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description Publicationkeyboard_double_arrow_right Article , Other literature type 2017Embargo end date: 02 Oct 2018 GermanyPublisher:The Electrochemical Society Zachary Lebens-Higgins; Nicholas Faenza; Pinaki Mukherjee; Shawn Sallis; Fadwa Badway; Nathalie Pereira; Christoph Schlueter; Tien-Lin Lee; Frederic Cosandey; Glenn Amatucci;Louis F.J. Piper;
Louis F.J. Piper
Louis F.J. Piper in OpenAIREFor layered oxide cathodes, aluminum doping has widely been shown to improve performance, particularly at high degrees of delithiation. While this has led to increased interest in Al-doped systems, including $\mathrm{LiNi_{0.8}Co_{0.15}Al_{0.05}O_{2}}$ (NCA), the aluminum surface environment has not been thoroughly investigated. Using hard x-ray photoelectron spectroscopy measurements of the Al 1s core region for NCA electrodes, we examined the evolution of the surface aluminum environment under electrochemical and thermal stress. By correlating the aluminum environment to transition metal reduction and electrolyte decomposition, we provide further insight into the cathode-electrolyte interface layer. A remarkable finding is that Al-O coatings in LiPF$_6$ electrolyte mimic the evolution observed for the aluminum surface environment in doped layered oxides. ECS transactions 80(10), 197 - 206 (2017). doi:10.1149/08010.0197ecst Published by Pennington, NJ
add ClaimPlease grant OpenAIRE to access and update your ORCID works.This Research product is the result of merged Research products in OpenAIRE.
You have already added works in your ORCID record related to the merged Research product.This Research product is the result of merged Research products in OpenAIRE.
You have already added works in your ORCID record related to the merged Research product.All Research productsarrow_drop_down <script type="text/javascript"> <!-- document.write('<div id="oa_widget"></div>'); document.write('<script type="text/javascript" src="https://beta.openaire.eu/index.php?option=com_openaire&view=widget&format=raw&projectId=10.1149/08010.0197ecst&type=result"></script>'); --> </script>
For further information contact us at helpdesk@openaire.eu4 citations 4 popularity Average influence Average impulse Average Powered by BIP!
more_vert add ClaimPlease grant OpenAIRE to access and update your ORCID works.This Research product is the result of merged Research products in OpenAIRE.
You have already added works in your ORCID record related to the merged Research product.This Research product is the result of merged Research products in OpenAIRE.
You have already added works in your ORCID record related to the merged Research product.All Research productsarrow_drop_down <script type="text/javascript"> <!-- document.write('<div id="oa_widget"></div>'); document.write('<script type="text/javascript" src="https://beta.openaire.eu/index.php?option=com_openaire&view=widget&format=raw&projectId=10.1149/08010.0197ecst&type=result"></script>'); --> </script>
For further information contact us at helpdesk@openaire.eudescription Publicationkeyboard_double_arrow_right Article 2024Publisher:Oxford University Press (OUP) Authors:Nicholas P Burnett;
Nicholas P Burnett
Nicholas P Burnett in OpenAIRETalia Y Moore;
Talia Y Moore
Talia Y Moore in OpenAIREdoi: 10.1093/icb/icae109
pmid: 38982321
Synopsis The biological structures that fill the environment around us are derived from materials produced by organisms. These biological materials are key to the mechanical function of organisms. The pathways and growth processes that produce biological materials can influence the mechanical properties of the materials, which can in turn shape the higher level function of the system into which the materials are incorporated. Characterizing a biological system requires thorough knowledge of the underlying materials, including their mechanical function, diversity, evolution, and sensitivity to the environment. Anthropogenic activity is driving rapid and widespread changes to the natural environment and global climate, which are influencing organismal growth and physiology in myriad ways. Here, we briefly introduce a collection of articles that focus on the intersection of anthropogenic activity and the mechanical function of biological materials, as part of the “Global Change in a Material World” bundle for Integrative and Comparative Biology. In addition, we provide an analysis of the current scientific literature in this field, highlighting an urgent need to better understand how changes to our world, driven by human activity, are influencing the fundamental architecture and mechanical performance of organisms across the globe.
Integrative and Comp... arrow_drop_down Integrative and Comparative BiologyArticle . 2024 . Peer-reviewedLicense: OUP Standard Publication ReuseData sources: Crossrefadd ClaimPlease grant OpenAIRE to access and update your ORCID works.This Research product is the result of merged Research products in OpenAIRE.
