物理化学学报
物理化學學報
물이화학학보
ACTA PHYSICO-CHIMICA SINICA
2015年
2期
353-359
,共7页
张洁%张江浩%张长斌%贺泓
張潔%張江浩%張長斌%賀泓
장길%장강호%장장빈%하홍
MnO2催化剂%低温催化氧化%乙醇完全氧化%挥发性有机物%晶格氧
MnO2催化劑%低溫催化氧化%乙醇完全氧化%揮髮性有機物%晶格氧
MnO2최화제%저온최화양화%을순완전양화%휘발성유궤물%정격양
MnO2 catalyst%Low temperature catalytic oxidation%Ethanol complete oxidation%Volatile organic compound%Lattice oxygen
采用水热合成法制备了α-MnO2、β-MnO2、γ-MnO2和δ-MnO2催化剂,运用N2吸脱附实验、X射线衍射(XRD)、X射线光电子能谱(XPS)和H2程序升温还原(H2-TPR)等方法对催化剂进行了表征,并将催化剂用于催化完全氧化乙醇反应中,考察了不同晶型MnO2催化剂催化氧化乙醇活性的差异,探讨了催化剂晶型结构与催化氧化活性的关联.结果表明,不同晶型的MnO2催化剂催化氧化乙醇活性差异显著,活性顺序为α-MnO2>δ-MnO2>γ-MnO2>β-MnO2.系列表征结果显示,晶体结晶度和比表面积不是影响不同晶型MnO2催化剂活性的主要原因,α-MnO2催化剂具有的较高晶格氧浓度和较高的可还原性是其具有良好催化氧化乙醇活性的关键因素.
採用水熱閤成法製備瞭α-MnO2、β-MnO2、γ-MnO2和δ-MnO2催化劑,運用N2吸脫附實驗、X射線衍射(XRD)、X射線光電子能譜(XPS)和H2程序升溫還原(H2-TPR)等方法對催化劑進行瞭錶徵,併將催化劑用于催化完全氧化乙醇反應中,攷察瞭不同晶型MnO2催化劑催化氧化乙醇活性的差異,探討瞭催化劑晶型結構與催化氧化活性的關聯.結果錶明,不同晶型的MnO2催化劑催化氧化乙醇活性差異顯著,活性順序為α-MnO2>δ-MnO2>γ-MnO2>β-MnO2.繫列錶徵結果顯示,晶體結晶度和比錶麵積不是影響不同晶型MnO2催化劑活性的主要原因,α-MnO2催化劑具有的較高晶格氧濃度和較高的可還原性是其具有良好催化氧化乙醇活性的關鍵因素.
채용수열합성법제비료α-MnO2、β-MnO2、γ-MnO2화δ-MnO2최화제,운용N2흡탈부실험、X사선연사(XRD)、X사선광전자능보(XPS)화H2정서승온환원(H2-TPR)등방법대최화제진행료표정,병장최화제용우최화완전양화을순반응중,고찰료불동정형MnO2최화제최화양화을순활성적차이,탐토료최화제정형결구여최화양화활성적관련.결과표명,불동정형적MnO2최화제최화양화을순활성차이현저,활성순서위α-MnO2>δ-MnO2>γ-MnO2>β-MnO2.계렬표정결과현시,정체결정도화비표면적불시영향불동정형MnO2최화제활성적주요원인,α-MnO2최화제구유적교고정격양농도화교고적가환원성시기구유량호최화양화을순활성적관건인소.
α-MnO2,β-MnO2,γ-MnO2, andδ-MnO2 catalysts were synthesized by hydrothermal methods, and their catalytic performances towards the oxidation of ethanol were evaluated in detail. The as-synthesized MnO2 catalysts were characterized by N2 adsorption-desorption measurements, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and H2 temperature-programmed reduction (H2-TPR). Theα-MnO2 catalyst showed the best activity of the catalysts tested for the combustion of ethanol and the trend in the activity of different MnO2 catalysts towards the oxidation of ethanol was of the orderα-MnO2>δ-MnO2>γ-MnO2>β-MnO2. The effect of the crystal phase structure on the activity of the MnO2 catalysts was investigated. The XRD results showed that there were differences in the crystal inities of theα-,β-,γ-,δ-MnO2 catalysts, but these differences did not have a significant effect on their catalytic performances towards the oxidation of ethanol. The BET surface areas of theα-,β-,γ-,δ-MnO2 catalysts exhibited similar tendencies to their ethanol oxidation activities, although the results of standardization calculations showed that the surface area was not the main factor affecting their catalytical activities. The XPS results showed that the lattice oxygen concentration played an important role in defining the catalytic performance of the MnO2. The α-MnO2 catalyst showed the best reducibility of al of the MnO2 catalysts tested, as determined by H2-TPR. The excel ent performance ofα-MnO2 was attributed to its higher lattice oxygen concentration and reducibility, which were identified as the main factors affecting the activity of the MnO2 towards the complete oxidation of ethanol.