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
Electrochemical CO_(2)reduction to formate is a potential approach to achieving global carbon neutrality.Here,Cu1Bi1bimetallic catalyst was prepared by a co-precipitation method.It has a ginger like composite structur...Electrochemical CO_(2)reduction to formate is a potential approach to achieving global carbon neutrality.Here,Cu1Bi1bimetallic catalyst was prepared by a co-precipitation method.It has a ginger like composite structure(CuO/CuBi_(2)O_(4))and exhibited a high formate faradaic efficiency of 98.07%at–0.98 V and a large current density of–56.12 mA.cm^(-2)at–1.28 V,which is twice as high as Bi2O3catalyst.Especially,high selectivity(FE^(–)_(HCOO)>85%)is maintained over a wide potential window of 500 mV.In-situ Raman measurements and structure characterization revealed that the reduced Cu1Bi1bimetallic catalyst possesses abundant Cu-Bi interfaces and residual Bi-O structures.The abundant Cu-Bi interface structures on the catalyst surface can provide abundant active sites for CO_(2)RR,while the Bi-O structures may stabilize the CO_(2)^(*–)intermediate.The synergistic effect of abundant Cu-Bi interfaces and Bi-O species promotes the efficient synthesis of formate by following the OCHO^(*)pathway.展开更多
The development of novel single-atom catalysts with optimal electron configuration and economical noble-metal cocatalyst for efficient photocatalytic hydrogen production is of great importance,but still challenging.He...The development of novel single-atom catalysts with optimal electron configuration and economical noble-metal cocatalyst for efficient photocatalytic hydrogen production is of great importance,but still challenging.Herein,we fabricate Pt and Co single-atom sites successively on polymeric carbon nitride(CN).In this Pt_(1)-Co_(1)/CN bimetallic single-atom catalyst,the noble-metal active sites are maximized,and the single-atomic Co_(1)N_4sites are tuned to Co_(1)N_3sites by photogenerated electrons arising from the introduced single-atomic Pt_(1)N_4sites.Mechanism studies and density functional theory(DFT)calculations reveal that the 3d orbitals of Co_(1)N_3single sites are filled with unpaired d-electrons,which lead to the improved visible-light response,carrier separation and charge migration for CN photocatalysts.Thereafter,the protons adsorption and activation are promoted.Taking this advantage of long-range electron synergy in bimetallic single atomic sites,the photocatalytic hydrogen evolution activity over Pt_(1)-Co_(1)/CN achieves 915.8 mmol g^(-1)Pt h^(-1),which is 19.8 times higher than Co_(1)/CN and 3.5 times higher to Pt_(1)/CN.While this electron-synergistic effect is not so efficient for Pt nanoclusters.These results demonstrate the synergistic effect at electron-level and provide electron-level guidance for the design of efficient photocatalysts.展开更多
Carbon dioxide reduction reaction(CO_(2)RR) represents an efficient approach to achieving carbon neutrality and simultaneously generating clean energy.However,the strong stability of CO_(2) molecules and the diversity...Carbon dioxide reduction reaction(CO_(2)RR) represents an efficient approach to achieving carbon neutrality and simultaneously generating clean energy.However,the strong stability of CO_(2) molecules and the diversity of products pose significant challenges.As an emerging material,bimetallic catalysts have been widely reported for their unique advantages,such as tunable electronic structures,suitable adsorption/desorption of CO_(2) and intermediates,and optimizable d-band centers of active sites through bimetallic synergy.These catalysts provide a remarkable platform for converting CO_(2) into high value-added chemicals.This review comprehensively summarizes recent research advances in bimetallic catalysts for CO_(2)RR.Firstly,the challenges associated with CO_(2)RR,including activity and selectivity are analyzed,followed by a discussion on the unique advantages of bimetallic catalysts.Next,their synthesis strategies are categorized into dual-atom site catalysts(DACs),bimetallic nanoparticles and nanoclusters,binary metal semiconductors,and layered double hydroxides(LDHs).Additionally,advanced characterization techniques of bimetallic catalysts and their applications in CO_(2)RR are thoroughly introduced.Finally,the prospects and challenges for the application of bimetallic materials are highlighted.This review aims to provide inspiration for CO_(2)RR into high-value chemicals and shed light on the research of bimetallic materials.展开更多
Microbial fuel cell(MFC) is one synchronous power generation device for wastewater treatment that takes into account environmental and energy issues, exhibiting promising potential. Sluggish oxygen reduction reaction(...Microbial fuel cell(MFC) is one synchronous power generation device for wastewater treatment that takes into account environmental and energy issues, exhibiting promising potential. Sluggish oxygen reduction reaction(ORR) kinetics on the cathode remains by far the most critical bottleneck hindering the practical application of MFC. An ideal cathode catalyst should possess excellent ORR activity, stability, and costeffectiveness, experiments have demonstrated that bimetallic catalysts are one of the most promising ORR catalysts currently. Based on this, this review mainly analyzes the reaction mechanism(ORR mechanisms, synergistic effects), advantages(combined with characterization technologies), and typical synthesis methods of bimetallic catalysts, focusing on the application effects of early Pt-M(M = Fe, Co, and Ni) alloys to bifunctional catalysts in MFC, pointing out that the main existing challenges remain economic analysis, long-term durability and large-scale application, and looking forward to this. At last, the research trend of bimetallic catalysts suitable for MFC is evaluated, and it is considered that the development and research of metal-organic framework(MOF)-based bimetallic catalysts are still worth focusing on in the future, intending to provide a reference for MFC to achieve energy-efficient wastewater treatment.展开更多
