Direct catalytic transformation of syngas(CO/H_(2)) into high value-added hydrocarbons has been one of the most attractive,yet challenging issues in C1 chemistry. In recent years, the concept of oxide-zeolite(OXZEO) b...Direct catalytic transformation of syngas(CO/H_(2)) into high value-added hydrocarbons has been one of the most attractive,yet challenging issues in C1 chemistry. In recent years, the concept of oxide-zeolite(OXZEO) bifunctional catalysis has emerged and spurred renewed enthusiasm in this field [1,2]. This method describes the use of selected oxide-zeolite-based composite catalysts for the direct syngas-to-hydrocarbons conversion.展开更多
Direct conversion of syngas to aromatics over metal oxide and zeolite(OXZEO) composite catalysts is promising.However,the selectivity of more valuable products such as benzene,toluene and xylenes(BTX) is limited due t...Direct conversion of syngas to aromatics over metal oxide and zeolite(OXZEO) composite catalysts is promising.However,the selectivity of more valuable products such as benzene,toluene and xylenes(BTX) is limited due to undesired secondary methylation of BTX.Herein,we report that the introduction of SAPO-34 into MnCrO_(x)-ZSM-5 catalyst enhances significantly the formation of BTX without sacrificing the aromatics selectivity.Under optimized conditions,the fraction of BTX in aromatics reaches 64.7% versus 28.9% over the catalyst without SAPO-34.A number of model reaction tests and characterizations reveal that SAPO-34 consumes partially the intermediates such as ketene,by converting them to light olefins.Thus,the methylation of BTX by ketene to heavy aromatics is inhibited over the external acid sites of ZSM-5,leading to an enhanced BTX selectivity in the products.This hybrid catalyst provides an efficient method for highly selective synthesis of BTX from syngas.展开更多
Direct conversion of syngas to aromatics(STA)over oxide-zeolite composite catalysts is promising as an alternative method for aromatics production.However,the structural effect of the oxide component in composite cata...Direct conversion of syngas to aromatics(STA)over oxide-zeolite composite catalysts is promising as an alternative method for aromatics production.However,the structural effect of the oxide component in composite catalysts is still ambiguous.Herein,we investigate the size effect by selecting ZnCr_(2)O_(4)spinel,as a probe oxide,mixing with H-ZSM-5 zeolite as a composite catalyst for STA reaction.The CO conversion,aromatics selectivity and space-time yield(STY)of aromatics are all significantly improved with the crystal size of ZnCr_(2)O_(4)oxide decreases,which can mainly attribute to the higher oxygen vacancy concentration and thus the rapid generation of more C1oxygenated intermediate species.Based on the understanding of the size-performance relationship,ZnCr_(2)O_(4)-400 with a smaller size mixing with H-ZSM-5 can achieve32.6%CO conversion with 76%aromatics selectivity.The STY of aromatics reaches as high as 4.79 mmol g_(cat)^(-1)h^(-1),which outperforms the previously reported some typical catalysts.This study elucidates the importance of regulating the size of oxide to design more efficient oxidezeolite composite catalysts for conversion of syngas to value-added chemicals.展开更多
Direct conversion of syngas to aromatics has great potential to decrease fossil fuel dependence.Here,a unique structured hybrid catalyst composed of Fe_(3)O_(4) nanoparticles intimately dispersed inside an acidic zeol...Direct conversion of syngas to aromatics has great potential to decrease fossil fuel dependence.Here,a unique structured hybrid catalyst composed of Fe_(3)O_(4) nanoparticles intimately dispersed inside an acidic zeolite is developed.1 to 4 nm sized Fe_(3)O_(4) nanoparticles end up evenly dispersed in an acidic and slightly mesoporous Al-ZSM-5 based on Fe_(3)O_(4) restructuring during co-hydro thermal synthesis using organosilane modification.A very high aromatic productivity of 214 mmolaromatics h^(-1) gFe^(-1) can be obtained with a remarkable 62%aromatic selectivity in hydrocarbons.This catalyst has excellent sintering resistance ability and maintains stable aromatics production over 570 h.The synthetic insights that postulate a mechanism for the metastable oxide-zeolite reorganization during hydrothermal synthesis could serve as a generic route to sinter-resistant oxide-zeolite composite materials with uniform,well-dispersed oxide nanoparticles in close intimacy with-and partially confined in-a zeolite matrix.展开更多
The metal-organic framework(MOF)derived Ni–Co–C–N composite alloys(NiCCZ)were“embedded”inside the carbon cloth(CC)strands as opposed to the popular idea of growing them upward to realize ultrastable energy storag...The metal-organic framework(MOF)derived Ni–Co–C–N composite alloys(NiCCZ)were“embedded”inside the carbon cloth(CC)strands as opposed to the popular idea of growing them upward to realize ultrastable energy storage and conversion application.The NiCCZ was then oxygen functionalized,facilitating the next step of stoichiometric sulfur anion diffusion during hydrothermal sulfurization,generating a flower-like metal hydroxysulfide structure(NiCCZOS)with strong partial implantation inside CC.Thus obtained NiCCZOS shows an excellent capacity when tested as a supercapacitor electrode in a three-electrode configuration.Moreover,when paired with the biomass-derived nitrogen-rich activated carbon,the asymmetric supercapacitor device shows almost 100%capacity retention even after 45,000 charge–discharge cycles with remarkable energy density(59.4 Wh kg^(-1)/263.8μWh cm^(–2))owing to a uniquely designed cathode.Furthermore,the same electrode performed as an excellent bifunctional water-splitting electrocatalyst with an overpotential of 271 mV for oxygen evolution reaction(OER)and 168.4 mV for hydrogen evolution reaction(HER)at 10 mA cm−2 current density along with 30 h of unhinged chronopotentiometric stability performance for both HER and OER.Hence,a unique metal chalcogenide composite electrode/substrate configuration has been proposed as a highly stable electrode material for flexible energy storage and conversion applications.展开更多
