Co-based catalysts have shown promising application prospects in propane dehydrogenation (PDH) due to their excellent C-H bond activation ability and environmental friendliness. However, issues such as unclear active sites and insufficient stability during the reaction process limit the application. In this work, a Co2+ embedding strategy was proposed to suppress carbon deposition, thereby achieving high propylene selectivity and long-term stability. Utilizing the "memory effect" of ammonium aluminum carbonate hydroxide (AACH), cobalt species are embedded into the lattice during the crystal reconstruction of AACH, successfully achieving a Co2+-embedded Co/Al-0.1 catalyst. By systematically adjusting the Co/Al molar ratio (0.05-0.6), rational regulation of Co2+ content is achieved. The Co/Al-0.1 with stably embedded Co2+ maintains propylene selectivity of above 90%, with a coking rate of 1.32 h-1, one third that of Co/Al2O3-IMP prepared by impregnation. Correspondingly, Co/ Al-0.1 exhibits a high long-term stability with a deactivation rate constant kd of 0.0075 h-1, less than one fifth that of Co/Al2O3-IMP (kd = 0.0406 h-1). In situ propylene adsorption-desorption infrared spectroscopy and theoretical calculations indicate that propylene easily desorbed from the stable embedded Co2+, thereby inhibiting deep dehydrogenation of propylene and C-C bond cleavage, which enhances propylene selectivity and anti-coking performance.

Terpenoids are widely distributed and contain suitable polycyclic structures to easily synthesize highperformance fuels. However, synthesizing and testing the performance of each fuel compound result in a huge workload, thus necessitating a rational design of molecules. In this work, we designed abundant fuel molecules based on alkylation and cyclization derivatives of terpenoid (isoprene, myrcene, farnesene) and calculated their properties through group contribution, quantum calculation and molecular dynamics calculation. Random forest model was used to identify the key variables including the number of C and H atoms, H/C ratio and the standard molar enthalpy of formation. The results show that the boiling and flash points, critical pressure and specific impulse have quadratic function relationships respectively with the C atoms number, the H atoms number and the standard molar enthalpy of formation, while the fuel density is linearly correlated with H/C ratio. Residual analysis is applied to cyclization effect analysis, revealing that three-and four-membered rings significantly increase flash point, density and specific impulse. Potential biofuel compounds are selected based on the RP-3 standard and Z-score standardization, in which myrcene-derived fuels show the best performance, followed by farnesene-derived and isoprene-derived fuels. A tricyclic cyclopropane myrcene-derived fuel compound has been selected as potential biofuel, which possess a high density (1.034 g & centerdot;cm-3), low freezing point (219.05 K) and high heat value (43.8 kJ & centerdot;g-1 ). These findings are beneficial for future biofuel design and synthesis. (c) 2025 The Chemical Industry and Engineering Society of China, and Chemical Industry Press Co., Ltd. All rights are reserved, including those for text and data mining, AI training, and similar technologies.

Structured catalysts take advantage of high diffusion efficiency and low heat transfer resistance, effectively boosting reactions in non‐adiabatic gas–solid processes. However, traditional coating catalysts face problems of weak bond strength. Nanosized zeolites with rich hydroxyl as crystal seeds could effectively improve the binding strength of zeolite coatings, but their poor crystallinity resulted in low growth content. Here, we designed large‐size hollow zeolites and anatase as seeds to prepare metal@Silicalite‐1 structured catalysts. Hollow zeolites provided abundant nucleation sites and increased the growth content of zeolite by 1.8 times. Meanwhile, the abundant Si‐OH and the enriched surface Ti‐OH significantly strengthened the adhesion stability of the coatings. In the propane dehydrogenation reaction, the optimized PtZn@S‐1‐10HT exhibited a high specific activity of 14.1 mol C3H6 mol Pt −1 s −1 with propylene selectivity up to 96.4% at 600°C. This strategy breaks the inherent contradiction between high loading and strong binding ability of coating catalysts, which broadens the avenues for industrial applications.

