最新刊期
卷 50 ， 期 11 ， 2025
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摘要：Anaerobic methane (CH4) coupling catalyzed by dielectric barrier discharge (DBD) plasma is a significant pathway for the efficient conversion of CH4 into high-value hydrocarbons (such as C2 hydrocarbons). However, its reaction efficiency is influenced by multiple factors. Through a series of experiments, the effects of key parameters such as discharge power, temperatures, total gas flow rates, auxiliary gas types and contents (volume fraction, the same below) on CH4 conversion rates and C2 hydrocarbon selectivities were systematically investigated. The experimental results indicate that total gas flow rate is a critical parameter for controlling the residence time of reactants. When the total gas flow rate increases, the average residence time of the gas in the plasma region shortens, leading to a decrease in CH4 conversion rate. Auxiliary gas types significantly regulate the reaction pathway. When N2 is used as an auxiliary gas, the CH4 conversion rate is significantly increased by exciting high-energy electrons, and the C2 hydrocarbon selectivity can reach up to 40%. When H2 is used as an auxiliary gas, the CH4 conversion rate decreases, but the C2H6 selectivity increases to more than 90% due to hydrogen radical-mediated hydrogenation reactions. The microscopic morphology of the electrode surface directly affects discharge characteristics. After treating the electrode surface with the 0.10 mol/L lysine solution for one day, the CH4 conversion rate significantly increases compared to untreated electrodes. The synergistic optimization mechanism of these multiple parameters will provide critical design guidelines for the scale-up of plasma-catalytic CH4 conversion reactors and deepen the theoretical understanding of the mechanism in plasma-catalytic systems.关键词：anaerobic methane coupling;dielectric barrier discharge plasma;plasma catalysis15|0|0更新时间：2025-11-25 -
摘要：The preparation of methanol from coal gasification is an important clean energy chemical technology, which can reduce carbon emission and environmental pollution, but methanol from syngas requires high catalyst activity and thermal stability, and targeted optimization of catalyst performance is a research hotspot in this direction. Based on MC17 commercial catalyst, ternary, binary and pure-phase model catalysts were prepared by co-precipitation method. The physicochemical properties were analyzed by XRD, N2 adsorption/desorption and so on. The reaction mechanism and structure-activity relationship of the catalyst were investigated by changing the copper-zinc ratio (m(CuO):m(ZnO)) of the catalyst, and the regulation of Al on the catalyst was investigated. The results show that the copper-zinc ratio can affect the structure and catalytic activity of the catalyst. The appropriate copper-zinc ratio is 3:1 to 2:1. CO conversion rate of the catalysts reaches 67.2%, and the retention of activity after simulated deactivation is above 86%. The optimization of the copper-zinc ratio and the introduction of aluminium can effectively improve the activity and stability of the methanol synthesis catalysts, which provides a reference for the design and optimization of methanol synthesis catalysts.关键词：methanol synthesis catalysts;precursors;Cu-based catalysts;synergy30|0|0更新时间：2025-11-25 -
摘要：To enhance the catalytic activity for CO2 hydrogenation to methanol and improve the atom economy of the synthesis process, Cu/ZnO/ZrO2 catalysts were prepared using the ammonia evaporation method instead of the traditional co-precipitation method, and their performance for CO2 hydrogenation to methanol was investigated. The effects of the synthesis method and ammonia evaporation temperatures on the structures and catalytic performances of catalysts were systematically studied. The phase compositions, crystallite sizes and specific surface areas of the catalysts were characterized by XRD, N2 adsorption/desorption, and UV-Vis spectroscopy. The results show that compared with the catalyst prepared by the co-precipitation method, the catalyst synthesized via