Over the past decade,a growing number of studies have reported transcription factor-based in situ reprogramming that can directly conve rt endogenous glial cells into functional neurons as an alternative approach for ...Over the past decade,a growing number of studies have reported transcription factor-based in situ reprogramming that can directly conve rt endogenous glial cells into functional neurons as an alternative approach for n euro regeneration in the adult mammalian central ne rvous system.Howeve r,many questions remain regarding how a terminally differentiated glial cell can transform into a delicate neuron that forms part of the intricate brain circuitry.In addition,concerns have recently been raised around the absence of astrocyte-to-neuron conversion in astrocytic lineage-tra cing mice.In this study,we employed repetitive two-photon imaging to continuously capture the in situ astrocyte-to-neuron conversion process following ecto pic expression of the neural transcription factor NeuroD1 in both prolife rating reactive astrocytes and lineage-tra ced astrocytes in the mouse cortex.Time-lapse imaging over several wee ks revealed the ste p-by-step transition from a typical astrocyte with numero us short,tapered branches to a typical neuro n with a few long neurites and dynamic growth cones that actively explored the local environment.In addition,these lineage-converting cells were able to migrate ra dially or to ngentially to relocate to suitable positions.Furthermore,two-photon Ca2+imaging and patch-clamp recordings confirmed that the newly generated neuro ns exhibited synchronous calcium signals,repetitive action potentials,and spontaneous synaptic responses,suggesting that they had made functional synaptic connections within local neural circuits.In conclusion,we directly visualized the step-by-step lineage conversion process from astrocytes to functional neurons in vivo and unambiguously demonstrated that adult mammalian brains are highly plastic with respect to their potential for neuro regeneration and neural circuit reconstruction.展开更多
The fructose-to-furfural transformation is facing major challenges in the selectivity and high efficiency. Herein, we have developed a simple and effective approach for the selective conversion of fructose to furfural...The fructose-to-furfural transformation is facing major challenges in the selectivity and high efficiency. Herein, we have developed a simple and effective approach for the selective conversion of fructose to furfural using Hβ zeolite modified by organic acids for dealuminization to regulate its textural and acidic properties. It was found that citric acid-dealuminized Hβ zeolite possessed high specific surface areas, wide channels and high Brønsted acid amount, which facilitated the selective conversion of fructose to furfural with a maximum yield of 76.2% at433 K for 1 h in the γ-butyrolactone(GBL)-H_(2)O system, as well as the concomitant formation of 83.0% formic acid. The^(13)C-isotope labelling experiments and the mechanism revealed that the selective cleavage of C1–C2 or C5–C6 bond on fructose was firstly occurred to form pentose or C5 intermediate by weak Brønsted acid, which was then dehydrated to furfural by strong Brønsted acid. Also this dealuminized Hβ catalyst showed the great recycling performance and was active for the conversion of glucose and mannose.展开更多
Electro-reduction of carbon dioxide(ERCO_(2)) is considered an effective method to alleviate the greenhouse effect and produce value-added chemicals.Achieving the dominant selectivity of Zn-based catalysts for formate...Electro-reduction of carbon dioxide(ERCO_(2)) is considered an effective method to alleviate the greenhouse effect and produce value-added chemicals.Achieving the dominant selectivity of Zn-based catalysts for formate remains a challenge.In this article,the ZnIn-E_(12) catalyst is successfully prepared by solvent assisted ligand exchange(SALE) method to convert organic ligands,achieving a Faradaic efficiency of 72.28% for formate at-1.26 V vs.RHE(V_(RHE)),which is 1.42 times higher than the original catalyst.Evidence shows that the successful conversion of organic ligands can transform the catalyst from the original large size polyhedron to cross-linked network of particles with a diameter of about 30 nm.The increased specific surface area can expose more active sites and facilitate the electrocatalytic conversion of CO_(2) to formate.This work is expected to provide inspiration for the regulation of formate selectivity and catalyst size in Zn-based catalysts.展开更多
A series of carbon nitride(CN)materials represented by graphitic carbon nitride(g-C3N4)have been widely used in bioimaging,biosensing,and other fields in recent years due to their nontoxicity,low cost,and high lumines...A series of carbon nitride(CN)materials represented by graphitic carbon nitride(g-C3N4)have been widely used in bioimaging,biosensing,and other fields in recent years due to their nontoxicity,low cost,and high luminescent quantum efficiency.What is more attractive is that the luminescent properties such as wavelength and intensity can be regulated by controlling the structure at the molecular level.Hence,it is time to summarize the related research on CN structural evolution and make a prospect on future developments.In this review,we first summarize the research history and multiple structural evolution of CN.Then,the progress of improving the luminescence performance of CN through structural evolution was discussed.Significantly,the relationship between CN structure evolution and energy conversion in the forms of photoluminescence,chemiluminescence,and electrochemiluminescence was reviewed.Finally,key challenges and opportunities such as nanoscale dispersion strategy,luminous efficiency improving methods,standardization evaluation,and macroscopic preparation of CN are highlighted.展开更多
Electrochemical C-C and C-N coupling reactions with the conversion of abundant and inexpensive small molecules,such as CO_(2) and nitrogencontaining species,are considered a promising route for increasing the value of...Electrochemical C-C and C-N coupling reactions with the conversion of abundant and inexpensive small molecules,such as CO_(2) and nitrogencontaining species,are considered a promising route for increasing the value of CO_(2) reduction products.The development of high-performance catalysts is the key to the both electrocatalytic reactions.In this review,we present a systematic summary of the reaction systems for electrocatalytic CO_(2) reduction,along with the coupling mechanisms of C-C and C-N bonds over outstanding electrocatalytic materials recently developed.The key intermediate species and reaction pathways related to the coupling as well as the catalyst-structure relationship will be also discussed,aiming to provide insights and guidance for designing efficient CO_(2) reduction systems.展开更多
BACKGROUND Hepatocellular carcinoma(HCC)is one of the leading causes of death due to its complexity,heterogeneity,rapid metastasis and easy recurrence after surgical resection.We demonstrated that combination therapy ...BACKGROUND Hepatocellular carcinoma(HCC)is one of the leading causes of death due to its complexity,heterogeneity,rapid metastasis and easy recurrence after surgical resection.We demonstrated that combination therapy with transcatheter arterial chemoembolization(TACE),hepatic arterial infusion chemotherapy(HAIC),Epclusa,Lenvatinib and Sintilimab is useful for patients with advanced HCC.CASE SUMMARY A 69-year-old man who was infected with hepatitis C virus(HCV)30 years previously was admitted to the hospital with abdominal pain.Enhanced computed tomography(CT)revealed a low-density mass in the right lobe of the liver,with a volume of 12.9 cm×9.4 cm×15 cm,and the mass exhibited a“fast-in/fast-out”pattern,with extensive filling defect areas in the right branch of the portal vein and an alpha-fetoprotein level as high as 657 ng/mL.Therefore,he was judged to have advanced HCC.During treatment,the patient received three months of Epclusa,three TACE treatments,two HAIC treatments,three courses of sintilimab,and twenty-one months of lenvatinib.In the third month of treatment,the patient developed severe side effects and had to stop immunotherapy,and the Lenvatinib dose had to be halved.Postoperative pathological diagnosis indicated a complete response.The patient recovered well after the operation,and no tumor recurrence was found.CONCLUSION Multidisciplinary conversion therapy for advanced enormous HCC caused by HCV infection has a significant effect.Individualized drug adjustments should be made during any treatment according to the patient's tolerance to treatment.展开更多
