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@ARTICLE{Gonalves:885517,
author = {Gonçalves, Liliana P. L. and Wang, Jianguang and Vinati,
Simone and Barborini, Emanuele and Wei, Xian-Kui and Heggen,
Marc and Franco, Miguel and Sousa, Juliana P. S. and
Petrovykh, Dmitri Y. and Soares, Olívia Salomé G. P. and
Kovnir, Kirill and Akola, Jaakko and Kolen'ko, Yury V.},
title = {{C}ombined experimental and theoretical study of acetylene
semi-hydrogenation over {P}d/{A}l2{O}3},
journal = {International journal of hydrogen energy},
volume = {45},
number = {2},
issn = {0360-3199},
address = {New York, NY [u.a.]},
publisher = {Elsevier},
reportid = {FZJ-2020-03897},
pages = {1283 - 1296},
year = {2020},
abstract = {The semi-hydrogenation of acetylene (C2H2 + H2 = C2H4, ΔH
= −172 kJ mol−1) is a well-studied reaction that is
important for purification of ethylene, C2H4, feed used in
polyethylene production. Pd-based catalysts are most
commonly used to remove acetylene from ethylene feed prior
to Ziegler–Natta polymerization because acetylene is a
poison for Ziegler–Natta catalysts. New applications of
the analogous catalytic processes, with similar requirements
for the conversion and selectivity, are considered for the
storage of H2 within the context of the H2 economy. Here, a
combination of experimental and theoretical studies was
employed to explore the performance of synthesized Pd
nanoparticles and the feasibility of using computational
modelling for predicting their catalytic properties.
Specifically, a model $5\%Pd/Al2O3$ nanocatalyst was
successfully synthesized using high-throughput flame spray
pyrolysis (FSP) method. As a catalyst for acetylene
semi-hydrogenation, the material shows high conversion of
$97\%,$ a modest selectivity of $62\%,$ and a turnover
frequency of ethylene formation of 5 s−1. The experimental
data were further supported by computational modelling of
catalytic properties. Results of microkinetic simulations,
based on parameters obtained from DFT calculations, over a
Pd30/Al2O3(100) model system were correlated with
experiments. The insights from this direct comparison of
theory and experiments provide indications for future
improvements of the theoretical predictions and for novel
types of materials with improved catalytic properties.},
cin = {ER-C-1},
ddc = {620},
cid = {I:(DE-Juel1)ER-C-1-20170209},
pnm = {143 - Controlling Configuration-Based Phenomena (POF3-143)
/ CritCat - Towards Replacement of Critical Catalyst
Materials by Improved Nanoparticle Control and Rational
Design (686053)},
pid = {G:(DE-HGF)POF3-143 / G:(EU-Grant)686053},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000514012200008},
doi = {10.1016/j.ijhydene.2019.04.086},
url = {https://juser.fz-juelich.de/record/885517},
}