83 research outputs found
Biocatalysis in organic synthesis
The first chapter provides an overview of the use of biocatalysis for the synthesis of pharmaceutical intermediates and natural products. This review focuses, in particular, on the impact of recent developments in technologies which enable the increased use of biocatalysts. These developments include: • the immobilisation of biocatalysts to enhance stability and ease of use, and enabling use in combination with metal and organocatalysts leading to dynamic kinetic resolution, as well as in continuous flow. • discovery and development of novel enzymes using molecular biology for enzyme engineering and metagenomics. The second chapter describes the lipase-mediated kinetic resolution of 2-phenylalkanols by tuning the steric properties of the acyl group to control the efficiency and selectivity of the resolution. In contrast to literature reports, efficient resolution was achieved using short-chain acyl groups through careful process control and substrate modification. The effect of increased steric demand at the stereocentre was also explored. Chapter three describes proof of concept that a hydrolase-catalysed dynamic kinetic resolution of a lactol is possible. By taking advantage of the spontaneous racemisation of the unreacted starting material, the dynamic kinetic resolution was carried out without the need for a separate racemisation catalyst. While the kinetic resolution was effective in a model system, the biotransformation was inhibited by the introduction of a second, remote stereocentre. Chapter four describes a dynamic kinetic resolution of synthetically versatile nitroalcohols by combination of a lipase-mediated resolution and the reversible intramolecular nitroaldol (Henry) reaction. Significant challenges in effecting the combination of the base-mediated racemisation step and the lipase-mediated resolution step were encountered. Reaction engineering allowed design of a sequential one-pot reaction system which furnished the products with excellent enantioselectivity, and good diastereoselectivity. Chapter five describes the use of novel transaminases in the kinetic resolution of model amine substrates and pharmaceutical intermediates by oxidative deamination, including exploration of the substrate scope of these novel biocatalysts. While transaminase-mediated reductive amination is an attractive method for asymmetric synthesis of chiral amines, the reductive amination is generally thermodynamically disfavoured. Preliminary investigation of approaches to favour the reductive amination is described. The final chapter contains the full experimental details, including spectroscopic and analytical data of all the compounds synthesised in this project; details of chiral phase HPLC analysis are included in the appendix
Electric vehicle: infrastructure regulatory requirements
In 2009 the European Union (EU) Directive on Renewable Energy placed an obligation on each Member State to ensure that 10% of transport energy (excluding aviation and marine transport) come from renewable sources by 2020. The Irish Government intends to achieve part of this target by making sure that 10% of all vehicles in its transport fleet are powered by electricity by 2020. Stakeholder groups include but are not limited to policy makers, the public, regulatory bodies, participants in the electricity retail market, the transmission and distribution system grid operators, the automotive industry, private enterprise, civil engineers, electrical engineers, electricians, architects, builders, building owners, building developers, building managers, fleet managers and EV owners. Currently it appears both internationally and Nationally the automotive industry is focused on EV manufacture, governments and policy makers have highlighted the potential environmental and job creation opportunities while the electricity sector is preparing for an additional electrical load on the grid system. The focus of this paper is to produce an international EV roadmap. A review of current international best practice and guidelines under consideration or recommended is presented. An update on any EV infrastructure charging equipment standards is also provided. Finally the regulatory modifications to existing National legislation as well as additional infrastructure items which may need control via new regulations are identified
The impact of recent developments in technologies which enable the increased use of biocatalysts
While biocatalytic transformations are very powerful in enantioselective synthesis, frequently occurring under mild conditions, and proceed with extraordinary selectivity, there are practical challenges associated with the use of biocatalysis, such as limited substrate scope, stability, and reusability. Recent technological developments, for example immobilization, continuous flow, and molecular biology, all contribute towards enhancing the use of enzymes in synthesis
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Developing future retail electricity markets with a customer-centric focus
Future retail electricity markets require development to accelerate the net-zero carbon transition. Adopting a customer-centric approach to market design is necessary to fully utilise smart grid technologies. In this perspective we postulate that empowering energy consumers to become an integral component of the smart grid will lead to heightened renewable energy deployment and network flexibility
Life cycle assessment of a short-rotation coppice willow riparian buffer strip for farm nutrient mitigation and renewable energy production
Publication history: Accepted - 13 January 2022; Published online - 2 February 2022.As agricultural activity intensifies across Europe there is growing concern over water quality. Agricultural run-off
is a leading cause of freshwater degradation. Simultaneously there is a continually increasing drive to promote
renewable energy and reduce greenhouse gas emissions. Willow coppice planted as a riparian buffer has been
suggested as a solution to help mitigate these problems. However, there is limited research into the use of such a
system and several key knowledge gaps remain, such as, the energy ratio of the system is not known, and a fully
harvested site has yet to be analysed in the literature. The aim of this research is to fill these knowledge gaps to
help inform agri-environmental policy. To do this a life cycle assessment was carried out on an established
willow buffer system, considering the global warming potential, eutrophication potential, acidification potential
and cumulative energy demand impact categories, alongside the calculation of the energy ratio. To our
knowledge it is the first site to be fully harvested and for which a full life cycle assessment has been carried out.