Hydrogen energy has become one of the recognized clean energy sources worldwide due to its advantages such as low cost,renewable energy,and green environmental protec-tion.Electrolytic water is currently one of the mo...Hydrogen energy has become one of the recognized clean energy sources worldwide due to its advantages such as low cost,renewable energy,and green environmental protec-tion.Electrolytic water is currently one of the most promising solutions for providing hydrogen fuel.Nickel iron bimetallic electrocatalysts have abundant sources,low cost,clean and pollution-free properties,and strong catalytic performance,This article mainly reviews the development and research of bimetallic nickel iron oxides and nickel iron alloys in recent years,and explores their synthesis methods,properties,and stability in depth.展开更多
The bifunctional oxygen catalyst is essential for zinc-air batteries(ZABs).Here,an efficient bifunctional oxygen catalyst,PPcFeCo/3D-G,is obtained throughπ-πinteraction between the conjugated polymerized iron-cobalt...The bifunctional oxygen catalyst is essential for zinc-air batteries(ZABs).Here,an efficient bifunctional oxygen catalyst,PPcFeCo/3D-G,is obtained throughπ-πinteraction between the conjugated polymerized iron-cobalt phthalocyanine(PPcFeCo)with excellent thermal stability and three-dimensional graphene(3D-G).The bimetallic synergistic effect of PPcFeCo,verified by DFT(Density functional theory)calculation,andπ-πinteractions enhances the catalytic activity and durability of the PPcFeCo/3D-G.Regarding electrochemical performance,the PPcFeCo/3D-G with a high electron transfer number(3.98,@0.768 V vs.RHE)has excellent half-wave potential(E_(1/2)=0.890 V vs.RHE)and exhibits outstanding reversibility(ΔE=0.700 V,ΔE=Ej=10-E_(1/2)).The liquid ZAB(LZAB)employed PPcFeCo/3D-G displays a high power density(222 m W cm^(-2)),a specific capacity(792 m A h g-1),and excellent durability(120 h).This work has guiding significance for the preparation of high-efficiency bifunctional catalysts.展开更多
Catalytic hydrogenation of CO_(2) using renewable hydrogen not only reduces greenhouse gas emissions,but also provides industrial chemicals.Herein,a Co-Fe bimetallic catalyst was developed by a facile reactive ball-mi...Catalytic hydrogenation of CO_(2) using renewable hydrogen not only reduces greenhouse gas emissions,but also provides industrial chemicals.Herein,a Co-Fe bimetallic catalyst was developed by a facile reactive ball-milling method for highly active and selective hydrogenation of CO_(2) to value-added hydrocarbons.When reacted at 320℃,1.0 MPa and 9600 mL h^(-1) g_(cat)^(-1),the selectivity to light olefin(C_(2)^(=)-C_(4)^(=)) and C_(5)+ species achieves 57.3% and 22.3%,respectively,at a CO_(2) co nversion of 31.4%,which is superior to previous Fe-based catalysts.The CO_(2) activation can be promoted by the CoFe phase formed by reactive ball milling of the Fe-Co_(3)O_(4) mixture,and the in-situ Co_(2)C and Fe_(5)C_(2) formed during hydrogenation are beneficial for the C-C coupling reaction.The initial C-C coupling is related to the combination of CO species with the surface carbon of Fe/Co carbides,and the sustained C-C coupling is maintained by self-recovery of defective carbides.This new strategy contributes to the development of efficient catalysts for the hydrogenation of CO_(2) to value-added hydrocarbons.展开更多
Nitrate from the application of nitrogen-based fertilizers in intensive agriculture is a notorious waste product, though it lacks cost-effective solutions for its removal from potential drinking water resources. Catal...Nitrate from the application of nitrogen-based fertilizers in intensive agriculture is a notorious waste product, though it lacks cost-effective solutions for its removal from potential drinking water resources. Catalytic reduction appears to be a promising technique for converting nitrates to benign nitrogen gas. Mesoporous silica SBA-15 is a frequently used catalyst support that has large surface areas and highly ordered nanopores. In this work, mesoporous silica SBA-15 bimetallic catalysts for nitrate reduction were investigated. The catalyst was optimized for the selection of promoter metal (Sn and Cu), noble metal (Pd and Pt) and loading ratios of these metals at different temperatures and reduction conditions. The catalysts prepared were characterized by FT-IR, N2 physisorption, XRD, SEM, and ICP. All catalysts showed the presence of cylindrical mesoporous channels and uniform pore structures that remained even after metals loading. In the presence of a CO<sub>2</sub> buffer, the catalysts 4Pd-1Cu/SBA-15 and 1Pt-1Cu/SBA-15 reduced at 100?C under H2 and 1Pd-1Cu/SBA-15 reduced at 200°C under H2 demonstrated very high nitrate conversion. Furthermore, the forementioned Pd catalysts had higher N2 selectivity (88% - 87%) compared to Pt catalyst (80%). Nitrate conversion by the 4Pd-1Cu/SBA-15 catalyst was significantly decreased to 81% in the absence of CO<sub>2</sub>.展开更多
A systematic study was carried out to investigate the promotion effect of manganese on the performance of a coprecipitated iron-manganese bimetallic catalyst for the light olefins synthesis from syngas. The catalyst s...A systematic study was carried out to investigate the promotion effect of manganese on the performance of a coprecipitated iron-manganese bimetallic catalyst for the light olefins synthesis from syngas. The catalyst samples were characterized by N2 physisorption, transmis- sion electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), powder X-ray diffraction (XRD), Mossbauer spectroscopy, H2- differential thermogravimetric analysis (H2-DTG), CO temperature-programmed reduction (CO-TPR) and CO2 temperature-programmed des- orption (CO2-TPD). The Fischer-Tropsch synthesis (FTS) performance of the catalyst was measured at 1.5 MPa, 250 ℃ and syngas with H2/CO ratio of 2.0. The characterization results indicated that the addition of manganese decreases the catalyst crystallite size, and improves the catalyst BET surface area and pore volume. The presence of manganese suppresses the catalyst reduction and carburization in H2, CO and syngas, respectively. The addition of manganese improves the catalytic activity of water-gas shift reaction and suppresses the oxidation of iron carbides in the FTS reaction. The incorporation of manganese improves the catalyst surface basicity and results in a significant improvement in the selectivities to light olefins and heavy hydrocarbons (C5+), and furthermore an inhibition of methane formation in FTS. The pure iron catalyst (Mn-00) has the highest initial FTS catalytic activity (65%) and the lowest selectivity (17.35 wt%) to light olefins (C2=-C4=). The addition of an appropriate amount of manganese can improve the catalyst FTS activity.展开更多
