


In the context of global climate change,carbon capture, utilization and storage (CCUS) technology has received widespread attention as a key technology for reducing greenhouse gas CO2 emissions and achieving the “dual carbon” goal.The operating cost of CO2 capture technology accounts for 70% of the total CCUS cost and is the core of CCUS technology.The PCET (proton-coupled electron transfer) reaction mechanism,as a crucial reaction pathway in the fields of energy conversion and environmental protection,has demonstrated significant application potential in CO2 capture technology.This article introduces the mechanism of PCET,summarizes the latest research progress of PCET application in electrocatalytic CO2 capture,deeply analyzes the advantages of related technologies,and further looks forward to future development directions,providing theoretical references for CO2 capture.
Catalytic combustion is currently one of the most effective methods to purify volatile organic compounds (VOCs).The design of effective catalysts for VOCs combustion is of great importance.An overview of domestic and foreign patent applications in this field and the primary applicants are herein subjected to statistical analysis.The area of volatile organic compounds catalytic purification is investigated in detail with an emphasis patent of the main catalytic systems and the evolving processes of the respective technical systems.Based on the state of art development in this field,rationalized recommendations are given for the development of catalysts for purification of volatile organic compounds,aiming to provide reference and inspiration for the subsequent development of highly active,highly stable,widely applicable catalysts and their industrial applications,and to provide valuable references for patent applications and layouts.
Mechanical strength serves as a critical prerequisite for solid catalysts to exhibit optimal performance,while forming processes provide solid-phase catalysts with appropriate morphology,dimensions,and superior mechanical robustness.Among various forming techniques,extrusion molding has been extensively employed in the processing of catalytic materials and ceramic products due to its advantages of high production efficiency,process continuity,cost-effectiveness,and broad applicability.During catalyst extrusion molding,mechanical strength is influenced by multiple factors related to forming conditions and thermal treatment processes.This paper systematically reviews the fundamental mechanisms of catalyst extrusion molding,operational parameters during extrusion,and heat treatment procedures.Key influencing factors and corresponding control strategies are discussed,including powder particle size,mixing duration and methodology,water-to-powder ratio,peptizing agents,extrusion aids,binding agents,as well as drying and calcination processes.These investigations hold significant implications for fabricating stable and controllable high-strength catalysts while extending the operational lifespan of industrial catalysts.
Silver catalyst is the only industrial catalyst for the production of ethylene oxide (EO),but there are problems such as complex catalyst structure,unclear mechanism,low conversion,low reactant partial pressure,high energy consumption for recycle flow and product separation,and high CO2 emission.The single-atom catalysts (SACs) show great application prospects in ethylene epoxidation reaction based on their outstanding advantages such as clear structure,clear mechanism,and controllable structure and performance,as well as their high atom utilization,high activity and selectivity.And the current relevant catalyst design strategies are mainly categorized into single-atom thermal catalysts and single-atom electrocatalysts.This review detailed the current research progress and challenges in this field,and gave some methods and suggestions to solve the dilemmas based on relevant research reports,including stability improvement of SACs,scale-up preparation techniques,design of novel SACs,and in-depth exploration of the mechanism as an aid.
Aiming at the problems of topological competition,templating agent dependence and high solvent consumption during the synthesis of SAPO-5/SAPO-18 eutectic molecular sieves,this study proposes a solvent-free green synthesis strategy,and systematically explores the influence laws of crystallization time,temperature and precursor ratios on the formation of eutectic structures.By optimizing the molar ratio of raw materials (Al2O3∶P2O5∶SiO2∶DIEA=1.0∶0.73∶0.6∶1.5) and the crystallization conditions (180 ℃,24 h),SAPO-5/SAPO-18 eutectic molecular sieves with high crystallinity were successfully prepared.XRD analysis showed that SAPO-18 (AEI phase) dominated at the early stage of crystallization,and SAPO-5 (AFI phase) gradually nucleated after prolonging the crystallization time to form a two-phase eutectic structure.An increase in crystallisation temperature promotes AFI phase generation,whereas a decrease in silicon content (SiO2/Al2O3=0.4) or template dose (DIEA/Al2O3=1.0) significantly reduces the AEI backbone crystallinity.By changing the crystallization conditions,effective control of the crystal structure and morphology of SAPO-5,SAPO-18,and SAPO-5/18 eutectic zeolites can be achieved.The solvent-free synthesis provides a new way for the green synthesis and industrial catalytic application of eutectic molecular sieves.
