最新刊期
卷 51 ， 期 6 ， 2026
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摘要：CO2 methanation is one of the important chemical strategies to achieve “carbon neutrality”. However, developing catalysts with high methane (CH4) selectivity remains challenging. CeO2 supports with different morphologies were prepared via calcination or hydrothermal method, and Rh-CeO2 catalysts with different exposed facets of CeO2 were prepared by loading 0.5% (mass fraction) Rh. The effects of the exposed facets of CeO2 on catalytic performances of Rh-CeO2 catalysts for CO2 methanation were systematically investigated. The results show that 0.5Rh-CeO2-NC (NC represents nano-cube) exhibits the best catalytic performance with CH4 selectivity of 76% and CH4 yield of 29.19% at 400 ℃. The CeO2(100) facet facilitates the formation of surface oxygen vacancies after reduction pretreatment, which promotes CO2 activation, and electron-rich Rh single atoms aggregate into nanoparticles, enhancing H2 activation and promoting CH4 formation. In situ DRIFTS confirms that CO2 methanation with Rh-CeO2 catalysts follows a dual-path mechanism of formate pathway and CO pathway, and the competition between these two pathways is regulated by CeO2 exposed facets.关键词：CO2 methanation;Rh-CeO2 catalysts;CeO2 exposed facets68|124|0更新时间：2026-06-25 -
摘要：Under the background of climate issues caused by the increase in CO2 concentration in the atmosphere and the promotion of “dual carbon” goal, although perovskite-type PbTiO3 has the potential for photocatalytic applications, its catalytic performance is limited due to the wide band gap and low photogenerated electron-hole separation efficiency in pure-phase PbTiO3. Rare earth ions doping is regarded as an effective method to enhance its photocatalytic performance. Pure-phase PbTiO3 and PbTiO3 with La, Sm, Pr, Dy and Tm rare earth ions doping were prepared by the hydrothermal method. The phases, morphologies and photoelectric properties of catalysts were characterized by XRD, SEM and UV-Vis DRS, and the photocatalytic CO2 reduction performances were evaluated. The results show that PbTiO3 with 1% (mole fraction) Pr3+ doping presents a polygonal block shape with the size range of 500 nm to 1000 nm. After 2 hours of irradiation with a 300 W xenon lamp under CO2, the CO and CH4 yields of the catalyst reach 1.70 μmol/(g·h) and 0.55 μmol/(g·h), respectively. Moreover, it exhibits good stability. Under 60%N2/40%CO2 mixed gas (other conditions remaining unchanged), the CO production of the catalyst increases to 2.82 μmol/g, because Pr3+ doping provides 4f orbitals for PbTiO3, narrows the band gap, promotes photogenerated electron-hole separation, and significantly enhances the photocatalytic CO2 reduction performance.关键词：photocatalytic CO2 reduction;rare earth doping;PbTiO378|0|0更新时间：2026-06-25 -
摘要：To address the challenges of deep CO removal from hydrogen produced by carbon-based fuel reforming and the replacement of Ru-based noble metal catalysts with non-noble metals, a two-stage selective methanation of CO (CO-SMET) technology over Ni/Ru-based dual catalysts was proposed. Ru-based and Ni-based catalysts with Cl loading were prepared, and their CO-SMET catalytic performances and CO methanation selectivities were investigated under inlet gas H2/CO2/CO (volume fractions of 75.0%, 24.5% and 0.5%, respectively). The results show that, in one-stage CO-SMET, the outlet CO concentration (mole fraction, the same below) is 17 μmol/mol, and the temperature is 310 ℃, and the CO methanation selectivity is 75.1% over Cat-10Ni5Cl, whereas the outlet CO concentration is 32 μmol/mol, and the temperature is 250 ℃, and the CO methanation selectivity is 65.9% over Cat-1.5Ru4.5Cl. In the two-stage CO-SMET over Ni/Ru-based dual catalysts, the outlet CO concentration is 8 μmol/mol, and the temperatures of first-stage and second-stage are 280 ℃ and 230 ℃, respectively, with the CO methanation selectivity of 80.0%. Cat-10Ni5Cl (as the first-stage catalyst) exhibits high CO methanation selectivity at lower temperatures, and Cat-1.5Ru4.5Cl (as the second-stage catalyst) exhibits high activity at low temperatures. Two-stage CO-SMET enables deep CO removal and partially replaces Ru-based noble metal catalysts.关键词：reforming hydrogen;methanation;CO removal;catalysts47|93|0更新时间：2026-06-25 -
