基于X射线光电子能谱(XPS)谱图信息研究焙烧温度对Mn基脱硝催化剂性能影响的机理  

Mechanism Study of the Influence of Calcination Temperature on Mn-based SCR De-NO_(x) Catalyst Activity Based on XPS Spectra Information

作　　者：陈静允 冯波 周佳丽 蒋复国 马琳鸽 CHEN Jingyun;FENG Bo;ZHOU Jiali;JIANG Fuguo;MA Lin'ge(National Institute of Clean-and-Low-Carbon Energy,Beijing 102209,China)

机构地区：[1]北京低碳清洁能源研究院,北京102209

出　　处：《中国无机分析化学》2025年第1期143-149,共7页Chinese Journal of Inorganic Analytical Chemistry

基　　金：国家重点研发计划项目(2019YFC1907500)。

摘　　要：Mn基脱硝催化剂中Mn的氧化态对其性能至关重要,但在利用X射线光电子能谱(XPS)分析Mn氧化物类型时,通常把Mn 2p3/2峰按照对称单峰进行分峰拟合,忽略了峰形不对称、多重分裂及振激卫星峰产生的峰形影响,为分析结果带来了一定的不确定性。基于Mn氧化态和性能的关系,综合利用XPS谱峰信息包括Mn 2p谱峰峰形对比、Mn 3s谱峰劈裂间距、催化剂表面吸附氧及所含元素的含量变化、Mn-Fe-Nb三元素的峰间距等,再结合XRD结果,确定了Mn-Fe-Nb/TiO_(2)脱硝催化剂在不同焙烧温度时Mn氧化物的类型,并解释了焙烧温度影响脱硝性能的机理:Mn氧化物类型、表面吸附氧量、Mn表面暴露量及元素间的相互作用均对催化剂的性能产生影响。通过对XPS谱图信息的综合利用,弥补了分峰拟合的不足,以期为更有效地利用XPS分析技术研究Mn基脱硝催化剂提供方法、为催化剂活性预测和配方优化提供更可靠的数据支撑。The oxidation state of manganese(Mn)in Mn-based denitrification(De-NO_(x))catalysts plays a crucial role in determining their activity.However,conventional X-ray photoelectron spectroscopy(XPS)analysis often over simplifies the fitting of the Mn 2p3/2 peak by assuming a symmetrical single peak,thereby neglecting the effects of peak asymmetries,multiple splitting and shake-up of satellite peaks,which introducing uncertainties into the analysis results.In this study,the XPS spectra information was used comprehensively,including the comparion of the peak-to-peak shape of the Mn 2p spectra,the Mn 3s spectra peak splitting spacing,the change of adsorbed oxygen and the content of elements on the catalyst surface,and peak intervals of Mn-Fe-Nb elements.Combined with the XRD phase analysis results,the different oxidation states and the mechanism of the influence of calcination temperature on De-NO_(x) catalyst activity were determined,of which included Mn oxides species,surface adsorbed oxygen,surface exposure of Mn element and interaction between elements.Through the comprehensive leveraging of XPS spectra information,this paper makes up for the deficiency of single use of XPS spectral peak fitting,and provides methods for more effective use of XPS analysis technology and more reliable data support for catalyst activity prediction and formulation optimization in the research of Mn-based De-NO_(x) catalysts.

关 键 词：X射线光电子能谱 Mn基脱硝催化剂 Mn氧化态 脱硝性能 

分 类 号：O652.2[理学—分析化学]