Ni/ZrO2 and Ni/TS-1 were prepared by the hydrothermal synthesis respectively,and Ni-TS-1@ZrO2 core-shell catalyst was prepared by coating ZrO2 on the surface of Ni/TS-1.The catalysts were analyzed by N2 adsorption-desorption,XRD,TEM,XPS.The effects of the core-shell structure possessed by Ni-TS-1@ZrO2 on the catalyst activity,stability,and anti-carbon accumulation performance were investigated.The results showed that Ni-TS-1@ZrO2 had the largest specific surface area and the largest number of mesopores.It was found that the reactivity of Ni-TS-1@ZrO2 with a core-shell structure was significantly increased,and the conversion of CH4 and CO2 was significantly improved after coating ZrO2.In the performance test,the reaction temperature was 700 ℃,the reaction time was 2 h,and the CH4 conversion over Ni-TS-1@ZrO2 was 86.1%,and the CO2 conversion was 91.4%.The ratio of H2/CO in the product was 0.91.As the temperature rised,the conversion over the Ni-TS-1@ZrO2 catalyst and the ratio of H2/CO increased.
A series of nanosheet ZSM-5 zeolites with different phosphorus precursors and loadings were synthesized using the impregnation method.The crystal structure,morphology,pore structure,and acidity of these materials were characterized by X-ray diffraction (XRD),scanning electron microscopy (SEM),N2 physical adsorption-desorption,and NH3 temperature-programmed desorption (NH3-TPD).The effects of phosphorus modification on the hydrothermal stability of nanosheet ZSM-5 and its performance in the co-cracking reaction of n-butene and methanol were systematically investigated.In this study,different phosphorus precursors[(NH4)2HPO4 and H3PO2]were used to modify the catalysts.After treatment at 800 ℃ under 100% steam for 4 hours,it was found that H3PO2 modification significantly improved the hydrothermal stability of the samples.Based on this,we further investigated the influence of H3PO2 loading on the hydrothermal stability and catalytic performance of the samples.The experimental results indicated that when the H3PO2 loading was mass fraction of 0.5%,the catalyst exhibited excellent stability and high light olefin yield in the co-cracking reaction of n-butene and methanol even after the aforementioned harsh hydrothermal treatment.The initial conversion of n-butene reached 68% after hydrothermal treatment,which was nearly 20 percentage points higher than that of the unmodified sample subjected to the same treatment.Additionally,the initial yield of ethylene and propylene increased by nearly 25 percentage points compared to the unmodified sample after hydrothermal treatment.After 340 hours of reaction,the total yield of ethylene and propylene still reached 40%.
Traditional powder photocatalysts face challenges such as aggregation-prone behavior,insufficient long-term stability,and difficult post-use recovery in practical applications.In contrast,monolithic photocatalysts can be directly applied in fixed-bed reactors or continuous-flow systems,offering facile separation and greater alignment with industrial requirements.However,current reports on monolithic photocatalysts for water splitting remain scarce,and existing synthesis protocols often involve complex procedures.There is an urgent need to develop more high-performance monolithic photocatalyst systems coupled with simple and rapid preparation methods.In this study,a Ni3S2-ZnIn2S4 heterojunction monolithic photocatalyst was controllably synthesized on nickel foam via a one-step hydrothermal method.The nickel foam not only serves as a robust structural scaffold but also acts as a nickel source for the in situ generation of Ni3S2 co-catalysts.The formed Ni3S2-ZnIn2S4 heterojunction significantly enhances photocatalytic activity and stability.The optimized Ni3S2-ZnIn2S4 monolithic catalyst demonstrates exceptional hydrogen evolution performance,achieving a cumulative hydrogen yield of 48.6 μmol over 5 hours,which is 3.4-fold higher than that of its powdered counterpart and surpasses many contemporary monolithic photocatalysts.This strategy exhibits simplicity,compatibility,and scalability,providing a novel pathway for the fabrication of large-scale photocatalytic water splitting systems.
The mechanism of ammonia decomposition on carbon nanotube-supported Co6 clusters (Co6@CNT) and Ni6 clusters (Ni6@CNT) was investigated by first-principles calculations.The most stable configurations of the species involved in the ammonia decomposition reaction were obtained through configuration optimization,and the adsorption energy of each species were obtained.It was found that carbon nanotubes as carriers significantly enhanced the adsorption ability of metal clusters.The transition states of the elementary reactions NH3→NH2+H,NH2→NH+H,NH→N+H and N+N→N2 involved in the ammonia decomposition process were searched,and the reaction heat and activation energy were obtained.The results show that carbon nanotubes as carriers significantly enhance the catalytic activity of Co6 clusters and Ni6 clusters.