摘要：In order to synthesize pure phase SAPO-34 zeolites with good catalytic performances for methanol to olefins, it is often necessary to add a large amount of organic template agent. However, a large amount of organic template agent not only increases the synthesis cost of SAPO-34 zeolites, but also pollutes the environment during the post-treatment process. With low-dosage template addition (n(triethylamine + tetraethylammonium hydroxide):n(P2O5) = 1.7:1.0), SAPO-34 zeolites were synthesized with and without ammonia. The results show that compared to SAPO-34 zeolite synthesized without ammonia (C-SAPO-34), the SAPO-34 zeolite synthesized with ammonia (L-SAPO-34) exhibits higher crystallinity, higher silicon content (mass fraction) in the crystal framework and higher acid strength. In the crystal framework of L-SAPO-34, silicon atoms exist in the form of Si(Al)4, then a higher content of silicon indicates the presence of more active sites. More active sites can reduce the partial pressure of methanol of each active site in MTO reaction, which is beneficial for improving the selectivity of dienes (ethylene + propylene), reducing the coking rate and prolonging the service life of zeolites.关键词：SAPO-34 zeolites;organic template;methanol to olefins;active sites103|0|0更新时间：2026-06-25 -
摘要：Coal-to-ethylene glycol (EG) route is a pivotal technology within the strategic framework of coal’s clean and efficient utilization in China, and dimethyl oxalate (DMO) hydrogenation to EG is the key step in the route. Due to its outstanding catalytic performance and controllable cost, Cu/SiO2-based catalysts have achieved industrial application in DMO hydrogenation to EG. However, present technologies are still limited by high energy cost of H2 circulation and short catalyst lifespans. Firstly, the reaction pathway of DMO hydrogenation, the active sites of the catalyst and their structure-activity relationships, as well as the deactivation mechanism were introduced. Then, from the perspectives of structure-activity relationship and industrial application, the active center regulation strategies such as the composite preparation process, promoter modification and microscopic-mesoscopic structure design of the catalyst were analyzed. Finally, the future developments of Cu/SiO2-based catalysts for DMO hydrogenation to EG were prospected, such as studying the dynamic evolution and deactivation mechanism of surface species of catalysts, seeking more effective active center regulation indicators and developing Cu/SiO2-based catalysts suitable for low n(H2)/n(DMO) and their supporting processes.关键词：ethylene glycol;dimethyl oxalate;Cu/SiO2-based catalysts;reaction mechanism;active center regulation96|0|0更新时间：2026-06-25 -
摘要：The hydrogenation of dimethyl oxalate (DMO) to produce ethylene glycol (EG) is a green route that combines economic viability with technical feasibility. Nanoparticle-, bulk- and sphere-shaped SiO2 supports were prepared by hydrothermal method for supporting Cu-based catalysts, aiming to investigate the effect of support morphologies on the stability of Cu/SiO2 in DMO hydrogenation. The physicochemical properties of the catalysts were characterized by XRD, SEM, XPS, H2-TPR and so on. The results show that the stability of the Cu/SiO2 catalyst is affected by the morphologies of the SiO2 support. After 70 h of hydrogenation of DMO to EG, the DMO conversion rate and EG selectivity of the Cu/SiO2-N (N represents nanoparticle-shaped) catalyst still reaches 98.4% and 89.5%, respectively, without significant deactivation. Compared with the bulk- and sphere-shaped SiO2-supported catalysts, as well as commercial catalysts, the Cu/SiO2-N catalyst exhibits higher stability. The improvement in stability is mainly due to the higher relative content ratio of Cu+ to Cu0 and better anti-carbon deposition performance.关键词：dimethyl oxalate;hydrogenation;ethylene glycol;support morphology;stability4|0|0更新时间：2026-06-25 -
摘要：The hydrogenation of dimethyl oxalate (DMO) to methyl glycolate (MG) has the advantages of being environmentally friendly and having relatively high MG yield. To optimize the structure and catalytic performances of catalysts for hydrogenation of DMO to MG, a series of Ni-modified Cu/SiO2 with different NiO mass fractions were prepared by synchronous ammonia evaporation method, and the catalysts were characterized by N2 physical adsorption/desorption, XRD and H2-TPR. The catalytic performances of the catalysts were evaluated on a fixed-bed micro-reaction device. The results show that the NiO mass fraction has no significant effect on the texture properties of the catalysts. Under the conditions of reaction temperature of 210 ℃, pressure of 2 MPa and n(H2)/n(DMO) = 100, 10Ni-Cu/SiO2 with NiO mass fraction of 10% exhibits good catalytic performance with DMO conversion rate of 98.3%, MG selectivity of 95.4% and MG yield of 93.8%, respectively. In addition, 10Ni-Cu/SiO2 has good stability, and its catalytic performance can remain stable within 500 h.关键词：synchronous ammonia evaporation method;Ni modification;dimethyl oxalate;hydrogenation;methyl glycolate61|0|0更新时间：2026-06-25 -
