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Highly Active and Stable Palladium Catalysts on Novel Ceria- Alumina Supports for Efficient Oxidation of Carbon Monoxide and Hydrocarbons

机译:在新型二氧化铈 - 氧化铝上的高活性和稳定的钯催化剂,用于有效氧化一氧化碳和碳氢化合物

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摘要

Precious metal catalysts with superior low-temperature activity and excellent thermal stability are highly needed in environmental catalysis field. In this work, a novel two-step incipient wetness impregnation (T-IWI) method was developed for the fabrication of a unique and highly stable CeO_2/Al_2O_3 support (CA-T). Pd anchored on CA-T exhibited a much higher low-temperature catalytic activity and superior thermal stability in carbon monoxide (CO) and hydrocarbon (HC) oxidations, compared to Pd anchored on conventional CeO_2/Al_2O_3 (CA), which was prepared by a one-step IWI method. After aging treatment at 800 °C, the CO oxidation rate on Pd/CA-T (1.69 mmol/(g_(pd) s)) at 120 °C was 4.1 and 84.5 times of those on Pd/ CA (0.41 mmol/(g_(pd) s)) and Pd/Al_2O_3 (0.02 mmol/(g_(pd) s)), respectively. It was revealed that the CA-T support with well-controlled small CeO_2 particles (ca. 12 nm) possessed abundant defects for Pd anchoring, which created rich Pd-CeO_2 interfaces with strengthened interaction between Pd and CeO_2 where oxygen could be efficiently activated. This resulted in the significantly improved oxidation activity and thermal stability of Pd/CA-T catalysts. The T-IWI method developed herein can be applied as a universal approach to prepare highly stable metal oxide-alumina-based supports, which have broad application in environmental catalyst design, especially for automobile exhaust aftertreatment.
机译:具有优异的低温活性和优异的热稳定性的贵金属催化剂是高度需要在环境催化领域。在这项工作中,一个新的两步初湿浸渍(T-IWI)方法为一个独特且高度稳定氧化铈/ Al_2O_3的支持(CA-T)的制造开发的。钯锚定在CA-T显示出一氧化碳(CO)和烃(HC)氧化反应高得多的低温催化活性和优异的热稳定性,相对于钯锚定在常规氧化铈/ Al_2O_3的(CA),将其通过一个制备一步法IWI方法。在120,在800℃下,在Pd / CA-T CO氧化速率(1.69毫摩尔/(G_(PD)3))时效处理后℃下为4.1和那些在Pd / CA 84.5倍(0.41毫摩尔/( G_(PD)3)),并分别的Pd / Al_2O_3的(0.02毫摩尔/(G_(PD)3))。据透露,具有良好控制的小粒子氧化铈(约12纳米)的CA-T载体具有对钯的锚固,其创建丰富的Pd-氧化铈接口与其中氧可有效地激活Pd和氧化铈之间加强相互作用丰富的缺陷。这导致了改进的显著氧化活性和Pd / CA-T催化剂的热稳定性。本文所开发的T-IWI方法可以应用于作为一种通用的方法来制备高度稳定的氧化铝的金属氧化物基载体,其具有在环境催化剂设计广泛的应用,特别是对于汽车排气后处理。

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  • 来源
    《Environmental Science & Technology》 |2021年第11期|7624-7633|共10页
  • 作者单位

    Department of Civil Environmental and Construction Engineering Catalysis Cluster for Renewable Energy and Chemical Transformations (REACT) NanoScience Technology Center (NSTC) University of Central Florida Orlando Florida 32816 United States;

    College of Environmental and Energy Engineering Beijing University of Technology Beijing 100124 China;

    Department of Civil Environmental and Construction Engineering Catalysis Cluster for Renewable Energy and Chemical Transformations (REACT) NanoScience Technology Center (NSTC) University of Central Florida Orlando Florida 32816 United States School of Chemistry and Chemical Engineering Jiangsu Key Laboratory of Vehicle Emissions Control Nanjing University Nanjing 210093 China;

    SEU-FE1 Nano-Pico Center Key Laboratory of MEMS of Ministry of Education Southeast University Nanjing 210096 China;

    Department of Civil Environmental and Construction Engineering Catalysis Cluster for Renewable Energy and Chemical Transformations (REACT) Nano Science Technology Center (NSTC) University of Central Florida Orlando Florida 32816 United States;

    National Synchrotron Light Source Ⅱ (NSLS-Ⅱ) Brookhaven National Laboratory Upton New York 11973 United States;

    National Synchrotron Light Source Ⅱ (NSLS-Ⅱ) Brookhaven National Laboratory Upton New York 11973 United States;

    CAS Key Laboratory of Standardization and Measurement for Nanotechnology National Center for Nanoscience and Technology Beijing 100190 China;

    School of Chemical and Biomedical Engineering Nanyang Technological University 637459 Singapore;

    SEU-FEI Nano-Pico Center Key Laboratory of MEMS of Ministry of Education Southeast University Nanjing 210096 China;

    College of Environmental and Energy Engineering Beijing University of Technology Beijing 100124 China;

    Department of Civil Environmental and Construction Engineering Catalysis Cluster for Renewable Energy and Chemical Transformations (REACT) NanoScience Technology Center (NSTC) University of Central Florida Orlando Florida 32816 United States;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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