Methanol,a crucial C1 intermediate,bridges traditional fossil-based chemical processes with emerging sustainable catalytic technologies by serving as both a versatile hydrogenation product from CO/CO_(2)and an active ...Methanol,a crucial C1 intermediate,bridges traditional fossil-based chemical processes with emerging sustainable catalytic technologies by serving as both a versatile hydrogenation product from CO/CO_(2)and an active intermediate for hydrocarbon synthesis.Despite significant progress in methanol-to-hydrocarbon(MTH)conversion,a comprehensive understanding of reaction mechanisms remains essential to enhance catalyst design and industrial applicability.This review critically synthesizes recent advances in mechanistic insights related to methanol conversion and methanol-mediated catalytic processes.Firstly,we systematically outline key reaction pathways involved in initial carbon–carbon(C–C)bond formation through direct and indirect mechanisms,emphasizing significant breakthroughs from spectroscopic analyses and theoretical calculations.Subsequently,we highlight the autocatalytic characteristics and dual-cycle mechanisms underlying MTH processes,critically evaluating the roles of zeolite structures,pore sizes,topology,and acidity in governing product selectivity and catalyst stability.Additionally,we discuss cutting-edge developments in tandem catalytic systems employing methanol as a pivotal intermediate for CO_(x)hydrogenation,emphasizing the transferable mechanistic principles and catalytic insights.Finally,we identify future research directions,including elucidating precise hydrocarbon pool(HCP)intermediates,optimizing zeolite structures through computational-guided design,and developing robust catalytic systems leveraging advanced characterization methods and artificial intelligence.By integrating multidisciplinary approaches from catalytic science,materials engineering,and reaction engineering,this review provides actionable guidance towards rational design and optimization of advanced catalytic systems for efficient methanol conversion processes.展开更多
Space exploration and manufacturing are of critical importance for scientific advancement,technological innovation,national security,and the acquisition of extraterrestrial resources.In view of this,chemical and biolo...Space exploration and manufacturing are of critical importance for scientific advancement,technological innovation,national security,and the acquisition of extraterrestrial resources.In view of this,chemical and biological nano-/micro-/meso-scale manufacturing provide complementary approaches to overcome key space exploration challenges by enabling the in-situ production of essential life-support materials,propellants,and other resources.This review examines the origin and historical evolution of space manufacturing and the latest advances across different environments—from orbital space stations and the lunar surface to Mars and asteroids.It is structured to present the current state of research,outline key manufacturing strategies and technologies,assess the technical and environmental challenges,and discuss emerging trends and future directions.Besides,the potential applications of emerging technologies such as synthetic biology and artificial intelligence in overcoming the limitations of microgravity,limited resources,and extreme conditions are discussed.Ultimately,this integrative review could serve to guide future development,from advancing space science and disruptive manufacturing to enabling interdisciplinary and application-level innovations.展开更多
Energy storage is a key factor in the drive for carbon neutrality and carbon nanotubes(CNTs)may have an important role in this.Their intrinsic sp2 covalent structure gives them excellent electrical conductivity,mechan...Energy storage is a key factor in the drive for carbon neutrality and carbon nanotubes(CNTs)may have an important role in this.Their intrinsic sp2 covalent structure gives them excellent electrical conductivity,mechanical strength,and chemical stability,making them suitable for many uses in energy storage,such as lithium-ion batteries(LIBs).Currently,their use in LIBs mainly focuses on conductive networks,current collectors,and dry electrodes.The review outlines advances in the use of CNTs in the cathodes and anodes of LIBs,especially in the electrode fabrication and mechanical sensors,as well as providing insights into their future development.展开更多
Existing organic halide synthesis routes typically employ elemental halogens(X_(2),X=Cl or Br),leading to low atom economy and significant environmental pollution.In this work,we developed an atom efficient electrosyn...Existing organic halide synthesis routes typically employ elemental halogens(X_(2),X=Cl or Br),leading to low atom economy and significant environmental pollution.In this work,we developed an atom efficient electrosynthesis and separation strategy for halogenation reagents—N-chlorosuccinimide(NCS)and N-bromosuccinimide(NBS)—at high current densities.Faradic efficiency(FE)of 91.0%and 81.3%was achieved for NCS and NBS generation on RuO_(x)/TiO_(2)/Ti in a batch cell,respectively.Electrosynthesis of NCS likely involves both heterogeneous catalytic and homogeneous tandem pathways,while NBS is likely formed in a Langmuir-Hinshelwood mechanism with a proton-coupled electron transfer as the rate-determining step.A coupled continuous electrocatalytic synthesis and in situ separation setup was developed for the efficient production of NCS and NBS,which yielded 0.77 g of NCS in 12000 s and 0.81 g of NBS in 15000 s,both with relative purity exceeding 95%.The halogenation of acetone using NCS and NBS enabled gram-scale production of the key intermediate in organic synthesis,1-halogenacetone,with over 95%recovery of succinimide.展开更多
5-Hydroxymethylfurfural(HMF),derived from biomass,is a promising sustainable resource that can be converted into valuable chemical compounds.One such compound,2,5-dihydroxymethylfuran(DHMF),produced through the electr...5-Hydroxymethylfurfural(HMF),derived from biomass,is a promising sustainable resource that can be converted into valuable chemical compounds.One such compound,2,5-dihydroxymethylfuran(DHMF),produced through the electrocatalytic hydrogenation of HMF,is widely used in industrial polymer manufacturing.However,the hydrogenation of high-concentration HMF remains challenging due to the tendency for undesirable dimerization.Acknowledging the critical role of adsorbed hydrogen(H*)in HMF hydrogenation,a series of transition metal-doped dual-cubic Cu electrocatalysts(M-Cu,where M=Mo,Pd,Pt,Au,and Ag)were synthesized to systematically investigate the effect of varying H*reactivity on HMF hydrogenation,A pronounced correlation between DHMF selectivity and H*coverage was observed.Increasing H*coverage can enhance the selectivity for DHMF and prevent undesired dimerization of adsorbed HMF molecules.While elevated H*coverage enhanced DHMF selectivity,excessive coverage adversely impacted Faradaic efficiency due to competing hydrogen evolution reaction.This underscores the critical importance of finely tuning H*coverage.The optimal electrocatalyst,achieved by fine-tuning the doping amount of Pt on Cu,demonstrated a Faradaic efficiency of over 90%for DHMF in highconcentration HMF at-0.3 V,marking the highest record reported to date.展开更多
