https://www.repository.cam.ac.uk/items/66efc6dd-3f21-48f2-bebf-eff6aa3b4705/full

*Author*
Daniel Warnes

2025

*Abstract*
Geoengineering refers to deliberate and large scale interventions in the
Earth’s climate, in this case, in pursuit of global warming mitigation.
Stratospheric aerosol injection (SAI) and marine cloud brightening (MCB)
are two methods of geoengineering that both aim to achieve solar radiation
management, by reducing the net magnitude of radiation reaching the Earth’s
surface. Solar radiation management via geoengineering could buy the world
time in the face of climate change, but it will not preclude the
requirement to meet global net zero emissions. In fact, solar
geoengineering strategies such as SAI and MCB have many potential negative
consequences, alongside their potential to limit or reverse global warming.
Sulfates and titanium dioxide are amongst the candidates being considered
for SAI. Whilst promising, they introduce a plethora of environmental
risks. This thesis focusses on a new candidate for SAI: cellulose
nanocrystals (CNCs) as a safe and possibly sustainable alternative. It will
also investigate the potential for CNCs to act as cloud condensation
nuclei, for deliberate or inadvertent MCB. CNCs are a bio-sourced
nanomaterial, isolated from naturally occurring cellulose. A recent,
specific, use has been cellulose as a sustainable alternative to light
scattering enhancers such as titanium dioxide, as a “white pigment” in
paints and cosmetics. It is hypothesised that cellulose could be effective
as a scattering enhancer in the aerosol form too. This thesis strives to
answer two research questions: First, can the aggregation of CNCs upon
aerosolisation be controlled? It is widely understood that surface
chemistry and mechanical treatment can impact aggregation in liquid
suspensions of CNCs. A detailed analysis of the morphology of aerosolised
CNCs was performed, and related to the behaviour of the initial CNC
suspensions. These results indicate that the colloidal stability of CNC
suspensions drives aggregation in CNC aerosols, unlocking a strategy to
tune CNC aerosol morphology. Second, how do CNC aerosols perform as solar
geoengineering candidates? The work in this thesis shows that, whilst
suboptimal for marine cloud brightening due to possessing only a moderate
hygroscopicity, CNCs are promising for stratospheric aerosol injection.
Desirable properties for agents of stratospheric aerosol injection include
an ability to scatter incident shortwave solar radiation from space and a
low propensity to absorb emitted longwave radiation from Earth. Multiphase
atmospheric simulation chamber experiments enabled the understanding of
optical, physical and chemical responses of CNCs to atmospheric ageing, and
compared favourably to an existing sulfate-based SAI candidate, and
similarly to novel solid aerosol particles that have been proposed in
literature. The single scattering albedo was found to be greater than 0.99
across the shortwave spectrum and the absorption of longwave radiation was
minimal. These findings are the first step towards understanding the
aerosolisation of CNCs and can be the foundation for detailed climate
modelling of CNCs as solar geoengineering candidates.

*Source: University of Cambridge*

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