Short Communication
Complete oxidation of formaldehyde at ambient temperature over
γ-Al
2
O
3
supported Au catalyst
Bing-bing Chen
a,b
, Xiao-bing Zhu
b
, Mark Crocker
c
, Yu Wang
a,b
, Chuan Shi
a,b,
⁎
a
Key Laboratory of Industrial Ecology and Environmental Engineering (MOE), Dalian University of Technology, Dalian, PR China
b
Laboratory of Plasma Physical Chemistry, Dalian University of Technology, Dalian, PR China
c
Center for Applied Energy Research, University of Kentucky, Lexington, KY 40511, USA
abstract article info
Article history:
Received 30 May 2013
Received in revised form 8 August 2013
Accepted 13 August 2013
Available online 22 August 2013
Keywords:
Formaldehyde
Catalytic oxidation
Au/γ-Al
2
O
3
Room temperature
Au supported on γ-Al
2
O
3
prepared by deposition–precipitation (DP) using urea is found to be a highly active
catalyst for the total oxidation of HCHO at room temperature under humid air, without the need for a reducible
oxide as support. In-situ DRIFTS studies suggested that the surface hydroxyl groups played a key role in the partial
oxidation of HCHO into the formate intermediates, which can be further oxidized into CO
2
and H
2
O with partic-
ipation of nano-Au. This study challenges the traditional idea of supporting noble metals on reducible oxides for
HCHO oxidation at room temperature.
© 2013 Elsevier B.V. All rights reserved.
1. Introduction
Given that formaldehyde is a major indoor air pollutant, significant
efforts have been directed at indoor HCHO removal to meet environ-
mental regulations and human health needs [1,2]. Catalytic oxidation
is recognized as the most promising HCHO removal technology. Indeed,
supported Pt catalysts such as Pt/TiO
2
and Pt/MnOx–CeO
2
have been
shown to be active for HCHO complete oxidation at room temperature
[3–6]. Moreover, in our previous study, 1% Au/CeO
2
catalyst was found
to provide 100% HCHO conversion at room temperature (RT). It was
suggested that HCHO was partially oxidized into [HCOO]
s
intermediates
on the support, further oxidation of these intermediates required the
participation of gas phase oxygen activated by Au nanoparticles [7].
In general, reducible oxides have been used as the support of choice
in past studies because of their high concentrations of oxygen defects
and their ability to stabilize high dispersions of Pt or Au.
With HCHO oxidation aside, γ-Al
2
O
3
is the most common support
material for metal catalysts, due to its low cost, thermal and chemical
stability, high surface area and amphoteric character [8,9]. However,
γ-Al
2
O
3
is considered to be a poor support for low temperature HCHO
oxidation catalysts due to its irreducibility [10]. It is generally agreed
that a reducible oxide such as ceria has strong surface interactions
with the supported metal which help to stabilize the latter. Such inter-
action might cause the charge transfer from the supported metal to the
support, which leads to the weakened bond of the support, such as
Ce\O bond [7,11,12]. That is the way that the surface oxygen species
become very active and normally believed to have key roles in low
temperature HCHO oxidation [13–15].
Herein, we report for the first time that γ-Al
2
O
3
supported Au is a
very active catalyst for HCHO oxidation at RT even in the presence of
moisture. It is found that although there is no active surface oxygen on
γ-Al
2
O
3
, surface hydroxyls have the ability to partially oxidize HCHO
into formate intermediates, which can be further oxidized into CO
2
and H
2
O by nano-Au. This study challenges the traditional idea of
supporting noble metals on reducible oxides for HCHO oxidation at RT.
2. Experimental section
2.1. Catalyst preparation
Au/γ-Al
2
O
3
catalysts with nominal gold loadings of 0.25, 0.5 and
1 wt.% were prepared by the deposition–precipitation method, using
urea as precipitant, according to a literature procedure [7]. The support-
ed gold catalysts were dried in air at 80 °C for 16 h, and calcined in air at
200 °C for 4 h.
2.2. Catalyst characterization
The catalysts were characterized by CO-chemisorption, UV–vis
spectra, transmission electron microscopy (TEM), H
2
temperature-
programmed reduction (H
2
-TPR), and diffuse reflectance infrared
Fourier transform (DRIFT) spectroscopy. The detailed procedures used
are described in the Supplementary data.
Catalysis Communications 42 (2013) 93–97
⁎ Corresponding author at: Key Laboratory of Industrial Ecology and Environmental
Engineering (MOE), Dalian University of Technology, Dalian, PR China. Tel.: +86 411
84986083.
E-mail address: chuanshi@dlut.edu.cn (C. Shi).
1566-7367/$ – see front matter © 2013 Elsevier B.V. All rights reserved.
http://dx.doi.org/10.1016/j.catcom.2013.08.008
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