahmad Khan Supareak Praserthdam Piyasan Praserthdam 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第7期486-507,共22页
The selective aqueous-phase glycerol hydrogenolysis is a promising reaction to produce commercially useful 1,3-propanediol(1,3-PDO).The Pt-WOx bifunctional catalyst can catalyse the glycerol hydrogenol-ysis but the ca... The selective aqueous-phase glycerol hydrogenolysis is a promising reaction to produce commercially useful 1,3-propanediol(1,3-PDO).The Pt-WOx bifunctional catalyst can catalyse the glycerol hydrogenol-ysis but the catalyst deactivation via sintering,metal leaching,and coking can predominantly occur in the aqueous phase reaction.In this work,the effect of reaction temperature,pressure and second promoter(Cu,Fe,Rh,Mn,Re,Ru,Ir,Sn,B,and P)on catalytic performance and deactivation behaviour of Pt/WOx/-Al2O3 was investigated.When doped with Rh,Mn,Re,Ru,Ir,B,and P,the second promoter boosts catalytic activity by promoting great dispersion of Pt on support and increasing Pt surface area.The increased Bronsted acid sites lead to selective synthesis of 1,3-PDO than 1,2-propanediol(1,2-PDO).The characterization studies of fresh and spent catalysts reveal that the main cause of catalyst deactivation is the Pt sintering,as interpreted based on XRD,CO chemisorption,and TEM analyses.The Pt sintering is affected depending on the second promoter that can either or reduce the interaction between Pt,WO_(χ)/γ and Al_(2)O_(3).As an electron acceptor of Pt in Pt/WO_(χ)/γ-Al_(2)O_(3),Re and Mn as second promoters resulted in increased Pt^(2+) on the catalytic surface,which strengthens the contact between Pt andγ-Al_(2)O_(3) and WO_(χ),resulting in a decrease in Pt sintering.The metal leaching and coking are not affected by the presence of second promoter.The catalyst modified with a second promoter possesses improved catalytic activity and 1,3-PDO production,however the stability continues to remain a challenge.The present work unrav-elled the determining parameters of catalytic activity and deactivation,thus providing a promising pro-tocol toward effective catalysts for glycerol hydrogenolysis. 展开更多
关键词 Glycerol hydrogenolysis 1 3-PROPANEDIOL Metal-support interaction Second promoter Liquid phase catalyst deactivation
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Elucidating the structure-activity relationship of Cu-Ag bimetallic catalysts for electrochemical CO_(2) reduction
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作者 Qining Huang Lili Wan +1 位作者 Qingxuan Ren Jingshan Luo 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第6期345-351,I0009,共8页
Developing bimetallic catalysts is an effective strategy for enhancing the activity and selectivity of electrochemical CO_(2) reduction reactions,where understanding the structure-activity relationship is essential fo... Developing bimetallic catalysts is an effective strategy for enhancing the activity and selectivity of electrochemical CO_(2) reduction reactions,where understanding the structure-activity relationship is essential for catalyst design.Herein,we prepared two Cu-Ag bimetallic catalysts with Ag nanoparticles attached to the top or the bottom of Cu nanowires.When tested in a flow cell,the Cu-Ag catalyst with Ag nanoparticles on the bottom achieved a faradaic efficiency of 54%for ethylene production,much higher than the catalyst with Ag nanoparticles on the top.The catalysts were further studied in the H-cell and zero-gap MEA cell.It was found that placing the two metals in the intensified reaction zone is crucial to triggering the tandem reaction of bimetallic catalysts.Our work elucidates the structure-activity relationship of bimetallic catalysts for CO_(2) reduction and demonstrates the importance of considering both catalyst structures and cell characteristics to achieve high activity and selectivity. 展开更多
关键词 Electrochemical CO_(2)reduction Bimetallic catalyst CU-AG Structure-activity relationship
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RuO_(2)/CoMO_(2)O_(x) Catalyst with Low Ruthenium Loading for Long-Term Acidic Oxygen Evolution
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作者 Yingying Wang Hui Pan +1 位作者 Zhikun Liu Peng Kang 《Transactions of Tianjin University》 EI CAS 2024年第5期395-405,共11页
We must urgently synthesize highly efficient and stable oxygen-evolution reaction(OER) catalysts for acidic media. Herein, we constructed a series of Ti mesh(TM)-supported RuO_(2)/CoMo_(y)O_(x) catalysts(RuO_(2)/CoMo_... We must urgently synthesize highly efficient and stable oxygen-evolution reaction(OER) catalysts for acidic media. Herein, we constructed a series of Ti mesh(TM)-supported RuO_(2)/CoMo_(y)O_(x) catalysts(RuO_(2)/CoMo_(y)O_(x)/TM) with heterogeneous structures. By optimizing the ratio of Co to Mo, RuO_(2)/CoMO_(2)O_(x)/TM with low Ru loading(0.079 mg/cm^(2)) achieves remarkable OER performance(η = 243 mV at 10 mA/cm^(2)) and high stability(300 h @ 10 mA/cm^(2)) in 0.5 mol/L H_(2)SO_(4) electrolyte. The activity of RuO_(2)/CoMo_yO_x/TM can be maintained for 50 h at 100 mA/cm^(2), and a water electrolyzer with RuO_(2)/CoMO_(2)O_(x)/TM as anode can operate for 40 h at 100 mA/cm~2, suggesting the remarkable OER durability of RuO_(2)/CoMo__(y)O__(x)/TM in acidic electrolyte. Owing to the heterogeneous interface between CoMO_(2)O_(x) and RuO_(2), the electronic structure of Ru atoms was optimized and electron-rich Ru was formed. With modulated electronic properties, the dissociation energy of H_(2)O is weakened, and the OER barrier is lowered. This study provides the design of low-cost noble metal catalysts with long-term stability in an acidic environment. 展开更多
