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Reaction engineering and catalysis

Editorial overview
Theodore T Tsotsis
Current Opinion in Chemical Engineering 2012,
1:269271
For a complete overview see the Issue
Available online 20th July 2012
2211-3398/$ see front matter, # 2012 Elsevier Ltd.
All rights reserved.
http://dx.doi.org/10.1016/j.coche.2012.07.001

Theodore T Tsotsis
Robert E. Vivian Professor of Energy
Resources, Mork Family Department of
Chemical Engineering and Materials Science,
University of Southern California, University
Park, Los Angles, CA 90089-1211, USA
e-mail: tsotsis@usc.edu
Theodore T. Tsotsis is the Robert E. Vivian
Professor of Energy Resources at the
University of Southern California. His current
research interests are in the areas of reaction
engineering, reactor design, membrane and
adsorbent preparation/characterization, and
the modelling of transport and reaction in
complex porous media.

Reaction and Reactor Engineering are among the oldest disciplines in the
field of Chemical Engineering and have played a pivotal role in the development of manufacturing, and the chemical and petrochemical industries. Despite their maturity, however, they continue to be the arena of many
lively and intensive R&D activities. This themed issue of Current Opinion
in Chemical Engineering contains ten short review articles that provide only
a small sampling of the so many new and exciting things which are currently
taking place in this all important area of Chemical Engineering. This writeup attempts to provide a short overview of the diverse mix of interesting
topics which are covered by these review papers.
Adesinas paper focuses on CO2 (dry as it is better known) reforming of light
hydrocarbons (C1C4) for syngas production, which has attracted considerable recent attention because of concerns about global warming, and the
obvious benefit of being able to utilize CO2. The process also has the added
flexibility of producing syngas with a H2:CO ratio more amenable to further
downstream use in FischerTropsch and methanol syntheses. Unfortunately, catalyst coking is a problem with dry reforming, and thus substantial
recent research activities are focusing on efforts to overcome this problem.
As detailed in the paper, they include the development of carbon-tolerant
catalysts, adding an oxidant to the reforming mixture, the distributed
feeding of reactants, and unsteady-state reactor operation. Adesina briefly
reviews such past efforts. He then proceeds to describe efforts by his group
in which CO2 is used as co-feed of a forced periodically operated reformer in
order to minimize coking even at the low steam to carbon ratio of 1. His
studies have also revealed that a basic oxide supported Ni-containing
catalyst promoted with alkaline-earth or rare-earth metals performs as well
or better than expensive noble metals.
Nature-inspired chemical engineering (NICE), which studies the fundamental mechanisms determining a desired property or function in nature,
particularly in biology, and attempts to apply the same mechanism/principles in the context of chemical engineering is the focus of Coppens paper.
He notes that application of biological mechanisms in reaction engineering
requires substantial adaptations, because the relevant time scales and
available building elements are different. For example, in reaction engineering one is able to manipulate parameters such as temperature and
pressure, which are much less tunable in biological systems. Coppens likens
NICE to an abstract portrait which preserves essential aspects of the
subject, without being its literal representation, emphasizing key features
that serve a desired objective. According to him, NICE aims to innovate
guided by nature but without mimicking it. Coppens uses three examples to
illustrate how biological mechanisms can be adapted to guide innovative

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Current Opinion in Chemical Engineering 2012, 1:269271

270 Reaction engineering and catalysis

solutions to technical challenges in Reaction and Reactor

Engineering. They include: first, the use of optimized,
hierarchical networks to bridge scales, and to minimize
transport limitations, and to realize efficient, scalable
solutions; second, careful balancing of forces at one or more
scales to achieve superior reactor performance, a key
example being enzyme nano-confinement; third, emergence of complex functions from simple components,
using dynamics as an organizing mechanism. Coppens
believes that NICE complements the ongoing revolution
in bio-inspired chemistry and materials synthesis, which
already finds applications in enzyme-mimics and antibody-mimics for catalysis, and in artificial photosynthesis.
Direct solid fuel use for electricity production using
chemical looping combustion (CLC) is discussed in the
paper by Fan and coworkers. According to the authors,
this novel approach shows the potential to have higher
energy efficiency than competing technologies in a carbon-constrained scenario, whereby CO2 must be separated and sequestered. The paper first focuses on the
selection of oxygen carriers via thermodynamic analysis,
with iron-based materials being considered as a particularly promising candidate. Then various CLC reactor
configurations are compared, based on the modes of
reducer design and operation, and are shown to significantly impact the overall system performance. The
authors conclude, based on a review of recent experimental studies by their group and others, that direct solid fuel
CLC is a promising technology, and they identify optimal
reducer design (to provide effective gassolid contact),
and favorable thermodynamics of the oxygen carrier as
the important challenges for the commercial scale application of the process.
With renewed focus on the use of energy sources other
than crude, such as coal and biomass, there has been in
recent years quite a bit of new interest in the Fischer
Tropsch Synthesis (FTS) reaction. The paper by Glasser,
Hildebrandt and coworkers reviews recent reaction and
reactor engineering advances in this area. As they note,
despite the fact that FTS has been studied for over 80
years an adequate description of its kinetics still seems to
be lacking. The authors report, for example, a number of
recent experimental results by their group and others that
are not explained by any of the existing kinetic models.
Their paper reviews some of these recent findings with
the goal of shedding light on phenomena occurring during
the FTS reaction that determine the overall rate and
selectivity, and in particular the olefin to paraffin ratios of
the lower MW hydrocarbon products. Their paper notes
that the volatile liquid-phase being present during FTS
may have a great effect on the observed kinetics, and
proposes that the FTS reactor maybe be best modeled as
a reactive distillation system, whereby the interaction
between phenomena such as vapor liquid equilibrium,
partial reaction equilibrium and kinetics can lead to
Current Opinion in Chemical Engineering 2012, 1:269271