Propane dehydrogenation (PDH) technology is a crucial pathway for propylene production,but its catalysts are prone to deactivation due to carbon deposition,resulting in performance decline.This study focuses on the moving-bed PDH process,investigating the effects of modulating the pore structure and mechanical strength of the support on catalyst performance.Alumina-based supports (RS-1 to RS-4) were prepared using different pore-enlarging agents (PET-1000,PET-5000,and PVP),and a series of catalysts (RSC-1 to RSC-4) were synthesized by loading Pt-based active components via the equal-volume co-impregnation method.Nitrogen adsorption-desorption and strength tests revealed that the addition of pore-enlarging agents significantly increased the support pore size (from 10.9 nm to 24.5 nm),and the introduction of PVP mitigated the strength reduction caused by pore enlargement by enhancing particle binding forces.Catalyst performance was evaluated under conditions of 600-620 ℃,atmospheric pressure,and an H2/C3H8 molar ratio of 0.5.The results showed that catalysts RSC-3 and RSC-4,prepared with large-pore supports,exhibited reduced carbon deposition due to optimized mass transfer processes,leading to significantly lower decay rates in conversion and selectivity,as well as superior stability compared to the small-pore catalyst (RSC-1).This study demonstrates that synergistic regulation of pore size expansion and mechanical strength can effectively enhance the carbon resistance and service life of PDH catalyst,providing key optimization direction for industrial catalyst design.Future research will focus on further optimizing the synergistic effects of additives and regeneration performance.
The process of catalytic liquid-phase selective oxidation of n-butane to prepare methyl ethyl ketone was studied using cobalt porphyrin/N-hydroxyphthalimide (NHPI) as catalyst and molecular oxygen as oxidant.Under optimized conditions (n-butane 64 mmol,cobalt porphyrin 1.0 × 10-3 mmol,NHPI molar fraction of 1.2%,100 ℃,1.0 MPa,4 h),the conversion of n-butane was 36.6%,and the selectivity of methyl ethyl ketone was 83.6%.Mechanistic studies demonstrated that the oxidation of n-butane was a reaction of free radical process.In situ UV spectroscopy demonstrated that cobalt porphyrin activated molecular oxygen to generate high valence active species,which combined with alkyl radicals to form methyl ethyl ketone.
In the continuous catalytic synthesis of 3-methyl-2-aminobenzoic acid from 3-methyl-2-nitrobenzoic acid,the effects of reaction temperature,pressure,molar ratio of hydrogen material and space velocity on the product distribution were studied,and the stability of the catalyst was evaluated.The results showed that the conversion and selectivity over the 1%Pt/C catalyst prepared with formic acid treatment carrier as the catalytic system were above 99% under the best reaction conditions of reaction temperature of 100 ℃,reaction pressure of 1.5 MPa,molar ratio of hydrogen material of 7 and space velocity of 0.6 h-1.The reaction stability is better under this catalytic system,and the catalyst life is longer.The results of this study can provide process parameters for industrial production and provide technical guidance for the modulation of industrial production results.
In order to study the feasibility of solving the problem of boiler air preheater ash deposition caused by the formation of ammonium bisulfate through the method by heating,a simultaneous thermal analyzer and Fourier transform infrared spectrometer were used to study the decomposition characteristics of ammonium bisulfate deposited in alumina,quartz sand,and coal ash samples in the range of 30~920 ℃.The samples were heated from 30 ℃ to 920 ℃ at a rate of 20 ℃/min in a N2 atmosphere.The results show that the decomposition characteristics of ammonium bisulfate on different deposits are different,and its decomposition characteristics are not only related to the type of deposits but also to the composition of the deposits.Among them,the thermal decomposition characteristics of ammonium bisulfate deposited on quartz sand are similar to ammonium bisulfate,primarily involving the thermal decomposition of ammonium bisulfate.However,the thermal decomposition characteristics of ammonium bisulfate deposited in alumina and coal ash are markedly different from those of pure ammonium bisulfate.This is primarily due to the reaction of ammonium bisulfate with the deposited substrate,which produces gases,and the subsequent decomposition of the generated solid into gases,leading to a reduction in mass.Furthermore,the melting point of the generated solid before decomposition is lower than that of ammonium bisulfate,thereby exacerbating ash fouling.