High pressure chemistry of solids and liquids
Lead Research Organisation:
University College London
Department Name: Chemistry
Abstract
We will explore new solid state chemistries occurring under extreme conditions of high pressure and high temperature, combining high-pressure synthesis in large-volume devices with in situ studies in the diamond anvil cell. We will focus our studies on developing the solid state chemistry of new light element , compounds, based on C, O, N, H, B etc. , These usually provide molecular gases, liquids and organic compounds, but they also give rise to superhard solids like diamond and cubic boron nitride. We will also explore metastable thermodynamic pathways to new materials prepared under high-pressure conditions, combining chemical precursor routes to yield unusual new compounds and materials, and metastable compression/decompression strategies to tune the properties of the resulting materials. We will study the physical chemistry of liquids and glasses at high pressure, to explore the new phenomena of density-driven phase transitions and polyamorphism that are reported to occur in liquids and glasses at constant chemical composition. This is a new area in the physical science of liquids that needs to be explored and developed.
Organisations
People |
ORCID iD |
Paul McMillan (Principal Investigator) |
Publications
Bailey E
(2010)
High pressure synthesis of superconducting nitrides in the MoN-NbN system
in Journal of Materials Chemistry
Bailey E
(2011)
Mechanical Properties of Titanium Nitride Nanocomposites Produced by Chemical Precursor Synthesis Followed by High-P,T Treatment.
in Materials (Basel, Switzerland)
Barkalov O
(2010)
Pressure-induced transformations and superconductivity of amorphous germanium
in Physical Review B
Boyko T
(2010)
Class of tunable wide band gap semiconductors ? - ( Ge x Si 1 - x ) 3 N 4
in Physical Review B
Briggs R
(2017)
High-pressure melting behavior of tin up to 105 GPa
in Physical Review B
Briggs R
(2012)
Melting of Sn to 1 Mbar
in Journal of Physics: Conference Series
Cao E
(2007)
Application of microfabricated reactors for operando Raman studies of catalytic oxidation of methanol to formaldehyde on silver
in Catalysis Today
Cao E.
(2007)
Microfabricated reactors for mechanistic and kinetic studies of formaldehyde synthesis on silver
in 2007 AIChE Annual Meeting
Daisenberger D
(2010)
Crystal-liquid interfaces and phase relations in stable and metastable silicon at positive and negative pressure
in Physical Review B
Daisenberger D
(2007)
High-pressure x-ray scattering and computer simulation studies of density-induced polyamorphism in silicon
in Physical Review B
Daisenberger D.
(2011)
Transformations among metastable amorphous and crystalline forms of silicon
Dzivenko D
(2008)
High-pressure high-temperature synthesis of novel binary and ternary nitride phases of group 4 and 14 elements
in Journal of Physics: Conference Series
Foglia F
(2016)
Water Dynamics in Shewanella oneidensis at Ambient and High Pressure using Quasi-Elastic Neutron Scattering.
in Scientific reports
Hadzifejzovic E
(2007)
Plasma electrochemistry: electroreduction in a flame.
in Physical chemistry chemical physics : PCCP
Hazael R
(2016)
Pressure as a Limiting Factor for Life.
in Life (Basel, Switzerland)
Hazael R
(2014)
Laboratory investigation of high pressure survival in Shewanella oneidensis MR-1 into the gigapascal pressure range.
in Frontiers in microbiology
Hazael R. T.
(2012)
High pressure studies in solid state chemistry and biology
Horvath-Bordon E
(2007)
High-pressure synthesis of crystalline carbon nitride imide, C2N2(NH).
in Angewandte Chemie (International ed. in English)
Hutchins Peter Thomas
(2007)
In situ synthesis studies of silicon clathrates
Kawashima T
(2007)
High-pressure synthesis and crystal structure of ?-Mo2N
in Physica C: Superconductivity and its Applications
Knapp C
(2010)
Synthesis, AACVD and X-ray crystallographic structures of group 13 monoalkoxometallanes
in Main Group Chemistry
Knapp CE
(2012)
Dimethylalkoxygallanes: monomeric versus dimeric gas-phase structures.
in Inorganic chemistry
Knapp CE
(2008)
Dimethylalkoxygallane incorporating a donor-functionalised alkoxide: the monomeric gas-phase structure.
in Dalton transactions (Cambridge, England : 2003)
Kroll P.
