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Title: Highly active subnanometer Rh clusters derived from Rh-doped SrTiO 3 for CO 2 reduction

Abstract

Here, sub-nanometer Rh clusters derived from Rh-doped SrTiO 3, demonstrated by in-situ X-ray Diffraction (XRD) and X-ray Absorption Fine Structure (XAFS) measurements, are applied as highly active catalysts for CO 2 reduction. Compared to the supported Rh/SrTiO 3, the catalyst synthesized by a doping-segregation method exhibits a higher space-time yield (STY) to CO with a selectivity of 95% for CO 2 reduction by hydrogen; it also shows a higher activity with a larger turnover frequency (TOF) for CO 2 reduction by ethane. According to the in-situ diffuse reflectance infrared Fourier transformed spectroscopy (DRIFTS) experiments, the higher CO selectivity for CO 2 hydrogenation is attributed to the lower CO binding strength resulted by the strong interactions (e.g., charge transfer) between Rh atoms and the oxide support with surface defects. The superior activity is suggested to be originated from the cooperative effect between the highly dispersed sub-nanometer Rh clusters for efficient dissociation of H 2/C 2H 6 and the reconstructed SrTiO 3 with oxygen vacancies for preferential adsorption/activation of CO 2. Finally, the doping-segregation method provides a unique opportunity to tune the size of active metal clusters and the physicochemical properties of the oxide support, offering the potential for applications in amore » variety of chemical reactions.« less

Authors:
 [1];  [2];  [2];  [2];  [3];  [4];  [5];  [5];  [4];  [2];  [6]
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  1. Tsinghua Univ., Beijing (China). Dept. of Chemical Engineering; Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Dept.
  2. Stony Brook Univ., NY (United States). Dept. of Materials Science and Chemical Engineering
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Dept.; Stony Brook Univ., NY (United States). Dept. of Materials Science and Chemical Engineering
  4. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
  5. Stony Brook Univ., NY (United States). Chemistry Dept.
  6. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Dept.; Columbia Univ., New York, NY (United States). Dept. of Chemical Engineering
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States); Stony Brook Univ., NY (United States); Tsinghua Univ., Beijing (China)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); National Natural Science Foundation of China (NNSFC)
OSTI Identifier:
1476271
Alternate Identifier(s):
OSTI ID: 1495314
Report Number(s):
BNL-209139-2018-JAAM
Journal ID: ISSN 0926-3373
Grant/Contract Number:  
SC0012704; AC02-76SF00515; FG02-03ER15476; 1254600; 21673125; DESC0012335
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Applied Catalysis B: Environmental
Additional Journal Information:
Journal Volume: 237; Journal ID: ISSN 0926-3373
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; CO2 reduction; subnanometer; perovskite; doping-segregation; selectivity

Citation Formats

Yan, Binhang, Wu, Qiyuan, Cen, Jiajie, Timoshenko, Janis, Frenkel, Anatoly I., Su, Dong, Chen, Xianyin, Parise, John B., Stach, Eric, Orlov, Alexander, and Chen, Jingguang G. Highly active subnanometer Rh clusters derived from Rh-doped SrTiO3 for CO2 reduction. United States: N. p., 2018. Web. doi:10.1016/j.apcatb.2018.06.074.
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Yan, Binhang, Wu, Qiyuan, Cen, Jiajie, Timoshenko, Janis, Frenkel, Anatoly I., Su, Dong, Chen, Xianyin, Parise, John B., Stach, Eric, Orlov, Alexander, & Chen, Jingguang G. Highly active subnanometer Rh clusters derived from Rh-doped SrTiO3 for CO2 reduction. United States. https://doi.org/10.1016/j.apcatb.2018.06.074
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Yan, Binhang, Wu, Qiyuan, Cen, Jiajie, Timoshenko, Janis, Frenkel, Anatoly I., Su, Dong, Chen, Xianyin, Parise, John B., Stach, Eric, Orlov, Alexander, and Chen, Jingguang G. Thu . "Highly active subnanometer Rh clusters derived from Rh-doped SrTiO3 for CO2 reduction". United States. https://doi.org/10.1016/j.apcatb.2018.06.074. https://www.osti.gov/servlets/purl/1476271.
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@article{osti_1476271,
title = {Highly active subnanometer Rh clusters derived from Rh-doped SrTiO3 for CO2 reduction},
author = {Yan, Binhang and Wu, Qiyuan and Cen, Jiajie and Timoshenko, Janis and Frenkel, Anatoly I. and Su, Dong and Chen, Xianyin and Parise, John B. and Stach, Eric and Orlov, Alexander and Chen, Jingguang G.},
abstractNote = {Here, sub-nanometer Rh clusters derived from Rh-doped SrTiO3, demonstrated by in-situ X-ray Diffraction (XRD) and X-ray Absorption Fine Structure (XAFS) measurements, are applied as highly active catalysts for CO2 reduction. Compared to the supported Rh/SrTiO3, the catalyst synthesized by a doping-segregation method exhibits a higher space-time yield (STY) to CO with a selectivity of 95% for CO2 reduction by hydrogen; it also shows a higher activity with a larger turnover frequency (TOF) for CO2 reduction by ethane. According to the in-situ diffuse reflectance infrared Fourier transformed spectroscopy (DRIFTS) experiments, the higher CO selectivity for CO2 hydrogenation is attributed to the lower CO binding strength resulted by the strong interactions (e.g., charge transfer) between Rh atoms and the oxide support with surface defects. The superior activity is suggested to be originated from the cooperative effect between the highly dispersed sub-nanometer Rh clusters for efficient dissociation of H2/C2H6 and the reconstructed SrTiO3 with oxygen vacancies for preferential adsorption/activation of CO2. Finally, the doping-segregation method provides a unique opportunity to tune the size of active metal clusters and the physicochemical properties of the oxide support, offering the potential for applications in a variety of chemical reactions.},
doi = {10.1016/j.apcatb.2018.06.074},
url = {https://www.osti.gov/biblio/1476271}, journal = {Applied Catalysis B: Environmental},
issn = {0926-3373},
number = ,
volume = 237,
place = {United States},
year = {2018},
month = {6}
}
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https://doi.org/10.1016/j.apcatb.2018.06.074
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Works referencing / citing this record:

A review of synthesis and morphology of SrTiO 3 for energy and other applications
journal, May 2019

A review of synthesis and morphology of SrTiO 3 for energy and other applications
journal, May 2019

Towards efficient use of noble metals via exsolution exemplified for CO oxidation
journal, January 2019

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