Project acronym BIOIONS
Project Biological ions in the gas-phase: New techniques for structural characterization of isolated biomolecular ions
Researcher (PI) Caroline Dessent
Host Institution (HI) UNIVERSITY OF YORK
Call Details Starting Grant (StG), PE4, ERC-2007-StG
Summary Recent intensive research on the laser spectroscopy of neutral gas-phase biomolecules has yielded a detailed picture of their structures and conformational preferences away from the complications of the bulk environment. In contrast, work on ionic systems has been sparse despite the fact that many important molecular groups are charged under physiological conditions. To address this probelm, we have developed a custom-built laser spectrometer, which incorporates a distincitive electrospray ionisation (ESI) cluster ion source, dedicated to producing biological anions (ATP,oligonucleotides) and their microsolvated clusters for structural characterization. Many previous laser spectrometers with ESI sources have suffered from producing "hot" congested spectra as the ions were produced at ambient temperatures. This is a particularly serious limitation for spectroscopic studies of biomolecules, since these systems can possess high internal energies due tothe presence of numerous low frequency modes. Our spectrometer overcomes this problem by exploiting the newly developed physics technique of "buffer gas cooling" to produce cold ESI molecular ions. In this proposal, we now seek to exploit the new laser-spectrometer to perform detailed spectroscopic interrogations of ESI generated biomolecular anions and clusters. In addition to traditional ion-dissociation spectroscopies, we propose to develop two new laser spectroscopy techniques (Two-color tuneable IR spectroscopy and Dipole-bound excited state spectroscopy) to give the broadest possible structural characterizations of the systems of interest. Studies will focus on ATP/GTP-anions, olignonucleotides, and sulphated and carboxylated sugars. These methodologies will provide a general approach for performing temperature-controlled spectroscopic characterizations of isolated biological ions, with measurements on the corresponding micro-solvated clusters providing details of how the molecules are perturbed by solvent.
Summary
Recent intensive research on the laser spectroscopy of neutral gas-phase biomolecules has yielded a detailed picture of their structures and conformational preferences away from the complications of the bulk environment. In contrast, work on ionic systems has been sparse despite the fact that many important molecular groups are charged under physiological conditions. To address this probelm, we have developed a custom-built laser spectrometer, which incorporates a distincitive electrospray ionisation (ESI) cluster ion source, dedicated to producing biological anions (ATP,oligonucleotides) and their microsolvated clusters for structural characterization. Many previous laser spectrometers with ESI sources have suffered from producing "hot" congested spectra as the ions were produced at ambient temperatures. This is a particularly serious limitation for spectroscopic studies of biomolecules, since these systems can possess high internal energies due tothe presence of numerous low frequency modes. Our spectrometer overcomes this problem by exploiting the newly developed physics technique of "buffer gas cooling" to produce cold ESI molecular ions. In this proposal, we now seek to exploit the new laser-spectrometer to perform detailed spectroscopic interrogations of ESI generated biomolecular anions and clusters. In addition to traditional ion-dissociation spectroscopies, we propose to develop two new laser spectroscopy techniques (Two-color tuneable IR spectroscopy and Dipole-bound excited state spectroscopy) to give the broadest possible structural characterizations of the systems of interest. Studies will focus on ATP/GTP-anions, olignonucleotides, and sulphated and carboxylated sugars. These methodologies will provide a general approach for performing temperature-controlled spectroscopic characterizations of isolated biological ions, with measurements on the corresponding micro-solvated clusters providing details of how the molecules are perturbed by solvent.