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more_vert Integrative and Comp... arrow_drop_down Integrative and Comparative BiologyArticle . 2024 . Peer-reviewedLicense: OUP Standard Publication ReuseData sources: Crossrefadd ClaimPlease grant OpenAIRE to access and update your ORCID works.This Research product is the result of merged Research products in OpenAIRE.
You have already added works in your ORCID record related to the merged Research product.This Research product is the result of merged Research products in OpenAIRE.
You have already added works in your ORCID record related to the merged Research product.All Research productsarrow_drop_down <script type="text/javascript"> <!-- document.write('<div id="oa_widget"></div>'); document.write('<script type="text/javascript" src="https://beta.openaire.eu/index.php?option=com_openaire&view=widget&format=raw&projectId=10.1093/icb/icae109&type=result"></script>'); --> </script>
For further information contact us at helpdesk@openaire.eudescription Publicationkeyboard_double_arrow_right Article 2024 United KingdomPublisher:International Association for Energy Economics (IAEE) Authors: Pollitt, MG;This paper examines the 2021-2023 energy crisis in Europe exacerbated by the energy consequences of the full-scale Russia – Ukraine war which began in February 2022. We show that this is an historically unprecedented price shock to both gas and electricity prices. We then draw on lessons from UK energy policy in World War Two to inform European energy policy during this crisis. In light of this, we highlight four good and three bad policy responses to observed across Europe. The EU has responsibility for the European single market in electricity and gas (which also formally includes Norway and effectively includes the UK). We examine its attempts to co-ordinate EU-27 responses to the crisis. We conclude with longer-run lessons for energy and climate policy arising from this gas and electricity price shock.
add ClaimPlease grant OpenAIRE to access and update your ORCID works.This Research product is the result of merged Research products in OpenAIRE.
You have already added works in your ORCID record related to the merged Research product.This Research product is the result of merged Research products in OpenAIRE.
You have already added works in your ORCID record related to the merged Research product.All Research productsarrow_drop_down <script type="text/javascript"> <!-- document.write('<div id="oa_widget"></div>'); document.write('<script type="text/javascript" src="https://beta.openaire.eu/index.php?option=com_openaire&view=widget&format=raw&projectId=10.5547/01956574.45.4.mpol&type=result"></script>'); --> </script>
For further information contact us at helpdesk@openaire.eu1 citations 1 popularity Average influence Average impulse Average Powered by BIP!
more_vert add ClaimPlease grant OpenAIRE to access and update your ORCID works.This Research product is the result of merged Research products in OpenAIRE.
You have already added works in your ORCID record related to the merged Research product.This Research product is the result of merged Research products in OpenAIRE.
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For further information contact us at helpdesk@openaire.eudescription Publicationkeyboard_double_arrow_right Thesis 2023Embargo end date: 26 Apr 2023 United KingdomPublisher:Apollo - University of Cambridge Repository Authors: Corsi, Giulio;doi: 10.17863/cam.96384
Over the past several years, online disinformation and misinformation concerning climate change have gained substantive attention within the scientific community. However, while the dynamics that drive the circulation of false online information have been analysed extensively, it remains unclear whether (and how) this phenomenon can be counteracted. This research project analyses the emerging role of bottom-up mobilisations as a form of noise-reduction, thereby examining how social movements may deploy peer-produced communication narra- tives to counteract the circulation of online disinformation and misinformation relating to climate change. To investigate this communication dynamic, this research applies techniques from computational social sciences to an original dataset of ≈ 250k Facebook posts produced by two movements that best embody this novel and innovative generation of radical envi- ronmental activism: Extinction Rebellion and Fridays for Future. The central thesis of this project forwards two original contributions to the fields of climate change communication and social movement studies. First, it analyses the emergence of a new generation of radical climate change movements and the significance of this new development in climate activism (Chapter II). Second, it offers interdisciplinary empirical evidence on how radical climate movements can act as a bottom-up force for what I term ‘epistemic activism’. It presents a theoretical framework where activist-led, peer-produced communication can provide a coun- tering force to both vertical disinformation and horizontal misinformation. It quantitatively analyses two channels through which these forms of false information can be opposed. For reducing vertical disinformation, this work assesses the use of naming and shaming against information polluters (Chapter III), while for horizontal misinformation, it evaluates the dissemination of scientific counter-narratives (Chapter IV). Ultimately, this thesis shows that the two movements under analysis engage extensively in epistemic activism, with great potential to influence the online climate change debate positively.