ammonia evaporation at 75 ℃ (CuZnZr-75) exhibits a more homogeneous distribution of Cu and Zn. After calcination, the resulting CuO crystallite size is smaller, leading to the formation of more Cu-Zn interfacial active sites. Under reaction conditions of n(H2):n(CO2) = 3:1, weight hourly space velocity (WHSV) of 24000 mL/(g·h), pressure of 2 MPa and temperature of 220 ℃, the catalytic performance was evaluated in a fixed-bed reactor. The results indicate that the ammonia evaporation method facilitates the construction of more highly active catalytic sites. Under optimal condition (CuZnZr-75), the methanol space-time yield per unit catalyst surface area increases from 3.96 mg/(m2·h) for the co-precipitated catalyst to 6.33 mg/(m2·h), and the CO2 conversion rate reaches 6.98%.关键词：Cu/ZnO/ZrO2 catalyst;ammonia evaporation method;CO2 hydrogenation;methanol72|0|0更新时间：2025-11-25 -
摘要：The preparation of methyl glycolate from ethylene glycol as raw material by oxidative esterification is an effective way to realize high value, low carbonization and diversified utilization of ethylene glycol. Nano-gold catalyst is a kind of commonly used catalysts for oxidative esterification, but its application in the reaction is limited due to its poor activity, large amount of precious metals used and high cost. Therefore, it is necessary to develop an efficient and relatively inexpensive catalyst. A series of palladium-based catalysts were prepared by equal volume impregnation method, and their catalytic performance for oxidative esterification of ethylene glycol to methyl glycolate was investigated. It is found that the catalyst activity and product selectivity can be significantly improved by introducing the second component into the palladium-based catalyst. The catalysts were characterized by XRD, TEM, XPS and H2-TPR. The results show that the second component forms intermetallic compounds with palladium, resulting in significant changes in the electronic properties of palladium, thereby improving catalyst activity and product selectivity. The types and contents of the second component, the reduction temperature of catalyst, the ratio of raw materials and the reaction temperature were investigated. It is found that the catalyst introducing bismuth has the best catalytic performance. Under the catalysis of Pd-Bi/Al2O3 catalyst with palladium and bismuth mass fractions of 1.00%, respectively and reduction temperature of 300 ℃, when n(ethylene glycol)/n(Na2CO3) = 200 and n(methanol)/n(ethylene glycol) = 20, the ethylene glycol conversion rate reaches 88.0% and methyl glycolate selectivity reaches 90.1% (120 ℃, 4 h).关键词：ethylene glycol;methyl glycolate;oxidative esterification reaction;palladium-based catalyst3|0|0更新时间：2025-11-25 -
摘要：As an important organic intermediate, epoxycyclohexane has shown a very broad application prospect in the field of chemistry and chemical engineering. However, current synthesis faces the problems of low selectivity and efficiency. Titanium silicate zeolites have unique porous structures and catalytic active centers, which can be used for efficient synthesis of epoxycyclohexane. Two types of titanium silicate zeolites (Ti-CHO-1 and Ti-CHO-2) were prepared, and their structures were characterized by XRD and UV-Raman spectroscopy, etc. The catalytic performance of Ti-CHO-1 and Ti-CHO-2 in synthesis of epoxycyclohexane by hydrogen peroxide (H2O2)oxidation of cyclohexene was studied, and the reaction conditions were optimized by optimal titanium silicate zeolites. The results indicate that compared to Ti-CHO-1, Ti-CHO-2 with hierarchical structure has a lower TiO2 content and lower acidity, resulting in better catalytic performance. Under the optimal conditions of acetonitrile solvent, temperature of 80 ℃, time of 4.0 h, cyclohexene dosage of 40 mmol, 30% (mass fraction) H2O2 dosage of 40 mmol (dropping time of 10 min), EDTA disodium salt dosage of 60 mg and Ti-CHO-2 dosage of 0.8 g, the conversion rate of cyclohexene, selectivity of epoxycyclohexane and yield of epoxycyclohexane are 87.2%, 83.1%, and 72.5%, respectively. Under optimal conditions for 5 cycles, the catalytic performance of Ti-CHO-2 can remain stable, which demonstrates that it has good recyclability.关键词：epoxycyclohexane;hydrogen peroxide;cyclohexene;catalytic oxidation;titanium silicate zeolites85|0|0更新时间：2025-11-25 -
