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Title: Confined Ultrathin Pd-Ce Nanowires with Outstanding Moisture and SO 2 Tolerance in Methane Combustion

Abstract

Here, an efficient strategy (enhanced metal oxide interaction and core–shell confinement to inhibit the sintering of noble metal) is presented confined ultrathin Pd-CeO x nanowire (2.4 nm) catalysts for methane combustion, which enable CH 4 total oxidation at a low temperature of 350 °C, much lower than that of a commercial Pd/Al 2O 3 catalyst (425 °C). Importantly, unexpected stability was observed even under harsh conditions (800 °C, water vapor, and SO 2), owing to the confinement and shielding effect of the porous silica shell together with the promotion of CeO 2. Pd-CeO x solid solution nanowires (Pd-Ce NW) as cores and porous silica as shells (Pd-CeNW@SiO 2) were rationally prepared by a facile and direct self-assembly strategy for the first time. Finally, this strategy is expected to inspire more active and stable catalysts for use under severe conditions (vehicle emissions control, reforming, and water–gas shift reaction).

Authors:
 [1];  [2];  [2];  [2];  [2];  [3]; ORCiD logo [3];  [4]; ORCiD logo [5]
  1. Nanchang Univ. (China). Inst. of Applied Chemistry. College of Chemistry; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
  2. Nanchang Univ. (China). Inst. of Applied Chemistry. College of Chemistry
  3. Shanghai Jiao Tong Univ. (China). School of Chemistry and Chemical Engineering
  4. Shanghai Jiao Tong Univ. (China). School of Chemistry and Chemical Engineering; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States); Nanchang Univ. (China); Shanghai Jiao Tong Univ. (China)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Key R&D Program of China; National Natural Science Foundation of China (NNSFC); Natural Science Foundation of Jiangxi Province (China); Foundation of State Key Lab. of Coal Clean Utilization and Ecological Chemical Engineering (China)
OSTI Identifier:
1479715
Alternate Identifier(s):
OSTI ID: 1459724
Grant/Contract Number:  
AC05-00OR22725; 2016YFC0205900; 21503106; 21567016; 21773106; 20171BCB23016; 20171BAB203024; 2016-15
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Volume: 57; Journal Issue: 29; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; cerium; core-shell materials; methane oxidation; palladium; solid solutions

Citation Formats

Peng, Honggen, Rao, Cheng, Zhang, Ning, Wang, Xiang, Liu, Wenming, Mao, Wenting, Han, Lu, Zhang, Pengfei, and Dai, Sheng. Confined Ultrathin Pd-Ce Nanowires with Outstanding Moisture and SO2 Tolerance in Methane Combustion. United States: N. p., 2018. Web. doi:10.1002/anie.201803393.
Peng, Honggen, Rao, Cheng, Zhang, Ning, Wang, Xiang, Liu, Wenming, Mao, Wenting, Han, Lu, Zhang, Pengfei, & Dai, Sheng. Confined Ultrathin Pd-Ce Nanowires with Outstanding Moisture and SO2 Tolerance in Methane Combustion. United States. doi:10.1002/anie.201803393.
Peng, Honggen, Rao, Cheng, Zhang, Ning, Wang, Xiang, Liu, Wenming, Mao, Wenting, Han, Lu, Zhang, Pengfei, and Dai, Sheng. Tue . "Confined Ultrathin Pd-Ce Nanowires with Outstanding Moisture and SO2 Tolerance in Methane Combustion". United States. doi:10.1002/anie.201803393. https://www.osti.gov/servlets/purl/1479715.
@article{osti_1479715,
title = {Confined Ultrathin Pd-Ce Nanowires with Outstanding Moisture and SO2 Tolerance in Methane Combustion},
author = {Peng, Honggen and Rao, Cheng and Zhang, Ning and Wang, Xiang and Liu, Wenming and Mao, Wenting and Han, Lu and Zhang, Pengfei and Dai, Sheng},
abstractNote = {Here, an efficient strategy (enhanced metal oxide interaction and core–shell confinement to inhibit the sintering of noble metal) is presented confined ultrathin Pd-CeOx nanowire (2.4 nm) catalysts for methane combustion, which enable CH4 total oxidation at a low temperature of 350 °C, much lower than that of a commercial Pd/Al2O3 catalyst (425 °C). Importantly, unexpected stability was observed even under harsh conditions (800 °C, water vapor, and SO2), owing to the confinement and shielding effect of the porous silica shell together with the promotion of CeO2. Pd-CeOx solid solution nanowires (Pd-Ce NW) as cores and porous silica as shells (Pd-CeNW@SiO2) were rationally prepared by a facile and direct self-assembly strategy for the first time. Finally, this strategy is expected to inspire more active and stable catalysts for use under severe conditions (vehicle emissions control, reforming, and water–gas shift reaction).},
doi = {10.1002/anie.201803393},
journal = {Angewandte Chemie (International Edition)},
issn = {1433-7851},
number = 29,
volume = 57,
place = {United States},
year = {2018},
month = {5}
}

Journal Article:
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Cited by: 6 works
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Figures / Tables:

Scheme 1 Scheme 1: Formation process and catalytic application of Pd-CeNW@SiO2.

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Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.