摘要：Covalent organic frameworks (COFs), owing to their structural designability, excellent thermal and chemical stability and ordered pore channels, exhibit great potential as matrix materials for solid-state electrolytes. However, existing sulfonic acid-functionalized COF-based solid-state electrolyte materials possess relatively simple structures, which limit their further performance enhancement. COF-Br containing bromine anchoring sites was synthesized via a solvothermal method. Through a Williamson ether synthesis reaction, sulfonic acid functional groups were successfully introduced, leading to the preparation of the functional COF-Br-SO3Li material. By compositing COF-Br-SO3Li with polyethylene oxide (PEO), a novel composite solid-state electrolyte film was obtained. Characterization results from XRD, FT-IR and TGA confirm that the prepared COFs possess good crystallinity, porosity and thermal stability. Electrochemical measurements demonstrate that at 30 ℃, the lithium-ion conductivity of the COF-Br-SO3Li solid-state electrolyte reaches 2.5 × 10-5 S/cm, with an activation energy of 0.25 eV, an electrochemical stability window extending up to 5.2 V and a lithium-ion transference number of 0.65. During the lithium symmetric cell cycling test (500 h), the solid-state electrolyte exhibits excellent interfacial stability and outstanding capability to suppress lithium dendrite growth.关键词：covalent organic frameworks;sulfonic acid functionalization;solid-state electrolytes;lithium-ion conduction46|166|0更新时间：2026-06-25 -
摘要：Studying the phase behavior of the oil-CO2 system is crucial for efficient shale oil and gas recovery. Considering the effects of capillary pressure and the shift of fluid critical points, a vapor-liquid equilibrium (VLE) model incorporating nano-confinement effects was developed, achieving a prediction relative error of less than or equal to 1.53%. On this basis, the phase behavior of CO2-shale oil systems was investigated using Eagle Ford and Wolfcamp shale oils as examples. The results indicate that the presence of nano-confinement suppresses the bubble-point pressure and delays gas liberation from the liquid phase, resulting in a lower gas-oil ratio, which is favorable for shale oil production. Under nano-confinement, the reduced gas-liquid density difference leads to a decrease in gas-liquid interfacial tension. Smaller pore radius of reservoir correspond to stronger nano-confinement effects and a greater tendency for CO2 and oil to become miscible. As the pore radius decreases, the gas-liquid interfacial tension first decreases slowly and then rapidly, with a pore radius of 20 nm identified as the turning point. In contrast, the capillary pressure first increases and then decreases, with the turning point occurring at a pore radius of 5 nm. This study can provide a reference for optimizing CO2 injection strategies and enhancing shale oil recovery.关键词：nano-confinement effect;phase behavior;shale oil;vapor-liquid equilibrium;gas-liquid interfacial tension91|123|0更新时间：2026-06-25 -
摘要：CF4 and NF3 are two important fluorinated electronic specialty gases, but due to their similar properties, the purification and separation are challenging. As a novel adsorbent with adjustable pore structure, the metal organic framework (MOF) materials are widely used for selective adsorption of gases. The research progress on various MOF materials applied to the adsorption and separation of CF4 and NF3 was reviewed. The adsorption capacity, CF4/N2 and NF3/N2 adsorption selectivities and cycle life of various MOF materials were summarized. And the effects of pore diameter, Lewis acidity of metal centers, electron donating ability of ligand substituents and other key factors on the adsorption performance were analyzed. Based on this, further research progress was explored on the removal of trace amounts of NF3 from CF4 and trace amounts of CF4 from NF3 by MOF materials. High throughput calculations can not only quickly obtain the adsorption performance of various MOF materials, but also provide guidance for the design and optimization of target MOF materials. Finally, the shortcomings of existing MOF materials in the adsorption and separation of CF4 and NF3 were analyzed, and the future research and development directions were discussed.关键词：metal organic framework;CF4;NF3;adsorption capacity;high throughput calculation2|0|0更新时间：2026-06-25 -