Silica, alumina, and activated carbon supported iron-cobalt catalysts were prepared by incipient wetness impregnation. These catalysts have been characterized by BET, X-ray diffraction (XRD), and temperature-program...Silica, alumina, and activated carbon supported iron-cobalt catalysts were prepared by incipient wetness impregnation. These catalysts have been characterized by BET, X-ray diffraction (XRD), and temperature-programmed reduction (TPR). Activity and selectivity of iron-cobalt supported on different carriers for CO hydrogenation were studied under the conditions of 1.5 MPa, 493 K, 630 h^-1, and H2/CO ratio of 1.6. The results indicate that the activity, C4 olefin/(C4 olefin+C4 paraffin) ratio, and C5 olefin/(C5 olefin+C5 paraffin) decrease in the order of Fe-Co/SiO2, Fe-Co/AC1, Fe-Co/Al2O3 and Fe- Co/AC2. The activity of Fe-Co/SiO2 reached a maximum. The results of TPR show that the Fe-Co/SiO2 catalyst is to some extent different. XRD patterns show that the Fe-Co/SiO2 catalyst differs significantly from the others; it has two diffraction peaks. The active spinel phase is correlated with the supports.展开更多
PVP-supported bimetallic catalyst, PVP-PdCl2-CdCl2, exhibits extremely high catalytic activity for the hydrogen transfer dechlorination of aryl chlorides in neutral environment. The yields of dechlorination products a...PVP-supported bimetallic catalyst, PVP-PdCl2-CdCl2, exhibits extremely high catalytic activity for the hydrogen transfer dechlorination of aryl chlorides in neutral environment. The yields of dechlorination products are high under mild reaction conditions and the operation is simple.展开更多
A non-phosgene route for the synthesis of hexamethylene-1,6-diisocyanate(HDI) was developed via catalytic decomposition of hexamethylene-1,6-dicarbamate(HDC) over Zn–Co bi-metallic supported ZSM-5 catalyst.The cataly...A non-phosgene route for the synthesis of hexamethylene-1,6-diisocyanate(HDI) was developed via catalytic decomposition of hexamethylene-1,6-dicarbamate(HDC) over Zn–Co bi-metallic supported ZSM-5 catalyst.The catalyst was characterized by FTIR and XRD analyses. Three solvents dioctyl sebacate(DOS), dibutyl sebacate(DBS) and 1-butyl-3-methylimidazolium tetrafluoroborate(BMIMBF_4) were investigated and compared; DOS gave better performance. The catalytic performances for thermal decomposition of HDC to HDI using DOS as solvent were then investigated, and the results showed that, under the optimized reaction conditions, i.e.,10 wt%concentration of HDC in DOS, 250 °C temperature, 60 min reaction time, 83.8% yield of HDI had been achieved over Zn–Co/ZSM-5. Decomposition of the intermediate hexamethylene-1-carbamate-6-isocyanate(HMI) over Zn–Co/ZSM-5 in DOS solvent was further studied and the results indicated that yield of HDI from HMI reached to 69.6%(98.6% HDI selectively) at 270 °C, which further increased the yield of the total HDI(HDI_(tol)) to as high as 95.0%. Recycling of catalyst showed that HDI and HMI yield slightly decreased, and by-product yield increased after the catalyst was reused for 4 times. At last possible reaction mechanism was proposed.展开更多
The electroreduction reaction of CO_(2)(ECO_(2)RR)requires high-performance catalysts to convert CO_(2)into useful chemicals.Transition metal-based atomically dispersed catalysts are promising for the high selectivity...The electroreduction reaction of CO_(2)(ECO_(2)RR)requires high-performance catalysts to convert CO_(2)into useful chemicals.Transition metal-based atomically dispersed catalysts are promising for the high selectivity and activity in ECO_(2)RR.This work presents a series of atomically dispersed Co,Fe bimetallic catalysts by carbonizing the Fe-introduced Co-zeolitic-imidazolate-framework(C-Fe-Co-ZIF)for the syngas generation from ECO_(2)RR.The synergistic effect of the bimetallic catalyst promotes CO production.Compared to the pure C-Co-ZiF,C-Fe-Co-ZIF facilitates CO production with a CO Faradaic efficiency(FE)boost of 10%,with optimal FE_(CO)of 51.9%,FE_(H_(2))of 42.4%at-0.55 V,and CO current density of 8.0 mA cm^(-2)at-0.7 V versus reversible hydrogen electrode(RHE).The H_(2)/CO ratio is tunable from 0.8 to 4.2 in a wide potential window of-0.35 to-0.8 V versus RHE.The total FE_(CO+H_(2))maintains as high as 93%over 10 h.The proper adding amount of Fe could increase the number of active sites and create mild distortions for the nanoscopic environments of Co and Fe,which is essential for the enhancement of the CO production in ECO_(2)RR.The positive impacts of Cu-Co and Ni-Co bimetallic catalysts demonstrate the versatility and potential application of the bimetallic strategy for ECO_(2)RR.展开更多
In the present work, a series of Pt-based catalysts, alloyed with a second metal, i.e., Re, Sn, Er, La, and Y, and supported on activated carbon, ordered mesoporous carbon, N-doped mesoporous carbon or reduced graphen...In the present work, a series of Pt-based catalysts, alloyed with a second metal, i.e., Re, Sn, Er, La, and Y, and supported on activated carbon, ordered mesoporous carbon, N-doped mesoporous carbon or reduced graphene oxide(rGO), have been developed for selective hydrogenation of cinnamaldehyde to cinnamylalcohol. Re and rGO were proved to be the most favorable metal dopant and catalyst support, respectively. Pt_(50) Re_(50)/rGO showed the highest cinnamylalcohol selectivity of 89% with 94% conversion of cinnamaldehyde at the reaction conditions of 120 °C, 2.0 MPaH_2 and 4 h.展开更多