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You have already added works in your ORCID record related to the merged Research product.This Research product is the result of merged Research products in OpenAIRE.
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For further information contact us at helpdesk@openaire.eu0 citations 0 popularity Average influence Average impulse Average Powered by BIP!
more_vert add ClaimPlease grant OpenAIRE to access and update your ORCID works.This Research product is the result of merged Research products in OpenAIRE.
You have already added works in your ORCID record related to the merged Research product.This Research product is the result of merged Research products in OpenAIRE.
You have already added works in your ORCID record related to the merged Research product.All Research productsarrow_drop_down <script type="text/javascript"> <!-- document.write('<div id="oa_widget"></div>'); document.write('<script type="text/javascript" src="https://beta.openaire.eu/index.php?option=com_openaire&view=widget&format=raw&projectId=10.17863/cam.96384&type=result"></script>'); --> </script>
For further information contact us at helpdesk@openaire.eudescription Publicationkeyboard_double_arrow_right Thesis 2023 United KingdomPublisher:Apollo - University of Cambridge Repository Authors: Gomezgil Yaspik, Vianney;doi: 10.17863/cam.102122
In recent decades, many societal changes have unfolded, including population ageing, reconfigurations of household structures, labour market transformation, and a secular deceleration of economic growth. These shifts pose considerable challenges to preexisting welfare states, particularly to the efficacy of countries’ pension systems. This dissertation examines the context and trajectory of pension reforms in Mexico, the United Kingdom, and the United States. Its contribution is to ascertain the viability and political feasibility of reforms that enhance the financial sustainability of their pension systems, while maintaining adequate income and coverage levels. The dissertation builds on political economy approaches and on the institutionalist literature, which highlight how the role of interest groups and structure of institutions and political systems shape policy outcomes. The frameworks of blame avoidance and credit-claiming are also considered, to provide a comprehensive analysis of the complex dynamics surrounding pension systems and reform efforts. This dissertation uses a mixed-methods approach – including public opinion surveys of 3,000+ individuals, semi-structured elite interviews, historical document analyses, and specialized fiscal and actuarial projections of selected pension reforms in the three selected countries. It addresses three core research questions: 1) What is the current context for pension reform in Mexico, the United Kingdom, and the United States given their histories? 2) Is the necessary (for achieving specific minimum levels of sustainability, adequacy, and coverage) pension reform politically feasible? 3) How do the characteristics of each reform affect its political feasibility? Corollary: The modification of which channel (benefits, contributions, retirement age) is perceived as more politically feasible for diverse stakeholders? The methodology chosen provides a timely picture of the context surrounding potential pension reforms in the three case studies. In Mexico, credit-claiming and the interests of private stakeholders explain the success of recent pension reforms, and partisan politics are the key determinants for future fiscal changes. For the United Kingdom, the institutionalist literature helps explain the reasons for the relatively easier reform avenues; the most politically feasible reforms are those in the private sector, while the housing market is of key importance for pensions. In the United States, the institutionalist literature and the framework of blame avoidance also help explain the current legislative gridlock and the reasons why no major reform has been enacted for decades. For Mexico and the United Kingdom there exist politically feasible reforms, notably a modification of the retirement age channel, that can increase the system’s sustainability while maintaining income adequacy and coverage; whereas based on the current context of extreme polarisation and legislative gridlock, there do not seem to exist politically feasible pension reforms that preserve the structure of Social Security in the United States. The dissertation brings the lens of political feasibility to bear on a previously technical literature on the structure of the pension systems in the three countries, and thus on the feasibility of reform to deliver financial sustainability, adequacy of retirement incomes, and adequate coverage of the old age population. It identifies the feasible routes for reform in Mexico and the United Kingdom, but concludes that the political economy context the United States has reached rules out feasible reforms of its current pension structures.
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You have already added works in your ORCID record related to the merged Research product.This Research product is the result of merged Research products in OpenAIRE.