摘要：The catalytic transfer hydrogenation of cinnamaldehyde to cinnamyl alcohol is of great practical significance, and the catalyst is the key to achieving selective hydrogenation of cinnamaldehyde. A series of ZrO(OH)2 catalysts were prepared by precipitation method at different aging temperatures, and ZrO2-25 was obtained by calcining ZrO(OH)2-25, which was aged at 25 ℃. The crystal phase structures, textural properties, microscopic morphologies, acid sites and —OH contents of ZrO(OH)2-25 and ZrO2-25 were characterized by XRD, N2 adsorption/desorption, SEM, Py-IR and XPS, respectively. The catalytic performances of the two catalysts were evaluated, and the effects of aging temperatures, reaction temperatures, cinnamaldehyde feeding amounts and hydrogen donor types on the catalytic performance of ZrO(OH)2-25 were investigated. The results show that ZrO(OH)2-25 exhibits amorphous state with specific surface area of 295 m2/g, while ZrO2-25 has tetragonal crystal structure with specific surface area of 144 m2/g. Under the optimal reaction conditions of 0.25 mmol cinnamaldehyde, 3 mL isopropanol as hydrogen donor, 40 mg ZrO(OH)2-25, 1 MPa N2, 700 r/min reaction temperature of 120 ℃ and reaction time of 4.0 h, the cinnamaldehyde conversion rate reaches 97.1% and the cinnamyl alcohol selectivity reaches 82.4%. The better catalytic performance of ZrO(OH)2-25 than ZrO2-25 under the same conditions is attributed to abundant —OH on its surface.关键词：cinnamaldehyde;catalytic transfer hydrogenation;cinnamyl alcohol;ZrO(OH)256|0|0更新时间：2025-11-25 -
摘要：γ-valerolactone (GVL) is an important biomass derivative, which is produced by “hydrolysis-hydrogenation” route of cellulose. However, at present, liquid acid and supported metal mixed catalysts are mainly used, which have the problem of low GVL yield. Therefore, a new route of “alcoholysis-hydrogenation” of cellulose and methanol was proposed. ZSM-5 molecular sieve pore confined Ru catalyst (Ru@ZSM-5) was designed with dual functional active sites of metal and acid by “ligand protection strategy” in-situ hydrothermal method, and Ru nanoclusters were encapsulated within the pore channels of ZSM-5 molecular sieve. TEM characterization and encapsulation degree test confirm that the average diameter of Ru clusters is only 0.57 nm, and a large number of Ru clusters (92.7%) are confined within the ten-membered ring cross pore channels of ZSM-5 molecular sieve. The results show that Ru@ZSM-5 exhibits excellent catalytic performance in the integrated conversion of cellulose and methanol to γ‑valerolactone. Under the conditions of 230 °C, 3 MPa H2 and volume ratio of water to methanol of 10%, the GVL yield is 51.1% (reaction for six hours), far superior to traditional supported Ru/ZSM-5, Ru/SiO2 + ZSM-5, and Ru/Al2O3 + ZSM-5 catalysts. Due to the confinement effect of ZSM-5 molecular sieve pores, Ru@ZSM-5 shows high stability, with the GVL yield of 51.5% and the particle size of Ru clusters remains 0.59 nm after five reaction cycles. However, Ru/ZSM-5 undergoes severe deactivation, and the Ru nanoparticles dispersed on the outer surface of ZSM-5 molecular sieve suffer from significant sintering, with the average particle size of 6.57 nm.关键词：cellulose;methanol;γ-valerolactone;Ru@ZSM-5;biomass29|0|0更新时间：2025-11-25 -
摘要：Due to the structural complexity of coal, its structural evolution is uncontrollable, which hinders the design and preparation of high-performance coal-based hard carbon materials. The effects of N-methylpyrrolidone (NMP) and NMP-CS2 (equal volume ratio) as extractants on structures and sodium storage properties of coal-based hard carbon materials were studied using Xinjiang nonstick coal as the raw material. The results show that the content of C==O groups on surface of the samples (HC-NMP) obtained with NMP as extractant is the highest, which is conducive to the construction of cross-linked structures during the preoxidation process. HC-NMP has large carbon layer distance and more disordered carbon structure, which are conducive to Na+ storage. At 20 mA/g, the reversible specific capacity of HC-NMP is 281.1 mAh/g, and the first cycle Coulomb efficiency is 84.1%. After 200 cycles at 100 mA/g, the reversible specific capacity of HC-NMP is 240.3 mAh/g.关键词：Xinjiang non-caking coal;extraction-peroxidation;extraction residue coal;coal-based hard carbon;sodium storage properties126|0|0更新时间：2025-11-25 -