The increase in anthropogenic carbon dioxide(CO_(2))emissions has exacerbated the deterioration of the global environment,which should be controlled to achieve carbon neutrality.Central to the core goal of achieving c...The increase in anthropogenic carbon dioxide(CO_(2))emissions has exacerbated the deterioration of the global environment,which should be controlled to achieve carbon neutrality.Central to the core goal of achieving carbon neutrality is the utilization of CO_(2) under economic and sustainable conditions.Recently,the strong need for carbon neutrality has led to a proliferation of studies on the direct conversion of CO_(2) into carboxylic acids,which can effectively alleviate CO_(2) emissions and create high-value chemicals.The purpose of this review is to present the application prospects of carboxylic acids and the basic principles of CO_(2) conversion into carboxylic acids through photo-,electric-,and thermal catalysis.Special attention is focused on the regulation strategy of the activity of abundant catalysts at the molecular level,inspiring the preparation of high-performance catalysts.In addition,theoretical calculations,advanced technologies,and numerous typical examples are introduced to elaborate on the corresponding process and influencing factors of catalytic activity.Finally,challenges and prospects are provided for the future development of this field.It is hoped that this review will contribute to a deeper understanding of the conversion of CO_(2) into carboxylic acids and inspire more innovative breakthroughs.展开更多
Different drillingfluid systems are designed according to mineral composition,lithology and wellbore stability of different strata.In the present study,the conversion of a non-dispersed polymer drillingfluid into a low ...Different drillingfluid systems are designed according to mineral composition,lithology and wellbore stability of different strata.In the present study,the conversion of a non-dispersed polymer drillingfluid into a low potas-sium anti-collapsing drillingfluid is investigated.Since the two drillingfluids belong to completely different types,the key to this conversion is represented by new inhibitors,dispersants and water-loss agents by which a non-dispersed drillingfluid can be turned into a dispersed drillingfluid while ensuring wellbore stability and reason-able rheology(carrying sand—inhibiting cuttings dispersion).In particular,the(QYZ-1)inhibitors and(FSJSS-2)dispersants are used.The former can inhibit the hydration expansion capacity of clay,reduce the dynamic shear force and weaken the viscosity;the latter can improve the sealing effect and reduce thefiltrate loss.The results have shown that after adding a reasonable proportion of these substances(QYZ-1:FSJSS-2)to the non-dispersed polymer drillingfluid,while the apparent viscosity,plastic viscosity,structural viscosity andfluidity index under-went almost negligible changes,the dynamic plastic ratio increased,and thefiltration loss decreased significantly,thereby indicating good compatibility.According to the tests(conducted in the Leijia area),the density was 1.293 g/cm3,and after standing for 24 h,the SF(static settlement factor)was 0.51.Moreover,thefiltration loss was reduced to 4.0 mL,the rolling recovery rate reached 96.92%,with excellent plugging and anti-collapse performances.展开更多
With the expansion of butene production capacity,clean and efficient conversion of mixed butene attracts increasing attention.Herein we report direct co-conversion of butene and syngas to highquality gasoline enabled ...With the expansion of butene production capacity,clean and efficient conversion of mixed butene attracts increasing attention.Herein we report direct co-conversion of butene and syngas to highquality gasoline enabled by a bifunctional OXZEO catalyst comprising ZnCrO_(x) oxide and ZSM-5 zeolite.A gasoline selectivity of 71.6% at 98.1% butene conversion and 26.2% CO conversion have been obtained under the reaction conditions of 360℃,3 MPa and 3000 mL g^(-1) h^(-1).The space time yield of gasoline of0.25 g·g^(-1) h^(-1) is achieved.Interestingly,the presence of syngas can effectively facilitate iso-paraffin production while hindering the formation of aromatics.This is attributed to the prohibited hydrogen transfer aromatization process of butene on ZSM-5 in the presence of H2.Fu rthermore,the formation of isomers of gasoline range hydrocarbons is favored because the active intermediates generated from CO/H_(2) activation over ZnCrO_(x) oxide could react with butene over ZSM-5 zeolite.Thus,the product distribution among gasoline range hydrocarbons is modulated with reduced heavy aromatics and improved iso-paraffins,which is desirable for application as fuels.This provides an alternative environmentally friendly technology to utilize still increasing mixed butene.展开更多
In the conversion process of syngas-to-C_(2)species,the OH species are inevitably produced accompanying the production of key intermediates CH_(x)(x=1-3),traditionally,the function of surface OH species is generally a...In the conversion process of syngas-to-C_(2)species,the OH species are inevitably produced accompanying the production of key intermediates CH_(x)(x=1-3),traditionally,the function of surface OH species is generally accepted as the hydrogenating reactive species.This work for the first time proposed and confirmed the assisted catalytic mechanism of surface OH species that performed as the promoter for syngas-to-C_(2)species on Cu-based catalysts.DFT and microkinetic modeling results reveal that the produced OH species accompanying the intermediates CH_(x)production on the MCu(M=Co,Fe,Rh)catalysts can stably exist to form OH/MCu catalysts,on which the presence of surface OH species as the promoter not only presented better activity and selectivity toward CH_(x)(x=1-3)compared to MCu catalysts,but also significantly suppressed CH_(3)OH production,providing enough CH_(x)sources to favor the production of C_(2)hydrocarbons and oxygenates.Correspondingly,the electronic properties analysis revealed the essential relationship between the electronic feature of OH/MCu catalysts and catalytic performance,attributing to the unique electronic micro-environment of the catalysts under the interaction of surface OH species.This new mechanism is called as OH-assisted catalytic mechanism,which may be applied in the reaction systems related to the generation of OH species.展开更多