The practical application of dry reforming of methane (DRM) is hindered by rapid carbon deposition on conventional Ni catalysts. Here, we report a highly coking-resistant Ni catalyst derived from A-site-substituted La1xSrxNiO3 perovskites. At an optimal Sr content (x = 0.2), the reduced catalyst features uniformly dispersed SrO clusters anchored on La2O3, creating a dual-support interface that induces a more electron-deficient surface Ni environment. Under DRM conditions at 800 degrees C with a CH4:CO2:N2 feed ratio of 1:1:1 and a GHSV of 36,000 mL & sdot;g & sdot;cat- 1 & sdot;h- 1, the catalyst derived from La0.8Sr0.2NiO3 delivers 91.7% CO2 and 89.4% CH4 conversions and exhibits stable performance over 50 h with minimal carbon accumulation. In contrast, the unsubstituted LaNiO3derived catalyst showed measurable deactivation within 15 h, with CO2 conversion decreasing from 90.1% to 87.8% and CH4 conversion decreasing from 88.3% to 86.0%. Mechanistic studies reveal that the SrO clusters function as CO2-capture promoters, dynamically cycling between SrO and SrCO3. This promotes the reversible La2O3/La2O2CO3 conversion via a tandem exchange step, establishing a carbonate-mediated oxygen-transfer pathway that rapidly oxidizes surface *C species and suppresses carbon growth. This study thus presents a perovskite-derived dual-support system whose dynamic oxygen cycle, driven by CO2 interaction between SrO and La2O3, provides a novel route to carbon-resistant DRM catalysis.

The development of highly efficient and durable acidic oxygen evolution reaction (OER) catalysts plays a crucial role in advancing proton exchange membrane water electrolysis (PEMWE). Iridium oxide (IrO2) is currently the most typical acidic OER catalyst, but its practical application is constrained by its limited intrinsic activity, sluggish charge-transfer dynamics, and insufficient structural stability. Despite attempts to modify IrO2 by introducing heteroatoms such as chromium, fundamental understanding remains insufficient. In this work, we report a chromium-incorporated IrO2 catalyst prepared via an improved molten-salt method. Cr modifies the local crystal structure of IrO2 and acts as an electronic modulator, leading to shortened Ir-O bond lengths. Density functional theory (DFT) calculations reveal that Cr, acting as an electron donor, induces an upshift of the Ir d-band center, thereby enhancing the adsorption energies of reaction intermediates. Benefiting from these effects, the optimized catalyst achieves a low overpotential (eta 10= 255 +/- 3 mV) and maintains an industrialstandard current density of 2 A cm-2 at 1.77 V for approximately 420 h in PEMWE tests.

Abstract Pd‐based catalysts often suffer from low H 2 O 2 selectivity and productivity due to O‐O bond cleavage. Herein, we address this challenge by constructing a well‐defined Pd‐SnO 2 interface on carbon nanotubes through a precisely controlled N 2 ‐thermal treatment. This key step ensures the reduction of Pd oxides while maintaining SnO 2 in an oxidized state, inducing moderate electron transfer from SnO 2 to Pd. The optimized Pd‐SnO 2 /CNTs catalyst exhibits outstanding H 2 O 2 productivity of 38,925 mol·kg Pd −1 ·h −1 , with 47.1% H 2 conversion and 52.7% H 2 O 2 selectivity, alongside excellent stability over five cycles. DFT simulations and experimental analysis reveal the Pd‐SnO 2 interface induces a moderate downshift in the d ‐band center of Pd, weakening the adsorption of reaction species on Pd 0 sites. A synergistic dual‐site mechanism occurs via H 2 dissociation and spilled‐over H* species on Pd 0 , while adjacent SnO 2 domains act as active sites for the sequential hydrogenation of activated O 2 , leading to the selective formation of H 2 O 2 .