You have already added works in your ORCID record related to the merged Research product.All Research productsarrow_drop_down <script type="text/javascript"> <!-- document.write('<div id="oa_widget"></div>'); document.write('<script type="text/javascript" src="https://beta.openaire.eu/index.php?option=com_openaire&view=widget&format=raw&projectId=10.17863/cam.102122&type=result"></script>'); --> </script>
For further information contact us at helpdesk@openaire.euAccess RoutesGreen 0 citations 0 popularity Average influence Average impulse Average Powered by BIP!
more_vert add ClaimPlease grant OpenAIRE to access and update your ORCID works.This Research product is the result of merged Research products in OpenAIRE.
You have already added works in your ORCID record related to the merged Research product.This Research product is the result of merged Research products in OpenAIRE.
You have already added works in your ORCID record related to the merged Research product.All Research productsarrow_drop_down <script type="text/javascript"> <!-- document.write('<div id="oa_widget"></div>'); document.write('<script type="text/javascript" src="https://beta.openaire.eu/index.php?option=com_openaire&view=widget&format=raw&projectId=10.17863/cam.102122&type=result"></script>'); --> </script>
For further information contact us at helpdesk@openaire.eudescription Publicationkeyboard_double_arrow_right Article , Journal 2016 ItalyPublisher:Elsevier BV Funded by:EC | NASCENTEC| NASCENTAuthors: Manuel Schnabel;Sergi Hernández;
Sergi Hernández
Sergi Hernández in OpenAIREJ. López-Vidrier;
Philipp Löper; +4 AuthorsJ. López-Vidrier
J. López-Vidrier in OpenAIREManuel Schnabel;Sergi Hernández;
Sergi Hernández
Sergi Hernández in OpenAIREJ. López-Vidrier;
Philipp Löper;J. López-Vidrier
J. López-Vidrier in OpenAIREMariaconcetta Canino;
B. Garrido; Caterina Summonte; Stefan Janz;Mariaconcetta Canino
Mariaconcetta Canino in OpenAIREThe optical and photovoltaic properties of Si NCs / SiC multilayers (MLs) are investigated using a membrane-based solar cell structure. By removing the Si substrate in the active cell area, the MLs are studied without any bulk Si substrate contribution. The occurrence is confirmed by scanning electron microscopy and light-beam induced current mapping . Optical characterization combined with simulations allows us to determine the absorption within the ML absorber layer, isolated from the other cell stack layers. The results indicate that the absorption at wavelengths longer than 800 nm is only due to the SiC matrix. The measured short-circuit current is significantly lower than that theoretically obtained from absorption within the ML absorber, which is ascribed to losses that limit carrier extraction. The origin of these losses is discussed in terms of the material regions where recombination takes place. Our results indicate that carrier extraction is most efficient from the Si NCs themselves, whereas recombination is strongest in SiC and residual a-Si domains . Together with the observed onset of the external quantum efficiency (EQE) at 700-800 nm, this fact is an evidence of quantum confinement in Si NCs embedded in SiC on device level.
CNR ExploRA arrow_drop_down Solar Energy Materials and Solar CellsArticle . 2016 . Peer-reviewedLicense: Elsevier TDMData sources: Crossrefadd ClaimPlease grant OpenAIRE to access and update your ORCID works.This Research product is the result of merged Research products in OpenAIRE.
You have already added works in your ORCID record related to the merged Research product.This Research product is the result of merged Research products in OpenAIRE.
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For further information contact us at helpdesk@openaire.euAccess RoutesGreen bronze 11 citations 11 popularity Top 10% influence Average impulse Top 10% Powered by BIP!
more_vert CNR ExploRA arrow_drop_down Solar Energy Materials and Solar CellsArticle . 2016 . Peer-reviewedLicense: Elsevier TDMData sources: Crossrefadd ClaimPlease grant OpenAIRE to access and update your ORCID works.This Research product is the result of merged Research products in OpenAIRE.
You have already added works in your ORCID record related to the merged Research product.This Research product is the result of merged Research products in OpenAIRE.