Oxide-Zeolite(OX-ZEO) bifunctional catalyst design concept has been exemplified in several processes to direct conversion syngas to value-added chemicals and fuels such as mixed light olefins, ethylene, aromatics and ...Oxide-Zeolite(OX-ZEO) bifunctional catalyst design concept has been exemplified in several processes to direct conversion syngas to value-added chemicals and fuels such as mixed light olefins, ethylene, aromatics and gasoline.Herein we demonstrate that the product can be steered toward liquefied petroleum gas(LPG) with a selectivity up to 89% in hydrocarbons especially propane selectivity reaching 80% at CO conversion of 63% using ZnCrOx-H-SSZ-39 catalyst.Interestingly, the quantity of the acid sites of SSZ-39 does not influence obviously the hydrocarbon distribution but the strength is crucial for selective formation of propane.This finding provides an alternative route of LPG synthesis from a variety of carbon resources via syngas.展开更多
CexZr1-xO2 mixed oxides with different Ce/Zr ratios were prepared by coprecipitation. The characterizations of mixed oxides were studied by X-ray diffraction (XRD) and H2-TPR. And the performances were tested in a fix...CexZr1-xO2 mixed oxides with different Ce/Zr ratios were prepared by coprecipitation. The characterizations of mixed oxides were studied by X-ray diffraction (XRD) and H2-TPR. And the performances were tested in a fixed-bed quartz reactor. The results indicated that lattice oxygen of CexZr1-xO2 could oxidate methane to syngas and the incorporation of zirconium into the ceria lattice could improve the O2- mobility. The Ce0.7Zr0.3O2 had the best activity in investigative temperature ranging from 600 to 900 ℃. Effects of reaction time on H2/CO ratio were studied at 850 ℃ when using Ce0.7Zr0.3O2 as catalyst. The results indicated that the ratio was closed to 2 values in the first 10 min, however, it rapidly increased with reaction time after >10 min. The possible reason was that the direct partial oxidation of methane reaction was dominant in the first 10 min. However, the methane pyrogenation was responsible for the rapid increase of H2/CO ratio after 10 min. Thus, if syngas with H2/CO ratio of 2 wanted to be obtained, the reaction time needed to be controlled.展开更多
Realizing high CO conversion and high aromatics selectivity simultaneously in syngas-to-aromatics(STA)reaction is still challenging.Herein,we report a 57.5%CO conversion along with 74%aromatics selectivity over a comp...Realizing high CO conversion and high aromatics selectivity simultaneously in syngas-to-aromatics(STA)reaction is still challenging.Herein,we report a 57.5%CO conversion along with 74%aromatics selectivity over a composite catalyst consisting of Fe/ZnCr_(2)O_(4)(Fe modified ZnCr_(2)O_(4)spinel)oxide and H-ZSM-5 zeolite.Impregnation of only 3 wt%of Fe onto ZnCr_(2)O_(4)can remarkably increase CO conversion without sacrificing the aromatics selectivity.Oxygen vacancy concentration is improved after impregnating Fe.The highly dispersed iron carbide species is formed during the reaction over Fe/ZnCr_(2)O_(4)spinel oxide.The synergistic effect of oxygen vacancy and iron carbide results in a rapid formation of abundant oxygenated intermediate species,which can be continuously transformed to aromatics in H-ZSM-5.This study provides a new insight into the design of highly efficient catalyst for syngas conversion.展开更多
Syngas conversion to fuels and chemicals is one of the most challenging subjects in the field of C1 chemistry. It is considered as an attractive alternative non-petroleum-based production route. The direct synthesis o...Syngas conversion to fuels and chemicals is one of the most challenging subjects in the field of C1 chemistry. It is considered as an attractive alternative non-petroleum-based production route. The direct synthesis of olefins and alcohols as high value-added chemicals from syngas has drawn particular attention due to its process simplicity, low energy consumption and clean utilization of carbon resource, which conforms to the principles of green carbon science. This review describes the recent advances for the direct production of lower olefins and higher alcohols via syngas conversion. Recent progress in the development of new catalyst systems for enhanced catalytic performance is highlighted. We also give recommendations regarding major challenges for further research in syngas conversion to various chemicals.展开更多
A series of ZnO-ZrO_(2) solid solutions with different Zn contents were synthesized by the urea coprecipitation method,which were coupled with H-ZSM-5 zeolite to form bifunctional catalysts.As a new benzene alkylation...A series of ZnO-ZrO_(2) solid solutions with different Zn contents were synthesized by the urea coprecipitation method,which were coupled with H-ZSM-5 zeolite to form bifunctional catalysts.As a new benzene alkylation reagent,syngas was used instead of methanol to realize the efficient conversion of syngas and benzene into toluene and xylene.A suitable ratio of ZnO-ZrO_(2) led to the significant improvement in the catalytic performance,and a suitable amount of acid helped to increase the selectivity of toluene/xylene and reduce the selectivity of the by-products ethylbenzene and C^(9+) aromatics.The highest benzene conversion of 89.2%and toluene/xylene selectivity of 88.7%were achieved over 10%ZnO-ZrO_(2)&H-ZSM-5(Si/Al=23)at a pressure of 3 MPa and a temperature of 450℃.In addition,the effect of the zeolite framework structure on product distribution was examined.Similar to the molecular dynamics of aromatic hydrocarbons,H-ZSM-5 zeolites comprise 10-membered-ring pores,which are beneficial to the activation of benzene;hence,the conversion of benzene is higher.H-ZSM-35 and HMOR zeolites exhibited small eight-membered-ring channels,which were not conducive to the passage of benzene;hence,the by-product ethylbenzene exhibits a higher selectivity.The distance between the active centers of the bifunctional catalysts was the main factor affecting the catalytic performance,and the powder mixing method was more conducive to the conversion of syngas and benzene.展开更多
基金supported by the National Natural Science Foundation of China(Grant No.21773230,91945302,21902158,22002165)the Liao Ning Revitalization Talents Program(XLYC1807207)+5 种基金the China National Postdoctoral Program for Innovative Talents(BX20190321)the China Postdoctoral Science Foundation(2019M651161,2019M651154)the DICP&QIBEBT UN201808the DICP I202104the EPSRC Institutional Sponsorship for funding(EP/P511353/1)The DNP MAS NMR experiments were performed at the Nottingham DNP MAS NMR Facility which is funded by the University of Nottingham and EPSRC(EP/L022524/1 and EP/R042853/1)。
文摘Direct catalytic transformation of syngas(CO/H_(2)) into high value-added hydrocarbons has been one of the most attractive,yet challenging issues in C1 chemistry. In recent years, the concept of oxide-zeolite(OXZEO) bifunctional catalysis has emerged and spurred renewed enthusiasm in this field [1,2]. This method describes the use of selected oxide-zeolite-based composite catalysts for the direct syngas-to-hydrocarbons conversion.