Renewable energy-driven bicarbonate conversion to valuable chemicals presents an attractive strategy for mitigating CO_(2)emissions,as bicarbonate can be efficiently generated from the capture of atmospheric CO_(2)usi...Renewable energy-driven bicarbonate conversion to valuable chemicals presents an attractive strategy for mitigating CO_(2)emissions,as bicarbonate can be efficiently generated from the capture of atmospheric CO_(2)using alkaline solutions with reactive absorption.In this work,we present a CO_(2)-mediated bicarbonate conversion to pure formate using a cation exchange membrane-based electrolyzer with a 25 cm^(2)electrode area.Our electrolysis achieved selectivities exceeding 75%for formate at a total current of 2.5 A,achieving formate concentrations up to 1.2 M and yields as high as 95%over extended periods.The techno-economic assessment confirmed the economic viability of the process,highlighting the potential for bicarbonate electrolysis as a sustainable method for producing valuable chemicals.展开更多
The electrocatalytic oxidation of glycerol toward formic acid is one of the most promising pathways for transformation and utilization of glycerol.Herein,a series of well-defined Ni_(n)(SR)_(2n) nanoclusters(n=4,5,6;d...The electrocatalytic oxidation of glycerol toward formic acid is one of the most promising pathways for transformation and utilization of glycerol.Herein,a series of well-defined Ni_(n)(SR)_(2n) nanoclusters(n=4,5,6;denoted as Ni NCs)were prepared for the electrocatalytic glycerol oxidation toward formic acid,in which Ni_(6)-PET-50CV afforded the most excellent electrocatalytic performance with a high formic acid selectivity of 93% and a high glycerol conversion of 86%.This was attributed to the lowest charge transfer impedance and the most rapid reaction kinetics.Combined electrochemical measurements and X-ray absorption fine structure measurements revealed that the structures of Ni NCs remained intact after CV scanning pretreatment and electrocatalysis via forming the Ni–O bond.Additionally,the kinetic studies and in-situ Fourier transformed infrared suggested a sequential oxidation mechanism,in which the main reaction steps of glycerol→glyceraldehyde→glyceric acid were very rapid to produce a high selectivity of formic acid even though the low glycerol conversion.This work presents an opportunity to study Ni NCs for the efficient electrocatalytic oxidation of biomass-derived polyhydroxyl platform molecules to produce value-added carboxylic acids.展开更多
Limited by the sluggish kinetics at the cathode of proton exchange membrane fuel cells(PEMFCs),optimizing platinum-based alloy catalysts for oxygen reduction reaction remains a key target toward industrialization.Stra...Limited by the sluggish kinetics at the cathode of proton exchange membrane fuel cells(PEMFCs),optimizing platinum-based alloy catalysts for oxygen reduction reaction remains a key target toward industrialization.Strain engineering is widely employed to tune Pt-M catalysts,but its impact on the structure-property relationship is often interwoven with multiple factors.In this work,we propose a bi-stage strain tuning method and demonstrate it on the most common PtCo catalysts.Macro-strain is introduced by synthesizing single-crystal PtCo nanodendrites,whereas mild acid etching introduces micro-strain to the surface.The half-wave potential of as-treated catalysts reaches 0.959 V,and mass activity is up to 0.69 A mg^(−1)_(Pt).A minimal decrease of 2 mV is observed for half-wave potential after 10,000 cycles.Detailed analysis using advanced transmission electron microscopy,wide-angle X-ray scattering,etc.provides direct evidence that surface disorder at the atomic scale accounts for the enhanced activity and stability.In contrast,the simplicity of this approach allows for scaling up on Pt-M catalysts,as demonstrated on PEMFCs.The bi-stage strain tuning strategy provides a new perspective and reference for improving the activity and durability of Pt-M catalysts.展开更多
Plastics have become omnipresent in modern life due to their versatility and durability.However,this convenience comes at the cost of substantial waste generation.The inherent chemical stability of plastics complicate...Plastics have become omnipresent in modern life due to their versatility and durability.However,this convenience comes at the cost of substantial waste generation.The inherent chemical stability of plastics complicates its recycling,leading to environmental pollution and ecological threats.This mini-review highlights recent advancements in addressing this challenge by oxidative transformation of polyethylene(PE)into new functional polymers,value-added chemicals,and carbon-based materials.We first discuss the introduction of hydroxyl,carbonyl groups onto PE with a focus on the functionalization degree and selectivity.Subsequently,approaches for PE oxidation into dicarboxylic acids and short-chain oxidized PE are described and compared,with an emphasis on the tandem reactions for converting mixed dicarboxylic acids into other value-added chemicals.We also briefly discuss the oxidative transformation of PE into carbon-based materials and summarize the progress in qualitative and quantitative analysis of oxidation products.Finally,we conclude this mini-review by highlighting the challenges and opportunities in the field.展开更多
Lithium(Li)metal battery is regarded as a promising candidate in pursuit of high-energy-density secondary batteries[1].However,Li metal batteries suffer from rapid capacity decay and anxious safety concerns,primarily ...Lithium(Li)metal battery is regarded as a promising candidate in pursuit of high-energy-density secondary batteries[1].However,Li metal batteries suffer from rapid capacity decay and anxious safety concerns,primarily due to nonuniform Li plating/stripping[2].Derived from the spontaneous reduction decomposition of electrolytes.展开更多
