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Title: Nanoassemblies of ultrasmall clusters with remarkable activity in carbon dioxide conversion into C1 fuels

Abstract

Cu nanoassemblies formed transiently during reaction from size-selected subnanometer Cu 4 clusters supported on amorphous OH-terminated alumina convert CO 2 into methanol and hydrocarbons under near-atmospheric pressure at rates considerably higher than those of individually standing Cu 4 clusters. An in situ characterization reveals that the clusters self-assemble into 2D nanoassemblies at higher temperatures which then disintegrate upon cooling down to room temperature. DFT calculations postulate a formation mechanism of these nanoassemblies by hydrogen-bond bridges between the clusters and H 2O molecules, which keep the building blocks together while preventing their coalescence.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1];  [1]; ORCiD logo [1];  [1]; ORCiD logo [1];  [3]; ORCiD logo [3]; ORCiD logo [4]
  1. Argonne National Lab. (ANL), Lemont, IL (United States)
  2. Aristotle Univ., Thessaloniki (Greece)
  3. Okinawa Inst. of Science and Technology Graduate Univ., Okinawa (Japan)
  4. Argonne National Lab. (ANL), Lemont, IL (United States); Univ. of Chicago, Chicago, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
Okinawa Institute of Science and Technology Graduate University (OIST); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1495230
Alternate Identifier(s):
OSTI ID: 1506238
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Published Article
Journal Name:
Nanoscale
Additional Journal Information:
Journal Volume: 11; Journal Issue: 11; Journal ID: ISSN 2040-3364
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY

Citation Formats

Halder, Avik, Kioseoglou, Joseph, Yang, Bing, Kolipaka, Karthika Lakshmi, Seifert, Soenke, Ilavsky, Jan, Pellin, Michael, Sowwan, Mukhles, Grammatikopoulos, Panagiotis, and Vajda, Stefan. Nanoassemblies of ultrasmall clusters with remarkable activity in carbon dioxide conversion into C1 fuels. United States: N. p., 2019. Web. doi:10.1039/c8nr06664g.
Halder, Avik, Kioseoglou, Joseph, Yang, Bing, Kolipaka, Karthika Lakshmi, Seifert, Soenke, Ilavsky, Jan, Pellin, Michael, Sowwan, Mukhles, Grammatikopoulos, Panagiotis, & Vajda, Stefan. Nanoassemblies of ultrasmall clusters with remarkable activity in carbon dioxide conversion into C1 fuels. United States. doi:10.1039/c8nr06664g.
Halder, Avik, Kioseoglou, Joseph, Yang, Bing, Kolipaka, Karthika Lakshmi, Seifert, Soenke, Ilavsky, Jan, Pellin, Michael, Sowwan, Mukhles, Grammatikopoulos, Panagiotis, and Vajda, Stefan. Wed . "Nanoassemblies of ultrasmall clusters with remarkable activity in carbon dioxide conversion into C1 fuels". United States. doi:10.1039/c8nr06664g.
@article{osti_1495230,
title = {Nanoassemblies of ultrasmall clusters with remarkable activity in carbon dioxide conversion into C1 fuels},
author = {Halder, Avik and Kioseoglou, Joseph and Yang, Bing and Kolipaka, Karthika Lakshmi and Seifert, Soenke and Ilavsky, Jan and Pellin, Michael and Sowwan, Mukhles and Grammatikopoulos, Panagiotis and Vajda, Stefan},
abstractNote = {Cu nanoassemblies formed transiently during reaction from size-selected subnanometer Cu4 clusters supported on amorphous OH-terminated alumina convert CO2 into methanol and hydrocarbons under near-atmospheric pressure at rates considerably higher than those of individually standing Cu4 clusters. An in situ characterization reveals that the clusters self-assemble into 2D nanoassemblies at higher temperatures which then disintegrate upon cooling down to room temperature. DFT calculations postulate a formation mechanism of these nanoassemblies by hydrogen-bond bridges between the clusters and H2O molecules, which keep the building blocks together while preventing their coalescence.},
doi = {10.1039/c8nr06664g},
journal = {Nanoscale},
number = 11,
volume = 11,
place = {United States},
year = {2019},
month = {2}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1039/c8nr06664g

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