Cu-x-Fe-y/SiO2 catalysts were prepared using urea-assisted sol-gel method. The structure and physicochemical properties of the catalysts were characterized using N-2 adsorption-desorption, transmission electron micros...Cu-x-Fe-y/SiO2 catalysts were prepared using urea-assisted sol-gel method. The structure and physicochemical properties of the catalysts were characterized using N-2 adsorption-desorption, transmission electron microscopy, H-2-temperature-programmed reduction, powder X-ray diffraction, and X-ray photoelectron spectroscopy. Compared with monometallic Cu or Fe catalysts, the bimetallic Cu-x-Fe-y/SiO2 catalysts exhibited enhanced catalytic performance for the selective hydrogenation of diethyl malonate to 1,3-propanediol. The bimetallic catalyst with an optimal Cu/Fe atomic ratio of 2 exhibited the highest activity, which yielded 96.3% conversion to diethyl malonate and 93.3% selectivity to 1,3-propanediol under the optimal reaction conditions. Characterization results revealed that interactions between Cu and Fe contributed to the improvement of diethyl malonate conversion and selectivity to 1,3-propanediol. The X-ray photoelectron spectroscopy results revealed that the addition of appropriate amount of Fe species enhanced the reduction of Cu2+ species, thereby increasing the Cu-0 species on the surface of bimetallic catalyst. It led to a better chemisorption capacity of hydrogen and further promoted of the activation of hydrogen molecule. The ethyl acetate temperature-programmed desorption results indicated that the FeOx species provided the additional adsorption sites for substrate molecules, and they activated the C=O bond. The improved catalytic performance of bimetallic Cu-x-Fe-y/SiO2 catalyst was mainly attributed to the synergistic effect between Cu-0 and FeOx species. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.展开更多
The aerobic oxidation of glycerol provides an economically viable route to glyceraldehyde, dihydroxyacetone and glyceric acid with versatile applications, for which monometallic Pt, Au and Pd and bimetallic Au-Pt, Au-...The aerobic oxidation of glycerol provides an economically viable route to glyceraldehyde, dihydroxyacetone and glyceric acid with versatile applications, for which monometallic Pt, Au and Pd and bimetallic Au-Pt, Au- Pd and Pt-Pd catalysts on TiO2 were examined under base-free conditions. Pt exhibited a superior activity relative to Pd, and Au-Pd and Pt-Pd while Au was essentially inactive. The presence of Au on the Au-Pt/TiO2 catalysts led to their higher activities (normalized per Pt atom) in a wide range of Au/Pt atomic ratios (i.e. 1/3-7/1 ), and the one with the Au/Pt ratio of 3/1 exhibited the highest activity. Such promoting effect is ascribed to the increased electron density on Pt via the electron transfer from Au to Pt, as characterized by the temperature-programmed desorption of CO and infra-red spectroscopy for CO adsorption. Meanwhile, the presence of Au on Au-Pt/TiO2, most like due to the observed electron transfer, changed the product selectivity, and facilitated the oxidation of the secondary hydroxyl groups in glycerol, leading to the favorable formation of dihydroxyacetone over glyceraldehyde and glyceric acid that were derived from the oxidation of the primary hydroxyl groups. The synergetic effect between Au and Pt demonstrates the feasibility in the efficient oxidation of glycerol to the targeted products, for example, by rational tuning of the electronic properties of metal catalysts.展开更多
In this study,a MOF-derived bimetallic Co@NiO catalyst was synthesized and doped into MgH_(2)to improve the hydrogen desorption and resorption kinetics.The Co@NiO catalyst decreased the onset dehydrogenation temperatu...In this study,a MOF-derived bimetallic Co@NiO catalyst was synthesized and doped into MgH_(2)to improve the hydrogen desorption and resorption kinetics.The Co@NiO catalyst decreased the onset dehydrogenation temperature of MgH_(2)by 160℃,compared with un-doped MgH_(2).The MgH^(2+)9%(mass)Co@NiO composite released 6.6%(mass)hydrogen in 350 s at 315℃and uptook 5.4%(mass)hydrogen in500 s at 165℃,showing greatly accelerated de/rehydrogenation rates.Besides,the desorption activation energy of MgH^(2+)9%(mass)Co@NiO was decreased to(93.8±8.4)kJ·mol^(-1).Noteworthy,symbiotic Mg_(2)NiH_(4)/Mg_(2)CoH_(5)clusters were in-situ formed from bimetallic precursors and inlaid on MgH_(2)surface,which are considered as"multi-step hydrogen pumps",and provides surface pathways for hydrogen absorption.Meanwhile,the introduced Mg_(2)NiH_(4)/Mg_(2)CoH_(5)interfaces could provide numerous low energy barrier H diffusion channels,therefore accelerating the hydrogen release and uptake.This research proposes new insights to design high-efficiency bimetallic catalyst for MgH_(2)hydrogen storage.展开更多
The water gas shift reaction is of vital significance for the generation and transition of energy due to the application in hydrogen production and industries such as ammonia synthesis and fuel cells.The influence of ...The water gas shift reaction is of vital significance for the generation and transition of energy due to the application in hydrogen production and industries such as ammonia synthesis and fuel cells.The influence of support doping and bimetallic alloying on the catalytic performance of Pt/Ce O_(2)-based nanocatalysts in water gas shift reaction was reported in this work.Various lanthanide ions and 3d transition metals were respectively introduced into the Ce O_(2)support or Pt to form Pt/Ce O_(2):Ln(Ln=La,Nd,Gd,Tb,Yb)and Pt M/Ce O_(2)(M=Fe,Co,Ni)nanocatalysts.The sample of Pt/Ce O_(2):Tb showed the highest activity(TOF at 200℃=0.051 s^(-1))among the Pt/Ce O_(2):Ln and the undoped Pt/Ce O_(2)catalysts.Besides,the sample of Pt Fe/Ce O_(2)exhibited the highest activity(TOF at 200℃=0.12 s^(-1))among Pt M/Ce O_(2)catalysts.The results of the multiple characterizations indicated that the catalytic activity of Pt/Ce O_(2):Ln catalysts was closely correlated with the amount of oxygen vacancies in doped ceria support.However,the different activity of Pt M/Ce O_(2)bimetallic catalysts was owing to the various Pt oxidation states of the bimetals dispersed on ceria.The study of the reaction pathway indicated that both the samples of Pt/Ce O_(2)and Pt/Ce O_(2):Tb catalyzed the reaction through the formate pathway,and the enhanced activity of the latter derived from the increased concentration of oxygen vacancies along with promoted water dissociation.As for the sample of Pt Fe/Ce O_(2),its catalytic mechanism was the carboxyl route with a higher reaction rate due to the moderate valence of Pt along with improved CO activation.展开更多
基金the funding support from the National Key Research and Development Program of China(2019YFE0123400)the Tianjin Distinguished Young Scholars Fund(20JCJQJC00260)+4 种基金the Major Science and Technology Project of Anhui Province(202203f07020007)the Anhui Conch Group Co.,Ltdthe“111”Project(B16027)the funding support from the Natural Science Foundation of China(22209081)the fellowship of China Postdoctoral Science Foundation(2021M690082)。
文摘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.
