低浓度甲烷在钙钛矿/BN-La上的高效燃烧:增强的催化性能和基本动力学分析

IF 4.6 2区 工程技术 Q2 ENGINEERING, CHEMICAL
Qiang Ni , Aikun Tang , Lu Xiao , Tao Cai , Leiqi Yang
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引用次数: 0

摘要

催化燃烧是从废气中去除低浓度甲烷的一种有效方法,其关键挑战是开发高效的催化剂。本研究以氮化硼为高导热载体,La为甲烷高效燃烧添加剂,开发了一种复合粉末钙钛矿MFC/BN。该催化剂可在455.7℃条件下实现甲烷完全燃烧,在800℃条件下高效运行25 h以上(甲烷转化率97%)。结构和化学表征(XRD, BET, SEM和XPS)表明,比表面积增加(28.8 m2/g), Mn4+含量增加(46.31%)。BN载体优良的导热性改善了传热,同时减少了催化剂的老化和烧结,与MFC的相互作用减小了钙钛矿晶粒尺寸,增加了比表面积。La可以诱导表面形成更多的Mn4+、Fe3+和Olat。通过动力学分析,得到了反应的指前因子(1.42 × 109 mol·g−1·s−1·kPa−1)和反应活化能(73.6 kJ/mol)的幂函数表达式,明确了反应物与催化剂表面的关系。机理表明甲烷脱氢和氧化是控制速率的步骤,BN和La促进CH4脱氢生成CH3、CH2和CHO中间体。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Efficient combustion of low concentration methane over perovskite/BN-La: Enhanced catalytic performance and fundamental kinetic analysis

Efficient combustion of low concentration methane over perovskite/BN-La: Enhanced catalytic performance and fundamental kinetic analysis
Catalytic combustion is an efficient method for removing low concentration methane from exhaust gases, with the key challenge being the development of highly effective catalysts. This study develops a composite powder perovskite MFC/BN using BN as a high thermal conductivity carrier and La as an additive for efficient methane combustion. This catalyst can achieve complete methane combustion at 455.7 °C, and run efficiently for over 25 h at 800 °C (methane conversion rate > 97 %). The structural and chemical characterizations (XRD, BET, SEM, and XPS) reveal an increased specific surface area (28.8 m2/g) and Mn4+ species (46.31 %). The excellent thermal conductivity of BN carrier improves heat transfer while reducing catalyst aging and sintering, and its interaction with MFC decreases perovskite grain size and increases the specific surface area. La can induce the formation of more Mn4+, Fe3+ and Olat species on the surface. Then, kinetic analysis demonstrates the pre-exponential factor (1.42 × 109 mol·g−1·s−1·kPa−1) and reaction activation energy (73.6 kJ/mol) in the reaction with a power function, and clarifies the relationship between the reactant and the catalyst surface. The mechanism shows that methane dehydrogenation and oxidation are rate-controlling steps, with BN and La facilitating CH4 dehydrogenation to form CH3, CH2, and CHO intermediates.
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来源期刊
Powder Technology
Powder Technology 工程技术-工程:化工
CiteScore
9.90
自引率
15.40%
发文量
1047
审稿时长
46 days
期刊介绍: Powder Technology is an International Journal on the Science and Technology of Wet and Dry Particulate Systems. Powder Technology publishes papers on all aspects of the formation of particles and their characterisation and on the study of systems containing particulate solids. No limitation is imposed on the size of the particles, which may range from nanometre scale, as in pigments or aerosols, to that of mined or quarried materials. The following list of topics is not intended to be comprehensive, but rather to indicate typical subjects which fall within the scope of the journal's interests: Formation and synthesis of particles by precipitation and other methods. Modification of particles by agglomeration, coating, comminution and attrition. Characterisation of the size, shape, surface area, pore structure and strength of particles and agglomerates (including the origins and effects of inter particle forces). Packing, failure, flow and permeability of assemblies of particles. Particle-particle interactions and suspension rheology. Handling and processing operations such as slurry flow, fluidization, pneumatic conveying. Interactions between particles and their environment, including delivery of particulate products to the body. Applications of particle technology in production of pharmaceuticals, chemicals, foods, pigments, structural, and functional materials and in environmental and energy related matters. For materials-oriented contributions we are looking for articles revealing the effect of particle/powder characteristics (size, morphology and composition, in that order) on material performance or functionality and, ideally, comparison to any industrial standard.
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