ZSM-48 zeolite, featuring a one-dimensional ten-membered-ring channel system, exhibits excellent support properties for hydroisomerization of long-chain alkanes. However, the intrinsically unbalanced distribution of acid sites significantly increases the probability of undesired cracking side reactions, making it challenging to simultaneously achieve high isomer selectivity at high conversion level. In this work, an in-situ acid-regulated crystallization strategy is developed to markedly enhance the hydroisomerization performance of ZSM-48. A series of ZSM-48-X samples are synthesized under different acid-regulated conditions, of which the physicochemical properties, particularly silanol nest concentration and acid characteristics, exhibit a strong dependence on the initial synthesis pH and type of anion in acid. The resulting ZSM-48-X zeolites with increased silanol nest density and reduced strong Br & Oslash;nsted acid sites exhibit substantially improved catalytic performance, achieving a general increase in isomer yield from 77.7% to above 85%. Symbolic regression of catalyst characteristics and reaction data by sparse identification of selected operators (SISSO) demonstrates the primary roles of silanol nests and strong Br & Oslash;nsted acid sites on facilitating isomerization reaction in a nonlinear manner. In-situ DRIFTS experiments on the catalysts further demonstrate that abundant silanol nests and optimized density of Br & Oslash;nsted acid sites in ZSM-48 weaken the adsorption strength of long-chain alkanes and promote the desorption of isomerized products, providing molecular-level mechanism insights into the promotional function of acid-regulated ZSM-48 for hydroisomerization determined by SISSO. This in-situ acid-regulated crystallization strategy broadens the scope of conventional zeolite synthesis and acidity modulation, offering a simple and efficient approach for tailoring silanol nests and providing valuable guidance for rational design of high-performance zeolite catalysts.

Oxidation of methylene compounds remains a critical challenge due to the difficult activation of C-H bond. Herein, Ce-Al composite oxide was prepared and employed for oxidation of 2-alkyl-anthrone and anthracene to corresponding anthraquinone (AQ) which is used widely in the H2O2 production by the anthraquinone process and fine chemical industries, with air at mild conditions. Characterization results show that incorporation of Ce, existing partially in CeAlO3 phase, results in the generation of oxygen vacancies and enhancement of reducibility. The optimal Ce-Al composite oxide (10%CeAl) exhibits superior performance in oxidation of 2-alkyl-anthrone and anthracene to AQ. The conversion of 100% could be achieved for 2-alkyl-anthrone to AQ at reaction time of 8 h and for 2-alkyl-anthracene to AQ at 15 h over 10%CeAl, with 100% selectivity. In-situ electron paramagnetic resonance measurements and DFT calculations reveal that the Ce-O-Al structure in CeAlO3 phase promotes the formation of carbon-centered radical R center dot through altering the C-H cleavage mechanism from hydrogen atom transfer to proton-coupled electron transfer (PCET), and superoxide anion radicals (O2 center dot-) formed on oxygen vacancies promote oxidation of R center dot.

The low-temperature deep hydrogenation of polycyclic aromatic hydrocarbons (PAHs) remains a challenge for producing high-value chemicals or high-density fuels. Herein, Ru/anatase TiO2 (101) catalysts were prepared using an electrostatic adsorption method combined with different reduction treatments (NaBH4, N2H4& centerdot;H2O, and H2/Ar as reductants). The metal-support interaction (SMI) was tailored, and uniformly dispersed Ru nanoparticles (size <2 nm) were obtained for all catalysts. For the Ru/TiO2 catalyst reduced by NaBH4 (Ru/TiO2-NaBH4), the overencapsulation effect of TiO2-x overlayer induced by SMSI is eliminated using NaBH4 reduction to expose more metal sites. The moderated metal-support interaction favors the generation of more electron-deficient Ru species (Rudelta+). These active Rudelta+ species exhibit excellent ability to promote H2 dissociation and enhance the isomerization rate of saturated aromatic compounds. Due to the enhanced adsorption of aromatic molecules, Ru/TiO2-NaBH4 exhibits superior hydrogenation performance and good stability. Under mild conditions (60 degrees C, 4 MPa), Ru/TiO2-NaBH4 achieves 87.9% conversion of acenaphthene (Ace) within 1 h and then up to 100% conversion with a 94.4% cis-selectivity of PHA within 3 h, with a high turnover frequency (TOF) of 2797.7 h-1, and the catalyst could be reused three times without significant loss of activity. This study provides new insights into the rational design of highly efficient PAHs deep hydrogenation catalysts under low-temperature conditions.