基金financially supported by the National Natural Science Foundation of China(22172082,21978137,and 21878162)the Natural Science Foundation of Tianjin(20JCZDJC00770)+1 种基金the NCC Fund(NCC2020FH05)the Fundamental Research Funds for the Central Universities。
文摘Electrochemical CO_(2)reduction to formate is a potential approach to achieving global carbon neutrality.Here,Cu1Bi1bimetallic catalyst was prepared by a co-precipitation method.It has a ginger like composite structure(CuO/CuBi_(2)O_(4))and exhibited a high formate faradaic efficiency of 98.07%at–0.98 V and a large current density of–56.12 mA.cm^(-2)at–1.28 V,which is twice as high as Bi2O3catalyst.Especially,high selectivity(FE^(–)_(HCOO)>85%)is maintained over a wide potential window of 500 mV.In-situ Raman measurements and structure characterization revealed that the reduced Cu1Bi1bimetallic catalyst possesses abundant Cu-Bi interfaces and residual Bi-O structures.The abundant Cu-Bi interface structures on the catalyst surface can provide abundant active sites for CO_(2)RR,while the Bi-O structures may stabilize the CO_(2)^(*–)intermediate.The synergistic effect of abundant Cu-Bi interfaces and Bi-O species promotes the efficient synthesis of formate by following the OCHO^(*)pathway.
基金the support of the National Natural Science Foundation of China (22002118,22208262,52271228,52202298,52201279,51834009,51801151)the Natural Science Foundation of Shaanxi Province (2021JQ-468,2020JZ-47)+2 种基金the Natural Science Foundation of Shaanxi Provincial Department of Education (21JP086)the Postdoctoral Research Foundation of China (2020 M683528,2020TQ0245,2018M633643XB)the Hundred Talent Program of Shaanxi Province。
文摘The development of novel single-atom catalysts with optimal electron configuration and economical noble-metal cocatalyst for efficient photocatalytic hydrogen production is of great importance,but still challenging.Herein,we fabricate Pt and Co single-atom sites successively on polymeric carbon nitride(CN).In this Pt_(1)-Co_(1)/CN bimetallic single-atom catalyst,the noble-metal active sites are maximized,and the single-atomic Co_(1)N_4sites are tuned to Co_(1)N_3sites by photogenerated electrons arising from the introduced single-atomic Pt_(1)N_4sites.Mechanism studies and density functional theory(DFT)calculations reveal that the 3d orbitals of Co_(1)N_3single sites are filled with unpaired d-electrons,which lead to the improved visible-light response,carrier separation and charge migration for CN photocatalysts.Thereafter,the protons adsorption and activation are promoted.Taking this advantage of long-range electron synergy in bimetallic single atomic sites,the photocatalytic hydrogen evolution activity over Pt_(1)-Co_(1)/CN achieves 915.8 mmol g^(-1)Pt h^(-1),which is 19.8 times higher than Co_(1)/CN and 3.5 times higher to Pt_(1)/CN.While this electron-synergistic effect is not so efficient for Pt nanoclusters.These results demonstrate the synergistic effect at electron-level and provide electron-level guidance for the design of efficient photocatalysts.
基金the financial support provided by National Natural Science Foundation of China (22008163)Postgraduate Research & Practice Innovation Program of Jiangsu Province+2 种基金Open Project Program of the State Key Laboratory of Photocatalysis on Energy and Environment (SKLPEE-KF202309)Natural Science Research Project of Higher Education Institutions in Jiangsu Province (20KJB150042, 21KJB150038)Natural Science Foundation of Jiangsu Province (BK20231342, BK20210867)。
文摘Carbon dioxide reduction reaction(CO_(2)RR) represents an efficient approach to achieving carbon neutrality and simultaneously generating clean energy.However,the strong stability of CO_(2) molecules and the diversity of products pose significant challenges.As an emerging material,bimetallic catalysts have been widely reported for their unique advantages,such as tunable electronic structures,suitable adsorption/desorption of CO_(2) and intermediates,and optimizable d-band centers of active sites through bimetallic synergy.These catalysts provide a remarkable platform for converting CO_(2) into high value-added chemicals.This review comprehensively summarizes recent research advances in bimetallic catalysts for CO_(2)RR.Firstly,the challenges associated with CO_(2)RR,including activity and selectivity are analyzed,followed by a discussion on the unique advantages of bimetallic catalysts.Next,their synthesis strategies are categorized into dual-atom site catalysts(DACs),bimetallic nanoparticles and nanoclusters,binary metal semiconductors,and layered double hydroxides(LDHs).Additionally,advanced characterization techniques of bimetallic catalysts and their applications in CO_(2)RR are thoroughly introduced.Finally,the prospects and challenges for the application of bimetallic materials are highlighted.This review aims to provide inspiration for CO_(2)RR into high-value chemicals and shed light on the research of bimetallic materials.
基金supported by the National Key R&D Program of China (2019YFC1804102)the National Natural Science Foundation of China (32171615)。
文摘Microbial fuel cell(MFC) is one synchronous power generation device for wastewater treatment that takes into account environmental and energy issues, exhibiting promising potential. Sluggish oxygen reduction reaction(ORR) kinetics on the cathode remains by far the most critical bottleneck hindering the practical application of MFC. An ideal cathode catalyst should possess excellent ORR activity, stability, and costeffectiveness, experiments have demonstrated that bimetallic catalysts are one of the most promising ORR catalysts currently. Based on this, this review mainly analyzes the reaction mechanism(ORR mechanisms, synergistic effects), advantages(combined with characterization technologies), and typical synthesis methods of bimetallic catalysts, focusing on the application effects of early Pt-M(M = Fe, Co, and Ni) alloys to bifunctional catalysts in MFC, pointing out that the main existing challenges remain economic analysis, long-term durability and large-scale application, and looking forward to this. At last, the research trend of bimetallic catalysts suitable for MFC is evaluated, and it is considered that the development and research of metal-organic framework(MOF)-based bimetallic catalysts are still worth focusing on in the future, intending to provide a reference for MFC to achieve energy-efficient wastewater treatment.