You have already added works in your ORCID record related to the merged Research product.All Research productsarrow_drop_down <script type="text/javascript"> <!-- document.write('<div id="oa_widget"></div>'); document.write('<script type="text/javascript" src="https://beta.openaire.eu/index.php?option=com_openaire&view=widget&format=raw&projectId=10.1016/j.solmat.2015.10.006&type=result"></script>'); --> </script>
For further information contact us at helpdesk@openaire.eudescription Publicationkeyboard_double_arrow_right Article 2024Publisher:AIP Publishing Authors:Yiwei Hu;
Yiwei Hu
Yiwei Hu in OpenAIREBenlei Wang;
Benlei Wang
Benlei Wang in OpenAIREZhanghua Wu;
Jianying Hu; +2 AuthorsZhanghua Wu
Zhanghua Wu in OpenAIREYiwei Hu;
Yiwei Hu
Yiwei Hu in OpenAIREBenlei Wang;
Benlei Wang
Benlei Wang in OpenAIREZhanghua Wu;
Jianying Hu;Zhanghua Wu
Zhanghua Wu in OpenAIREErcang Luo;
Ercang Luo
Ercang Luo in OpenAIREJingyuan Xu;
Jingyuan Xu
Jingyuan Xu in OpenAIREThermoacoustic technology emerges as a sustainable and low-carbon method for energy conversion, leveraging environmentally friendly working mediums and independence from electricity. This study presents the development of a multimode heat-driven thermoacoustic system designed to utilize medium/low-grade heat sources for room-temperature cooling and heating. We constructed both a simulation model and an experimental prototype for a single-unit direct-coupled thermoacoustic system, exploring its performance in heating-only, cooling-only, and hybrid heating and cooling modes. Internal characteristic analysis including an examination of internal exergy loss and a distribution analysis of key parameters was first conducted in the hybrid cooling and heating mode. The results indicated a positive-focused traveling-wave-dominant acoustic field within the thermoacoustic core unit, enhancing energy conversion efficiency. The output system performance was subsequently tested under different working conditions in the heating-only and cooling-only modes. A maximum output heating power of 2.3 kW and a maximum COPh of 1.41 were observed in the heating-only mode. Meanwhile, a cooling power of 748 W and a COPc of 0.4 were obtained in the typical cooling condition at 7 °C when operating in cooling-only mode. These findings underscore the promising potential of thermoacoustic systems for efficiently utilizing medium/low-grade heat sources for cooling and/or heating applications in the future.
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You have already added works in your ORCID record related to the merged Research product.This Research product is the result of merged Research products in OpenAIRE.
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more_vert add ClaimPlease grant OpenAIRE to access and update your ORCID works.This Research product is the result of merged Research products in OpenAIRE.
You have already added works in your ORCID record related to the merged Research product.This Research product is the result of merged Research products in OpenAIRE.
You have already added works in your ORCID record related to the merged Research product.All Research productsarrow_drop_down <script type="text/javascript"> <!-- document.write('<div id="oa_widget"></div>'); document.write('<script type="text/javascript" src="https://beta.openaire.eu/index.php?option=com_openaire&view=widget&format=raw&projectId=10.1063/5.0196770&type=result"></script>'); --> </script>
For further information contact us at helpdesk@openaire.eudescription Publicationkeyboard_double_arrow_right Thesis 2024 United KingdomPublisher:Apollo - University of Cambridge Repository Authors: Wing, Trevelyan Sherman;doi: 10.17863/cam.112842
This thesis explores Germany’s *Energiewende* (‘energy transition’) and the role of citizen/community energy democracy initiatives at municipal and state levels in shaping developments that underpin this society-wide transformation - examining how grassroots agitation, in particular, has prompted meaningful action and policy change on the part of government at multiple levels. Using Berlin and Hamburg - Germany’s largest urban centers and leading city-states in the country’s federal system - as case studies, the research examines how citizens’ initiatives in both cities have campaigned for the remunicipalization of local energy networks to expedite, democratize, and incorporate social justice goals into each region’s Energiewende. Finally, this study pivots to consider the progress of the transition nationally in recent years, investigating how major events like the Covid-19 pandemic, watershed federal elections in 2021, war in Ukraine, and the resultant energy crisis have affected the evolution and direction of the Energiewende, and the important contributions of citizen/community energy initiatives to the national response here. The analytical framework draws on over 100 interviews conducted with relevant stakeholders and experts involved in the transition, representing different perspectives (e.g. on remunicipalization and the Energiewende itself) and diverse levels of government (e.g. from the district to federal level). This extensive body of original research is complemented by a wide array of other relevant source material that has likewise been consulted to inform this work and further evaluate the impacts of bottom-up energy democracy initiatives on the broader transition in Germany’s regions - and, by extension, nationally - as they continue to affect the pace and trajectory of the now-famous Energiewende. Ultimately, this study contributes an in-depth, ground-level analysis to the literature of key elements that have driven energy system change in Germany, shining a fresh light on the complex and interrelated nexus of sustained grassroots action, policy responses, and shifting sociopolitical realities that form the context in which the Energiewende has been (re)launched, reformed, and reimagined over the decades.