基金supported by the National Natural Science Foundation of China (22321002 and 22008234)the Natural Science Foundation of Liaoning Province (2022011086-JH3/107)+1 种基金Dalian High-level Talent Innovation Program (2021RQ111)the Innovation Research Fund of Dalian Institute of Chemical Physics (DICP I202240)。
文摘Direct conversion of syngas to aromatics over metal oxide and zeolite(OXZEO) composite catalysts is promising.However,the selectivity of more valuable products such as benzene,toluene and xylenes(BTX) is limited due to undesired secondary methylation of BTX.Herein,we report that the introduction of SAPO-34 into MnCrO_(x)-ZSM-5 catalyst enhances significantly the formation of BTX without sacrificing the aromatics selectivity.Under optimized conditions,the fraction of BTX in aromatics reaches 64.7% versus 28.9% over the catalyst without SAPO-34.A number of model reaction tests and characterizations reveal that SAPO-34 consumes partially the intermediates such as ketene,by converting them to light olefins.Thus,the methylation of BTX by ketene to heavy aromatics is inhibited over the external acid sites of ZSM-5,leading to an enhanced BTX selectivity in the products.This hybrid catalyst provides an efficient method for highly selective synthesis of BTX from syngas.
基金financial support from the National Natural Science Foundation of China(Grant No.21978285,21991093,21991090)the“Transformational Technologies for Clean Energy and Demonstration”,Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDA21030100)。
文摘Direct conversion of syngas to aromatics(STA)over oxide-zeolite composite catalysts is promising as an alternative method for aromatics production.However,the structural effect of the oxide component in composite catalysts is still ambiguous.Herein,we investigate the size effect by selecting ZnCr_(2)O_(4)spinel,as a probe oxide,mixing with H-ZSM-5 zeolite as a composite catalyst for STA reaction.The CO conversion,aromatics selectivity and space-time yield(STY)of aromatics are all significantly improved with the crystal size of ZnCr_(2)O_(4)oxide decreases,which can mainly attribute to the higher oxygen vacancy concentration and thus the rapid generation of more C1oxygenated intermediate species.Based on the understanding of the size-performance relationship,ZnCr_(2)O_(4)-400 with a smaller size mixing with H-ZSM-5 can achieve32.6%CO conversion with 76%aromatics selectivity.The STY of aromatics reaches as high as 4.79 mmol g_(cat)^(-1)h^(-1),which outperforms the previously reported some typical catalysts.This study elucidates the importance of regulating the size of oxide to design more efficient oxidezeolite composite catalysts for conversion of syngas to value-added chemicals.
基金supported financially by the National Natural Science Foundation of China(51776206)the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(2017BT01N092)+4 种基金the National Key R&D Program of China(2018YFB1501504)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX20_0095)the Fundamental Research Funds for the Central Universities(3203002104D)the Research Foundation-Flanders(FWO,grant 12E8617N)for funding and KU Leuven grant C14/20/086visiting scholar(2017-20202)at the Guangzhou Institute of Energy Conversion,Chinese Academy of Sciences。
文摘Direct conversion of syngas to aromatics has great potential to decrease fossil fuel dependence.Here,a unique structured hybrid catalyst composed of Fe_(3)O_(4) nanoparticles intimately dispersed inside an acidic zeolite is developed.1 to 4 nm sized Fe_(3)O_(4) nanoparticles end up evenly dispersed in an acidic and slightly mesoporous Al-ZSM-5 based on Fe_(3)O_(4) restructuring during co-hydro thermal synthesis using organosilane modification.A very high aromatic productivity of 214 mmolaromatics h^(-1) gFe^(-1) can be obtained with a remarkable 62%aromatic selectivity in hydrocarbons.This catalyst has excellent sintering resistance ability and maintains stable aromatics production over 570 h.The synthetic insights that postulate a mechanism for the metastable oxide-zeolite reorganization during hydrothermal synthesis could serve as a generic route to sinter-resistant oxide-zeolite composite materials with uniform,well-dispersed oxide nanoparticles in close intimacy with-and partially confined in-a zeolite matrix.
基金supported by the Basic Science Research Program through the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(2021R1A4A2000934).
文摘The metal-organic framework(MOF)derived Ni–Co–C–N composite alloys(NiCCZ)were“embedded”inside the carbon cloth(CC)strands as opposed to the popular idea of growing them upward to realize ultrastable energy storage and conversion application.The NiCCZ was then oxygen functionalized,facilitating the next step of stoichiometric sulfur anion diffusion during hydrothermal sulfurization,generating a flower-like metal hydroxysulfide structure(NiCCZOS)with strong partial implantation inside CC.Thus obtained NiCCZOS shows an excellent capacity when tested as a supercapacitor electrode in a three-electrode configuration.Moreover,when paired with the biomass-derived nitrogen-rich activated carbon,the asymmetric supercapacitor device shows almost 100%capacity retention even after 45,000 charge–discharge cycles with remarkable energy density(59.4 Wh kg^(-1)/263.8μWh cm^(–2))owing to a uniquely designed cathode.Furthermore,the same electrode performed as an excellent bifunctional water-splitting electrocatalyst with an overpotential of 271 mV for oxygen evolution reaction(OER)and 168.4 mV for hydrogen evolution reaction(HER)at 10 mA cm−2 current density along with 30 h of unhinged chronopotentiometric stability performance for both HER and OER.Hence,a unique metal chalcogenide composite electrode/substrate configuration has been proposed as a highly stable electrode material for flexible energy storage and conversion applications.