Max ERC Funding
1 250 000 €
Duration
Start date: 2008-10-01, End date: 2015-06-30
Project acronym CHEMBIOMECH
Project Exploring mechanism in chemical biology by high-throughput approaches
Researcher (PI) Florian Hollfelder
Host Institution (HI) THE CHANCELLOR MASTERS AND SCHOLARS OF THE UNIVERSITY OF CAMBRIDGE
Call Details Starting Grant (StG), PE4, ERC-2007-StG
Summary In the biomedical sciences, where endless combinatorial diversity of genes, proteins and synthetic molecules is involved, miniaturisation has not simply allowed an increase in the speed at which experiment can be performed: it has given birth to new areas such as combinatorial chemistry and biology, proteomics, genomics, and more recently, systems and synthetic biology. In all these areas, the synthesis, assay and analysis of large molecular ensembles has become the essence of experimental progress. However, it is the systematic analysis of the enormous amounts of data generated that will ultimately lead to an understanding of fundamental chemical and biological problems. This proposal deals with approaches in which libraries of molecules are employed to give such mechanistic insight – into how enzyme catalysis is brought about in proteins and polymeric enzyme models and into the molecular recognition and cell biology of drug delivery reagents. In each case considerable technical challenges are involved in the way diversity is brought about and probed: ranging from either using the tools of synthetic chemistry to using gene repertoires in emulsion microdroplet reactors with femtolitre volumes, handled in microfluidic devices.
Summary
In the biomedical sciences, where endless combinatorial diversity of genes, proteins and synthetic molecules is involved, miniaturisation has not simply allowed an increase in the speed at which experiment can be performed: it has given birth to new areas such as combinatorial chemistry and biology, proteomics, genomics, and more recently, systems and synthetic biology. In all these areas, the synthesis, assay and analysis of large molecular ensembles has become the essence of experimental progress. However, it is the systematic analysis of the enormous amounts of data generated that will ultimately lead to an understanding of fundamental chemical and biological problems. This proposal deals with approaches in which libraries of molecules are employed to give such mechanistic insight – into how enzyme catalysis is brought about in proteins and polymeric enzyme models and into the molecular recognition and cell biology of drug delivery reagents. In each case considerable technical challenges are involved in the way diversity is brought about and probed: ranging from either using the tools of synthetic chemistry to using gene repertoires in emulsion microdroplet reactors with femtolitre volumes, handled in microfluidic devices.
Max ERC Funding
563 848 €
Duration
Start date: 2008-09-01, End date: 2013-08-31
Project acronym DeCO-HVP
Project Decouple Electrochemical Reduction of Carbon Dioxide to High Value Products
Researcher (PI) Kathryn Ellen TOGHILL
Host Institution (HI) UNIVERSITY OF LANCASTER
Call Details Starting Grant (StG), PE4, ERC-2018-STG
Summary This programme aims to convert carbon dioxide into high value hydrocarbon products using carbon neutral electrochemical methods. High value products are materials that may be used as carbon based chemical feedstocks and as synthetic fuels, reducing the ever-present demand on oil and natural gas to fulfil these needs. The project is within the remit of an international ambition to valorise carbon dioxide waste and reduce environmentally harmful greenhouse gas generation, as opposed to stopping at carbon capture and sequestration. This proposal outlines an alternative route to carbon dioxide utilisation (CDU), in which a mediated approach that decouples the electrochemical reduction from the catalytic process is explored. Novel bimetallic catalysts will be synthesised and studied, meditating electron donating solutions will be generated, and a robust and comprehensive analytical arrangement will be implemented to allow total identification and quantification of the wide range of possible products.
Electrocatalytic CO2 reduction is one of the key approaches to CDU, as it has a direct pathway to carbon neutral renewable electricity. Nonetheless it is a field that has shown minimal progress in the past 30 years. A paradigm shift is necessary in the approach to electrochemical CO2 reduction, where conventional heterogeneous interfacial catalysis is limited by mass transport, passivation, and CO2 solubility. This proposal outlines the use of electron donating mediators generated separately to the catalysed chemical reduction of CO2, such that the electrolyte becomes the electrode. This opens a whole new avenue for catalyst research, and here target bimetallic catalysts that suppress side reactions and promote high value product synthesis are described.
Summary
This programme aims to convert carbon dioxide into high value hydrocarbon products using carbon neutral electrochemical methods. High value products are materials that may be used as carbon based chemical feedstocks and as synthetic fuels, reducing the ever-present demand on oil and natural gas to fulfil these needs. The project is within the remit of an international ambition to valorise carbon dioxide waste and reduce environmentally harmful greenhouse gas generation, as opposed to stopping at carbon capture and sequestration. This proposal outlines an alternative route to carbon dioxide utilisation (CDU), in which a mediated approach that decouples the electrochemical reduction from the catalytic process is explored. Novel bimetallic catalysts will be synthesised and studied, meditating electron donating solutions will be generated, and a robust and comprehensive analytical arrangement will be implemented to allow total identification and quantification of the wide range of possible products.