Understanding interphase mass transfer is crucial for the efficient design and operation of gas–solid fluidized beds,which are widely used in various industrial processes.However,research on mass transfer behavior in...Understanding interphase mass transfer is crucial for the efficient design and operation of gas–solid fluidized beds,which are widely used in various industrial processes.However,research on mass transfer behavior in such systems,particularly at high temperatures(e.g.,>1000℃),remains sparse.This study,dedicated to Profs.Yong Jin and Zhiqing Yu's contributions to fluidization,elucidates the mass transfer behavior of gas-solid bubbling fluidized beds at temperatures up to 1600℃by modeling gas residence time distribution data using a two-phase model.We examine the effects of temperature,gas velocity,bed height,and particle size on mass transfer characteristics.The results reveal that the mass transfer flux increases with temperature up to 800℃,peaking within this range before stabilizing above 1200℃.This trend is closely linked to the behavior of bubble dynamics,where bubble size initially decreases significantly as temperature rises,eventually reaching a plateau at higher temperatures.Experimental pressure fluctuation analysis validates this behavior,further supporting the observed temperature effects on bubble dynamics.Higher gas velocity reduces the mass transfer flux and mitigates back-mixing,while bed height and particle size affect bubble dynamics in a nonlinear manner.Experimental validation confirms the potential of these findings for optimizing the design and operation of high-temperature bubbling fluidized bed reactors.展开更多
Propane dehydrogenation using CO_(2)as a mild oxidizer(CO_(2)-ODP)is a promising technology for high propylene production and CO_(2)reduction utilization.Among them,the reverse water gas shift reaction(RWGS)can change...Propane dehydrogenation using CO_(2)as a mild oxidizer(CO_(2)-ODP)is a promising technology for high propylene production and CO_(2)reduction utilization.Among them,the reverse water gas shift reaction(RWGS)can change the reaction equilibrium to increase the propylene yield,and the Boudouard reaction can assist in the carbon accumulation elimination.However,the efficiency of the catalysts developed so far is limited,we introduced the Cr active component during the synthesis of porous silica spheres to form a CO_(2)-ODP catalyst,with a uniform distribution of active sites via(NH_(4))_(3)[CrMo_(6)O_(24)H_(6)]·7H_(2)O produce a derivative.As anα-type Anderson series of polyoxometalates(POMs),this six octahedral structure formed by Mo participation surrounds the central atom Cr,which is more stable in structure by electrostatic effect,its derivatives generated after calcination are stably bound to the silica-based carrier,which reduces the formation of inertα-Cr_(2)O_(3)by CrO_(x)aggregation during the catalytic process.Meanwhile,the oxygen atoms rich in polyoxometalates are more likely to form Si-O bonds with the carrier,which makes the active sites evenly and stably branched in the inner wall of the pores of mesoporous silica spheres,reduces the influence of carbon accumulation,and facilitates the activation and regeneration.The CO_(2)conversion of the catalyst CrMoO_(x)@mesoporous silica spheres(MSS)is typically greater than 20%under selected ideal conditions.This synthesis method of assembling POMs with mesoporous materials opens a new pathway for developing propane dehydrogenation catalysts.Compared to traditional impregnation synthesis,this catalyst contains a lower Cr content while achieving higher CO_(2)consumption efficiency.展开更多
Conducting polymer hydrogels offer promising electrical interfaces with biological tissues for electrophysio-logical signal recording,sensing,and stimulation due to their favorable electrical properties,biocompatibili...Conducting polymer hydrogels offer promising electrical interfaces with biological tissues for electrophysio-logical signal recording,sensing,and stimulation due to their favorable electrical properties,biocompatibility,and stability.Among them,Poly(3,4-ethylenedioxythiophene):Polystyrene sulfonate(PEDOT:PSS)is widely used as a conductive filler,forming a network of conjugated nanofibers within the hydrogel matrix.This structure enables robust electronic conductivity while preserving ionic transport and biocompatibility in phys-iological environments.However,the mechanical integrity of these hydrogels is often compromised by micellar microstructures in aqueous colloidal dispersions.The absence of interconnected conducting polymer nanofibers to maintain mechanical integrity during swelling hinders the mechanical properties of hydrogels.Here,three modification strategies were explored to enhance the flexibility and stretchability:constructing an inter-penetrating network,phase separation induced by ionic compounds,and pure conductive hydrogels formed through polar solvent additives and dry-annealing.These strategies synergistically enhance conductivity and flexibility by controlling interchain entanglement and redesigning the distribution of conjugated crystal regions and soft regions.The resulting hydrogels exhibit excellent conductivity(1.99-5.25 S/m),softness(elastic modulus as low as 280 Pa),and elasticity(tensile properties up to 800%).When used as epidermal or implantable bioelectrodes,they provided a soft interface,ensuring longer-lasting and more stable electromyo-gram,electrocardiogram,and electroencephalogram signals compared to commercial gel electrodes,with a signal-to-noise ratio of up to 20.0 dB.Therefore,the conducting polymer hydrogels developed in this study leverage the synergy between conductivity and flexibility,paving the way for further transformative applications in bioelectronics.展开更多
Aromatics,as essential basic chemical raw materials,are widely used in rubber,nylon,resins,solvents,and other products.Light aromatics such as benzene,toluene,and xylene serve as cornerstones of modern chemical indust...Aromatics,as essential basic chemical raw materials,are widely used in rubber,nylon,resins,solvents,and other products.Light aromatics such as benzene,toluene,and xylene serve as cornerstones of modern chemical industries.Conventional aromatic production predominantly relies on petroleum resources.Compared with traditional petroleum-derived aromatic production processes,syngas to aromatics technology offer signifi cant advantages in terms of energy consumption,environmental emissions,and production costs.Notably,coal-based syngas to aromatics technology offers several advantages,including a shorter process flow,lower hydrogen-to-carbon ratio requirements,and improved pressure compatibility with existing systems.Therefore,syngas to aromatics technology is poised to play an increasingly vital role in future energy transitions,driving the evolution of green,low-carbon chemical industries.One of the key challenges in the technology of synthesizing aromatics from coal-based syngas lies in the construction of the catalytic system.Another challenge lies in the design of the reactor equipment.Based on the above key challenges,this review systematically summarizes three major catalytic mechanisms:the modified Fischer-Tropsch synthesis pathway,the methanol-mediated pathway,and the formaldehyde-mediated pathway,deeply analyses the factors influencing the catalytic performance in the syngas to aromatics process,discusses the role of reactor design in this process;on this basis,it further explores the potential and prospects of coal-based syngas to aromatics technology in promoting the development of green and low-carbon chemical industry.展开更多