文摘Hydrogen energy has become one of the recognized clean energy sources worldwide due to its advantages such as low cost,renewable energy,and green environmental protec-tion.Electrolytic water is currently one of the most promising solutions for providing hydrogen fuel.Nickel iron bimetallic electrocatalysts have abundant sources,low cost,clean and pollution-free properties,and strong catalytic performance,This article mainly reviews the development and research of bimetallic nickel iron oxides and nickel iron alloys in recent years,and explores their synthesis methods,properties,and stability in depth.
基金financially supported by the National Natural Science Foundation of China(22172093 and 21776167)。
文摘The bifunctional oxygen catalyst is essential for zinc-air batteries(ZABs).Here,an efficient bifunctional oxygen catalyst,PPcFeCo/3D-G,is obtained throughπ-πinteraction between the conjugated polymerized iron-cobalt phthalocyanine(PPcFeCo)with excellent thermal stability and three-dimensional graphene(3D-G).The bimetallic synergistic effect of PPcFeCo,verified by DFT(Density functional theory)calculation,andπ-πinteractions enhances the catalytic activity and durability of the PPcFeCo/3D-G.Regarding electrochemical performance,the PPcFeCo/3D-G with a high electron transfer number(3.98,@0.768 V vs.RHE)has excellent half-wave potential(E_(1/2)=0.890 V vs.RHE)and exhibits outstanding reversibility(ΔE=0.700 V,ΔE=Ej=10-E_(1/2)).The liquid ZAB(LZAB)employed PPcFeCo/3D-G displays a high power density(222 m W cm^(-2)),a specific capacity(792 m A h g-1),and excellent durability(120 h).This work has guiding significance for the preparation of high-efficiency bifunctional catalysts.
基金supported by the National Natural Science Foundation of China (22008098, 21978156, 42002040)the Program for Innovative Research Team (in Science and Technology) in University of Henan Province (21IRTSTHN004)+1 种基金the Program for Science & Technology Innovation Talents in Universities of Henan Province (22HASTIT008)the Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering (2022-K34)。
文摘Catalytic hydrogenation of CO_(2) using renewable hydrogen not only reduces greenhouse gas emissions,but also provides industrial chemicals.Herein,a Co-Fe bimetallic catalyst was developed by a facile reactive ball-milling method for highly active and selective hydrogenation of CO_(2) to value-added hydrocarbons.When reacted at 320℃,1.0 MPa and 9600 mL h^(-1) g_(cat)^(-1),the selectivity to light olefin(C_(2)^(=)-C_(4)^(=)) and C_(5)+ species achieves 57.3% and 22.3%,respectively,at a CO_(2) co nversion of 31.4%,which is superior to previous Fe-based catalysts.The CO_(2) activation can be promoted by the CoFe phase formed by reactive ball milling of the Fe-Co_(3)O_(4) mixture,and the in-situ Co_(2)C and Fe_(5)C_(2) formed during hydrogenation are beneficial for the C-C coupling reaction.The initial C-C coupling is related to the combination of CO species with the surface carbon of Fe/Co carbides,and the sustained C-C coupling is maintained by self-recovery of defective carbides.This new strategy contributes to the development of efficient catalysts for the hydrogenation of CO_(2) to value-added hydrocarbons.
文摘Nitrate from the application of nitrogen-based fertilizers in intensive agriculture is a notorious waste product, though it lacks cost-effective solutions for its removal from potential drinking water resources. Catalytic reduction appears to be a promising technique for converting nitrates to benign nitrogen gas. Mesoporous silica SBA-15 is a frequently used catalyst support that has large surface areas and highly ordered nanopores. In this work, mesoporous silica SBA-15 bimetallic catalysts for nitrate reduction were investigated. The catalyst was optimized for the selection of promoter metal (Sn and Cu), noble metal (Pd and Pt) and loading ratios of these metals at different temperatures and reduction conditions. The catalysts prepared were characterized by FT-IR, N2 physisorption, XRD, SEM, and ICP. All catalysts showed the presence of cylindrical mesoporous channels and uniform pore structures that remained even after metals loading. In the presence of a CO<sub>2</sub> buffer, the catalysts 4Pd-1Cu/SBA-15 and 1Pt-1Cu/SBA-15 reduced at 100?C under H2 and 1Pd-1Cu/SBA-15 reduced at 200°C under H2 demonstrated very high nitrate conversion. Furthermore, the forementioned Pd catalysts had higher N2 selectivity (88% - 87%) compared to Pt catalyst (80%). Nitrate conversion by the 4Pd-1Cu/SBA-15 catalyst was significantly decreased to 81% in the absence of CO<sub>2</sub>.
基金supported by Natural Science Foundation of Chongqing Three Gorges University (12ZD14)Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education, Southeast University
文摘A systematic study was carried out to investigate the promotion effect of manganese on the performance of a coprecipitated iron-manganese bimetallic catalyst for the light olefins synthesis from syngas. The catalyst samples were characterized by N2 physisorption, transmis- sion electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), powder X-ray diffraction (XRD), Mossbauer spectroscopy, H2- differential thermogravimetric analysis (H2-DTG), CO temperature-programmed reduction (CO-TPR) and CO2 temperature-programmed des- orption (CO2-TPD). The Fischer-Tropsch synthesis (FTS) performance of the catalyst was measured at 1.5 MPa, 250 ℃ and syngas with H2/CO ratio of 2.0. The characterization results indicated that the addition of manganese decreases the catalyst crystallite size, and improves the catalyst BET surface area and pore volume. The presence of manganese suppresses the catalyst reduction and carburization in H2, CO and syngas, respectively. The addition of manganese improves the catalytic activity of water-gas shift reaction and suppresses the oxidation of iron carbides in the FTS reaction. The incorporation of manganese improves the catalyst surface basicity and results in a significant improvement in the selectivities to light olefins and heavy hydrocarbons (C5+), and furthermore an inhibition of methane formation in FTS. The pure iron catalyst (Mn-00) has the highest initial FTS catalytic activity (65%) and the lowest selectivity (17.35 wt%) to light olefins (C2=-C4=). The addition of an appropriate amount of manganese can improve the catalyst FTS activity.
基金the China High-Tech Development 863 Program,Guangdong Province Sci & Tech Bureau(No.2006B12401006)Guangzhou Sci & Tech Bureau(No.2005U13D2031,2007Z2-D2031)financial support of this work National University of Singapore for financial support.