complex behavior and, thus, explain the conflicting

reports among various researchers studying the system.
The topic of NOx reduction in lean-burn vehicle engines
is discussed in the paper by Harold. Its particular focus is
the so-called lean NOx trap (LNT), which is an adsorptive
catalytic reactor in which NOx is stored (in the form of
nitrates) in the presence of excess O2, and is subsequently
reduced during a brief regeneration. As Harold notes, this
is a transient multi-functional reactor that is called upon
to carry out NO oxidation, NOx storage, and reduction, all
within a 12 min cycle, attaining in the process NOx
conversions exceeding 95%. The paper reviews studies
by Harolds group on the coupling, under transient conditions, between reaction and transport, and describes the
current insight linking catalyst composition and structure
to conversion and selectivity. The current technical hurdles facing the emerging lean NOx reduction technologies are also nicely described.
One of the primary challenges in the conversion of
biomass to renewable fuels and chemicals is removing
the oxygen-containing functional groups. The paper by
Kruger, Nicolakis and Vlachos discusses catalytic dehydration as an effective way to deoxygenate biomass that
avoids the environmental challenges facing the current
approaches using inorganic acids. The paper reviews the
use of microporous and mesoporous catalysts for this
reaction, and tries to correlate their characteristics such
as degree and type of acidity, mesoporosity, and hydrophobicity to their performance. Review of recent studies
indicates that heterogeneous catalysts show good
promise, but the lack of fundamental understanding
may be limiting their commercial use; potential technical
barriers that need to be overcome are discussed.
Ethylene oxide is one of the most important intermediates in the chemical industry, being used to produce a
variety of chemicals, including various glycols, glycol
ethers and polyols, ethoxylates, ethanolamines, among
others. Direct catalytic epoxidation of ethylene by air or
oxygen is currently the dominant production technology
having today largely replaced the earlier, more complex
routes. Salmi and coworkers note in their paper that no
general agreement exists presently concerning its reaction mechanism and kinetics. They describe using microreactors as a tool for the rapid and precise investigations of
epoxidation kinetics. Their paper reviews and screens
rival kinetic models, and proposes a more general kinetic
model for ethylene oxide formation consistent with their
experimental data on silver catalysts.
Fuel cells find today application in many diverse areas.
Sundmacher and coworkers in their paper indicate that
despite significant progress that has been made in the last
two decades, substantial further improvements in performance and reduction in costs are potentially possible.
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Editorial overview Tsotsis 271

They identify, in particular, four areas in fuel cell research

where chemical reaction engineers can make significant
contributions. They include: first, understanding their
nonlinear dynamic electrochemical behavior, second,
improving mass and heat integration, third, being
able to use renewable biomass as a primary energy source,
and fourth, using enzymes for catalyzing the electrode
reactions.
The focus of the paper by Subramanian is on nontraditional solvents and on how they may be exploited
to develop sustainable chemical processes. The emphasis, in particular, is on gas-expanded liquids (GXL) generated by mixing liquid solvents and compressed nearcritical gases, such as CO2 and light olefins. Subramanians group and others have shown, in lab-scale studies,
that the enhanced solubility and transport properties of
GXL compared to conventional liquid solvents allow
them to carry out reactions at mild conditions, with
increased selectivity, and also provide for the facile

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separation of catalyst and products. Examples are provided of using GXL for industrially important hydroformylations and epoxidations. According to Subramanian,
GXL show particularly good promise for application in
the biorefining industry.
Liu, Sahimi and Tsotsis summarize in their paper recent
efforts by their team in producing hydrogen from coal and
biomass using membrane-based reactive separations.
They report on the development of a technology, they
term the one-box process, to produce pure hydrogen
from coal-derived and biomass-derived syngas in the
presence of its common impurities via the water gas shift
reaction, and by using commercial-scale carbon molecular
sieve membranes and impurity-tolerant commercial catalysts. They also discuss, in addition, the use of commercial-size Pd and Pd-alloy membranes during
production of ultra-pure hydrogen from coal and biomass.
Details about the recent field-testing of the technology
are also provided.

Current Opinion in Chemical Engineering 2012, 1:269271