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Conventional packed-bed catalysts suffer from single-scale porosity, insufficient mechanical strength, and suboptimal mass transfer efficiency. Inspired by the fractal structure of the lung bronchi, a design and 3D printing method for gradient meta-structural catalysts is proposed by integrating synthesized LaFeNiO (LFN) perovskite with pseudo-boehmite, achieving ultralow pressure drop and high catalytic efficiency. Computational fluid dynamics and reaction simulations guide the design of uniform and gradient-structured catalysts with hierarchical woodpile channels (0.5-3 mm). Compared with homogeneous catalysts, the gradient design theoretically exhibits 1.5-fold and 1.1-fold increases in flow velocity and hydrogen production, respectively. Meta-structural catalysts are fabricated with gradient multi-peak pore distribution (9.32 nm, 103.75 nm) by regionally modulating unit cell sizes and LFN content (11-35%) combined with the dehydroxylation of pseudo-boehmite. 3D-printed perovskite catalysts demonstrate a 78.7-fold increase in specific surface area (102.26 m g) and compressive strength of 8.48 MPa. In dry reforming of methane (DRM) tests, it achieves 82.13% CH conversion, and 9.69 mmol g syngas yield, outperforming conventional powder-packed beds by 10% efficiency. This study achieves mass transfer and catalytic performance coupling by tuning gradient hierarchical pores and tailoring flow dynamics, offering a paradigm for robust, high-efficiency catalyst design across diverse applications.
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http://dx.doi.org/10.1002/adma.202508078 | DOI Listing |
Phys Chem Chem Phys
September 2025
Chemical Sciences, Faculty of Science, Universiti Brunei Darussalam, Jalan Tungku Link, Gadong, BE 1410, Brunei Darussalam.
The crossover of methanol from the anode to the cathode presents a significant challenge, adversely affecting the efficacy of direct methanol fuel cells (DMFCs) by poisoning the cathode catalyst. Here, LaBO (B = Mn, Fe, Co, and Ni) perovskite oxides synthesized by the sol-gel method, followed by calcination, are shown to represent a compelling solution to this challenge by effectively reducing the methanol crossover effect and concurrently improving the sluggish cathodic oxygen reduction reaction (ORR). X-ray diffraction, FTIR, and XPS analyses reveal the establishment of phase-pure LaMnO, LaFeO, LaCoO, and LaNiO, perovskite oxides.
View Article and Find Full Text PDFACS Appl Nano Mater
August 2025
Department of Chemistry, Bilkent University, Ankara 06800, Turkey.
Perovskites have significant potential to improve efficiency, reduce the costs of conventional oxidation catalysts, and contribute to cleaner and more sustainable energy solutions. However, numerous structural factors influencing their catalytic performance are still a subject to debate. In this study, simple perovskite nanoparticles in the form of LaCoO (LC) and LaMnO (LM), as well as LaCo Mn O (LCM)-mixed B-site perovskites with different B-site cations, were synthesized and their performances in CO oxidation and NO oxidation reactions were examined.
View Article and Find Full Text PDFInorg Chem
September 2025
School of Physics and Material Science, Nanchang University, Nanchang, Jiangxi 330031, P. R. China.
In this report, we demonstrate the first application of lead-free double perovskite microcrystals (CsAgBiBr MCs) in sustainable C-C coupling reactions. The CsAgBiBr MCs catalyst exhibits ultrahigh activity and selectivity in the α-alkylation of aldehyde and 2-bromoacetophenone, achieving a reaction rate of 2687.5 mmolgh, a turnover number (TON) value of 22854.
View Article and Find Full Text PDFJ Am Chem Soc
September 2025
Department of Chemistry, Tsinghua University, Beijing 100084, China.
The inherent trade-off between activity and stability in platinum single-atom catalysts (SACs) poses a significant challenge for catalytic oxidation reactions. High-coordination Pt sites have good stability, but their overoxidation often passivates activity. In contrast, metastable low-coordination Pt structures typically display high activity but are prone to oxidation and aggregation under harsh conditions.
View Article and Find Full Text PDFAdv Sci (Weinh)
August 2025
Wolfson Catalysis Centre, Department of Chemistry, University of Oxford, Oxford, OX1 3QR, UK.
Photocatalytic ammonia decomposition offers a sustainable route for hydrogen production, but its development is limited by low catalytic efficiency and poorly understood mechanisms. Here, a protonated layered perovskite, HPrNbO (HPNO), is reported as an efficient catalyst for ammonia decomposition under mild photo-thermal conditions. Upon exposure to NH at elevated temperatures, HPNO promotes the in situ formation and intercalation of hydrazine intermediates within its interlayer galleries, enabled by thermally generated oxygen vacancies and hydrogen bonding.
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