Electrocatalytic CO2 reduction is one of the key approaches to CDU, as it has a direct pathway to carbon neutral renewable electricity. Nonetheless it is a field that has shown minimal progress in the past 30 years. A paradigm shift is necessary in the approach to electrochemical CO2 reduction, where conventional heterogeneous interfacial catalysis is limited by mass transport, passivation, and CO2 solubility. This proposal outlines the use of electron donating mediators generated separately to the catalysed chemical reduction of CO2, such that the electrolyte becomes the electrode. This opens a whole new avenue for catalyst research, and here target bimetallic catalysts that suppress side reactions and promote high value product synthesis are described.
Max ERC Funding
1 499 994 €
Duration
Start date: 2018-10-01, End date: 2023-09-30
Project acronym DESI_JEDI-IMAGING
Project Development of mass spectrometric techniques for 3D imaging and in-vivo analysis of biological tissues
Researcher (PI) Zoltan Takats
Host Institution (HI) IMPERIAL COLLEGE OF SCIENCE TECHNOLOGY AND MEDICINE
Call Details Starting Grant (StG), PE4, ERC-2007-StG
Summary Recent development of atmospheric pressure desorption ionization methods has opened a unique area of application for analytical mass spectrometry. Most of these methods do not require any modification of samples, and this feature, together with the minimal invasiveness of these methods allows direct analytical interrogation of biological tissues, even the real-time, in-vivo observation of biochemical processes. The proposed research focuses on the development of atmospheric pressure desorption ionization mass spectrometric methods for the characterization of biological tissues. The first question to answer is aimed at the nature of information which can be obtained, using a variety of desorption ionization methods including desorption electrospray ionization and jet desorption ionization methods. Preliminary results show, that APDI-MS methods provide information on lipids, metabolic compounds, drugs and certain proteins. First task of the proposed research is to implement a chemical imaging system, which is capable of producing 3D concentration distribution functions for various constituents of tissue samples. The developed methodology will be used to tackle fundamental pathophysiological problems including development of various malignant tumors. A database will be created for the unequivocal identification of various tissues including healthy and malignant tissue samples. In-vivo applications of MS will also be developed. JeDI-MS,similarly to water jet surgery, also utilizes high velocity water jet can directly be used as an intelligent scalpel. Real-time in-situ tissue identification has the potential of revolutionizing cancer surgery, since this way the amount of removed tissue can be minimized, while the tumor removal efficiency is maximized. The identical experimental platform can also be used to gather real-time in-situ metabolic information, which can help to understand pathophysiological changes.
Summary
Recent development of atmospheric pressure desorption ionization methods has opened a unique area of application for analytical mass spectrometry. Most of these methods do not require any modification of samples, and this feature, together with the minimal invasiveness of these methods allows direct analytical interrogation of biological tissues, even the real-time, in-vivo observation of biochemical processes. The proposed research focuses on the development of atmospheric pressure desorption ionization mass spectrometric methods for the characterization of biological tissues. The first question to answer is aimed at the nature of information which can be obtained, using a variety of desorption ionization methods including desorption electrospray ionization and jet desorption ionization methods. Preliminary results show, that APDI-MS methods provide information on lipids, metabolic compounds, drugs and certain proteins. First task of the proposed research is to implement a chemical imaging system, which is capable of producing 3D concentration distribution functions for various constituents of tissue samples. The developed methodology will be used to tackle fundamental pathophysiological problems including development of various malignant tumors. A database will be created for the unequivocal identification of various tissues including healthy and malignant tissue samples. In-vivo applications of MS will also be developed. JeDI-MS,similarly to water jet surgery, also utilizes high velocity water jet can directly be used as an intelligent scalpel. Real-time in-situ tissue identification has the potential of revolutionizing cancer surgery, since this way the amount of removed tissue can be minimized, while the tumor removal efficiency is maximized. The identical experimental platform can also be used to gather real-time in-situ metabolic information, which can help to understand pathophysiological changes.