文摘Novel Cu-Ni/C has been prepared and utilized as an efficient catalyst system in direct synthesis of DMC from CH3OH and CO2.
文摘Silica, alumina, and activated carbon supported iron-cobalt catalysts were prepared by incipient wetness impregnation. These catalysts have been characterized by BET, X-ray diffraction (XRD), and temperature-programmed reduction (TPR). Activity and selectivity of iron-cobalt supported on different carriers for CO hydrogenation were studied under the conditions of 1.5 MPa, 493 K, 630 h^-1, and H2/CO ratio of 1.6. The results indicate that the activity, C4 olefin/(C4 olefin+C4 paraffin) ratio, and C5 olefin/(C5 olefin+C5 paraffin) decrease in the order of Fe-Co/SiO2, Fe-Co/AC1, Fe-Co/Al2O3 and Fe- Co/AC2. The activity of Fe-Co/SiO2 reached a maximum. The results of TPR show that the Fe-Co/SiO2 catalyst is to some extent different. XRD patterns show that the Fe-Co/SiO2 catalyst differs significantly from the others; it has two diffraction peaks. The active spinel phase is correlated with the supports.
文摘PVP-supported bimetallic catalyst, PVP-PdCl2-CdCl2, exhibits extremely high catalytic activity for the hydrogen transfer dechlorination of aryl chlorides in neutral environment. The yields of dechlorination products are high under mild reaction conditions and the operation is simple.
基金Supported by the National Natural Science Foundation of China(21476244,21406245)Transformational Technologies for Clean Energy and Demonstration,Strategic Priority Research Program of the Chinese Academy of Sciences,(XDA 21030600)the Youth Innovation Promotion Association CAS(2016046)
文摘A non-phosgene route for the synthesis of hexamethylene-1,6-diisocyanate(HDI) was developed via catalytic decomposition of hexamethylene-1,6-dicarbamate(HDC) over Zn–Co bi-metallic supported ZSM-5 catalyst.The catalyst was characterized by FTIR and XRD analyses. Three solvents dioctyl sebacate(DOS), dibutyl sebacate(DBS) and 1-butyl-3-methylimidazolium tetrafluoroborate(BMIMBF_4) were investigated and compared; DOS gave better performance. The catalytic performances for thermal decomposition of HDC to HDI using DOS as solvent were then investigated, and the results showed that, under the optimized reaction conditions, i.e.,10 wt%concentration of HDC in DOS, 250 °C temperature, 60 min reaction time, 83.8% yield of HDI had been achieved over Zn–Co/ZSM-5. Decomposition of the intermediate hexamethylene-1-carbamate-6-isocyanate(HMI) over Zn–Co/ZSM-5 in DOS solvent was further studied and the results indicated that yield of HDI from HMI reached to 69.6%(98.6% HDI selectively) at 270 °C, which further increased the yield of the total HDI(HDI_(tol)) to as high as 95.0%. Recycling of catalyst showed that HDI and HMI yield slightly decreased, and by-product yield increased after the catalyst was reused for 4 times. At last possible reaction mechanism was proposed.
基金This work is supported financially by the Natural Sciences and Engineering Research Council of Canada(NSERC),the Fonds de Recherche du Québec-Nature et Technologies(FRQNT)Centre Québécois sur les Materiaux Fonctionnels(CQMF),the Canada Foundation for Innovation(CFI)+1 种基金Institut National de la Recherche Scientifique(INRS).The XAS characterizations were performed at the Canadian Light Source(CLS),which is financially supported by NSERC,CFIthe University of Saskatchewan,the Government of Saskatchewan,Western Economic Diversification Canada,the National Research Council of Canada,and the Canadian Institutes of Health Research。
文摘The electroreduction reaction of CO_(2)(ECO_(2)RR)requires high-performance catalysts to convert CO_(2)into useful chemicals.Transition metal-based atomically dispersed catalysts are promising for the high selectivity and activity in ECO_(2)RR.This work presents a series of atomically dispersed Co,Fe bimetallic catalysts by carbonizing the Fe-introduced Co-zeolitic-imidazolate-framework(C-Fe-Co-ZIF)for the syngas generation from ECO_(2)RR.The synergistic effect of the bimetallic catalyst promotes CO production.Compared to the pure C-Co-ZiF,C-Fe-Co-ZIF facilitates CO production with a CO Faradaic efficiency(FE)boost of 10%,with optimal FE_(CO)of 51.9%,FE_(H_(2))of 42.4%at-0.55 V,and CO current density of 8.0 mA cm^(-2)at-0.7 V versus reversible hydrogen electrode(RHE).The H_(2)/CO ratio is tunable from 0.8 to 4.2 in a wide potential window of-0.35 to-0.8 V versus RHE.The total FE_(CO+H_(2))maintains as high as 93%over 10 h.The proper adding amount of Fe could increase the number of active sites and create mild distortions for the nanoscopic environments of Co and Fe,which is essential for the enhancement of the CO production in ECO_(2)RR.The positive impacts of Cu-Co and Ni-Co bimetallic catalysts demonstrate the versatility and potential application of the bimetallic strategy for ECO_(2)RR.
基金Supported by the National Natural Science Foundation of China(21476211)the Zhejiang Provincial Natural Science Foundation of China(LY16B060004 and LY18B060016)
文摘In the present work, a series of Pt-based catalysts, alloyed with a second metal, i.e., Re, Sn, Er, La, and Y, and supported on activated carbon, ordered mesoporous carbon, N-doped mesoporous carbon or reduced graphene oxide(rGO), have been developed for selective hydrogenation of cinnamaldehyde to cinnamylalcohol. Re and rGO were proved to be the most favorable metal dopant and catalyst support, respectively. Pt_(50) Re_(50)/rGO showed the highest cinnamylalcohol selectivity of 89% with 94% conversion of cinnamaldehyde at the reaction conditions of 120 °C, 2.0 MPaH_2 and 4 h.