Due to the high structural flexibility and controllable thermal expansion,cubic double ReO_(3)-type negative thermal expansion(NTE)fluorides provide a solution for solving the prominent phenomenon of thermal expansion...Due to the high structural flexibility and controllable thermal expansion,cubic double ReO_(3)-type negative thermal expansion(NTE)fluorides provide a solution for solving the prominent phenomenon of thermal expansion mismatch between materials.However,the expensive raw materials and complex synthesis steps limit its practical application.In this work,we have designed a more advantageous method for the synthesis of NTE material CaZrF_(6),and it is expected to be generalized to the synthesis of other double ReO_(3)-fluorides.Intriguingly,a new orthorhombic phase CaZrF_(6)has been synthesized via this method in a lower temperature.Unlike the strong isotropic NTE of the cubic phase CaZrF_(6),the orthorhombic phase shows the strong anisotropic positive thermal expansion(PTE).The combined analysis of temperature-dependent X-ray diffraction(XRD),Raman spectra,and first-principles calculations shows that the low frequency phonon vibration mode with negative Grüneisen parameter in cubic CaZrF_(6)are strongly correlated with the transverse thermal vibration of F atoms and dominates the NTE of the material.展开更多
Particle segregation and mixing behavior play a crucial role in industrial processes.This study investigates the saturated jetsam fraction,which indicates the maximum capacity of flotsam to entrain jetsam,in an initia...Particle segregation and mixing behavior play a crucial role in industrial processes.This study investigates the saturated jetsam fraction,which indicates the maximum capacity of flotsam to entrain jetsam,in an initially separated binary fluidized bed with particle size differences.According to the value of saturated jetsam fraction,three distinct regimes-segregation,mixing,and an intermediate regime-are identified.Moreover,intriguing relationships between the saturated jetsam fraction and superficial gas velocity are observed,exhibiting monotonic trends in both the segregation and mixing regimes,while a unique volcano-shaped curve in the intermediate regime.Additionally,a comprehensive entrainment model based on two-fluid model elucidates the observed phenomena,emphasizing the significance of mixing behavior in fluidized layer on the saturated jetsam fraction.This work offers potential insights for evaluating segregation in industrial applications.展开更多
Turbulent fluidized bed proves effective in industrial processes due to superior heat and mass transfer and chemical reaction performance. However, understanding the transition to turbulent fluidization remains limite...Turbulent fluidized bed proves effective in industrial processes due to superior heat and mass transfer and chemical reaction performance. However, understanding the transition to turbulent fluidization remains limited, especially at temperatures exceeding 1000 ℃, making it challenging to develop high-temperature fluidized bed applications. This paper presents an experimental investigation on the turbulent fluidization onset velocity (U_(c)), measured in a 30 mm diameter bed using corundum particles with average diameters from 0.68 mm to 1.58 mm in temperatures from ambient to 1600 ℃. Experimental results reveal that U_(c) increases with temperature up to 600 ℃, stabilizes within the 600–1200 ℃ range, and then decreases above 1200 ℃, demonstrating the varying relative significance of hydrodynamic and interparticle forces at different temperatures. To help design and operate high-temperature applications of turbulent fluidization, we developed U_(c) correlations based on experimental data from both literature sources and this study, covering temperatures of up to 1600 ℃ and particles of Groups A to D.展开更多
The development of clean and efficient renewable energy is of great strategic importance to realize green energy conversion and low-carbon growth.Hydrogen energy,as a renewable energy with“zero carbon emission”,can ...The development of clean and efficient renewable energy is of great strategic importance to realize green energy conversion and low-carbon growth.Hydrogen energy,as a renewable energy with“zero carbon emission”,can be efficiently converted into hydrogen energy and electric energy by electrolysis of water to hydrogen technology.Anion-exchange membrane water electrolysis(AEMWE),substantially advanced by nonprecious metal electrocatalysts,is among the most cost-effective and promising water electrolysis technologies,combining the advantages of proton exchange membranes with the proven technology of traditional alkaline water electrolysis and potentially eliminating the disadvantages of both.In this paper,the latest results of AEMWE research in recent years are summarized,including the AEMWE mechanism study and the hot issues of low-cost transition metal hydrogen evolution reaction and oxygen evolution reaction electrocatalyst design in recent years.The key factors affecting the performance of AEMWE are pointed out,and further challenges and opportunities encountered in large-scale industrialization are discussed.Finally,this review provides strong guidance for advancing AEMWE.展开更多
基金the Inner Mongolia Natural Science Foundation(2023ZD05,2025JQ028,2025MS02001)the National Natural Science Foundation of China(22278238,22238004)+3 种基金the National Key Research and Development Program of China(2024YFE0211400)the Major Science and Technology Program of Inner Mongolia Autonomous Region(20212120326)the“Elite Talents Revitalize Inner Mongolia”Initiative–Tier-1 Talent Team(202410)the Ordos Science and Technology Breakthrough(JBGS2024003),and Ordos Laboratory for their financial support.