摘要：The presence of hydrogen sulfide (H2S) and carbonyl sulfide (COS) in coal gas (including gasification gas, coke oven gas and blast furnace gas) can lead to catalyst poisoning, equipment corrosion and environmental pollution, making gas desulfurization crucial. The research progress on the dry gas desulfurization mechanism based on density functional theory (DFT) was summarized. Firstly, the adsorption mechanisms of H2S on the surfaces of various metal oxides, metal-organic framework materials (MOFs) and activated carbon materials were examined, along with an analysis of the desulfurization reaction pathways on commonly used metal oxides in industrial applications. Secondly, the dissociation and reaction mechanisms of O2 on the surface of metal sulfides during the regeneration of desulfurizers were elucidated, further revealing the microscopic mechanisms by which dopant modification influences the desulfurization and regeneration behavior of metal oxides. Additionally, the sulfur release mechanism during desulfurization was analyzed. Regarding the catalytic hydrolysis and hydrogenolysis of COS, the adsorption and transformation mechanisms of COS on catalyst surfaces were explored. Finally, existing challenges in the research field were summarized, and future research directions were proposed.关键词：density functional theory;hydrogen sulfide;carbonyl sulfide;adsorption mechanism;gas desulfurization228|0|0更新时间：2025-11-25 -
摘要：Sulfur hexafluoride (SF6) has become a key target of global emission reduction efforts due to its extremely strong greenhouse effect and high chemical inertness. However, existing technologies such as thermal catalysis and photocatalysis generally face problems such as low degradation efficiency and high energy consumption. A novel cerium-aluminum composite catalyst (i-AlCeO2) was prepared via the sol-gel method, and combined with dielectric barrier discharge (DBD) plasma technology to achieve efficient degradation of SF6. The physicochemical properties of the catalyst were characterized, and key parameters such as n(Al)/n(Ce) (i = 7/1, 5/3, 3/5 and 1/7) in the catalyst and the DBD input power (40 W to 60 W) were optimized. Meanwhile, the transformation mechanism of Ce3+ to Ce4+ and the generation of oxygen vacancies on the catalyst surface under plasma excitation were analyzed based on XPS characterization. The results show that adjusting n(Al)/n(Ce) and input power could significantly enhance the degradation efficiency of SF6. Under the conditions of using Ar as the carrier gas, the SF6 volume fraction of 1.53% and the input power of 50 W, the 3/5-AlCeO2 catalyst exhibits excellent catalytic degradation performance, achieving a degradation efficiency of 99.8% and a energy yield of 28.99 g/(kW·h), and the degradation efficiency remains stable over 99% after continuous operation about 40 min. Analysis reveals that the 3/5-AlCeO2 possesses a large pore size of 13.08 nm and abundant surface oxygen, which in synergy with the pre-dissociation effect of high-energy electrons generated by DBD on SF6, promotes the Ce3+-mediated attack of oxygen radicals (·O) on S—F bonds, thereby achieving deep degradation of SF6. This study aims to overcome the technical bottleneck of efficient and low-energy SF6 degradation through multi-scale catalyst design and plasma synergistic excitation strategy, and to clarify the structure-activity relationship and reaction mechanism, providing a reference for related research.关键词：SF6;DBD;cerium-aluminum composite catalyst;degradation efficiency12|0|0更新时间：2025-11-25 -
