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Incorporating Pb2+ Templates into the CrystallineStructure of MnO2 Catalyst Supported on Monolith: Applications in H2O2 Decomposition

机译:将Pb2 +模板整合到结晶中整体支撑的MnO2催化剂的结构:在H2O2分解中的应用

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摘要

Several MnO2 catalysts, promoted with Pb2+ ions and supported on a wash-coated monolith (WMon), briefly, xPbyMn-WMon (x = 0, 0.5, 1.0, 1.5, 2, and 2.5 and y = 8 wt %), were prepared. The presence of Pb2+ affects the manganese oxidation state, crystalline phase, thermal resistance, metal dispersion, and catalytic performance. According to XPS spectra, XRD patterns and HRTEM images, manganese was dispersed on the monolith surface as Mn3+ and Mn4+ species in both α and β crystalline phases. The ratios of Mn4+/Mn3+ states and α/β phases were highly enhanced, and the desired PbxMn8O16 phase (coronadite) was formed. Concentrations of the defect oxygen (Mn–O–H) and oxygen vacancies, which improve the catalyst reducibility and the MnO2 reduction temperature, were also increased. Further, based on the H2 chemisorption analysis, the Pb2+ template would increase the manganese dispersion and the reaction sites. Meanwhile, the average MnO2 crystallite size was decreased from 13.26 to 8.15 nm. The optimum catalyst 1.5Pb8Mn-WMon exhibited an activity 149% more than the manganese-only catalyst indecomposition of H2O2. Evaluation of catalyststability in the presence of Pb2+ after 10 recycles showedonly a 6.8% decrease. The catalytic reaction was evaluated based ondifferent criteria.
机译:几种MnO2催化剂,由Pb 2 + 离子促进并负载在洗涂的整料(WMon)上,简要地说是xPbyMn-WMon(x = 0、0.5、1.0、1.5、2和2.5以及制备y = 8wt%。 Pb 2 + 的存在会影响锰的氧化态,晶相,耐热性,金属分散性和催化性能。根据XPS光谱,XRD图谱和HRTEM图像,锰在α和β晶相中均以Mn 3 + 和Mn 4 + 的形式分散在整料表面。 Mn 4 + / Mn 3 + 态与α/β相的比率大大提高,并形成了所需的PbxMn8O16相(钴镍铁矿)。缺陷氧(Mn–O–H)和氧空位的浓度也增加了,从而提高了催化剂的还原能力和MnO2还原温度。此外,基于H2的化学吸附分析,Pb 2 + 模板会增加锰的分散度和反应位点。同时,平均MnO2微晶尺寸从13.26 nm减小到8.15 nm。最佳催化剂1.5Pb8Mn-WMon的活性比纯锰催化剂高149%。H2O2分解。催化剂评估Pb 2 + 存在10次循环后的稳定性仅下降了6.8%。催化反应基于不同的标准。

著录项

  • 期刊名称 ACS Omega
  • 作者单位
  • 年(卷),期 2019(4),15
  • 年度 2019
  • 页码 16638–16650
  • 总页数 13
  • 原文格式 PDF
  • 正文语种
  • 中图分类
  • 关键词

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