Shrinkage and porosity defects critically impair the quality of 12Cr2Mo1V alloy ingots used in high-temperature, high-pressure applications. This study employs finite-element simulations to systematically investigate the effects of pouring temperature, mold preheating temperature, and pouring rate on the filling and solidification behavior of this alloy during low-speed metal mold gravity casting. A numerical model incorporating the Niyama criterion was established and validated against metallographic observations to predict defect formation. The results demonstrate that increasing the pouring temperature from 1535 to 1655 °C causes porosity volume to first decrease and then increase, while defect locations progressively shift away from the riser. Elevating the mold preheating temperature from 150 to 350 °C prolongs solidification time by up to 22

Pd-based catalysts often suffer from low H2O2 selectivity and productivity due to O-O bond cleavage. Herein, we address this challenge by constructing a well-defined Pd-SnO2 interface on carbon nanotubes through a precisely controlled N-2-thermal treatment. This key step ensures the reduction of Pd oxides while maintaining SnO2 in an oxidized state, inducing moderate electron transfer from SnO2 to Pd. The optimized Pd-SnO2/CNTs catalyst exhibits outstanding H2O2 productivity of 38,925 mol & centerdot;kgPd (-1)& centerdot;h(-1), with 47.1% H2 conversion and 52.7% H2O2 selectivity, alongside excellent stability over five cycles. DFT simulations and experimental analysis reveal the Pd-SnO2 interface induces a moderate downshift in the d-band center of Pd, weakening the adsorption of reaction species on Pd0 sites. A synergistic dual-site mechanism occurs via H-2 dissociation and spilled-over H* species on Pd0, while adjacent SnO(2 )domains act as active sites for the sequential hydrogenation of activated O-2, leading to the selective formation of H2O2 .

Constructing a robust solid electrolyte interphase (SEI) is critical for batteries. Conventional SEI is formed and repaired through cyclic electrochemical processes that consume active lithium from the cathode, leading to Coulombic losses and capacity decay. Here, we demonstrate an electron-decoupled chemical approach that builds a robust pre-fluorinated SEI through the catalytic reaction of parasitic LiPF6 hydrolysis at the interface between electrolyte and a designed nanoscale Cu/SiOx catalytic layer (CL) on micro-sized silicon. The formed LiF-rich SEI is further fortified by the electrocatalytic conversion of the preceding HF byproducts. The resulting anode exhibits a 7% improved initial Coulombic efficiency of 89.3%, remarkable stability over 1600 cycles, and superior rate performance (2670 mAh g-1 at 5 A g-1). This strategy of catalytic pre-fluorination offers a powerful pathway to stabilize dynamic electrode interfaces.

Electrocatalytic semi-hydrogenation (ECSH) of alkynes using water as a hydrogen source is expected to provide a revolutionary solution for upgrading the traditional hydrogenation process. An ingenious design of the electrocatalyst is required to break the tradeoff between activity, selectivity, and Faradaic efficiency (FE). Herein, a non-noble metal catalytic system, containing well-defined Ni-Fe atom pairs and Ni clusters on N-doped carbon, is constructed by a two-step annealing method for energy-efficient ECSH of alkynols. The optimized catalyst with collaborative Ni-Fe pairs and Ni clusters effectively suppresses hydrogen evolution reaction (HER) competition and C═C over-hydrogenation, and simultaneously accomplishes three critical objectives at ultra-low applied potential (-0.125 V vs. RHE): nearly 100% conversion, 100% selectivity, and high FE of up to 98% (for 2 h). Joint experiments and theoretical calculations demonstrate that adjacent Ni-Fe pairs electronically tune the neighboring Ni clusters, and the resulting synergy enables complementary functions of the two sites: Ni-Fe pairs accelerate H2O dissociation, whereas Ni clusters regulate alkynol/alkenol adsorption for selective semi-hydrogenation. The excellent stability, wide substrate universality, ultrahigh TOF, and low energy consumption of this low-cost catalyst distinguish it from noble-metal-based systems with poor FE, offering a promising strategy for designing efficient polymorphic component catalysts.

