The remarkable activity and stability of a highly dispersive beta-brass Cu-Zn catalyst for the production of ethylene glycol.

Abstract:

:Incorporation of Zn atoms into a nanosize Cu lattice is known to alter the electronic properties of Cu, improving catalytic performance in a number of industrially important reactions. However the structural influence of Zn on the Cu phase is not well studied. Here, we show that Cu nano-clusters modified with increasing concentration of Zn, derived from ZnO support doped with Ga(3+), can dramatically enhance their stability against metal sintering. As a result, the hydrogenation of dimethyl oxalate (DMO) to ethylene glycol, an important reaction well known for deactivation from copper nanoparticle sintering, can show greatly enhanced activity and stability with the CuZn alloy catalysts due to no noticeable sintering. HRTEM, nano-diffraction and EXAFS characterization reveal the presence of a small beta-brass CuZn alloy phase (body-centred cubic, bcc) which appears to greatly stabilise Cu atoms from aggregation in accelerated deactivation tests. DFT calculations also indicate that the small bcc CuZn phase is more stable against Cu adatom migration than the fcc CuZn phase with the ability to maintain a higher Cu dispersion on its surface.

journal_name

Sci Rep

journal_title

Scientific reports

authors

Li MM,Zheng J,Qu J,Liao F,Raine E,Kuo WC,Su SS,Po P,Yuan Y,Tsang SC

doi

10.1038/srep20527

subject

Has Abstract

pub_date

2016-02-09 00:00:00

pages

20527

issn

2045-2322

pii

srep20527

journal_volume

6

pub_type

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