基金supported by the National Natural Science Foundation of China,No.31970906(to WLei)the Natural Science Foundation of Guangdong Province,No.2020A1515011079(to WLei)+4 种基金Key Technologies R&D Program of Guangdong Province,No.2018B030332001(to GC)Science and Technology Projects of Guangzhou,No.202206060002(to GC)the Youth Science Program of the National Natural Science Foundation of China,No.32100793(to ZX)the Pearl River Innovation and Entrepreneurship Team,No.2021ZT09 Y552Yi-Liang Liu Endowment Fund from Jinan University Education Development Foundation。
文摘Over the past decade,a growing number of studies have reported transcription factor-based in situ reprogramming that can directly conve rt endogenous glial cells into functional neurons as an alternative approach for n euro regeneration in the adult mammalian central ne rvous system.Howeve r,many questions remain regarding how a terminally differentiated glial cell can transform into a delicate neuron that forms part of the intricate brain circuitry.In addition,concerns have recently been raised around the absence of astrocyte-to-neuron conversion in astrocytic lineage-tra cing mice.In this study,we employed repetitive two-photon imaging to continuously capture the in situ astrocyte-to-neuron conversion process following ecto pic expression of the neural transcription factor NeuroD1 in both prolife rating reactive astrocytes and lineage-tra ced astrocytes in the mouse cortex.Time-lapse imaging over several wee ks revealed the ste p-by-step transition from a typical astrocyte with numero us short,tapered branches to a typical neuro n with a few long neurites and dynamic growth cones that actively explored the local environment.In addition,these lineage-converting cells were able to migrate ra dially or to ngentially to relocate to suitable positions.Furthermore,two-photon Ca2+imaging and patch-clamp recordings confirmed that the newly generated neuro ns exhibited synchronous calcium signals,repetitive action potentials,and spontaneous synaptic responses,suggesting that they had made functional synaptic connections within local neural circuits.In conclusion,we directly visualized the step-by-step lineage conversion process from astrocytes to functional neurons in vivo and unambiguously demonstrated that adult mammalian brains are highly plastic with respect to their potential for neuro regeneration and neural circuit reconstruction.
基金supported by Program for National Natural Science Foundation of China(Nos.22178135,21978104 and 22278419)the National Key Research and Development Program of China(No.2021YFC2101601)。
文摘The fructose-to-furfural transformation is facing major challenges in the selectivity and high efficiency. Herein, we have developed a simple and effective approach for the selective conversion of fructose to furfural using Hβ zeolite modified by organic acids for dealuminization to regulate its textural and acidic properties. It was found that citric acid-dealuminized Hβ zeolite possessed high specific surface areas, wide channels and high Brønsted acid amount, which facilitated the selective conversion of fructose to furfural with a maximum yield of 76.2% at433 K for 1 h in the γ-butyrolactone(GBL)-H_(2)O system, as well as the concomitant formation of 83.0% formic acid. The^(13)C-isotope labelling experiments and the mechanism revealed that the selective cleavage of C1–C2 or C5–C6 bond on fructose was firstly occurred to form pentose or C5 intermediate by weak Brønsted acid, which was then dehydrated to furfural by strong Brønsted acid. Also this dealuminized Hβ catalyst showed the great recycling performance and was active for the conversion of glucose and mannose.
基金financially supported by the National Natural Science Foundation of China(22072087)。
文摘Electro-reduction of carbon dioxide(ERCO_(2)) is considered an effective method to alleviate the greenhouse effect and produce value-added chemicals.Achieving the dominant selectivity of Zn-based catalysts for formate remains a challenge.In this article,the ZnIn-E_(12) catalyst is successfully prepared by solvent assisted ligand exchange(SALE) method to convert organic ligands,achieving a Faradaic efficiency of 72.28% for formate at-1.26 V vs.RHE(V_(RHE)),which is 1.42 times higher than the original catalyst.Evidence shows that the successful conversion of organic ligands can transform the catalyst from the original large size polyhedron to cross-linked network of particles with a diameter of about 30 nm.The increased specific surface area can expose more active sites and facilitate the electrocatalytic conversion of CO_(2) to formate.This work is expected to provide inspiration for the regulation of formate selectivity and catalyst size in Zn-based catalysts.
基金supported by the Natural Science Foundation of Hebei Province(Grant No.E2022209039)Key Research Project of North China University of Science and Technology(Grant No.ZD-YG-202301)Tangshan Talent Funding Project(Grant No.A202202007).
文摘A series of carbon nitride(CN)materials represented by graphitic carbon nitride(g-C3N4)have been widely used in bioimaging,biosensing,and other fields in recent years due to their nontoxicity,low cost,and high luminescent quantum efficiency.What is more attractive is that the luminescent properties such as wavelength and intensity can be regulated by controlling the structure at the molecular level.Hence,it is time to summarize the related research on CN structural evolution and make a prospect on future developments.In this review,we first summarize the research history and multiple structural evolution of CN.Then,the progress of improving the luminescence performance of CN through structural evolution was discussed.Significantly,the relationship between CN structure evolution and energy conversion in the forms of photoluminescence,chemiluminescence,and electrochemiluminescence was reviewed.Finally,key challenges and opportunities such as nanoscale dispersion strategy,luminous efficiency improving methods,standardization evaluation,and macroscopic preparation of CN are highlighted.
基金support from the Tangshan Talent Funding Project(Grant No.A202202007)National Natural Science Foundation of China(Grant Nos.22102136 and 21703065)+2 种基金Natural Science Foundation of Hebei Province(Grant Nos.B2018209267 and E2022209039)Natural Science Foundation of Hubei Province(Grant No.2022CFB1001)Department of Education of Hubei Province(Grant No.Q20221701).
文摘Electrochemical C-C and C-N coupling reactions with the conversion of abundant and inexpensive small molecules,such as CO_(2) and nitrogencontaining species,are considered a promising route for increasing the value of CO_(2) reduction products.The development of high-performance catalysts is the key to the both electrocatalytic reactions.In this review,we present a systematic summary of the reaction systems for electrocatalytic CO_(2) reduction,along with the coupling mechanisms of C-C and C-N bonds over outstanding electrocatalytic materials recently developed.The key intermediate species and reaction pathways related to the coupling as well as the catalyst-structure relationship will be also discussed,aiming to provide insights and guidance for designing efficient CO_(2) reduction systems.
基金Supported by Shanghai Hospital Development Center Foundation,No.SHDC2022CRS033.