The electrocatalytic reduction of CO2 (CO2RR) to methane (CH4) using renewable electricity represents a pivotal technology for closing the anthropogenic carbon cycle. However, achieving high CH4 Faradaic efficiency at industrially relevant current density remains challenging. This is primarily due to the complex multiple adsorption, activation, and reaction steps for CH4 production, in which each process needs to occur efficiently at its matching catalytic active sites, so the kinetic bottlenecks exceed the capacity of single or dual-site catalysts. To address this, we engineered a Cu/Al-based multi-site heterogeneous electrocatalyst featuring atomically dispersed Cu clusters (1.5 wt.%) on a gamma-Al2O3 matrix. Experimental and theoretical studies reveal that Cu and gamma-Al2O3 sites predominantly serve as CO2 (forming *CO) and H2O molecule (yielding *H) activation centers, respectively, whereas Cu/gamma-Al2O3 interfacial sites primarily accelerate the *CO and *H coupling to form rate-determining step intermediates (*CHO). The optimized Cu1.5 wt.%/gamma-Al2O3 multi-site catalyst exhibited a high CH4 Faradaic efficiency of 72% at the current density of 500 mA cm-2, outperforming the reported Cu-based single-site and dual-site catalysts. This study establishes combinatorial site engineering as a paradigm for overcoming scaling relations in multi-step CO2 hydrogenation, with broad applicability in catalyst design.

Dry reforming of methane (DRM) is plagued by rapid catalyst deactivation, primarily due to carbon deposition exacerbated by exposed Al2O3 surfaces in conventional mixed-phase supports. Herein, we construct a well-defined Pt/TiO2-Al2O3 interface by depositing an ultra-thin anatase TiO2 overlayer onto Al2O3 via an in situ growth strategy to eliminate detrimental Al2O3 exposure. Characterization coupled with DFT calculations reveal that the Al2O3 support induces lattice contraction and electron enrichment of the ultra-thin TiO2 layer through interfacial stress and charge transfer. This concurrently activates lattice oxygen (Ti-O) and optimizes Pt charge density, endowing the catalyst with balanced CH4 activation and a heightened CH* → C* barrier. The resulting Pt/TiO2-Al2O3 catalyst achieves exceptional durability, maintaining 91% CH4 conversion at 800 °C for 100 h with negligible carbon deposition, outperforming Pt/Al2O3 and Pt/TiO2 benchmarks. This work demonstrates that engineering a continuous ultra-thin TiO2 overlayer on Al2O3 is a superior alternative to mixed-phase supports, providing a generalizable blueprint for coke-resistant catalyst design via precise interface control.

Seawater batteries (SWBs) that rely on the dissolved oxygen reduction reaction (ORR) on the cathode are a crucial choice for the long-term power supply of underwater equipment. However, chloride ions (Cl-) poisoning and the lean-oxygen condition in seawater severely suppress the ORR kinetics, leading to rapid activity decay and poor durability of catalysts. Herein, we present a Cl--resilient ORR catalyst of CoSn alloy anchored on nitrogen-doped carbon substrate (CoSn@NC). The introduction of p-block Sn atoms effectively tunes the d-band center of Co, weakening the adsorption of competitive Cl- while simultaneously optimizing the binding strength with oxygenated intermediates. This dual regulation mitigates chloride-induced surface poisoning even in a lean-oxygen environment. The obtained CoSn@NC exhibits superior ORR activity and durability in natural seawater, delivering the higher half-wave potential of 0.72 V and enhanced kinetic current density compared with commercial Pt/C. Furthermore, a SWB prototype employing CoSn@NC as cathode demonstrates excellent rate capability and a stable 1.49 V operating voltage sustained for over 130 h. Promisingly, we demonstrate stable SWB operation beneath the sea-ice layer in the Bohai Bay, which confirms that CoSn@NC can sustain ORR under the Cl- corrosion and low temperature, thereby giving guidance for the design of practical SWBs in a harsh marine environment.