摘要：Zinc oxide (ZnO) is widely used as a precise desulfurization agent in industrial processes, but its regeneration is difficult, making recycling challenging. Existing studies mainly focus on the effects of operating conditions, such as temperature, oxygen concentration and space velocity, on the regeneration rate, composition and structure of ZnO. However, the effect of the particle size of the desulfurization product zinc sulfide (ZnS) on the cyclic desulfurization-regeneration performance of ZnO remains unclear. ZnS samples with different particle sizes (13.98 nm, 18.48 nm and 33.00 nm) were prepared via a hydrothermal method, and oxidative regeneration/desulfurization cycle tests were conducted. Characterization techniques including XRD, N2 adsorption/desorption and XPS were used to compare the composition and structure of the samples during three oxidative regeneration cycles, and to investigate the effect of ZnS particle size on the cyclic desulfurization-regeneration performance of ZnO. The results show that ZnS particle size has a significant effect on the oxidation regeneration rate, the crystallite size and the textural properties of regenerated ZnO. Smaller ZnS particles lead to faster oxidation regeneration, with the oxidation time shortened by up to 60 min, and produce regenerated ZnO with smaller crystallite sizes and larger specific surface areas, resulting in higher desulfurization activity during the oxidative regeneration/desulfurization cycles tests. However, after three cycles, ZnO regenerated from small-particle ZnS exhibits the largest increase in crystallite size (68.7%), the greatest decrease in specific surface area (29.0%), and generates the most zinc sulfate (ZnSO4), thereby showing the largest decrease in desulfurization performance (32.6%).关键词：ZnS;ZnO;oxidative regeneration;desulfurization;particle size effect55|71|0更新时间：2026-06-25 -
摘要：Liquid organic hydrogen carriers (LOHC) represent a promising hydrogen storage strategy owing to their high safety and mild reaction conditions. However, the dehydrogenation reaction of LOHC imposes stringent requirements on the catalysts, thus the development of highly efficient catalysts capable of achieving dehydrogenation under low-temperature conditions is essential. A series of titanium nanotube (TNT) supports were synthesized via high-temperature hydrothermal method, and various supported Pd-based catalysts were prepared by loading Pd onto the supports through the impregnation method and the dehydrogenation performance for 8H-N-methylindole (8H-NMID) was evaluated. The physicochemical properties of catalysts were characterized by XRD, SEM, TEM, XPS, etc., and the structure-activity relationships of catalysts were explored. The results show that hydrothermal treatment increases the catalyst’s specific surface area and oxygen vacancy density, among which the Pd/TNT-150-24 catalyst exhibits the maximum specific surface area and oxygen vacancy density. Pd/TNT-150-24 displays excellent catalytic performance. After reacting at 180 ℃ for 6 h, it can achieve complete dehydrogenation of 8H-NMID. The conversion rate of 8H-NMID and the selectivity of N-methylindole (NMID) of this catalyst can both reach 100%. The dehydrogenation reaction rate of 8H-NMID is positively correlated with reaction temperature, with an apparent activation energy of 134.48 kJ/mol. Additionally, Pd/TNT-150-24 demonstrates good stability, retaining a dehydrogenation efficiency of 84.8% after five consecutive reaction cycles.关键词：TiO2 nanotubes;N-methylindole;dehydrogenation catalyst66|0|0更新时间：2026-06-25 -
摘要：Due to the low density of hydrogen, transportation via high-pressure tube trailers is economically inefficient. Blending hydrogen into natural gas pipelines is considered one of the effective approaches for long-distance, large-scale hydrogen transport. An experimental study was conducted on the coupled membrane-pressure swing adsorption (PSA) process for hydrogen separation from natural gas with hydrogen blending ratios of 5.0% to 20.0% (volume fraction, the same below). The main factors affecting hydrogen separation efficiency, such as the natural gas hydrogen blending ratio, pressure, flow rate, and carbon dioxide content, etc., were analyzed. The results show that the hydrogen blending ratio in natural gas has the most significant impact on hydrogen separation efficiency, with higher blending ratios leading to lower hydrogen separation costs. Higher pressure