文摘BACKGROUND Hepatocellular carcinoma(HCC)is one of the leading causes of death due to its complexity,heterogeneity,rapid metastasis and easy recurrence after surgical resection.We demonstrated that combination therapy with transcatheter arterial chemoembolization(TACE),hepatic arterial infusion chemotherapy(HAIC),Epclusa,Lenvatinib and Sintilimab is useful for patients with advanced HCC.CASE SUMMARY A 69-year-old man who was infected with hepatitis C virus(HCV)30 years previously was admitted to the hospital with abdominal pain.Enhanced computed tomography(CT)revealed a low-density mass in the right lobe of the liver,with a volume of 12.9 cm×9.4 cm×15 cm,and the mass exhibited a“fast-in/fast-out”pattern,with extensive filling defect areas in the right branch of the portal vein and an alpha-fetoprotein level as high as 657 ng/mL.Therefore,he was judged to have advanced HCC.During treatment,the patient received three months of Epclusa,three TACE treatments,two HAIC treatments,three courses of sintilimab,and twenty-one months of lenvatinib.In the third month of treatment,the patient developed severe side effects and had to stop immunotherapy,and the Lenvatinib dose had to be halved.Postoperative pathological diagnosis indicated a complete response.The patient recovered well after the operation,and no tumor recurrence was found.CONCLUSION Multidisciplinary conversion therapy for advanced enormous HCC caused by HCV infection has a significant effect.Individualized drug adjustments should be made during any treatment according to the patient's tolerance to treatment.
基金financial support from the King Abdullah University of Science and Technology(KAUST).
文摘The increase in anthropogenic carbon dioxide(CO_(2))emissions has exacerbated the deterioration of the global environment,which should be controlled to achieve carbon neutrality.Central to the core goal of achieving carbon neutrality is the utilization of CO_(2) under economic and sustainable conditions.Recently,the strong need for carbon neutrality has led to a proliferation of studies on the direct conversion of CO_(2) into carboxylic acids,which can effectively alleviate CO_(2) emissions and create high-value chemicals.The purpose of this review is to present the application prospects of carboxylic acids and the basic principles of CO_(2) conversion into carboxylic acids through photo-,electric-,and thermal catalysis.Special attention is focused on the regulation strategy of the activity of abundant catalysts at the molecular level,inspiring the preparation of high-performance catalysts.In addition,theoretical calculations,advanced technologies,and numerous typical examples are introduced to elaborate on the corresponding process and influencing factors of catalytic activity.Finally,challenges and prospects are provided for the future development of this field.It is hoped that this review will contribute to a deeper understanding of the conversion of CO_(2) into carboxylic acids and inspire more innovative breakthroughs.
文摘Different drillingfluid systems are designed according to mineral composition,lithology and wellbore stability of different strata.In the present study,the conversion of a non-dispersed polymer drillingfluid into a low potas-sium anti-collapsing drillingfluid is investigated.Since the two drillingfluids belong to completely different types,the key to this conversion is represented by new inhibitors,dispersants and water-loss agents by which a non-dispersed drillingfluid can be turned into a dispersed drillingfluid while ensuring wellbore stability and reason-able rheology(carrying sand—inhibiting cuttings dispersion).In particular,the(QYZ-1)inhibitors and(FSJSS-2)dispersants are used.The former can inhibit the hydration expansion capacity of clay,reduce the dynamic shear force and weaken the viscosity;the latter can improve the sealing effect and reduce thefiltrate loss.The results have shown that after adding a reasonable proportion of these substances(QYZ-1:FSJSS-2)to the non-dispersed polymer drillingfluid,while the apparent viscosity,plastic viscosity,structural viscosity andfluidity index under-went almost negligible changes,the dynamic plastic ratio increased,and thefiltration loss decreased significantly,thereby indicating good compatibility.According to the tests(conducted in the Leijia area),the density was 1.293 g/cm3,and after standing for 24 h,the SF(static settlement factor)was 0.51.Moreover,thefiltration loss was reduced to 4.0 mL,the rolling recovery rate reached 96.92%,with excellent plugging and anti-collapse performances.
基金supported by the Ministry of Science and Technology of China (2018YFA0704503)the National Natural Science Foundation of China (Grant Nos. 22002153, 91945302)+2 种基金the Youth Innovation Promotion Association of Chinese Academy of Sciences (2019184)the Natural Science Foundation of Liaoning (2020-BS019)Dalian Science and Technology Innovation Fund (2020JJ26GX028)。
文摘With the expansion of butene production capacity,clean and efficient conversion of mixed butene attracts increasing attention.Herein we report direct co-conversion of butene and syngas to highquality gasoline enabled by a bifunctional OXZEO catalyst comprising ZnCrO_(x) oxide and ZSM-5 zeolite.A gasoline selectivity of 71.6% at 98.1% butene conversion and 26.2% CO conversion have been obtained under the reaction conditions of 360℃,3 MPa and 3000 mL g^(-1) h^(-1).The space time yield of gasoline of0.25 g·g^(-1) h^(-1) is achieved.Interestingly,the presence of syngas can effectively facilitate iso-paraffin production while hindering the formation of aromatics.This is attributed to the prohibited hydrogen transfer aromatization process of butene on ZSM-5 in the presence of H2.Fu rthermore,the formation of isomers of gasoline range hydrocarbons is favored because the active intermediates generated from CO/H_(2) activation over ZnCrO_(x) oxide could react with butene over ZSM-5 zeolite.Thus,the product distribution among gasoline range hydrocarbons is modulated with reduced heavy aromatics and improved iso-paraffins,which is desirable for application as fuels.This provides an alternative environmentally friendly technology to utilize still increasing mixed butene.
基金financially supported by Key Projects of National Natural Science Foundation of China(No.21736007)National Natural Science Foundation of China(Nos.22078221,21776193,21476155)Top Young Innovative Talents of Shanxi。
文摘In the conversion process of syngas-to-C_(2)species,the OH species are inevitably produced accompanying the production of key intermediates CH_(x)(x=1-3),traditionally,the function of surface OH species is generally accepted as the hydrogenating reactive species.This work for the first time proposed and confirmed the assisted catalytic mechanism of surface OH species that performed as the promoter for syngas-to-C_(2)species on Cu-based catalysts.DFT and microkinetic modeling results reveal that the produced OH species accompanying the intermediates CH_(x)production on the MCu(M=Co,Fe,Rh)catalysts can stably exist to form OH/MCu catalysts,on which the presence of surface OH species as the promoter not only presented better activity and selectivity toward CH_(x)(x=1-3)compared to MCu catalysts,but also significantly suppressed CH_(3)OH production,providing enough CH_(x)sources to favor the production of C_(2)hydrocarbons and oxygenates.Correspondingly,the electronic properties analysis revealed the essential relationship between the electronic feature of OH/MCu catalysts and catalytic performance,attributing to the unique electronic micro-environment of the catalysts under the interaction of surface OH species.This new mechanism is called as OH-assisted catalytic mechanism,which may be applied in the reaction systems related to the generation of OH species.