Max ERC Funding
1 750 000 €
Duration
Start date: 2008-09-01, End date: 2013-08-31
Project acronym ENERGYBIOCATALYSIS
Project Understanding and Exploiting Biological Catalysts for Energy Cycling: Development of Infrared Spectroelectrochemistry for Studying Intermediates in Metalloenzyme Catalysis
Researcher (PI) Kylie Alison Vincent
Host Institution (HI) THE CHANCELLOR, MASTERS AND SCHOLARS OF THE UNIVERSITY OF OXFORD
Call Details Starting Grant (StG), PE4, ERC-2010-StG_20091028
Summary Advanced catalysts for energy cycling will be essential to a future sustainable energy economy. Interconversion of water and hydrogen allows solar and other green electricity to be stored in transportable form as H2 - a fuel for electricity generation on demand. Precious metals (Pt) are the best catalysts currently available for H2 oxidation in fuel cells. In contrast, readily available Ni/Fe form the catalytic centres of robust enzymes used by micro-organisms to oxidise or produce H2 selectively, at rates rivalling platinum. Metalloenzymes also efficiently catalyse redox reactions of the nitrogen and carbon cycles. Electrochemistry of enzyme films on a graphite electrode provides a direct route to studying and exploiting biocatalysis, for example a fuel cell that produces electricity from dilute H2 in air using an electrode modified with hydrogenase. Understanding structures and complex chemistry of enzyme active sites is now an important challenge that underpins exploitation of enzymes and design of future catalysts. This project develops sensitive IR methods for metalloenzymes on conducting surfaces or particles. Ligands with strong InfraRed vibrational signatures (CO, CN-) are exploited as probes of active site chemistry for hydrogenases and carbon-cycling enzymes. The proposal unites physical techniques (surface vibrational spectroscopy, electrochemistry), microbiology (mutagenesis, microbial energy cycling), inorganic chemistry (reactions at unusual organometallic centres) and technology development (energy-catalysis) in addressing enzyme chemistry. Understanding the basis for the extreme catalytic selectivity of enzymes will contribute to knowledge of biological energy cycling and provide inspiration for new catalysts.
Summary
Advanced catalysts for energy cycling will be essential to a future sustainable energy economy. Interconversion of water and hydrogen allows solar and other green electricity to be stored in transportable form as H2 - a fuel for electricity generation on demand. Precious metals (Pt) are the best catalysts currently available for H2 oxidation in fuel cells. In contrast, readily available Ni/Fe form the catalytic centres of robust enzymes used by micro-organisms to oxidise or produce H2 selectively, at rates rivalling platinum. Metalloenzymes also efficiently catalyse redox reactions of the nitrogen and carbon cycles. Electrochemistry of enzyme films on a graphite electrode provides a direct route to studying and exploiting biocatalysis, for example a fuel cell that produces electricity from dilute H2 in air using an electrode modified with hydrogenase. Understanding structures and complex chemistry of enzyme active sites is now an important challenge that underpins exploitation of enzymes and design of future catalysts. This project develops sensitive IR methods for metalloenzymes on conducting surfaces or particles. Ligands with strong InfraRed vibrational signatures (CO, CN-) are exploited as probes of active site chemistry for hydrogenases and carbon-cycling enzymes. The proposal unites physical techniques (surface vibrational spectroscopy, electrochemistry), microbiology (mutagenesis, microbial energy cycling), inorganic chemistry (reactions at unusual organometallic centres) and technology development (energy-catalysis) in addressing enzyme chemistry. Understanding the basis for the extreme catalytic selectivity of enzymes will contribute to knowledge of biological energy cycling and provide inspiration for new catalysts.