(2007)
Single-crystals of a new carbon nitride phase with All-sp3 carbon
in Materials Research Society Symposium Proceedings
Machon D
(2014)
The Physics and Chemistry of Inorganic Clathrates
Machon D
(2014)
Pressure-induced amorphization and polyamorphism: Inorganic and biochemical systems
in Progress in Materials Science
Makwana NM
(2015)
Photocatalytic water disinfection by simple and low-cost monolithic and heterojunction ceramic wafers.
in Photochemical & photobiological sciences : Official journal of the European Photochemistry Association and the European Society for Photobiology
Martin L
(2007)
Metallic molecular crystals containing chiral or racemic guest molecules
in CrystEngComm
Martin L
(2007)
Multi-layered molecular charge-transfer salts containing alkali metal ions
in Journal of Materials Chemistry
McMillan P
(2007)
Treatise on Geophysics
McMillan P
(2008)
Direct density determination of low- and high-density glassy polyamorphs following a liquid-liquid phase transition in Y2O3-Al2O3 supercooled liquids
in Journal of Non-Crystalline Solids
McMillan P
(2009)
Graphitic carbon nitride C6N9H3·HCl: Characterisation by UV and near-IR FT Raman spectroscopy
in Journal of Solid State Chemistry
McMillan P
(2013)
Liquid Polymorphism
McMillan P
(2010)
High-Pressure Crystallography
McMillan P
(2010)
Going supercritical
in Nature Physics
McMillan P
(2009)
Water-soluble amorphous alumina-based ceramic precursors and alumosols: Structural and chemical characterization
in Journal of Non-Crystalline Solids
McMillan P
(2007)
Metastable phase transitions and structural transformations in solid-state materials at high pressure
in Phase Transitions
McMillan P.F.
(2010)
High-pressure synthesis of materials
in NATO Science for Peace and Security Series B: Physics and Biophysics
McMillan P.F.
(2010)
Amorphous x-ray diffraction at high pressure: Polyamorphic silicon and amyloid fibrils
in NATO Science for Peace and Security Series B: Physics and Biophysics
Mcmillan P.F.
(2013)
Polyamorphism and liquid-liquid phase transitions in amorphous silicon and supercooled Al2O3-Y2O3 liquids
in Advances in Chemical Physics
McMillan Paul F.
(2013)
POLYAMORPHISM AND LIQUID-LIQUID PHASE TRANSITIONS IN AMORPHOUS SILICON AND SUPERCOOLED Al
2O
3-Y
2O
3 LIQUIDS
in LIQUID POLYMORPHISM
McMillan PF
(2008)
Ceramic materials: levitating liquids.
in Nature materials
McMillan PF
(2007)
High-pressure chemistry: benzene bridges under pressure.
in Nature materials
Meersman F
(2009)
Compressibility of insulin amyloid fibrils determined by X-ray diffraction in a diamond anvil cell
in High Pressure Research
Description | We investigated synthesis of new nitride materials from chemical precursor routes using high pressure-high temperature approaches. We discovered a new carbon nitride hydride compound C2N3H that was recoverable to room pressure : this is the first example of a series of new dense light element phases. We produced titanium nitride amorphous-crystalline nanocomposites and tested their mechanical properties. These did not have high hardness as expected but showed signs of unusual brittle-ductile behaviour under applied load. We investigated high pressure structures and phase transitions in oxide pyrochlores to understand their dielectric properties and in photocatalytically active titanium oxonitride. We adapted our high pressure techniques to form polycrystalline discs of TiO2 for photocatalytic testing, and developed new encapsulation in Teflon containers for experiments to introduce and trap Cs+ ions inside zeolites. That work has implications for radioactive waste immobilisation. We also investigated the high pressure structural behaviour and amorphisation of zirconolite that is proposed as a refractory ceramic radionuclide host. We investigated pressure-induced amorphous-amorphous phase transitions between glasses and liquids with different density. That constitutes a new branch of physical chemistry research. We investigated the formation and recovery of high-density metallic and superconducting forms of amorphous silicon and germanium, and the emergence of a low density "polyamorph" of glassy yttria-alumina mixtures following a liquid-liquid phase transition. That project is leading to creation of new ceramic/matrix nanocomposite materials. We used the EPSRC Senior Research Fellowship to open up new areas in high pressure biology and biophysics as well as soft matter studies. We Investigated the mechanical properties of cellulose resolving a long-standing issue between compression resistance along and between the chains, and studied amyloid fibrils compressed in different media to help distinguish between different structural models. We used our new Teflon high pressure cells developed for the Cs incorporation study to begin new investigations of bacterial survival into the GigaPascal range, long thought to be impossible. Our first results showed existence of E. coli populations to at least 2 GPa following sequential cloning of pressure-adapted survivors. We also applied our facilities and expertise to investigate Raman and fluorescence spectroscopy applied to collagen and cartilage samples, and developed a new methodology for investigation of early cartilage disease. Likewise we brought the fibre-optic and microbeam Raman techniques to bear on operando and in situ studies of catalysis in microchannel flow conditions. These "spin-out" activities are now incorporated in other projects including commercial development. |
