Metal oxide decorated porous carbons from controlled calcination of a metal-organic framework

Gregory S. Day; Jialuo Li; Elizabeth A. Joseph; Peter C. Metz; Zachary Perry; Matthew R. Ryder; Katharine Page; Hong Cai Zhou

doi:10.1039/c9na00720b

Metal oxide decorated porous carbons from controlled calcination of a metal-organic framework

Gregory S. Day, Jialuo Li, Elizabeth A. Joseph, Peter C. Metz, Zachary Perry, Matthew R. Ryder, Katharine Page, Hong Cai Zhou

Neutron & X-Ray Scattering, & Thermophys

Research output: Contribution to journal › Article › peer-review

15 Scopus citations

Abstract

Thermal decomposition of an iron-based MOF was conducted under controlled gas environments to understand the resulting porous carbon structure. Different phases and crystallite sizes of iron oxide are produced based on the specific gas species. In particular, air resulted in iron(iii) oxide, and D2O and CO2 resulted in the mixed valent iron(ii,iii) oxide. Performing the carbonization under non-oxidative or reducing conditions (N2, He, H2) resulted in the formation of a mixture of both iron(ii,iii) oxide and iron(iii) oxide. Based on in situ and air-free handling experiments, it was observed that this is partially due to the formation of zero-valent iron metal that is rapidly oxidized when exposed to air. Neutron pair distribution function analysis provided insight into the effect of the gas environment on the local structure of the porous carbon, indicating a noticeable change in local order between the D2O and the N2 calcined samples.

Original language	English
Pages (from-to)	2758-2767
Number of pages	10
Journal	Nanoscale Advances
Volume	2
Issue number	7
DOIs	https://doi.org/10.1039/c9na00720b
State	Published - Jul 2020

Funding

The work was supported by the U.S. Department of Energy (DOE) Office of Science Graduate Student Research (SCGSR) program and the Center for Gas Separations Relevant to Clean Energy Technologies, an Energy Frontier Research Center funded by the DOE Office of Science (Basic Energy Sciences) under Contract Number DE-SC0001015. The SCGSR program is administered by the Oak Ridge Institute for Science and Education (ORISE) for the DOE under contract number DESC0014664. M. R. R. acknowledges the DOE Office of Science (Basic Energy Sciences) for additional research funding and the National Energy Research Scientic Computing Center (NERSC), a DOE Office of Science User Facility operated under Contract No. DE-AC02-05CH11231 for access to supercomputing resources. H.-C. Z. acknowledges the Robert A. Welch Foundation for a Welch Endowed Chair (A-0030). The research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. The authors also acknowledge the Texas A&M Microscopy and Imaging Center and Materials Characterization Facility.

Funders	Funder number
DOE Office of Science
National Energy Research Scientic Computing Center
Office of Science Graduate Student Research
Robert A. Welch Foundation	A-0030
SCGSR
U.S. Department of Energy
Basic Energy Sciences	DE-SC0001015
Oak Ridge Institute for Science and Education	DESC0014664

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title = "Metal oxide decorated porous carbons from controlled calcination of a metal-organic framework",

abstract = "Thermal decomposition of an iron-based MOF was conducted under controlled gas environments to understand the resulting porous carbon structure. Different phases and crystallite sizes of iron oxide are produced based on the specific gas species. In particular, air resulted in iron(iii) oxide, and D2O and CO2 resulted in the mixed valent iron(ii,iii) oxide. Performing the carbonization under non-oxidative or reducing conditions (N2, He, H2) resulted in the formation of a mixture of both iron(ii,iii) oxide and iron(iii) oxide. Based on in situ and air-free handling experiments, it was observed that this is partially due to the formation of zero-valent iron metal that is rapidly oxidized when exposed to air. Neutron pair distribution function analysis provided insight into the effect of the gas environment on the local structure of the porous carbon, indicating a noticeable change in local order between the D2O and the N2 calcined samples.",

author = "Day, {Gregory S.} and Jialuo Li and Joseph, {Elizabeth A.} and Metz, {Peter C.} and Zachary Perry and Ryder, {Matthew R.} and Katharine Page and Zhou, {Hong Cai}",

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AU - Day, Gregory S.

AU - Li, Jialuo

AU - Joseph, Elizabeth A.

AU - Metz, Peter C.

AU - Perry, Zachary

AU - Ryder, Matthew R.

AU - Page, Katharine

AU - Zhou, Hong Cai

PY - 2020/7

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N2 - Thermal decomposition of an iron-based MOF was conducted under controlled gas environments to understand the resulting porous carbon structure. Different phases and crystallite sizes of iron oxide are produced based on the specific gas species. In particular, air resulted in iron(iii) oxide, and D2O and CO2 resulted in the mixed valent iron(ii,iii) oxide. Performing the carbonization under non-oxidative or reducing conditions (N2, He, H2) resulted in the formation of a mixture of both iron(ii,iii) oxide and iron(iii) oxide. Based on in situ and air-free handling experiments, it was observed that this is partially due to the formation of zero-valent iron metal that is rapidly oxidized when exposed to air. Neutron pair distribution function analysis provided insight into the effect of the gas environment on the local structure of the porous carbon, indicating a noticeable change in local order between the D2O and the N2 calcined samples.

AB - Thermal decomposition of an iron-based MOF was conducted under controlled gas environments to understand the resulting porous carbon structure. Different phases and crystallite sizes of iron oxide are produced based on the specific gas species. In particular, air resulted in iron(iii) oxide, and D2O and CO2 resulted in the mixed valent iron(ii,iii) oxide. Performing the carbonization under non-oxidative or reducing conditions (N2, He, H2) resulted in the formation of a mixture of both iron(ii,iii) oxide and iron(iii) oxide. Based on in situ and air-free handling experiments, it was observed that this is partially due to the formation of zero-valent iron metal that is rapidly oxidized when exposed to air. Neutron pair distribution function analysis provided insight into the effect of the gas environment on the local structure of the porous carbon, indicating a noticeable change in local order between the D2O and the N2 calcined samples.

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Metal oxide decorated porous carbons from controlled calcination of a metal-organic framework

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