Max ERC Funding
1 373 322 €
Duration
Start date: 2011-02-01, End date: 2016-01-31
Project acronym IMAGEMS
Project Exploring applications of spatial-map and velocity-map imaging mass spectrometry
Researcher (PI) Claire Vallance
Host Institution (HI) THE CHANCELLOR, MASTERS AND SCHOLARS OF THE UNIVERSITY OF OXFORD
Call Details Starting Grant (StG), PE4, ERC-2007-StG
Summary Our aim is to develop a next-generation mass spectrometer with unique imaging capabilities. For each mass, the new instrument will image the complete velocity or spatial distribution of the ions at their point of formation. The velocity distributions of fragment ions are highly sensitive to the detailed dynamics of the fragmentation process, such that in velocity imaging mode the new instrument will provide a powerful alternative to conventional tandem mass spectrometry approaches for fragmentation studies. In addition to the mechanistic and structural information encoded the images, the set of photofragment velocity distributions constitutes a unique ‘fingerprint’ for the parent molecule that may be used in molecular identification. In spatial imaging mode, there are clear applications in the areas of surface analysis and high throughput sampling, both of which will be explored over the course of the project. The spectrometer will utilise the method of velocity/spatial-map imaging, a technique originally developed for studying the photofragmentation dynamics of small molecules. A standard velocity-map imaging measurement yields the detailed speed and angular distributions for a single fragment. However, by employing advanced detector technology, our instrument will be capable of recording such distributions for all fragments simultaneously, opening the way for the study of much larger molecules with complex fragmentation pathways. A working prototype of the spectrometer will be constructed within the first year of the project, with further developments and improvements taking place over the remaining four years. The instrument will be calibrated using results from previous studies, and its capabilities in both spatial and velocity-map imaging modes will then be explored using a number of carefully chosen chemical systems. These include fundamental dynamics studies, ultraviolet photodissociation of peptides, and imaging of biomolecules and single cells on surfaces.
Summary
Our aim is to develop a next-generation mass spectrometer with unique imaging capabilities. For each mass, the new instrument will image the complete velocity or spatial distribution of the ions at their point of formation. The velocity distributions of fragment ions are highly sensitive to the detailed dynamics of the fragmentation process, such that in velocity imaging mode the new instrument will provide a powerful alternative to conventional tandem mass spectrometry approaches for fragmentation studies. In addition to the mechanistic and structural information encoded the images, the set of photofragment velocity distributions constitutes a unique ‘fingerprint’ for the parent molecule that may be used in molecular identification. In spatial imaging mode, there are clear applications in the areas of surface analysis and high throughput sampling, both of which will be explored over the course of the project. The spectrometer will utilise the method of velocity/spatial-map imaging, a technique originally developed for studying the photofragmentation dynamics of small molecules. A standard velocity-map imaging measurement yields the detailed speed and angular distributions for a single fragment. However, by employing advanced detector technology, our instrument will be capable of recording such distributions for all fragments simultaneously, opening the way for the study of much larger molecules with complex fragmentation pathways. A working prototype of the spectrometer will be constructed within the first year of the project, with further developments and improvements taking place over the remaining four years. The instrument will be calibrated using results from previous studies, and its capabilities in both spatial and velocity-map imaging modes will then be explored using a number of carefully chosen chemical systems. These include fundamental dynamics studies, ultraviolet photodissociation of peptides, and imaging of biomolecules and single cells on surfaces.
Max ERC Funding
1 499 969 €
Duration
Start date: 2008-06-01, End date: 2013-05-31
Project acronym InsideChromatin
Project Towards Realistic Modelling of Nucleosome Organization Inside Functional Chromatin Domains
Researcher (PI) Rosana COLLEPARDO GUEVARA
Host Institution (HI) THE CHANCELLOR MASTERS AND SCHOLARS OF THE UNIVERSITY OF CAMBRIDGE
Call Details Starting Grant (StG), PE4, ERC-2018-STG
Summary Reading the genome is one thing – finding out how it functions, is something else altogether. The next big challenge to understand gene behaviour is deciphering (a) how the genome is organized in space and (b) how this organization influences its function. Inside Eukaryotic cells, genomic DNA is packed together with proteins into a remarkable structure known as chromatin. Nucleosomes, the building blocks of chromatin, interact with each other to enable high-density packaging. Our understanding of chromatin structure is limited by the lack of ‘close up views’ and molecular-level mechanistic information of how nucleosome interactions are regulated in vivo by many highly coupled factors.
InsideChromatin aims to develop a groundbreaking multiscale approach that will push the current limits of realistic computational modelling of in vivo chromatin structure. The vision is to achieve the first multiscale simulation study that describes nucleosome organization inside functionally different kilobase-scale domains, while explicitly accounting for the combination of epigenetic marks, the binding of architectural proteins, and nucleosome remodelling activity that distinguishes each domain. InsideChromatin will integrate atomistic simulations with two levels of coarse-graining and experimental data for validation to understand how nucleosome organization at kilobase scales leads to physical properties at megabase scales. The output from InsideChromatin will bring us closer to the ‘holy grail’ of deciphering the connection between genome characteristics, structure, and function.
