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Despite extensive research on alkali resistance of denitrification (de-NO) catalysts, the synergistic poisoning mechanism of alkali and alkaline-earth metals on de-NO catalysts, particularly Mn-based catalysts, remains unresolved. This study investigates the co-poisoning effects of K and Ca on the de-NO activity of Mn-based quasi-MOF (Metal Organic Framework) catalysts, specifically TEOS&Mn-BTC (a catalyst previously designed by our team, TEOS and BTC represent tetraethyl orthosilicate and trimesic acid, respectively). We found that the coexistence of K and Ca elevates the d-band center, which improves the electron mobility ability of the catalyst, thus enhancing the electron transfer between Mn and O in the Si-O-Mn electron-metal-carrier coordination structure, which further promotes the occurrence of acid and redox circulations while strengthening the electron-metal-carrier interaction. Moreover, the increase in the d-band center enhances the charge transfer between the catalyst and the adsorbate, thereby further enhancing the adsorption of NH and NO. These findings elucidate the anti-poisoning mechanism of TEOS&Mn-BTC and provide theoretical insights for designing alkali/alkaline-earth-resistant de-NO catalysts.
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http://dx.doi.org/10.1016/j.jhazmat.2025.139714 | DOI Listing |
J Hazard Mater
August 2025
State Key Laboratory of Electrical Insulation and Power Equipment, School of Electrical Engineering, Xi'an Jiaotong University, Xi'an 710049, China. Electronic address:
Despite extensive research on alkali resistance of denitrification (de-NO) catalysts, the synergistic poisoning mechanism of alkali and alkaline-earth metals on de-NO catalysts, particularly Mn-based catalysts, remains unresolved. This study investigates the co-poisoning effects of K and Ca on the de-NO activity of Mn-based quasi-MOF (Metal Organic Framework) catalysts, specifically TEOS&Mn-BTC (a catalyst previously designed by our team, TEOS and BTC represent tetraethyl orthosilicate and trimesic acid, respectively). We found that the coexistence of K and Ca elevates the d-band center, which improves the electron mobility ability of the catalyst, thus enhancing the electron transfer between Mn and O in the Si-O-Mn electron-metal-carrier coordination structure, which further promotes the occurrence of acid and redox circulations while strengthening the electron-metal-carrier interaction.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
September 2025
MOE Key Laboratory of Pollution Processes and Environmental Criteria, Tianjin Key Laboratory of Environmental Remediation and Pollution Control, College of Environmental Science and Engineering, Nankai University, Tianjin, 300350, P.R. China.
Selective catalytic reduction of nitrogen oxides (NO) with NH (NH-SCR) poses considerable potential in the abatement of NO emissions. However, the efficient adsorption and speedy reaction of reactants following the specific mechanism in a favorable way is still a challenge for enhancing catalysis. Herein, we propose the strategy aimed at adjusting electronic properties of Ce-O-W acid-base pairs through constructing oxygen vacancies on Ce/WO, thereby fostering SCR activity.
View Article and Find Full Text PDFChem Sci
April 2025
New Energy Technologies Group, Department of Applied Physics, Aalto University School of Science FI-00076 Aalto Finland
Solid electrolyte membrane reactors (SEMRs) can be operated at high temperatures with distinct reaction kinetics, or at lower temperatures (300-500 °C) for industrially relevant energy applications (such as solid oxide fuel/electrolysis cells, direct carbon fuel cells, and metal-air batteries), chemical (such as alkane dehydrogenation, C-C coupling, and NH synthesis), environmental (De-NO , CO utilization, and separation), as well as their combined (one-step coupled CO/HO co-electrolysis and methanation reaction, power and chemical cogeneration) applications. SEMRs can efficiently integrate electrical, chemical, and thermal energy sectors, thereby circumventing thermodynamic constraints and production separation issues. They offer a promising way to achieve carbon neutrality and improve chemical manufacturing processes.
View Article and Find Full Text PDFJ Hazard Mater
January 2025
Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education of the People's Republic of China, School of Chemistry and Materials, Heilongjiang University, No.74 Xuefu Road, Harbin 150080, PR China. Electronic address:
The MnNbTiO (a = 0.6-0.9) catalysts for NH selective catalytic reduction denitration were prepared using the co-precipitation method.
View Article and Find Full Text PDFRSC Adv
November 2024
Department of Chemical System Engineering, School of Engineering, The University of Tokyo 7-3-1 Hongo Bunkyo-ku Tokyo 113-8656 Japan
Manganese octahedral molecular sieves with an α-MnO crystal structure (OMS-2) and their related materials have attracted significant attention for the selective catalytic reduction of NO using NH (NH-SCR) at low temperatures. Further lowering their operating temperature should be an effective method to develop an environmentally friendly de-NO system; however, their catalytic activity at low temperatures, especially below 100 °C, remains poor. This study describes a post-synthetic approach to develop Mn-based catalysts superior to those in the literature that operate at ultralow temperatures.
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