摘要：With the increasing severity of the global climate change problem, CO2 emission control has become the focus of attention. Combustion process of carbon-based fuel is one of the main sources of CO2 emission, and the development of efficient CO2 capture technology is of great significance to mitigate the greenhouse effect. In recent years, CO2 capture technologies based on carbon-based materials have received increasing attention. Research progress of carbon-based materials for CO2 capture (post-combustion capture) was reviewed, focusing on analyzing the CO2 capture mechanisms of carbon-based materials, mainly including physical adsorption, chemical adsorption and gas exchange, etc. The characteristics of different types of carbon-based materials and their applications for CO2 capture were summarized, and the effects of different modification methods on the CO2 capture performance of biochar were analyzed. Finally, the technical bottlenecks and future development directions of carbon-based materials for CO2 capture were analyzed and prospected.关键词：carbon-based materials;CO2 capture;biochar;doped modification164|0|0更新时间：2025-11-25 -
摘要：Due to the severe challenges caused by global climate change, carbon capture, utilization and storage (CCUS) technology has become the key to the green transformation of the chemical industry. Electrochemical technology has shown great potential in carbon dioxide (CO2) capture and conversion due to its high energy conversion efficiency and environmental friendliness. However, it still faces many challenges in industrial scale applications. The latest progress of electrochemical mediated carbon dioxide capture technology (EMCC) and electrochemical carbon dioxide conversion technology (ECCT) was reviewed. The impact of adsorbent optimization, electrode material selection, reactor design innovation, and multi-technology coupling integrated application on improving CO2 capture efficiency, products selectivity and system stability was systematically analyzed. It is found that although electrochemical technology has advantages in CCUS, it still needs further breakthroughs in material stability, system integration complexity and cost control. Future research should focus on developing efficient and stable materials, optimizing system integration strategies, reducing application costs, and exploring the synergistic effect of electrochemical technology and other CCUS technologies to achieve its wide application and industrialization process in industrial scale, providing robust support for the low-carbon chemical industry and environmental sustainability.关键词：CO2 capture and conversion;electrochemical technology;CCUS;electrocatalysis508|0|0更新时间：2025-11-25 -
摘要：CO2 capture from flue gas is an effective method to improve the climate change and achieve “carbon neutral”. The development of adsorbents with large CO2 adsorption capacity, excellent selectivity, rapid adsorption/desorption and simple regeneration is the key to achieving low energy consumption CO2 capture. Although metal-organic framework materials (MOFs) have a high saturation CO2 adsorption capacity, they suffer from slow adsorption rates. On the basis of Al(HCOO)3 MOFs (ALF), the modified adsorbents were synthesized by doping Mg, and their synthesis process were explored. The results show that the synthesis temperature and synthesis time have a great influence on the crystal structure and grain size of the adsorbents in the study of synthesis process of Mg(OH)2 doped modified adsorbents. Under synthesis temperature of 100 ℃ and synthesis time of 24 h, the CO2 adsorption capacity of AMHF-2 is 14.3 mL/g higher than that of ALF within 3 min. AMHF-2 and ALF have the same main structure. Compared with ALF, AMHF-2 has smaller crystallite size and higher crystallite dispersion, and has a faster adsorption rate and higher CO2 adsorption capacity in a short period of time. Therefore it becomes possible to apply to large-scale pressure swing adsorption flue gas decarbonization.关键词：ALF materials;MOFs;structure modulation;CO2 adsorption129|0|0更新时间：2025-11-25 -