Efficient synthesis of aviation fuels from biomass-derived compounds is highly desirable. Herein, the selective one-pot production of high-density fuel from lignocellulose-derived methyl benzaldehyde and cyclopentanone was developed by combining the aldol condensation and subsequent hydrodeoxygenation (HDO) over the cocatalyst of efficient titanate nanotubes and Ru/Al2O3. The PTNT-10M-0.5 nanotubes with one-dimensional multilayered walls and large surface areas were fabricated by controlling the NaOH concentration and HNO3 post-treatment. The nanotube surface was enriched with Br & Oslash;nsted acid sites and exposed to stronger acidic active sites in the inner layer. The medium-strong Br & Oslash;nsted acid sites were the active sites and very crucial for activating the C=O/C-O bonds, making the PTNT-10M-0.5 catalyst highly active in the aldol condensation and HDO process. The possible reaction mechanisms were also proposed that the medium-strong Br & Oslash;nsted acid sites localized on the inner surface of PTNT-10M-0.5 actively mediate the catalytic activation of the aldol condensation between methyl benzaldehyde and cyclopentanone. The synergistic effect of PTNT-10M-0.5 and Ru/Al2O3 co-catalyst promoted the selective preparation of high-density tricyclic alkanes (>= 80.6 %) in one pot under mild conditions. This work provides a simple and effective route for synthesizing high-density aviation fuels from lignocellulose platform compounds.

The electrocatalytic reduction of CO 2 (CO 2 RR) to methane (CH 4 ) using renewable electricity represents a pivotal technology for closing the anthropogenic carbon cycle. However, achieving high CH 4 Faradaic efficiency at industrially relevant current density remains challenging. This is primarily due to the complex multiple adsorption, activation, and reaction steps for CH 4 production, in which each process needs to occur efficiently at its matching catalytic active sites, so the kinetic bottlenecks exceed the capacity of single or dual‐site catalysts. To address this, we engineered a Cu/Al‐based multi‐site heterogeneous electrocatalyst featuring atomically dispersed Cu clusters (1.5 wt.%) on a γ‐Al 2 O 3 matrix. Experimental and theoretical studies reveal that Cu and γ‐Al 2 O 3 sites predominantly serve as CO 2 (forming *CO) and H 2 O molecule (yielding *H) activation centers, respectively, whereas Cu/γ‐Al 2 O 3 interfacial sites primarily accelerate the *CO and *H coupling to form rate‐determining step intermediates (*CHO). The optimized Cu 1.5 wt.% /γ‐Al 2 O 3 multi‐site catalyst exhibited a high CH 4 Faradaic efficiency of 72% at the current density of 500 mA cm −2 , outperforming the reported Cu‐based single‐site and dual‐site catalysts. This study establishes combinatorial site engineering as a paradigm for overcoming scaling relations in multi‐step CO 2 hydrogenation, with broad applicability in catalyst design.

Herein, a series of Ni/ZrO2 catalysts with tunable ZrO2 crystal phases were synthesized by controlling the calcination temperature of Ni/UiO-66(Zr). Ni/ZrO2-500 (t-ZrO2) exhibited higher activity than Ni/ZrO2-700 (m-ZrO2) in the photothermal Sabatier reaction, which was mainly attributed to a larger concentration of oxygen vacancies on the t-ZrO2 surface.