Summary
Reading the genome is one thing – finding out how it functions, is something else altogether. The next big challenge to understand gene behaviour is deciphering (a) how the genome is organized in space and (b) how this organization influences its function. Inside Eukaryotic cells, genomic DNA is packed together with proteins into a remarkable structure known as chromatin. Nucleosomes, the building blocks of chromatin, interact with each other to enable high-density packaging. Our understanding of chromatin structure is limited by the lack of ‘close up views’ and molecular-level mechanistic information of how nucleosome interactions are regulated in vivo by many highly coupled factors.
InsideChromatin aims to develop a groundbreaking multiscale approach that will push the current limits of realistic computational modelling of in vivo chromatin structure. The vision is to achieve the first multiscale simulation study that describes nucleosome organization inside functionally different kilobase-scale domains, while explicitly accounting for the combination of epigenetic marks, the binding of architectural proteins, and nucleosome remodelling activity that distinguishes each domain. InsideChromatin will integrate atomistic simulations with two levels of coarse-graining and experimental data for validation to understand how nucleosome organization at kilobase scales leads to physical properties at megabase scales. The output from InsideChromatin will bring us closer to the ‘holy grail’ of deciphering the connection between genome characteristics, structure, and function.
Max ERC Funding
1 490 380 €
Duration
Start date: 2019-04-01, End date: 2024-03-31
Project acronym INTRODUCING SPRITES
Project Real-Time Observation of Biological Reactions Using Femtosecond 2D-IR Spectroscopy – Introducing SPRITES
Researcher (PI) Neil Terence Hunt
Host Institution (HI) UNIVERSITY OF STRATHCLYDE
Call Details Starting Grant (StG), PE4, ERC-2007-StG
Summary A fundamental question facing physical chemistry and biology is to determine the basic mechanisms by which biological molecules react and change structure. Ultrafast two dimensional infrared (2D-IR) spectroscopy has emerged as an exciting new tool for probing the structure and dynamics of bio-systems. This proposal is the first concerted application of transient 2D-IR spectroscopy to answer pressing questions relating to reactions of biological systems. The unique combination of ultrafast time resolution and structural insight makes 2D-IR the perfect platform to observe real-time structure changes during reactions. We will exploit this ability by developing SPRITES – Structure changes in Protein Reactions via Infrared Time Evolution Spectroscopy. We will trigger reactions in peptide and enzyme systems and use 2D-IR as a time-delayed probe of molecular structure to follow them in unprecedented real-time detail. This ambitious project will be split into three stages for reasons of risk management: In stage one, simple photochemical reactions of model compounds of the hydrogenase enzyme active site will be initiated and the structural evolution of the reactants followed using 2D-IR. In stage two, the novel pH-jump SPRITES technique will be developed to study peptide folding reactions. These experiments will lead to a “molecular movie” of a folding peptide in a natural environment, representing a unique scientific development. The final stage of the project will use pH-jump SPRITES to initiate and observe the reaction of a complete hydrogenase enzyme. This ambitious final stage will yield unprecedented insight into the mechanisms of biological reactions. The purpose of the proposal is to assist the PI in consolidating the independence gained through the award of a prestigious EPSRC Fellowship. The proposal seeks funding to create a research team of two postdoctoral research associates and two PhD students. This team will be managed and directed by the PI.