of hydrogen-enriched natural gas results in a higher hydrogen recovery rate. However, an increase in flow rate leads to a decrease in the hydrogen recovery rate. Carbon dioxide and hydrogen exhibit strong permeation competition when passing through the polymer membrane, and carbon dioxide significantly affects hydrogen separation efficiency. Under natural gas pressure of 4.0 MPa and hydrogen blending ratios of 5.0% to 20.0%, high-purity hydrogen with a purity of 99.999% (volume fraction) can be efficiently separated from hydrogen-enriched natural gas, achieving a total hydrogen recovery rate of 90% and a theoretical energy consumption of 0.5 kWh/m3 to 1.0 kWh/m3 (based on hydrogen).关键词：hydrogen-blended natural gas;hydrogen separation and purification;membrane separation;pressure swing adsorption2|0|0更新时间：2026-06-25 -
摘要：CO2 hydrate-based technology exhibits broad application potential for carbon capture and storage (CCS). However, its industrial deployment is still hindered by several key challenges, including sluggish hydrate nucleation and growth kinetics, insufficient stability, and high susceptibility to decomposition under fluctuating ambient temperature and pressure conditions. The promotion effect of nano-SiO2 on CO2 hydrate formation was investigated, as well as the underlying mechanism governing hydrate stability. Specifically, the nucleation induction time, formation rate and decomposition behavior of CO2 hydrate in both nano-SiO2 dispersions and pure water were characterized systematically. The results demonstrate that, with the addition of 0.5% (mass fraction) nano-SiO2 with particle size of 60 nm, the nucleation induction time of CO2 hydrate is significantly reduced from 36 min to 24 min, while the average formation rate increases from 0.198 mmol/min to 0.288 mmol/min, corresponding to a 45% enhancement. Furthermore, under ambient conditions (293.15 K, 101.325 kPa), the hydrate decomposition time is extended from 39 min to 90 min, confirming a remarkable improvement in hydrate stability. The reason is that nano-SiO2 reduces the nucleation energy barrier of CO2 hydrate through its high specific surface area and surface activity, which facilitates heterogeneous nucleation and reaction heat dissipation. Meanwhile, it can form a protective encapsulation layer on the hydrate surface to effectively retard heat transfer, thereby enhancing both the formation kinetics and stability of CO2 hydrate. The study can provide a valuable reference for the deployment of nanomaterial-enhanced hydrate technology in CCS applications.关键词：CO2 hydrate;nano-SiO2;formation rate;stability20|0|0更新时间：2026-06-25 -
摘要：Hydrate plugging is a major safety challenge in the development of deepwater oil and gas resources. Among them, the nucleation, agglomeration and instability of hydrates are the key processes in mitigating hydrate plugging. However, the effect of polyvinyl caprolactam (inhibitor) on the instability mechanism of natural gas hydrates has not yet been clearly elucidated. Molecular dynamics (MD) simulations and density functional theory (DFT) calculations were employed to investigate the instability process of natural gas hydrate aggregates under tensile and compressive loads in the presence of polyvinyl caprolactam. Key parameters within the aggregates, including instability stress, Young’s modulus, the number of cage structures, the number of water molecules and intermolecular interactions, were analyzed. The results indicate that the hydrate aggregates exhibit local unstable brittle fracture under tensile load, whereas under compressive load they display strain softening and overall unstable failure. The inhibitor significantly reduces the mechanical properties and structural stability of hydrate aggregates by enlarging the strength difference within the hydrogen bond network, generating repulsive interactions and exerting steric hindrance effects. Specifically, after adding the inhibitor, the tensile and compressive ultimate instability stresses of the hydrate aggregates decrease by approximately 44.17% and 29.62%, respectively, while their stiffness and resistance to external loads are also reduced. In addition, the inhibitor suppresses the ordered arrangement of water molecules, the formation of 51262-type cage structures and the recombination of hydrate cages, thereby making the aggregates more prone to structural deformation and instability failure under external load.关键词：natural gas hydrates;instability stress;inhibitor;molecular dynamics94|137|0更新时间：2026-06-25
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