摘要：In order to solve the corrosion problem of CO2 capture equipment of blast furnace gas in iron and steel enterprises, the ionic liquid anhydrous absorber diethylenetriamine formate-monoethanolamine-dimethylsulfoxide ([DETAH][HCOO]-MEA-DMSO) was prepared. The corrosivities of [DETAH][HCOO]-MEA-DMSO and aqueous absorbers (MEA-H2O, [DETAH][HCOO]-MEA-H2O) on 20# carbon steel sheet were studied by weight loss method and electrochemical method, respectively. The results show that when 20# carbon steel is corroded at 30 ℃ for 168 h, the corrosivity of fresh and saturated [DETAH][HCOO]-MEA-DMSO is very weak, with corrosion rates (weight loss method) of 3.12 × 10-4 mm/a and 9.56 × 10-4 mm/a, respectively, and the corrosion current densities (electrochemical method) are 4.09 × 10-7 A/cm2 and 13.20 × 10-7 A/cm2, respectively. The corrosivity of [DETAH][HCOO]-MEA-DMSO is not enhanced by increasing temperature and CO2 loading. The weak corrosivity of [DETAH][HCOO]-MEA-DMSO is related to the chelation effect of ionic liquid components to Fe2+.关键词：diethylenetriamine formate-monoethanolamine-dimethylsulfoxide;CO2 capture;corrosion characteristics;weight loss method;electrochemical method103|0|0更新时间：2025-11-25 -
摘要：Compared with the traditional ammonia synthesis process (Haber Bosch method), electrocatalytic nitrate reduction to ammonia offers advantages such as renewable energy input, mild reaction conditions and no secondary pollution. However, this reaction still faces challenges including insufficient catalytic activity, low product selectivity and poor stability. Copper-aluminum layered double hydroxides (CuxAl-LDH) with different ratios of Cu to Al (n(Cu)/n(Al) = x = 1.5, 2 or 3) were synthesized by hydrothermal method. Their structures were characterized, and their electrochemical performances were evaluated. The effects of Cu/Al ratio, initial NO -
摘要：Long-distance pipeline systems are the most efficient, economical and safe methods for large-scale green ammonia transportation. When a liquid ammonia pipeline leaks or requires maintenance, in order to prevent severe hazards caused by the direct release of highly toxic liquid ammonia to surrounding personnel and the environment, a release and recovery process is typically adopted. Based on the fundamental thermophysical properties and phase characteristics of ammonia, a simulation model of the release and recovery process for liquid ammonia pipelines was developed to investigate the variations in temperature and pressure under different operating conditions, as well as the associated low-temperature failure risks. The results show that during the release and recovery process of liquid ammonia pipelines, the internal pressure, temperature, liquid holdup and ammonia inventory all exhibit a trend of rapid initial decline followed by gradual stabilization. Moreover, the local temperature inside the pipeline may remain below the minimum allowable service temperature (-20 ℃) of commonly used pipeline materials for an extended period, significantly increasing the risk of brittle fracture due to low temperatures. The closer to the release point, the greater the drops in pressure and temperature, with temperatures potentially falling to around -30 ℃, and the fluctuations being more pronounced. Soil temperature has a limited effect on the pressure and temperature changes during the release and recovery process, but higher soil temperature significantly shortenes the recovery duration. A higher back pressure in the storage tank results in smaller pressure and temperature drops and reduced fluctuations, but prolongs the recovery time. Conversely, a larger valve opening leads to greater pressure and temperature drops and a shorter recovery time. Increasing the storage tank back pressure and reducing the valve opening can maintain the pipeline temperature within the safe range of -15 ℃ to -10 ℃. This study provides a reference for safety management in the emergency release and recovery processes of long-distance liquid ammonia pipelines.关键词：liquid ammonia pipelines;release and recovery;characteristic parameters;low-temperature brittle fracture;simulation model79|0|0更新时间：2025-11-25
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