The willow was combusted to fuel a district heating system. Key results showed emissions of 4.66 kg CO2eq
GJheatout -1 and 0.01 kg SO2eq GJheatout -1, both of which are significant reductions compared to an oil heating
system (95% reductions for both impact categories). The system also resulted in the permanent nutrient removal
of 55.36 kg PO43-eq ha-1 yr-1 and had an energy ratio of 17.4, which could rise to 64 depending on the harvest
method.This Bryden Centre project is supported by the European Union’s
INTERREG VA Programme, managed by the Special EU Programmes
Body (SEUPB). The views and opinions expressed in this paper do not
necessarily reflect those of the European Commission or the Special EU
Programmes Body (SEUPB). The work was also supported by Queen’s
University Belfast and the Agri-Food and Biosciences Institute in
Northern Ireland
Production pathways for profitability and valuing ecosystem services for willow coppice in intensive agricultural applications
Publication history: Accepted - 14 January 2023; Published online - 20 January 2023Increasing agricultural sustainability is a key challenge facing the globe today. Energy crops, planted as riparian buffers are one way to support this, simultaneously mitigating water quality degradation and climate change. However, the economics of implementing such riparian buffer systems is under researched. Hence this work conducted a bottom-up economic analysis of willow coppice riparian buffers on a Northern Irish dairy farm, which is indicative of agricultural intensification across Europe. This work includes an economic assessment of a willow coppice riparian buffer strip, using harvested yield data from an established willow buffer site for the first time. It also considered the impact of harvesting technology on the economic performance of a willow coppice riparian buffer strip for the first time. The analysis considered three willow production pathways: 1) direct chip harvesting, 2) full-stem harvesting, and 3) a scenario with a guaranteed purchasing contract for fresh chip. Economic performance was considered using net present value over a 25-year plantation lifetime. The full-stem scenario provided the highest economic return over its lifetime with an average yearly net present value of £497 ha−1 (in £ sterling). This system was then considered for integration into a typical dairy farm, assuming 5 % land usage and including government grants for establishing riparian zones. The result was a drop in value of £28 ha−1 yr−1 compared to a dairy-only scenario; however, per litre of milk the farm employing willow coppice riparian buffer strips outperformed a typical dairy farm both environmentally and economically. Further analysis considered a novel approach that included payments for ecosystem services in the economic analysis. This analysis found that the implementation of government payments for ecosystem services (nutrient removal) increased the economic return of the willow coppice riparian buffer system by £400 ha−1 yr−1, resulting in minimal impact on the return from dairy land.This Bryden Centre project is supported by the European Union's INTERREG VA Programme, managed by the Special EU Programmes Body (SEUPB). The views and opinions expressed in this paper do not necessarily reflect those of the European Commission or the Special EU Programmes Body (SEUPB). The work was also supported by Queen's University Belfast and the Agri-Food and Biosciences Institute in Northern Ireland. The authors would like to thank David Gilliland of Organic Resources and Alan Hegan of Hegan Biomass for the expert insight readily provided for this research
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Decarbonizing the pulp and paper industry: a critical and systematic review of sociotechnical developments and policy options
Paper has shaped society for centuries and is considered one of humanity's most important inventions. However, pulp and paper products can be damaging to social and natural systems along their lifecycle of material extraction, processing, transportation, and waste handling. The pulp and paper industry is among the top five most energy-intensive industries globally and is the fourth largest industrial energy user. This industry accounts for approximately 6% of global industrial energy use and 2% of direct industrial CO2 emissions. The pulp and paper industry is also the largest user of original or virgin wood, with deleterious impacts on both human health and local flora and fauna, including aquatic ecosystems. This critical and systematic review seeks to identify alternatives for mitigating the climate impacts of pulp and paper processes and products, thus making the pulp and paper industry more environmentally sustainable. This study reviews 466 studies to answer the following questions: what are the main determinants of energy and carbon emissions emerging from the pulp and paper industry? What are the benefits of this industry adopting low-carbon manufacturing processes, and what barriers will need to be tackled to enable such adoption? Using a sociotechnical lens, we answer these questions, identify barriers for the pulp and paper industry's decarbonization, and present promising avenues for future research
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