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Facile Synthesis of Highly Efficient Amorphous Mn‐MIL‐100 Catalysts: Formation Mechanism and Structure Changes during Application in CO Oxidation
Chemistry - A European Journal ( IF 3.9 ) Pub Date : 2018-05-30 , DOI: 10.1002/chem.201800773 Xiaodong Zhang 1 , Hongxin Li 1 , Xutian Lv 1 , Jingcheng Xu 2 , Yuxin Wang 3 , Chi He 4 , Ning Liu 1 , Yiqiong Yang 1 , Yin Wang 1
Chemistry - A European Journal ( IF 3.9 ) Pub Date : 2018-05-30 , DOI: 10.1002/chem.201800773 Xiaodong Zhang 1 , Hongxin Li 1 , Xutian Lv 1 , Jingcheng Xu 2 , Yuxin Wang 3 , Chi He 4 , Ning Liu 1 , Yiqiong Yang 1 , Yin Wang 1
Affiliation
A comprehensive study was carried out on amorphous metal‐organic frameworks Mn‐MIL‐100 as efficient catalysts for CO oxidation. This study focused on explaining the crystalline–amorphous–crystalline transformations during thermolysis of Mn‐MIL‐100 and studying the structure changes during the CO oxidation reaction. A possible formation mechanism of amorphous Mn‐MIL‐100 was proposed. Amorphous Mn‐MIL‐100 obtained by calcination at 250 °C (a‐Mn‐250) showed a smaller specific surface area (4 m2 g−1) but high catalytic activity. Furthermore, the structure of amorphous Mn‐MIL‐100 was labile during the reaction. When a‐Mn‐250 was treated with reaction atmosphere at high temperature (giving used‐a‐Mn‐250‐S), the amorphous catalysts transformed into Mn2O3. Meanwhile, the BET surface area (164 m2 g−1) and catalytic performance both sharply increased. In addition, used‐a‐Mn‐250‐S catalyst transformed from Mn2O3 into Mn3O4, and this resulted in a slight decrease of catalytic activity in the presence of 1 vol % water vapor in the feed stream. A schematic mechanism of the structure changes during the reaction process was proposed. The success of the synthesis relies on the increase in BET surface area by using CO as retreatment atmosphere, and the enhanced catalytic activity was attributed to the unique structure, a large quantity of surface active oxygen species, oxygen vacancies, and good low‐temperature reduction behavior.
中文翻译:
高效无定形Mn-MIL-100高效催化剂的合成:CO氧化过程中的形成机理和结构变化
对无定形金属-有机骨架Mn-MIL-100作为CO氧化的有效催化剂进行了全面的研究。这项研究的重点是解释Mn-MIL-100热解过程中的晶体-非晶态-晶体转变,以及研究CO氧化反应过程中的结构变化。提出了一种可能的非晶态Mn-MIL-100的形成机理。通过在250°C下煅烧得到的Mn-MIL-100(a-Mn-250)表现出较小的比表面积(4 m 2 g -1),但催化活性较高。此外,在反应过程中非晶态Mn-MIL-100的结构不稳定。当将a-Mn-250在高温下用反应气氛处理(使用过的a-Mn-250-S)时,无定形催化剂转化为Mn 2 O3。同时,BET表面积(164m 2 g -1)和催化性能均急剧增加。此外,用过的Mn-250-S催化剂从Mn 2 O 3转变为Mn 3 O 4,并且在进料流中存在1体积%水蒸气的情况下,这导致催化活性略有下降。提出了反应过程中结构变化的机理示意图。合成的成功取决于通过使用CO作为后处理气氛来增加BET表面积,而增强的催化活性归因于独特的结构,大量的表面活性氧种类,氧空位以及良好的低温还原性行为。
更新日期:2018-05-30
中文翻译:
高效无定形Mn-MIL-100高效催化剂的合成:CO氧化过程中的形成机理和结构变化
对无定形金属-有机骨架Mn-MIL-100作为CO氧化的有效催化剂进行了全面的研究。这项研究的重点是解释Mn-MIL-100热解过程中的晶体-非晶态-晶体转变,以及研究CO氧化反应过程中的结构变化。提出了一种可能的非晶态Mn-MIL-100的形成机理。通过在250°C下煅烧得到的Mn-MIL-100(a-Mn-250)表现出较小的比表面积(4 m 2 g -1),但催化活性较高。此外,在反应过程中非晶态Mn-MIL-100的结构不稳定。当将a-Mn-250在高温下用反应气氛处理(使用过的a-Mn-250-S)时,无定形催化剂转化为Mn 2 O3。同时,BET表面积(164m 2 g -1)和催化性能均急剧增加。此外,用过的Mn-250-S催化剂从Mn 2 O 3转变为Mn 3 O 4,并且在进料流中存在1体积%水蒸气的情况下,这导致催化活性略有下降。提出了反应过程中结构变化的机理示意图。合成的成功取决于通过使用CO作为后处理气氛来增加BET表面积,而增强的催化活性归因于独特的结构,大量的表面活性氧种类,氧空位以及良好的低温还原性行为。