Summary
A fundamental question facing physical chemistry and biology is to determine the basic mechanisms by which biological molecules react and change structure. Ultrafast two dimensional infrared (2D-IR) spectroscopy has emerged as an exciting new tool for probing the structure and dynamics of bio-systems. This proposal is the first concerted application of transient 2D-IR spectroscopy to answer pressing questions relating to reactions of biological systems. The unique combination of ultrafast time resolution and structural insight makes 2D-IR the perfect platform to observe real-time structure changes during reactions. We will exploit this ability by developing SPRITES – Structure changes in Protein Reactions via Infrared Time Evolution Spectroscopy. We will trigger reactions in peptide and enzyme systems and use 2D-IR as a time-delayed probe of molecular structure to follow them in unprecedented real-time detail. This ambitious project will be split into three stages for reasons of risk management: In stage one, simple photochemical reactions of model compounds of the hydrogenase enzyme active site will be initiated and the structural evolution of the reactants followed using 2D-IR. In stage two, the novel pH-jump SPRITES technique will be developed to study peptide folding reactions. These experiments will lead to a “molecular movie” of a folding peptide in a natural environment, representing a unique scientific development. The final stage of the project will use pH-jump SPRITES to initiate and observe the reaction of a complete hydrogenase enzyme. This ambitious final stage will yield unprecedented insight into the mechanisms of biological reactions. The purpose of the proposal is to assist the PI in consolidating the independence gained through the award of a prestigious EPSRC Fellowship. The proposal seeks funding to create a research team of two postdoctoral research associates and two PhD students. This team will be managed and directed by the PI.
Max ERC Funding
999 745 €
Duration
Start date: 2008-08-01, End date: 2012-07-31
Project acronym PHOTO-EM
Project Solar cells at the nanoscale: imaging active photoelectrodes in the transmission electron microscope
Researcher (PI) Caterina Ducati
Host Institution (HI) THE CHANCELLOR MASTERS AND SCHOLARS OF THE UNIVERSITY OF CAMBRIDGE
Call Details Starting Grant (StG), PE4, ERC-2010-StG_20091028
Summary The exploitation of renewable sources of energy is one of the biggest challenges of our time, with wide ranging implications in both Science and Society. The new generation of dye-sensitized solar cells and hybrid polymer-inorganic solar cells represents one of the most exciting developments in this field. These promising devices based on photoactive nanomaterials can be produced at low cost, but they have an overall power conversion efficiency of 10-12%, attributed to short charge carrier recombination times and diffusion lengths. If we hope to improve this performance we must learn how the solar cells behave at the nanoscale, under realistic working conditions.
To achieve this I propose to study photovoltaic materials in the transmission electron microscope, under photon irradiation. The three main areas to pursue are: a) In situ illumination technique development, b) Study of physical properties of solar cells, c) Theoretical interpretation of the spectroscopy results. The work plan of this ERC project will follow different strands in parallel, so that we can explore this novel field more efficiently.
Our in situ illumination technique will be exported to a new monochromated and aberration corrected transmission electron microscope with very high spatial and energy resolution. The ultimate challenge is to provide maps of the electronic properties and photovoltaic behaviour of a solar cell, in particular to evaluate –on the atomic level- the effect of grain boundaries and surfaces on the performance of the device.
We will study both dye-sensitized and bulk heterojunction solar cells, starting from the individual nanostructured components, with the aim of producing working cross-section devices to be mounted and operated inside the electron microscope. Efficient data processing and theoretical interpretation of the microscopy results will be essential to the success of this process, so we will build capabilities in these areas to support and guide the experimental work.
The team I want to lead in this scientific mission is ideally composed of a postdoctoral research assistant and two PhD students. The postdoc will take care of technique development and theoretical aspects, while the students will concentrate on the study of materials and devices.
Summary
The exploitation of renewable sources of energy is one of the biggest challenges of our time, with wide ranging implications in both Science and Society. The new generation of dye-sensitized solar cells and hybrid polymer-inorganic solar cells represents one of the most exciting developments in this field. These promising devices based on photoactive nanomaterials can be produced at low cost, but they have an overall power conversion efficiency of 10-12%, attributed to short charge carrier recombination times and diffusion lengths. If we hope to improve this performance we must learn how the solar cells behave at the nanoscale, under realistic working conditions.
To achieve this I propose to study photovoltaic materials in the transmission electron microscope, under photon irradiation. The three main areas to pursue are: a) In situ illumination technique development, b) Study of physical properties of solar cells, c) Theoretical interpretation of the spectroscopy results. The work plan of this ERC project will follow different strands in parallel, so that we can explore this novel field more efficiently.
Our in situ illumination technique will be exported to a new monochromated and aberration corrected transmission electron microscope with very high spatial and energy resolution. The ultimate challenge is to provide maps of the electronic properties and photovoltaic behaviour of a solar cell, in particular to evaluate –on the atomic level- the effect of grain boundaries and surfaces on the performance of the device.