文摘Methanol,a crucial C1 intermediate,bridges traditional fossil-based chemical processes with emerging sustainable catalytic technologies by serving as both a versatile hydrogenation product from CO/CO_(2)and an active intermediate for hydrocarbon synthesis.Despite significant progress in methanol-to-hydrocarbon(MTH)conversion,a comprehensive understanding of reaction mechanisms remains essential to enhance catalyst design and industrial applicability.This review critically synthesizes recent advances in mechanistic insights related to methanol conversion and methanol-mediated catalytic processes.Firstly,we systematically outline key reaction pathways involved in initial carbon–carbon(C–C)bond formation through direct and indirect mechanisms,emphasizing significant breakthroughs from spectroscopic analyses and theoretical calculations.Subsequently,we highlight the autocatalytic characteristics and dual-cycle mechanisms underlying MTH processes,critically evaluating the roles of zeolite structures,pore sizes,topology,and acidity in governing product selectivity and catalyst stability.Additionally,we discuss cutting-edge developments in tandem catalytic systems employing methanol as a pivotal intermediate for CO_(x)hydrogenation,emphasizing the transferable mechanistic principles and catalytic insights.Finally,we identify future research directions,including elucidating precise hydrocarbon pool(HCP)intermediates,optimizing zeolite structures through computational-guided design,and developing robust catalytic systems leveraging advanced characterization methods and artificial intelligence.By integrating multidisciplinary approaches from catalytic science,materials engineering,and reaction engineering,this review provides actionable guidance towards rational design and optimization of advanced catalytic systems for efficient methanol conversion processes.
基金supported by National Natural Science Foundation of China(22278241)a grant from the Institute Guo Qiang,Tsinghua University(2021GQG1016).
文摘Space exploration and manufacturing are of critical importance for scientific advancement,technological innovation,national security,and the acquisition of extraterrestrial resources.In view of this,chemical and biological nano-/micro-/meso-scale manufacturing provide complementary approaches to overcome key space exploration challenges by enabling the in-situ production of essential life-support materials,propellants,and other resources.This review examines the origin and historical evolution of space manufacturing and the latest advances across different environments—from orbital space stations and the lunar surface to Mars and asteroids.It is structured to present the current state of research,outline key manufacturing strategies and technologies,assess the technical and environmental challenges,and discuss emerging trends and future directions.Besides,the potential applications of emerging technologies such as synthetic biology and artificial intelligence in overcoming the limitations of microgravity,limited resources,and extreme conditions are discussed.Ultimately,this integrative review could serve to guide future development,from advancing space science and disruptive manufacturing to enabling interdisciplinary and application-level innovations.
文摘Energy storage is a key factor in the drive for carbon neutrality and carbon nanotubes(CNTs)may have an important role in this.Their intrinsic sp2 covalent structure gives them excellent electrical conductivity,mechanical strength,and chemical stability,making them suitable for many uses in energy storage,such as lithium-ion batteries(LIBs).Currently,their use in LIBs mainly focuses on conductive networks,current collectors,and dry electrodes.The review outlines advances in the use of CNTs in the cathodes and anodes of LIBs,especially in the electrode fabrication and mechanical sensors,as well as providing insights into their future development.
文摘Existing organic halide synthesis routes typically employ elemental halogens(X_(2),X=Cl or Br),leading to low atom economy and significant environmental pollution.In this work,we developed an atom efficient electrosynthesis and separation strategy for halogenation reagents—N-chlorosuccinimide(NCS)and N-bromosuccinimide(NBS)—at high current densities.Faradic efficiency(FE)of 91.0%and 81.3%was achieved for NCS and NBS generation on RuO_(x)/TiO_(2)/Ti in a batch cell,respectively.Electrosynthesis of NCS likely involves both heterogeneous catalytic and homogeneous tandem pathways,while NBS is likely formed in a Langmuir-Hinshelwood mechanism with a proton-coupled electron transfer as the rate-determining step.A coupled continuous electrocatalytic synthesis and in situ separation setup was developed for the efficient production of NCS and NBS,which yielded 0.77 g of NCS in 12000 s and 0.81 g of NBS in 15000 s,both with relative purity exceeding 95%.The halogenation of acetone using NCS and NBS enabled gram-scale production of the key intermediate in organic synthesis,1-halogenacetone,with over 95%recovery of succinimide.
基金supported financially by the Australian Research Council(CE230100032,DP230102027,DP240102575,FT200100062)。
文摘5-Hydroxymethylfurfural(HMF),derived from biomass,is a promising sustainable resource that can be converted into valuable chemical compounds.One such compound,2,5-dihydroxymethylfuran(DHMF),produced through the electrocatalytic hydrogenation of HMF,is widely used in industrial polymer manufacturing.However,the hydrogenation of high-concentration HMF remains challenging due to the tendency for undesirable dimerization.Acknowledging the critical role of adsorbed hydrogen(H*)in HMF hydrogenation,a series of transition metal-doped dual-cubic Cu electrocatalysts(M-Cu,where M=Mo,Pd,Pt,Au,and Ag)were synthesized to systematically investigate the effect of varying H*reactivity on HMF hydrogenation,A pronounced correlation between DHMF selectivity and H*coverage was observed.Increasing H*coverage can enhance the selectivity for DHMF and prevent undesired dimerization of adsorbed HMF molecules.While elevated H*coverage enhanced DHMF selectivity,excessive coverage adversely impacted Faradaic efficiency due to competing hydrogen evolution reaction.This underscores the critical importance of finely tuning H*coverage.The optimal electrocatalyst,achieved by fine-tuning the doping amount of Pt on Cu,demonstrated a Faradaic efficiency of over 90%for DHMF in highconcentration HMF at-0.3 V,marking the highest record reported to date.