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For further information contact us at helpdesk@openaire.eu0 citations 0 popularity Average influence Average impulse Average Powered by BIP!
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You have already added works in your ORCID record related to the merged Research product.This Research product is the result of merged Research products in OpenAIRE.
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For further information contact us at helpdesk@openaire.eudescription Publicationkeyboard_double_arrow_right Thesis 2022Embargo end date: 04 Nov 2022 United KingdomPublisher:Apollo - University of Cambridge Repository Authors: Smith, Collin;doi: 10.17863/cam.90350
Ammonia has been responsible for feeding population growth in the 20th century through synthetic fertilizer, and is poised to become the preferred energy storage medium for a society powered by renewable electricity in the 21st century. However, conventional brown ammonia production through the Haber-Bosch process is optimized for utilization of centralized and steady energy supply from fossil-fuels. When shifting to distributed and intermittent energy supply through wind and solar energy, a re-optimization is required for a low-capital and flexible green ammonia production processes. This thesis re-designs and Haber-Bosch process by targeting the integration of reaction and separation in a single process vessel at low pressures, thereby achieving the simplification and down-scaling of the high pressure recycle loop of the Haber-Bosch process. Materials are developed for this purpose, the feasibility of integration is demonstrated, and mathematical modeling is utilized for assessing the application of the single-vessel process to a range of renewable energy sources in comparison to competing ammonia production processes. Herein, a catalyst with low-temperature (< 350°C) and high-conversion (i.e. near equilibrium) activity is developed using ruthenium nanoparticles as the active metal supported on ceria and promoted with cesium to mitigate hydrogen and ammonia inhibition, respectively. This catalyst is compared to commercial iron-based catalyst from the perspective of the final application. Concurrently, a high-temperature (> 300°C) manganese chloride absorbent is developed that resists decomposition and is stable when supported on silica. These catalyst and absorbent are integrated in a layered reactor configuration to demonstrate the feasibility of the integrated process by exceeding single-pass reaction equilibrium. Mathematical modelling of ammonia production processes illustrates that at small-scales (< 1 t day-1) the single-vessel process is optimal compared to the Haber-Bosch process due to its modular design. In addition, it can achieve simpler ramping because the Haber-Bosch process is constrained by heat-integration in the recycle loop and the potential for runaway reaction. For final application, the pairing of ammonia production processes with examples of intermittent solar and wind sources demonstrates that the flexibility of the production process is essential when considering non-ideal sources of energy with a long-term (e.g. seasonal) oscillations. Flexible ammonia production also expands the economic usage of ammonia as an energy storage vector from the seasonal to the weekly time-scale, with advantage compared to batteries or hydrogen. The work of this thesis provides a framework for advancing the electrification of the chemical industry given the novel constrains of intermittent and distributed renewable energy. A systems level approach is applied from the ground up, starting from material design and progressing to optimized process design and application.
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You have already added works in your ORCID record related to the merged Research product.This Research product is the result of merged Research products in OpenAIRE.
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For further information contact us at helpdesk@openaire.euAccess RoutesGreen 0 citations 0 popularity Average influence Average impulse Average Powered by BIP!
more_vert add ClaimPlease grant OpenAIRE to access and update your ORCID works.This Research product is the result of merged Research products in OpenAIRE.
You have already added works in your ORCID record related to the merged Research product.This Research product is the result of merged Research products in OpenAIRE.