基金supported by the Natural Science Foundation of China (91545115,21473145,and 21403178)the Postgraduate Basic Innovative Research Program of Xiamen University (201412G001)the Program for Innovative Research Team in Chinese Universities (no.IRT_14R31)
文摘Cu-x-Fe-y/SiO2 catalysts were prepared using urea-assisted sol-gel method. The structure and physicochemical properties of the catalysts were characterized using N-2 adsorption-desorption, transmission electron microscopy, H-2-temperature-programmed reduction, powder X-ray diffraction, and X-ray photoelectron spectroscopy. Compared with monometallic Cu or Fe catalysts, the bimetallic Cu-x-Fe-y/SiO2 catalysts exhibited enhanced catalytic performance for the selective hydrogenation of diethyl malonate to 1,3-propanediol. The bimetallic catalyst with an optimal Cu/Fe atomic ratio of 2 exhibited the highest activity, which yielded 96.3% conversion to diethyl malonate and 93.3% selectivity to 1,3-propanediol under the optimal reaction conditions. Characterization results revealed that interactions between Cu and Fe contributed to the improvement of diethyl malonate conversion and selectivity to 1,3-propanediol. The X-ray photoelectron spectroscopy results revealed that the addition of appropriate amount of Fe species enhanced the reduction of Cu2+ species, thereby increasing the Cu-0 species on the surface of bimetallic catalyst. It led to a better chemisorption capacity of hydrogen and further promoted of the activation of hydrogen molecule. The ethyl acetate temperature-programmed desorption results indicated that the FeOx species provided the additional adsorption sites for substrate molecules, and they activated the C=O bond. The improved catalytic performance of bimetallic Cu-x-Fe-y/SiO2 catalyst was mainly attributed to the synergistic effect between Cu-0 and FeOx species. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.
基金supported by the National Basic Research Program of China (2011CB201400 and 2011CB808700)the National Natural Science Foundation of China (21373019, 21173008 and 21433001)
文摘The aerobic oxidation of glycerol provides an economically viable route to glyceraldehyde, dihydroxyacetone and glyceric acid with versatile applications, for which monometallic Pt, Au and Pd and bimetallic Au-Pt, Au- Pd and Pt-Pd catalysts on TiO2 were examined under base-free conditions. Pt exhibited a superior activity relative to Pd, and Au-Pd and Pt-Pd while Au was essentially inactive. The presence of Au on the Au-Pt/TiO2 catalysts led to their higher activities (normalized per Pt atom) in a wide range of Au/Pt atomic ratios (i.e. 1/3-7/1 ), and the one with the Au/Pt ratio of 3/1 exhibited the highest activity. Such promoting effect is ascribed to the increased electron density on Pt via the electron transfer from Au to Pt, as characterized by the temperature-programmed desorption of CO and infra-red spectroscopy for CO adsorption. Meanwhile, the presence of Au on Au-Pt/TiO2, most like due to the observed electron transfer, changed the product selectivity, and facilitated the oxidation of the secondary hydroxyl groups in glycerol, leading to the favorable formation of dihydroxyacetone over glyceraldehyde and glyceric acid that were derived from the oxidation of the primary hydroxyl groups. The synergetic effect between Au and Pt demonstrates the feasibility in the efficient oxidation of glycerol to the targeted products, for example, by rational tuning of the electronic properties of metal catalysts.
基金financial supports from the National Natural Science Foundation of China(51801078)the Natural Science Foundation of Jiangsu Province(BK20210884)。
文摘In this study,a MOF-derived bimetallic Co@NiO catalyst was synthesized and doped into MgH_(2)to improve the hydrogen desorption and resorption kinetics.The Co@NiO catalyst decreased the onset dehydrogenation temperature of MgH_(2)by 160℃,compared with un-doped MgH_(2).The MgH^(2+)9%(mass)Co@NiO composite released 6.6%(mass)hydrogen in 350 s at 315℃and uptook 5.4%(mass)hydrogen in500 s at 165℃,showing greatly accelerated de/rehydrogenation rates.Besides,the desorption activation energy of MgH^(2+)9%(mass)Co@NiO was decreased to(93.8±8.4)kJ·mol^(-1).Noteworthy,symbiotic Mg_(2)NiH_(4)/Mg_(2)CoH_(5)clusters were in-situ formed from bimetallic precursors and inlaid on MgH_(2)surface,which are considered as"multi-step hydrogen pumps",and provides surface pathways for hydrogen absorption.Meanwhile,the introduced Mg_(2)NiH_(4)/Mg_(2)CoH_(5)interfaces could provide numerous low energy barrier H diffusion channels,therefore accelerating the hydrogen release and uptake.This research proposes new insights to design high-efficiency bimetallic catalyst for MgH_(2)hydrogen storage.
基金financial support from the National Natural Science Foundation of China(21832001 and 21771009)the Beijing National Laboratory for Molecular Sciences(BNLMSCXXM-202104)。
文摘The water gas shift reaction is of vital significance for the generation and transition of energy due to the application in hydrogen production and industries such as ammonia synthesis and fuel cells.The influence of support doping and bimetallic alloying on the catalytic performance of Pt/Ce O_(2)-based nanocatalysts in water gas shift reaction was reported in this work.Various lanthanide ions and 3d transition metals were respectively introduced into the Ce O_(2)support or Pt to form Pt/Ce O_(2):Ln(Ln=La,Nd,Gd,Tb,Yb)and Pt M/Ce O_(2)(M=Fe,Co,Ni)nanocatalysts.The sample of Pt/Ce O_(2):Tb showed the highest activity(TOF at 200℃=0.051 s^(-1))among the Pt/Ce O_(2):Ln and the undoped Pt/Ce O_(2)catalysts.Besides,the sample of Pt Fe/Ce O_(2)exhibited the highest activity(TOF at 200℃=0.12 s^(-1))among Pt M/Ce O_(2)catalysts.The results of the multiple characterizations indicated that the catalytic activity of Pt/Ce O_(2):Ln catalysts was closely correlated with the amount of oxygen vacancies in doped ceria support.However,the different activity of Pt M/Ce O_(2)bimetallic catalysts was owing to the various Pt oxidation states of the bimetals dispersed on ceria.The study of the reaction pathway indicated that both the samples of Pt/Ce O_(2)and Pt/Ce O_(2):Tb catalyzed the reaction through the formate pathway,and the enhanced activity of the latter derived from the increased concentration of oxygen vacancies along with promoted water dissociation.As for the sample of Pt Fe/Ce O_(2),its catalytic mechanism was the carboxyl route with a higher reaction rate due to the moderate valence of Pt along with improved CO activation.