fau型和lta型沸石上歧化和配位对NO的高效吸附

IF 13.2 1区 工程技术 Q1 ENGINEERING, CHEMICAL Chemical Engineering Journal Pub Date : 2025-02-04 DOI:10.1016/j.cej.2025.160305
Kexin Xu, Li Wang, Xinghua Zhang, Xuehai Wang, Yimin Zhu
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引用次数: 0

摘要

沸石对NO的高效吸附不仅加速了催化NO浓缩成N2的过程,同时也揭示了低温低浓度去除NO的难点。本研究评价了12种商业沸石对NO的动态吸附-解吸行为,证明了13X和5A沸石具有高NO吸附能力和低再生温度的优良吸附剂。基于n2 -物理吸附、NH3-TPD、CO2-TPD、在线质谱和原位漂移等广泛表征,深入研究和讨论了NO吸附-解吸行为以及气体和表面物质的孔隙结构-性能关系、酸性-性能关系和碱性-性能关系。NO直接配位到强Lewis酸位点和强碱位点(即强Lewis酸碱对)上,分别形成NOδ+和NOδ-两种配位键。NO也直接歧化成N2O和NO2,然后NO2就地转化为硝酸盐。因此,确定了13X和5A沸石对NO高效吸附的配位和歧化机制,补充了目前沸石对NO吸附的认识,并为增强强Lewis酸碱对沸石对NO的吸附提供了新的策略。
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Disproportionation and coordination driven high-efficient NO adsorption on FAU-and LTA-type zeolites
High efficient NO adsorption on zeolites not only accelerates catalytic NO to N2 by concentrating, but also figures out the difficulty of removing NO with low temperature and low concentration. This study evaluates the dynamic NO adsorption–desorption behaviors on 12 commercial zeolites, demonstrating 13X and 5A zeolites as excellent adsorbents with high NO adsorption capacity and low regeneration temperature. Based on extensive characterizations including N2-physisorption, NH3-TPD, CO2-TPD, on-line MS and in-situ DRIFTS, the pore structure-performance relationship, acidity-performance relationship and basicity-performance relationship have been thoroughly investigated and discussed upon NO adsorption–desorption behaviors, together with the gaseous and surface species. NO directly coordinates to the strong Lewis acid sites and strong base sites (i.e., strong Lewis acid-base pairs), leading to coordinately bonded NOδ+ and NOδ- species, respectively. Besides, NO also directly disproportionates to N2O and NO2, followed by in-situ conversion of NO2 into nitrate species. Thus, the coordination and disproportionation mechanisms have been identified for high-efficient NO adsorption on 13X and 5A zeolites, which supplements the current understandings of NO adsorption on zeolites and provides a new strategy to strengthen NO adsorption on zeolites with strong Lewis acid-base pairs.
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来源期刊
Chemical Engineering Journal
Chemical Engineering Journal 工程技术-工程:化工
CiteScore
21.70
自引率
9.30%
发文量
6781
审稿时长
2.4 months
期刊介绍: The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.
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