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For further information contact us at helpdesk@openaire.eudescription Publicationkeyboard_double_arrow_right Thesis 2023Embargo end date: 14 Jul 2023 United KingdomPublisher:Apollo - University of Cambridge Repository doi: 10.17863/cam.99818
The aggravating global problems of energy crisis, rising atmospheric greenhouse gas concentrations and accumulation of persistent waste have attracted the attention of scientists, policy-makers and global organisations to come up with effective and expeditious solutions to address these challenges. In this context, the development of sustainable technologies driven by renewable energy sources for the production of clean fuels and commodity chemicals from diverse waste feedstocks is an appealing approach towards creating a circular economy. Over the years, semiconductor photocatalysts based on TiO₂, CdS, carbon-nitrides (CNx) and carbon dots (CDs) have been widely used for the photocatalytic reforming (PC reforming) of pre-treated waste substrates to organic products, accompanied with clean hydrogen (H₂) generation. However, these conventional solar-driven processes suffer from major drawbacks such as low production rates, poor product selectivity, CO₂ release, challenging process and catalyst optimisation, and harsh waste pre-treatment conditions, which limit their commercial applicability. These challenges are tackled in this thesis with the introduction of new and efficient photoelectrochemical (PEC) and chemoenzymatic processes for reforming a diverse range of waste feedstocks to sustainable fuels. Solar-driven PEC reforming based on halide perovskite light-absorber is first developed as an attractive alternative to PC reforming. The PEC systems consist of a perovskite|Pt photocathode for clean H₂ production and a Cu-Pd alloy anode for reforming diverse waste streams, including pre-treated cellulosic biomass, polyethylene terephthalate (PET) plastics, and industrial by-product glycerol into industrially-relevant, value-added chemicals (gluconic acid, glycolic acid and glyceric acid) without any externally applied bias or voltage. Additionally, the single light-absorber PEC systems can also convert the airborne waste stream and greenhouse gas CO₂ to diverse products with the simultaneous reforming of PET plastics with no applied voltage. The perovskite-based photocathode enables the integration of different CO₂ reduction catalysts such as a molecular cobalt porphyrin, a Cu-In alloy and formate dehydrogenase enzyme, which produce CO, syngas and formate, respectively. The versatile PEC systems, which can be assembled in either a ‘two-compartment’ or standalone ‘artificial leaf’ configurations achieve 60‒90% oxidation product selectivity (with no over-oxidation) and >100 µmol cm‾² h‾¹ product formation rates, corresponding to 10²‒10⁴ times higher activity than conventional PC reforming systems. In addition to developing PEC platforms, this thesis also explores avenues for circumventing the harsh alkaline pre-treatment strategies (pH >13, 60‒80 ºC) adopted for photoreforming waste substrates. For this purpose, a chemoenzymatic pathway is introduced whereby PET and polycaprolactone plastics were deconstructed using functional enzymes under benign conditions (pH 6‒8, 37‒65 ºC), followed by PC reforming using Pt loaded TiO₂ (TiO₂|Pt) or Ni₂P loaded carbon-nitride (CNx|Ni₂P) photocatalysts. The chemoenzymatic reforming process demonstrates versatility in upcycling polyester films and nanoplastics for H₂ production at high yields reaching ∼10³‒10⁴ µmol gsub‾¹ and activities at >500 µmol gcat‾¹ h‾¹. The utilisation of enzyme pre-treated plastics also allowed the coupling of plastic reforming with photocatalytic CO₂-to-syngas conversion using a phosphonated cobalt bis(terpyridine) co-catalyst immobilised on TiO₂ (TiO₂|CotpyP). Finally, moving beyond solar-driven systems, a bio-electrocatalytic flow process is demonstrated for the conversion of microbe pre-treated food waste to ethylene (an important feedstock in the chemical industry) on graphitic carbon electrodes via succinic acid as the central intermediate. In conclusion, with its focus on improving efficiencies, achieving selective product formation, building versatile platforms, diversifying substrate and product scope, and reducing carbon footprint and economic strain, this thesis aims to bring sustainable waste-to-fuel technologies a step closer to commercial implementation.
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more_vert add ClaimPlease grant OpenAIRE to access and update your ORCID works.This Research product is the result of merged Research products in OpenAIRE.
You have already added works in your ORCID record related to the merged Research product.This Research product is the result of merged Research products in OpenAIRE.
You have already added works in your ORCID record related to the merged Research product.All Research productsarrow_drop_down <script type="text/javascript"> <!-- document.write('<div id="oa_widget"></div>'); document.write('<script type="text/javascript" src="https://beta.openaire.eu/index.php?option=com_openaire&view=widget&format=raw&projectId=10.17863/cam.99818&type=result"></script>'); --> </script>
For further information contact us at helpdesk@openaire.eu