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Title: Growth of Nanoparticles with Desired Catalytic Functions by Controlled Doping-Segregation of Metal in Oxide

Abstract

Here, the size and morphology of metal nanoparticles (NPs) often play a critical role in defining the catalytic performance of supported metal nanocatalysts. However, common synthetic methods struggle to produce metal NPs of appropriate size and morphological control. Thus, facile synthetic methods that offer controlled catalytic functions are highly desired. Here we have identified a new pathway to synthesize supported Rh nanocatalysts with finely tuned spatial dimensions and controlled morphology using a doping-segregation method. We have analyzed their structure evolutions during both the segregation process and catalytic reaction using a variety of in situ spectroscopic and microscopic techniques. A correlation between the catalytic functional sites and activity in CO 2 hydrogenation over supported Rh nanocatalysts is then established. This study demonstrates a facile strategy to design and synthesize nanocatalysts with desired catalytic functions.

Authors:
ORCiD logo [1];  [2];  [1];  [1];  [3];  [1];  [3];  [3];  [1]; ORCiD logo [4]; ORCiD logo [5]; ORCiD logo [6];  [1]
  1. Stony Brook Univ., Stony Brook, NY (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States); Tsinghua Univ., Beijing (China)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States)
  4. Stony Brook Univ., Stony Brook, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
  5. Brookhaven National Lab. (BNL), Upton, NY (United States); Univ. of Pennsylvania, Philadelphia, PA (United States)
  6. Brookhaven National Lab. (BNL), Upton, NY (United States); Columbia Univ., New York, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1438305
Report Number(s):
BNL-205661-2018-JAAM
Journal ID: ISSN 0897-4756
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 30; Journal Issue: 5; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY

Citation Formats

Wu, Qiyuan, Yan, Binhang, Cen, Jiajie, Timoshenko, Janis, Zakharov, Dmitri N., Chen, Xianyin, Xin, Huolin L., Yao, Siyu, Parise, John B., Frenkel, Anatoly I., Stach, Eric A., Chen, Jingguang G., and Orlov, Alexander. Growth of Nanoparticles with Desired Catalytic Functions by Controlled Doping-Segregation of Metal in Oxide. United States: N. p., 2018. Web. doi:10.1021/acs.chemmater.7b04699.
Wu, Qiyuan, Yan, Binhang, Cen, Jiajie, Timoshenko, Janis, Zakharov, Dmitri N., Chen, Xianyin, Xin, Huolin L., Yao, Siyu, Parise, John B., Frenkel, Anatoly I., Stach, Eric A., Chen, Jingguang G., & Orlov, Alexander. Growth of Nanoparticles with Desired Catalytic Functions by Controlled Doping-Segregation of Metal in Oxide. United States. doi:10.1021/acs.chemmater.7b04699.
Wu, Qiyuan, Yan, Binhang, Cen, Jiajie, Timoshenko, Janis, Zakharov, Dmitri N., Chen, Xianyin, Xin, Huolin L., Yao, Siyu, Parise, John B., Frenkel, Anatoly I., Stach, Eric A., Chen, Jingguang G., and Orlov, Alexander. Mon . "Growth of Nanoparticles with Desired Catalytic Functions by Controlled Doping-Segregation of Metal in Oxide". United States. doi:10.1021/acs.chemmater.7b04699. https://www.osti.gov/servlets/purl/1438305.
@article{osti_1438305,
title = {Growth of Nanoparticles with Desired Catalytic Functions by Controlled Doping-Segregation of Metal in Oxide},
author = {Wu, Qiyuan and Yan, Binhang and Cen, Jiajie and Timoshenko, Janis and Zakharov, Dmitri N. and Chen, Xianyin and Xin, Huolin L. and Yao, Siyu and Parise, John B. and Frenkel, Anatoly I. and Stach, Eric A. and Chen, Jingguang G. and Orlov, Alexander},
abstractNote = {Here, the size and morphology of metal nanoparticles (NPs) often play a critical role in defining the catalytic performance of supported metal nanocatalysts. However, common synthetic methods struggle to produce metal NPs of appropriate size and morphological control. Thus, facile synthetic methods that offer controlled catalytic functions are highly desired. Here we have identified a new pathway to synthesize supported Rh nanocatalysts with finely tuned spatial dimensions and controlled morphology using a doping-segregation method. We have analyzed their structure evolutions during both the segregation process and catalytic reaction using a variety of in situ spectroscopic and microscopic techniques. A correlation between the catalytic functional sites and activity in CO2 hydrogenation over supported Rh nanocatalysts is then established. This study demonstrates a facile strategy to design and synthesize nanocatalysts with desired catalytic functions.},
doi = {10.1021/acs.chemmater.7b04699},
journal = {Chemistry of Materials},
number = 5,
volume = 30,
place = {United States},
year = {2018},
month = {2}
}

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