基金National Natural Science Foundation of China(22379083)State Key Laboratory of Chemical Engineering(SKL-ChE-23T02)+2 种基金financial support from Beijing National Laboratory for Molecular Sciencessupport from Tsinghua International School’s Research Mentoring Programsupport from Tsinglan School’s Research Mentoring Program。
文摘Renewable energy-driven bicarbonate conversion to valuable chemicals presents an attractive strategy for mitigating CO_(2)emissions,as bicarbonate can be efficiently generated from the capture of atmospheric CO_(2)using alkaline solutions with reactive absorption.In this work,we present a CO_(2)-mediated bicarbonate conversion to pure formate using a cation exchange membrane-based electrolyzer with a 25 cm^(2)electrode area.Our electrolysis achieved selectivities exceeding 75%for formate at a total current of 2.5 A,achieving formate concentrations up to 1.2 M and yields as high as 95%over extended periods.The techno-economic assessment confirmed the economic viability of the process,highlighting the potential for bicarbonate electrolysis as a sustainable method for producing valuable chemicals.
文摘The electrocatalytic oxidation of glycerol toward formic acid is one of the most promising pathways for transformation and utilization of glycerol.Herein,a series of well-defined Ni_(n)(SR)_(2n) nanoclusters(n=4,5,6;denoted as Ni NCs)were prepared for the electrocatalytic glycerol oxidation toward formic acid,in which Ni_(6)-PET-50CV afforded the most excellent electrocatalytic performance with a high formic acid selectivity of 93% and a high glycerol conversion of 86%.This was attributed to the lowest charge transfer impedance and the most rapid reaction kinetics.Combined electrochemical measurements and X-ray absorption fine structure measurements revealed that the structures of Ni NCs remained intact after CV scanning pretreatment and electrocatalysis via forming the Ni–O bond.Additionally,the kinetic studies and in-situ Fourier transformed infrared suggested a sequential oxidation mechanism,in which the main reaction steps of glycerol→glyceraldehyde→glyceric acid were very rapid to produce a high selectivity of formic acid even though the low glycerol conversion.This work presents an opportunity to study Ni NCs for the efficient electrocatalytic oxidation of biomass-derived polyhydroxyl platform molecules to produce value-added carboxylic acids.
基金the National Natural Science Foundation of China(NO.12274010,12474003)Beijing Nova Program(20240484584)+2 种基金the support from the Shanghai Key Laboratory of Material Frontiers Research in Extreme Environments,China(No.22dz2260800)the Shanghai Science and Technology Committee,China(No.22JC1410300)the National Natural Science Foundation of China(No.52103330)。
文摘Limited by the sluggish kinetics at the cathode of proton exchange membrane fuel cells(PEMFCs),optimizing platinum-based alloy catalysts for oxygen reduction reaction remains a key target toward industrialization.Strain engineering is widely employed to tune Pt-M catalysts,but its impact on the structure-property relationship is often interwoven with multiple factors.In this work,we propose a bi-stage strain tuning method and demonstrate it on the most common PtCo catalysts.Macro-strain is introduced by synthesizing single-crystal PtCo nanodendrites,whereas mild acid etching introduces micro-strain to the surface.The half-wave potential of as-treated catalysts reaches 0.959 V,and mass activity is up to 0.69 A mg^(−1)_(Pt).A minimal decrease of 2 mV is observed for half-wave potential after 10,000 cycles.Detailed analysis using advanced transmission electron microscopy,wide-angle X-ray scattering,etc.provides direct evidence that surface disorder at the atomic scale accounts for the enhanced activity and stability.In contrast,the simplicity of this approach allows for scaling up on Pt-M catalysts,as demonstrated on PEMFCs.The bi-stage strain tuning strategy provides a new perspective and reference for improving the activity and durability of Pt-M catalysts.
基金supported by the National Natural Science Foundation of China(22375113)Beijing Natural Science Foundation(Z240029)。
文摘Plastics have become omnipresent in modern life due to their versatility and durability.However,this convenience comes at the cost of substantial waste generation.The inherent chemical stability of plastics complicates its recycling,leading to environmental pollution and ecological threats.This mini-review highlights recent advancements in addressing this challenge by oxidative transformation of polyethylene(PE)into new functional polymers,value-added chemicals,and carbon-based materials.We first discuss the introduction of hydroxyl,carbonyl groups onto PE with a focus on the functionalization degree and selectivity.Subsequently,approaches for PE oxidation into dicarboxylic acids and short-chain oxidized PE are described and compared,with an emphasis on the tandem reactions for converting mixed dicarboxylic acids into other value-added chemicals.We also briefly discuss the oxidative transformation of PE into carbon-based materials and summarize the progress in qualitative and quantitative analysis of oxidation products.Finally,we conclude this mini-review by highlighting the challenges and opportunities in the field.
文摘Lithium(Li)metal battery is regarded as a promising candidate in pursuit of high-energy-density secondary batteries[1].However,Li metal batteries suffer from rapid capacity decay and anxious safety concerns,primarily due to nonuniform Li plating/stripping[2].Derived from the spontaneous reduction decomposition of electrolytes.
基金support from the National Natural Science Foundation of China(grant No.U22A20410)the Inner Mongolia Government(grant No.Ordoslab-2023002).
文摘Understanding interphase mass transfer is crucial for the efficient design and operation of gas–solid fluidized beds,which are widely used in various industrial processes.However,research on mass transfer behavior in such systems,particularly at high temperatures(e.g.,>1000℃),remains sparse.This study,dedicated to Profs.Yong Jin and Zhiqing Yu's contributions to fluidization,elucidates the mass transfer behavior of gas-solid bubbling fluidized beds at temperatures up to 1600℃by modeling gas residence time distribution data using a two-phase model.We examine the effects of temperature,gas velocity,bed height,and particle size on mass transfer characteristics.The results reveal that the mass transfer flux increases with temperature up to 800℃,peaking within this range before stabilizing above 1200℃.This trend is closely linked to the behavior of bubble dynamics,where bubble size initially decreases significantly as temperature rises,eventually reaching a plateau at higher temperatures.Experimental pressure fluctuation analysis validates this behavior,further supporting the observed temperature effects on bubble dynamics.Higher gas velocity reduces the mass transfer flux and mitigates back-mixing,while bed height and particle size affect bubble dynamics in a nonlinear manner.Experimental validation confirms the potential of these findings for optimizing the design and operation of high-temperature bubbling fluidized bed reactors.
