Conspectus
The central theme of this Account is the development
of intensified
and sustainable chemical processes for the sequestration of CO2 in synergism with the utilization of wastes of industrial,
urban, and agricultural origins. A challenge when working with solid
waste–fluid reactions is that mass transfer limitations across
solid–liquid, solid–gas, and gas–liquid interfaces
and unfavorable thermodynamics lead to slow reaction rates, incomplete
reaction conversions, high energy expenditure and processing costs,
and inadequate product properties. The traditional macroscale approaches
to overcoming slurry reaction limitations can be effective; however,
they come at a cost to the environment. In the treatment or valorization
of low-grade and waste resources, such conventional approaches are
often unfeasible on an industrial scale. Sustainable solutions are
thus needed.
In the last six years, we have been exploring and
developing approaches
to overcoming reaction rate limitations of slurry reactions of environmental
relevance by concurrently applying process intensification strategies
and multiscale engineering approaches. The scientific approach has
relied on laboratory-scale experiments to test and refine the devised
multiscale process intensification strategies, with thermodynamic
and computational modeling work supporting the experimental work and
with advanced characterization techniques being used to elucidate
reaction and transport mechanisms and aid the development of nanoscale
reaction models and micro- and macroscale process models. The research
streams, associated with the four key references, discussed next are
(a) brine carbonation; (b) mineral carbonation and enhanced weathering;
(c) process intensification and integration; and (d) characterization
techniques.
Within the four research streams, a number of mineral
carbonation
processes have been investigated and can be classified as (i) ambient
weathering and carbonation; (ii) gas-(wet) solid accelerated carbonation;
(iii) aqueous accelerated carbonation; (iv) supercritical accelerated
carbonation; and (v) CO2 mineralization from brine. In
some cases, the research was aimed at producing valuable products
with reduced environmental risk or a reduced carbon footprint, such
as an organomineral fertilizer and zeolites. In other cases, the aim
was to assess the reactivity of minerals to match the right feedstock
with the right carbonation process, in view of maximizing net carbon
sequestration. There were also cases where the carbonation process
was reimagined by the use of innovative reaction conditions, reactors,
and reagents. The experience with accelerated weathering and carbonation
in engineered processes has been translated into the field of enhanced
rock weathering (ERW) in agriculture, where the multidisciplinary
approach used has served to advance ERW science and technology in
ways that have had a resounding effect on recent commercial deployment.
The completed research serves to encourage the adoption of process
intensification technologies ...