Production of H2-free CO by decomposition of formic acid over ZrO2 catalysts

Hyun Ju Lee, Dong Chang Kang, Seung Hee Pyen, Mi Shin, Young Woong Suh, Haksoo Han, Chae Ho Shin

Research output: Contribution to journalArticle

17 Citations (Scopus)

Abstract

The decomposition of formic acid (HCOOH) over ZrO2 catalysts synthesized by precipitation method was investigated and their catalytic activity based on unit mass of catalyst was compared by varying the calcination temperature in the 500–1000 °C range. The calcined ZrO2 samples were characterized using temperature-programed desorption (TPD) of iso-propanol (IPA), H2O, and HCOOH as well as X-ray diffraction (XRD), pyridine-adsorbed infrared spectroscopy (Py-IR) and N2 sorption. The catalytic activity as a function of the calcination temperature of ZrO2 showed a volcano-type curve with a maximum at 900 °C. The catalytic activity of ZrO2 in the decomposition of HCOOH well correlated with Brönsted acid site density, and it was influenced by the crystalline phase of ZrO2. Furthermore, the evolution of the Brönsted acid site density measured by Py-IR as a function of the calcination temperature was in good accordance with the desorption temperature determined by IPA- and HCOOH-TPD experiments. When H2O vapor was added, the conversion of HCOOH slightly decreased, while the CO selectivity remained almost constant. However, when CO was supplied, the conversion of HCOOH decreased continuously, and the selectivity to H2 gradually increased, indicating that the formation of zirconium suboxides with characteristics approaching those of metals was successful using CO as a reductant.

Original languageEnglish
Pages (from-to)13-20
Number of pages8
JournalApplied Catalysis A: General
Volume531
DOIs
Publication statusPublished - 2017 Feb 5

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formic acid
Formic acid
Carbon Monoxide
Decomposition
Catalysts
Calcination
1-Propanol
Catalyst activity
Desorption
Propanol
Pyridine
Temperature
Infrared spectroscopy
Volcanoes
Acids
Reducing Agents
Zirconium
Sorption
Metals
Vapors

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Process Chemistry and Technology

Cite this

Lee, Hyun Ju ; Kang, Dong Chang ; Pyen, Seung Hee ; Shin, Mi ; Suh, Young Woong ; Han, Haksoo ; Shin, Chae Ho. / Production of H2-free CO by decomposition of formic acid over ZrO2 catalysts. In: Applied Catalysis A: General. 2017 ; Vol. 531. pp. 13-20.
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abstract = "The decomposition of formic acid (HCOOH) over ZrO2 catalysts synthesized by precipitation method was investigated and their catalytic activity based on unit mass of catalyst was compared by varying the calcination temperature in the 500–1000 °C range. The calcined ZrO2 samples were characterized using temperature-programed desorption (TPD) of iso-propanol (IPA), H2O, and HCOOH as well as X-ray diffraction (XRD), pyridine-adsorbed infrared spectroscopy (Py-IR) and N2 sorption. The catalytic activity as a function of the calcination temperature of ZrO2 showed a volcano-type curve with a maximum at 900 °C. The catalytic activity of ZrO2 in the decomposition of HCOOH well correlated with Br{\"o}nsted acid site density, and it was influenced by the crystalline phase of ZrO2. Furthermore, the evolution of the Br{\"o}nsted acid site density measured by Py-IR as a function of the calcination temperature was in good accordance with the desorption temperature determined by IPA- and HCOOH-TPD experiments. When H2O vapor was added, the conversion of HCOOH slightly decreased, while the CO selectivity remained almost constant. However, when CO was supplied, the conversion of HCOOH decreased continuously, and the selectivity to H2 gradually increased, indicating that the formation of zirconium suboxides with characteristics approaching those of metals was successful using CO as a reductant.",
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Production of H2-free CO by decomposition of formic acid over ZrO2 catalysts. / Lee, Hyun Ju; Kang, Dong Chang; Pyen, Seung Hee; Shin, Mi; Suh, Young Woong; Han, Haksoo; Shin, Chae Ho.

In: Applied Catalysis A: General, Vol. 531, 05.02.2017, p. 13-20.

Research output: Contribution to journalArticle

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AU - Pyen, Seung Hee

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AB - The decomposition of formic acid (HCOOH) over ZrO2 catalysts synthesized by precipitation method was investigated and their catalytic activity based on unit mass of catalyst was compared by varying the calcination temperature in the 500–1000 °C range. The calcined ZrO2 samples were characterized using temperature-programed desorption (TPD) of iso-propanol (IPA), H2O, and HCOOH as well as X-ray diffraction (XRD), pyridine-adsorbed infrared spectroscopy (Py-IR) and N2 sorption. The catalytic activity as a function of the calcination temperature of ZrO2 showed a volcano-type curve with a maximum at 900 °C. The catalytic activity of ZrO2 in the decomposition of HCOOH well correlated with Brönsted acid site density, and it was influenced by the crystalline phase of ZrO2. Furthermore, the evolution of the Brönsted acid site density measured by Py-IR as a function of the calcination temperature was in good accordance with the desorption temperature determined by IPA- and HCOOH-TPD experiments. When H2O vapor was added, the conversion of HCOOH slightly decreased, while the CO selectivity remained almost constant. However, when CO was supplied, the conversion of HCOOH decreased continuously, and the selectivity to H2 gradually increased, indicating that the formation of zirconium suboxides with characteristics approaching those of metals was successful using CO as a reductant.

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