关键词 Oxygen-evolution reaction Ru-based catalyst acidic media Heterostructure Long-term electrolysis Low precious metal
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“Capture-activation-recapture” mechanism-guided design of double-atom catalysts for electrocatalytic nitrogen reduction
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作者 Cheng He Shiqi Yan Wenxue Zhang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第9期437-447,共11页
Compared with the traditional industrial nitrogen fixation, electrocatalytic methods, especially those utilizing double-atom catalysts containing nonmetals, can give good consideration to the economy and environmental... Compared with the traditional industrial nitrogen fixation, electrocatalytic methods, especially those utilizing double-atom catalysts containing nonmetals, can give good consideration to the economy and environmental protection. However, the existing “acceptance-donation” mechanism is only applicable to bimetallic catalysts and nonmetallic double-atom catalysts containing boron atoms. Herein, a novel “capture-activation-recapture” mechanism for metal-nonmetal double-atom catalyst is proposed to solve the problem by adjusting the coordination environments of nonmetallic atoms and utilizing the activation effect of metal atoms on nitrogen. Based on this mechanism, the nitrogen reduction reaction (NRR) activity of 48 structures is calculated by density functional theory calculation, and four candidates are selected as outstanding electrocatalytic nitrogen reduction catalysts: Si-Fe@NG (U_(L) = –0.14 V), Si-Co@NG (U_(L)= –0.15 V), Si-Mo@BP1 (U_(L) = 0 V), and Si-Re@BP1 (U_(L) = –0.02 V). The analyses of electronic properties further confirm “capture-activation-recapture” mechanism and suggest that the difference in valence electron distribution between metal and Si atoms triggers the activation of N≡N bonds. In addition, a machine learning approach is utilized to generate an expression and an intrinsic descriptor that considers the coordination environment to predict the limiting potential. This study offers profound insight into the synergistic mechanism of TM and Si for NRR and guidance in the design of novel double-atom nitrogen fixation catalysts. 展开更多
关键词 "Capture-activation-recapture"mechanism Double-atom catalyst Nitrogen reduction reaction Density functional theory
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Non-thermal atmospheric-pressure positive pulsating corona discharge in degradation of textile dye Reactive Blue 19 enhanced by Bi_(2)O_(3) catalyst
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作者 Milica PETROVIC Dragan RADIVOJEVIC +4 位作者 Sasa RANCEV Nena VELINOV Milos KOSTIC Danijela BOJIC Aleksandar BOJIC 《Plasma Science and Technology》 SCIE EI CAS CSCD 2024年第2期104-113,共10页
In this work,monoclinic Bi_(2)O_(3) was applied for the first time,to the best of our knowledge,as a catalyst in the process of dye degradation by a non-thermal atmospheric-pressure positive pulsating corona discharge... In this work,monoclinic Bi_(2)O_(3) was applied for the first time,to the best of our knowledge,as a catalyst in the process of dye degradation by a non-thermal atmospheric-pressure positive pulsating corona discharge.The research focused on the interaction of the plasma-generated species and the catalyst,as well as the role of the catalyst in the degradation process.Plasma decomposition of the anthraquinone reactive dye Reactive Blue 19(RB 19) was performed in a selfmade reactor system.Bi_(2)O_(3) was prepared by electrodeposition followed by thermal treatment,and characterized by x-ray diffraction,scanning electron microscopy and energy-dispersive xray techniques.It was observed that the catalyst promoted decomposition of plasma-generated H_(2)O_(2) into ·OH radicals,the principal dye-degrading reagent,which further attacked the dye molecules.The catalyst improved the decolorization rate by 2.5 times,the energy yield by 93.4%and total organic carbon removal by 7.1%.Excitation of the catalyst mostly occurred through strikes by plasma-generated reactive ions and radical species from the air,accelerated by the electric field,as well as by fast electrons with an energy of up to 15 eV generated by the streamers reaching the liquid surface.These strikes transferred the energy to the catalyst and created the electrons and holes,which further reacted with H_(2)O_(2) and water,producing ·OH radicals.This was indentified as the primary role of the catalyst in this process.Decolorization reactions followed pseudo first-order kinetics.Production of H_(2)O_(2) and the dye degradation rate increased with increase in the input voltage.The optimal catalyst dose was 500 mg·dm^(-3).The decolorization rate was a little lower in river water compared with that in deionized water due to the side reactions of ·OH radicals with organic matter and inorganic ions dissolved in the river water. 展开更多
关键词 corona RB 19 Bi_(2)O_(3) catalyst DEGRADATION
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