基金supported by the Ministry of Science and Technology of China (No.2017YFB0602201)the Chinese Academy of Sciences (XDA21020400)+2 种基金the National Natural Science Foundation of China (Grant nos.91645204, 21425312 and 21621063)the Youth Innovation Promotion Association of Chinese Academy of Sciences (2019184)the INCOE (International Network of Centers of Excellence) project coordinated by BASF SE
文摘Oxide-Zeolite(OX-ZEO) bifunctional catalyst design concept has been exemplified in several processes to direct conversion syngas to value-added chemicals and fuels such as mixed light olefins, ethylene, aromatics and gasoline.Herein we demonstrate that the product can be steered toward liquefied petroleum gas(LPG) with a selectivity up to 89% in hydrocarbons especially propane selectivity reaching 80% at CO conversion of 63% using ZnCrOx-H-SSZ-39 catalyst.Interestingly, the quantity of the acid sites of SSZ-39 does not influence obviously the hydrocarbon distribution but the strength is crucial for selective formation of propane.This finding provides an alternative route of LPG synthesis from a variety of carbon resources via syngas.
基金the National Natural Science Foundation of China (50574046)National Natural Science Foundationof Major Research Projects (90610035)High School Doctoral Subject Special Science and Research Foundation of Ministry of Education (20040674005)
文摘CexZr1-xO2 mixed oxides with different Ce/Zr ratios were prepared by coprecipitation. The characterizations of mixed oxides were studied by X-ray diffraction (XRD) and H2-TPR. And the performances were tested in a fixed-bed quartz reactor. The results indicated that lattice oxygen of CexZr1-xO2 could oxidate methane to syngas and the incorporation of zirconium into the ceria lattice could improve the O2- mobility. The Ce0.7Zr0.3O2 had the best activity in investigative temperature ranging from 600 to 900 ℃. Effects of reaction time on H2/CO ratio were studied at 850 ℃ when using Ce0.7Zr0.3O2 as catalyst. The results indicated that the ratio was closed to 2 values in the first 10 min, however, it rapidly increased with reaction time after >10 min. The possible reason was that the direct partial oxidation of methane reaction was dominant in the first 10 min. However, the methane pyrogenation was responsible for the rapid increase of H2/CO ratio after 10 min. Thus, if syngas with H2/CO ratio of 2 wanted to be obtained, the reaction time needed to be controlled.
基金the financial support from the National Natural Science Foundation of China(Grant No.21978285,21991093,21991090),the‘‘Transformational Technologies for Clean Energy and Demonstration”the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDA21030100)。
文摘Realizing high CO conversion and high aromatics selectivity simultaneously in syngas-to-aromatics(STA)reaction is still challenging.Herein,we report a 57.5%CO conversion along with 74%aromatics selectivity over a composite catalyst consisting of Fe/ZnCr_(2)O_(4)(Fe modified ZnCr_(2)O_(4)spinel)oxide and H-ZSM-5 zeolite.Impregnation of only 3 wt%of Fe onto ZnCr_(2)O_(4)can remarkably increase CO conversion without sacrificing the aromatics selectivity.Oxygen vacancy concentration is improved after impregnating Fe.The highly dispersed iron carbide species is formed during the reaction over Fe/ZnCr_(2)O_(4)spinel oxide.The synergistic effect of oxygen vacancy and iron carbide results in a rapid formation of abundant oxygenated intermediate species,which can be continuously transformed to aromatics in H-ZSM-5.This study provides a new insight into the design of highly efficient catalyst for syngas conversion.
基金supported by the National Natural Science Foundation of China(91545112,21573271,21403278)Shanghai Municipal Science and Technology Commission,China(15DZ1170500)the Chinese Academy of Sciences(QYZDB-SSW-SLH035)
文摘Syngas conversion to fuels and chemicals is one of the most challenging subjects in the field of C1 chemistry. It is considered as an attractive alternative non-petroleum-based production route. The direct synthesis of olefins and alcohols as high value-added chemicals from syngas has drawn particular attention due to its process simplicity, low energy consumption and clean utilization of carbon resource, which conforms to the principles of green carbon science. This review describes the recent advances for the direct production of lower olefins and higher alcohols via syngas conversion. Recent progress in the development of new catalyst systems for enhanced catalytic performance is highlighted. We also give recommendations regarding major challenges for further research in syngas conversion to various chemicals.
基金financial support from the National Key Research&Development Program of China(2018YFB0604901)the National Natural Science Foundation of China(21706210)the Key Research&Development Program of Shaanxi Province(2020ZDLGY11-06)。
文摘A series of ZnO-ZrO_(2) solid solutions with different Zn contents were synthesized by the urea coprecipitation method,which were coupled with H-ZSM-5 zeolite to form bifunctional catalysts.As a new benzene alkylation reagent,syngas was used instead of methanol to realize the efficient conversion of syngas and benzene into toluene and xylene.A suitable ratio of ZnO-ZrO_(2) led to the significant improvement in the catalytic performance,and a suitable amount of acid helped to increase the selectivity of toluene/xylene and reduce the selectivity of the by-products ethylbenzene and C^(9+) aromatics.The highest benzene conversion of 89.2%and toluene/xylene selectivity of 88.7%were achieved over 10%ZnO-ZrO_(2)&H-ZSM-5(Si/Al=23)at a pressure of 3 MPa and a temperature of 450℃.In addition,the effect of the zeolite framework structure on product distribution was examined.Similar to the molecular dynamics of aromatic hydrocarbons,H-ZSM-5 zeolites comprise 10-membered-ring pores,which are beneficial to the activation of benzene;hence,the conversion of benzene is higher.H-ZSM-35 and HMOR zeolites exhibited small eight-membered-ring channels,which were not conducive to the passage of benzene;hence,the by-product ethylbenzene exhibits a higher selectivity.The distance between the active centers of the bifunctional catalysts was the main factor affecting the catalytic performance,and the powder mixing method was more conducive to the conversion of syngas and benzene.