We will study both dye-sensitized and bulk heterojunction solar cells, starting from the individual nanostructured components, with the aim of producing working cross-section devices to be mounted and operated inside the electron microscope. Efficient data processing and theoretical interpretation of the microscopy results will be essential to the success of this process, so we will build capabilities in these areas to support and guide the experimental work.
The team I want to lead in this scientific mission is ideally composed of a postdoctoral research assistant and two PhD students. The postdoc will take care of technique development and theoretical aspects, while the students will concentrate on the study of materials and devices.
Max ERC Funding
1 381 541 €
Duration
Start date: 2010-12-01, End date: 2015-11-30
Project acronym QUANTUMCRASS
Project Towards a fully quantum ab initio treatment of chemical reactions at solid surfaces
Researcher (PI) Angelos Michaelides
Host Institution (HI) UNIVERSITY COLLEGE LONDON
Call Details Starting Grant (StG), PE4, ERC-2007-StG
Summary The making and breaking of bonds involving hydrogen atoms at the surfaces of materials plays a major role in nature. For example, the formation and activation of C-H, N-H, and O-H bonds lies at the heart of heterogeneous catalysis and is no less important to other disciplines such as electrochemistry and astrophysics, not to mention the widely discussed “hydrogen economy” of the future. When dealing with hydrogen, quantum nuclear effects - tunnelling and quantum delocalization - can be significant at room temperature and below. Despite this fact, and despite growing economic and environmental incentives to carry out hydrogenation and dehydrogenation reactions at lower temperatures most theoretical studies neglect the role quantum nuclear effects play in such processes. Here, we will address this by developing and applying ab initio path integral techniques for the rigorous treatment of quantum nuclear effects in elementary diffusion and reaction events at solid surfaces. The path integral formalism of quantum mechanics provides a powerful approach for treating quantum nuclear effects and when done with an ab initio determination of the underlying potential energy surface highly accurate predictions can be achieved. This project will begin with ab initio path integral simulations of time independent quantum properties such as addressing the extent of quantum delocalisation of adsorbed hydrogen atoms and hydrogen atoms incorporated in molecules adsorbed on solid surfaces. Following this ab initio centroid molecular dynamics techniques specifically designed for the determination of quantum transition state theory rate constants and mechanisms of elementary reaction and diffusion processes at solid surfaces will be developed. This highly ambitious project will culminate in the fully quantum treatment of several elementary reactions at metal surfaces and in so doing open up a new research frontier: the fully quantum path integral treatment of surface chemistry.
Summary
The making and breaking of bonds involving hydrogen atoms at the surfaces of materials plays a major role in nature. For example, the formation and activation of C-H, N-H, and O-H bonds lies at the heart of heterogeneous catalysis and is no less important to other disciplines such as electrochemistry and astrophysics, not to mention the widely discussed “hydrogen economy” of the future. When dealing with hydrogen, quantum nuclear effects - tunnelling and quantum delocalization - can be significant at room temperature and below. Despite this fact, and despite growing economic and environmental incentives to carry out hydrogenation and dehydrogenation reactions at lower temperatures most theoretical studies neglect the role quantum nuclear effects play in such processes. Here, we will address this by developing and applying ab initio path integral techniques for the rigorous treatment of quantum nuclear effects in elementary diffusion and reaction events at solid surfaces. The path integral formalism of quantum mechanics provides a powerful approach for treating quantum nuclear effects and when done with an ab initio determination of the underlying potential energy surface highly accurate predictions can be achieved. This project will begin with ab initio path integral simulations of time independent quantum properties such as addressing the extent of quantum delocalisation of adsorbed hydrogen atoms and hydrogen atoms incorporated in molecules adsorbed on solid surfaces. Following this ab initio centroid molecular dynamics techniques specifically designed for the determination of quantum transition state theory rate constants and mechanisms of elementary reaction and diffusion processes at solid surfaces will be developed. This highly ambitious project will culminate in the fully quantum treatment of several elementary reactions at metal surfaces and in so doing open up a new research frontier: the fully quantum path integral treatment of surface chemistry.
Max ERC Funding
912 916 €
Duration
Start date: 2008-08-01, End date: 2012-07-31