基金financial support by“Grassland Talents”of Inner Mongolia Autonomous Region,Young Talents of Science and Technology in Universities of Inner Mongolia Autonomous Region(No.NJYT23030)Technology Breakthrough Engineering Hydrogen Energy Field"Unveiling and Leading"Project(No.2024KJTW0018)+4 种基金“Steed plan High level Talents”of Inner Mongolia University,Carbon neutralization research project(No.STZX202218)the National Natural Science Foundation of China(No.U22A20107)Inner Mongolia Autonomous Region Natural Science Foundation(No.2023MS02002)Guangdong Provincial Key Laboratory of Materials and Technologies for Energy Conversion(No.MATEC2024KF011)National Key R&D Program of China(No.2022YFA1205201).
文摘Propane dehydrogenation using CO_(2)as a mild oxidizer(CO_(2)-ODP)is a promising technology for high propylene production and CO_(2)reduction utilization.Among them,the reverse water gas shift reaction(RWGS)can change the reaction equilibrium to increase the propylene yield,and the Boudouard reaction can assist in the carbon accumulation elimination.However,the efficiency of the catalysts developed so far is limited,we introduced the Cr active component during the synthesis of porous silica spheres to form a CO_(2)-ODP catalyst,with a uniform distribution of active sites via(NH_(4))_(3)[CrMo_(6)O_(24)H_(6)]·7H_(2)O produce a derivative.As anα-type Anderson series of polyoxometalates(POMs),this six octahedral structure formed by Mo participation surrounds the central atom Cr,which is more stable in structure by electrostatic effect,its derivatives generated after calcination are stably bound to the silica-based carrier,which reduces the formation of inertα-Cr_(2)O_(3)by CrO_(x)aggregation during the catalytic process.Meanwhile,the oxygen atoms rich in polyoxometalates are more likely to form Si-O bonds with the carrier,which makes the active sites evenly and stably branched in the inner wall of the pores of mesoporous silica spheres,reduces the influence of carbon accumulation,and facilitates the activation and regeneration.The CO_(2)conversion of the catalyst CrMoO_(x)@mesoporous silica spheres(MSS)is typically greater than 20%under selected ideal conditions.This synthesis method of assembling POMs with mesoporous materials opens a new pathway for developing propane dehydrogenation catalysts.Compared to traditional impregnation synthesis,this catalyst contains a lower Cr content while achieving higher CO_(2)consumption efficiency.
基金supported by the National Natural Science Foundation of China(22278241)a grant from the Institute Guo Qiang,Tsing-hua University(2021GQG1016).
文摘Conducting polymer hydrogels offer promising electrical interfaces with biological tissues for electrophysio-logical signal recording,sensing,and stimulation due to their favorable electrical properties,biocompatibility,and stability.Among them,Poly(3,4-ethylenedioxythiophene):Polystyrene sulfonate(PEDOT:PSS)is widely used as a conductive filler,forming a network of conjugated nanofibers within the hydrogel matrix.This structure enables robust electronic conductivity while preserving ionic transport and biocompatibility in phys-iological environments.However,the mechanical integrity of these hydrogels is often compromised by micellar microstructures in aqueous colloidal dispersions.The absence of interconnected conducting polymer nanofibers to maintain mechanical integrity during swelling hinders the mechanical properties of hydrogels.Here,three modification strategies were explored to enhance the flexibility and stretchability:constructing an inter-penetrating network,phase separation induced by ionic compounds,and pure conductive hydrogels formed through polar solvent additives and dry-annealing.These strategies synergistically enhance conductivity and flexibility by controlling interchain entanglement and redesigning the distribution of conjugated crystal regions and soft regions.The resulting hydrogels exhibit excellent conductivity(1.99-5.25 S/m),softness(elastic modulus as low as 280 Pa),and elasticity(tensile properties up to 800%).When used as epidermal or implantable bioelectrodes,they provided a soft interface,ensuring longer-lasting and more stable electromyo-gram,electrocardiogram,and electroencephalogram signals compared to commercial gel electrodes,with a signal-to-noise ratio of up to 20.0 dB.Therefore,the conducting polymer hydrogels developed in this study leverage the synergy between conductivity and flexibility,paving the way for further transformative applications in bioelectronics.
文摘Aromatics,as essential basic chemical raw materials,are widely used in rubber,nylon,resins,solvents,and other products.Light aromatics such as benzene,toluene,and xylene serve as cornerstones of modern chemical industries.Conventional aromatic production predominantly relies on petroleum resources.Compared with traditional petroleum-derived aromatic production processes,syngas to aromatics technology offer signifi cant advantages in terms of energy consumption,environmental emissions,and production costs.Notably,coal-based syngas to aromatics technology offers several advantages,including a shorter process flow,lower hydrogen-to-carbon ratio requirements,and improved pressure compatibility with existing systems.Therefore,syngas to aromatics technology is poised to play an increasingly vital role in future energy transitions,driving the evolution of green,low-carbon chemical industries.One of the key challenges in the technology of synthesizing aromatics from coal-based syngas lies in the construction of the catalytic system.Another challenge lies in the design of the reactor equipment.Based on the above key challenges,this review systematically summarizes three major catalytic mechanisms:the modified Fischer-Tropsch synthesis pathway,the methanol-mediated pathway,and the formaldehyde-mediated pathway,deeply analyses the factors influencing the catalytic performance in the syngas to aromatics process,discusses the role of reactor design in this process;on this basis,it further explores the potential and prospects of coal-based syngas to aromatics technology in promoting the development of green and low-carbon chemical industry.
