Highly active copper-intercalated weakly crystallized δ-MnO2 for low-temperature oxidation of CO in dry and humid air

IF 6.1 2区 环境科学与生态学 Q2 ENGINEERING, ENVIRONMENTAL
Hao Zhang, Huinan Li, Pengyi Zhang, Tingxia Hu, Xianjie Wang
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Abstract

Copper intercalated birnessite MnO2 (δ-MnO2) with weak crystallinity and high specific surface area (421 m2/g) was synthesized by a one-pot redox method and investigated for low-temperature CO oxidation. The molar ratio of Cu/Mn was as high as 0.37, which greatly weakened the Mn-O bond and created a lot of low-temperature active oxygen species. In situ DRIFTS revealed strong bonding of copper ions with CO. As-synthesized MnO2-150Cu achieved 100% conversion of 250 ppm CO in normal air (3.1 ppm H2O) even at −10 °C under the weight-hourly space velocity (WHSV) of 150 L/(g·h). In addition, it showed high oxygen storage capacity to oxidize CO in inert atmosphere. Though the concurrent moisture in air significantly inhibited CO adsorption and its conversion at ambient temperature, MnO2-150Cu could stably convert CO in 1.3% moisture air at 70 °C owing to its great low-temperature activity and reduced competitive adsorption of water with increased temperature. This study discovers the excellent low-temperature activity of weakly crystallized δ-MnO2 induced by high content intercalated copper ions.

Abstract Image

用于在干燥和潮湿空气中低温氧化 CO 的高活性铜掺杂弱结晶 δ-MnO2
通过一锅氧化还原法合成了具有弱结晶性和高比表面积(421 m2/g)的铜插层桦烷石 MnO2(δ-MnO2),并研究了其在低温 CO 氧化中的应用。铜/锰摩尔比高达 0.37,大大削弱了 Mn-O 键,产生了大量低温活性氧。原位 DRIFTS 显示铜离子与 CO 有很强的结合力。合成的 MnO2-150Cu 在-10 °C、150 升/(克-小时)的重量小时空间速度(WHSV)条件下,对普通空气中 250 ppm CO(3.1 ppm H2O)的转化率达到 100%。此外,它在惰性气氛中氧化 CO 的储氧能力也很强。虽然在环境温度下,空气中同时存在的水分会严重抑制 CO 的吸附和转化,但由于 MnO2-150Cu 具有极高的低温活性,且随着温度的升高,其对水的竞争性吸附减少,因此它能在 70 °C、含水量为 1.3% 的空气中稳定地转化 CO。这项研究发现了高含量插层铜离子诱导的弱结晶 δ-MnO2 的优异低温活性。
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来源期刊
Frontiers of Environmental Science & Engineering
Frontiers of Environmental Science & Engineering ENGINEERING, ENVIRONMENTAL-ENVIRONMENTAL SCIENCES
CiteScore
10.90
自引率
12.50%
发文量
988
审稿时长
6.1 months
期刊介绍: Frontiers of Environmental Science & Engineering (FESE) is an international journal for researchers interested in a wide range of environmental disciplines. The journal''s aim is to advance and disseminate knowledge in all main branches of environmental science & engineering. The journal emphasizes papers in developing fields, as well as papers showing the interaction between environmental disciplines and other disciplines. FESE is a bi-monthly journal. Its peer-reviewed contents consist of a broad blend of reviews, research papers, policy analyses, short communications, and opinions. Nonscheduled “special issue” and "hot topic", including a review article followed by a couple of related research articles, are organized to publish novel contributions and breaking results on all aspects of environmental field.
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