Exploitation Route | The new high pressure materials especially nitrides have potential applications in photocatalysis and other optoelectronic device applications : however the research results are still highly "upstream" and need more fundamental research and development to achieve potentially useful technology. The work on liquid-liquid phase transitions and polyamorphism can lead to new generations of nanocomposite materials with designed mechanical and thermal properties. We are exploring this for ceramic aluminate-silicate-phosphate systems with colleagues in the USA. The new area of high pressure biology can have major implications for bionanotechnology in areas ranging from environmental remediation, food processing to electrically conducting nanonetworks and nanomaterials fabrication. We are currently exploring these possible extensions of our research. Our experience and expertise with optical spectroscopy along with high pressure techniques is leading to potentially new biomedical applications such as the patented process for cartilage disease detection. Our main route is via UCL Business that provides advice and support for developing patenting and licensing strategies, and interactions with potential industry partners and other institutions. We also seek to develop personal contacts and interactions with potential collaborators and development partners both informally and at organised workshops, seminars and conferences. Another main exploitation avenue for the research is in outreach to public/schools audiences, that we participate in regularly mainly through both organised talks and conference programmes and individually organised presentations. |
Sectors | Chemicals Education Energy Environment Healthcare |
Description | The award was designed to explore the chemistry and physical properties of new solids, liquids and amorphous materials under high pressure conditions. In the area of high pressure chemistry we developed new approaches based on combining designed chemical precursors with high pressure-high temperature treatment to achieve new nitrides and other materials, some have which have potential for future technological development. The techniques developed by our group are now being implemented in other research studies in the UK and internationally. Our work on liquids and solid amorphous materials has established a firm foundation for the new physical phenomena of liquid-liquid phase transitions and polyamorphism driven by the density rather than chemical composition. The outcomes at present are mainly academic but there could be technological potential development for creation of novel nanocomposite materials. Finally the new techniques and approaches allowed us to develop first studies in new areas of high pressure biophysics, soft matter research and experimental biology, as part of a rapidly emerging new field to understand the structure and function of biologically important macromolecules and organisms under extreme conditions. results have inspired others to follow similar approaches to discover new materials and physical phenomena. They have allowed us to initiate new fields of research in high pressure biology and biophysics studies. |
First Year Of Impact | 2003 |
Sector | Chemicals,Education,Energy |
Impact Types | Societal Economic |
Description | AWE |
Amount | £1,029,248 (GBP) |
Funding ID | Enhancement of AWEs hydrodynamics science capability |
Organisation | Atomic Weapons Establishment |
Sector | Private |
Country | United Kingdom |
Start | 05/2008 |
End | 06/2013 |
Description | Leverhulme Research grant scheme |
Amount | £164,159 (GBP) |
Funding ID | RPG-350 |
Organisation | The Leverhulme Trust |
Sector | Charity/Non Profit |
Country | United Kingdom |
Start | 02/2012 |
End | 09/2015 |
Description | Materials Innovation Impact Acceleration |
Amount | £40,000 (GBP) |
Organisation | Engineering and Physical Sciences Research Council (EPSRC) |
Sector | Public |
Country | United Kingdom |
Start | 04/2014 |
End | 04/2015 |
Title | Electrode for use in a lithum-ion electrochemical cell |
Description | Carbon nitride materials to be developed for use a lithium ion battery electrodes |
IP Reference | GB1311742.9 |
Protection | Patent application published |
Year Protection Granted | 2013 |
Licensed | No |
Impact | None to date |
Title | Tissue assessment |
Description | A method to evaluate cartilage disease grade using Raman spectroscopy. |
IP Reference | GB0808711.6 |
Protection | Patent granted |
Year Protection Granted | 2009 |
Licensed | No |
Impact | The application has been tested in vivo but no partners have expressed interest to date. |
Description | Schools and public lectures |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | International |
Primary Audience | Schools |
Results and Impact | Presentations including demonstration lectures about materials chemistry, high pressure science, glasses and amorphous materials to schools and general public audiences, throughout the UK, in France and the USA |
Year(s) Of Engagement Activity | Pre-2006,2006,2007,2008,2009,2011 |