基金supported by the National Natural Science Foundation of China(Nos.22071221,12374032,and U22A20107)the Natural Science Foundation of Henan Province(No.222301420040)+5 种基金China Postdoctoral Science Foundation(No.2023M743152)the State Key Laboratory of Refractories and Metallurgy(Wuhan University of Science and Technology)(No.G202306)“Grassland Talents”of Inner Mongolia Autonomous Region,Young Talents of Science and Technology in Universities of Inner Mongolia Autonomous Region(No.NJYT23030)“Steed plan High level Talents”of Inner Mongolia University,Carbon neutralization research project(No.STZX202218)Inner Mongolia Autonomous Region Natural Science Foundation(No.2023MS02002)the National Key R&D Program of China(No.2022YFA1205201).
文摘Due to the high structural flexibility and controllable thermal expansion,cubic double ReO_(3)-type negative thermal expansion(NTE)fluorides provide a solution for solving the prominent phenomenon of thermal expansion mismatch between materials.However,the expensive raw materials and complex synthesis steps limit its practical application.In this work,we have designed a more advantageous method for the synthesis of NTE material CaZrF_(6),and it is expected to be generalized to the synthesis of other double ReO_(3)-fluorides.Intriguingly,a new orthorhombic phase CaZrF_(6)has been synthesized via this method in a lower temperature.Unlike the strong isotropic NTE of the cubic phase CaZrF_(6),the orthorhombic phase shows the strong anisotropic positive thermal expansion(PTE).The combined analysis of temperature-dependent X-ray diffraction(XRD),Raman spectra,and first-principles calculations shows that the low frequency phonon vibration mode with negative Grüneisen parameter in cubic CaZrF_(6)are strongly correlated with the transverse thermal vibration of F atoms and dominates the NTE of the material.
基金support from the National Natural Science Foundation of China (Grant Nos.22308187,22208186,22278238,and 22238004)the Beijing Nova Program (Grant No.2022118)the Key Research and Development Program of Inner Mongolia and Ordos,and the Ordos-Tsinghua Innovative&Collaborative Research Program in Carbon Neutrality (Ordos Laboratory).
文摘Particle segregation and mixing behavior play a crucial role in industrial processes.This study investigates the saturated jetsam fraction,which indicates the maximum capacity of flotsam to entrain jetsam,in an initially separated binary fluidized bed with particle size differences.According to the value of saturated jetsam fraction,three distinct regimes-segregation,mixing,and an intermediate regime-are identified.Moreover,intriguing relationships between the saturated jetsam fraction and superficial gas velocity are observed,exhibiting monotonic trends in both the segregation and mixing regimes,while a unique volcano-shaped curve in the intermediate regime.Additionally,a comprehensive entrainment model based on two-fluid model elucidates the observed phenomena,emphasizing the significance of mixing behavior in fluidized layer on the saturated jetsam fraction.This work offers potential insights for evaluating segregation in industrial applications.
基金supported by the National Natural Science Foundation of China(grant No.U22A20410).
文摘Turbulent fluidized bed proves effective in industrial processes due to superior heat and mass transfer and chemical reaction performance. However, understanding the transition to turbulent fluidization remains limited, especially at temperatures exceeding 1000 ℃, making it challenging to develop high-temperature fluidized bed applications. This paper presents an experimental investigation on the turbulent fluidization onset velocity (U_(c)), measured in a 30 mm diameter bed using corundum particles with average diameters from 0.68 mm to 1.58 mm in temperatures from ambient to 1600 ℃. Experimental results reveal that U_(c) increases with temperature up to 600 ℃, stabilizes within the 600–1200 ℃ range, and then decreases above 1200 ℃, demonstrating the varying relative significance of hydrodynamic and interparticle forces at different temperatures. To help design and operate high-temperature applications of turbulent fluidization, we developed U_(c) correlations based on experimental data from both literature sources and this study, covering temperatures of up to 1600 ℃ and particles of Groups A to D.
基金support by“Grassland Talents”of Inner Mongolia Autonomous Region,Young Talents of Science and Technology in Universities of Inner Mongolia Autonomous Region(NJYT23030)Technology Breakthrough Engineering Hydrogen Energy Field“Unveiling and Leading”Project(2024KJTW0018)+4 种基金“Steed plan High level Talents”of Inner Mongolia University,Carbon neutralization research project(STZX202218)National Natural Science Foundation of China(U22A20107)Inner Mongolia Autonomous Region Natural Science Foundation(2023MS02002)Guangdong Provincial Key Laboratory of Materials and Technologies for Energy Conversion(MATEC2024KF011)National Key R&D Program of China(2022YFA1205201).
文摘The development of clean and efficient renewable energy is of great strategic importance to realize green energy conversion and low-carbon growth.Hydrogen energy,as a renewable energy with“zero carbon emission”,can be efficiently converted into hydrogen energy and electric energy by electrolysis of water to hydrogen technology.Anion-exchange membrane water electrolysis(AEMWE),substantially advanced by nonprecious metal electrocatalysts,is among the most cost-effective and promising water electrolysis technologies,combining the advantages of proton exchange membranes with the proven technology of traditional alkaline water electrolysis and potentially eliminating the disadvantages of both.In this paper,the latest results of AEMWE research in recent years are summarized,including the AEMWE mechanism study and the hot issues of low-cost transition metal hydrogen evolution reaction and oxygen evolution reaction electrocatalyst design in recent years.The key factors affecting the performance of AEMWE are pointed out,and further challenges and opportunities encountered in large-scale industrialization are discussed.Finally,this review provides strong guidance for advancing AEMWE.
