Predictive multiscale free energy simulations of hybrid transition metal catalysts
Lead Research Organisation:
UNIVERSITY COLLEGE LONDON
Department Name: Chemistry
Abstract
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Organisations
Publications
Abdul Nasir J
(2023)
Influence of Solvent on Selective Catalytic Reduction of Nitrogen Oxides with Ammonia over Cu-CHA Zeolite.
in Journal of the American Chemical Society
Abdul Nasir J
(2024)
The Rôle of Iron in Zeolite Beta for deNOx Catalysis
in Journal of Catalysis
Guan J
(2023)
Computational infrared and Raman spectra by hybrid QM/MM techniques: a study on molecular and catalytic material systems.
in Philosophical transactions. Series A, Mathematical, physical, and engineering sciences
Liu T
(2025)
Origins of intrinsic p-type conductivity, p-n transition and substoichiometry in SrO
in Journal of Materials Chemistry A
Lu Y
(2023)
Multiscale QM/MM modelling of catalytic systems with ChemShell.
in Physical chemistry chemical physics : PCCP
Zhang X
(2023)
Toward a Consistent Prediction of Defect Chemistry in CeO2.
in Chemistry of materials : a publication of the American Chemical Society
Zhang X
(2023)
Bulk and Surface Contributions to Ionisation Potentials of Metal Oxides
in Angewandte Chemie
Zhang X
(2024)
Environment-Driven Variability in Absolute Band Edge Positions and Work Functions of Reduced Ceria.
in Journal of the American Chemical Society
| Description | Theoretical vibrational spectroscopic techniques represent an important class of computational methods to answer some of the most important questions in the field of material chemistry. What we recently developed and implemented is a new set of approaches to address the large-/exa-scale computation of anharmonic vibrational Infrared and Raman spectra using hybrid QM/MM approaches. The new facility built herein helps advance the fields of theoretical vibrational spectroscopic techniques to study more realistic large-scale chemical systems using vibrational self-consistent field methods (VSCF) and related theories. Standard VSCF methods in the literature have been limited to gas-phase molecules over decades. However, the current method(s) developed here aims to lift this limit eventually. This also set the base for the development of more advanced techniques of new embedded modelling techniques. Several material systems of catalysis are under investigation using the newly developed approach, including but not limited to hydrogenation on polar ZnO surfaces and aromatic adsorbates in zeolite ZSM-5. Meanwhile, more intelligent sampling techniques have been seen and constantly developed to vastly accelerate the anharmonic vibrational calculation reliant on newly designed algorithmic techniques for VSCF. |
| Exploitation Route | Publications and open-source software |
| Sectors | Electronics Energy Environment Pharmaceuticals and Medical Biotechnology |
| Title | Vastly parallelised vibrational self-consistent field calculations under ChemShell |
| Description | A vastly parallelised vibrational self-consistent field computation infrastructure has been built and tested against molecular and catalytic material systems under ChemShell. New numerical solutions to vibrational self-consistent field theory have also been developed. |
| Type Of Material | Improvements to research infrastructure |
| Year Produced | 2023 |
| Provided To Others? | No |
| Impact | This new development enables new vibrational spectroscopy scientific studies and allows researchers to study much larger-scaled anharmonic vibrational effects, IR, Raman, and environmental impacts using hybrid QM/MM approaches. |
| Title | vibrational self-consistent field method (VSCF) redesigned for hybrid QM/MM |
| Description | A more productive VSCF development and implementation for computationally intensive hybrid QM/MM method, facilitated by more intelligent sampling techniques. |
| Type Of Material | Improvements to research infrastructure |
| Year Produced | 2025 |
| Provided To Others? | Yes |
| Impact | VSCF method has been majorly applied for gas-phase molecules with very limited application to large systems of material chemistry. Its full impacts have been limited by most standard theoretical development and implementation over the past few decades. In the current work, the algorithmic techniques are redesigned and implemented to support large systems modelled by hybrid QM/MM approaches, targeting more realistic studies of material chemistry. More advanced developments of hybrid QM/MM approaches rely on the current VSCF infrastructure. |
| Description | Cross Campus ECR Vibrational Spectroscopy Meeting (Harwell Lab, RAL) |
| Form Of Engagement Activity | A talk or presentation |
| Part Of Official Scheme? | No |
| Geographic Reach | National |
| Primary Audience | Postgraduate students |
| Results and Impact | Meeting of research community working on vibrational spectroscopy; Dr. Jingcheng Guan gave a talk on the latest development and findings from theoretical anharmonic infrared and Raman spectroscopic studies. |
| Year(s) Of Engagement Activity | 2024 |
| URL | https://www.rc-harwell.ac.uk/events/cross-campus-ecr-vibrational-spectroscopy-meeting |
| Description | International Conference on Theoretical Aspects of Catalysis 2024 (Seville, Spain) |
| Form Of Engagement Activity | A talk or presentation |
| Part Of Official Scheme? | No |
| Geographic Reach | International |
| Primary Audience | Postgraduate students |
| Results and Impact | A reputed international conference on theoretical computational aspects in catalysis science. Dr. Jingcheng Guan gave a talk at the event, and his talk sparked questions and insightful discussions on anharmonic vibrational calculations on exascale systems of interest. This activity leads to improvements in the current methodology related to vibrational self-consistent field and vibrational interaction theory. |
| Year(s) Of Engagement Activity | 2024 |
| URL | https://gestioneventos.us.es/xx-international-conference-on-theoretical-aspects-of-catalysis/prog-y-... |
| Description | MCC Workshop on the Modelling of Point Defects |
| Form Of Engagement Activity | A talk or presentation |
| Part Of Official Scheme? | No |
| Geographic Reach | National |
| Primary Audience | Postgraduate students |
| Results and Impact | A workshop targeted PhD students and postdocs working on point defects modelling; discussions on new developments and techniques have been made recently, in particular within the MCC research community, and new findings of properties of defects in various materials. Dr. Jingcheng Guan gave a talk on applying recently developed tools, for example, computational infra-red, Raman and EPR spectra, to further analyse the material defects and make a stronger correlation between theory and experimental observation. |
| Year(s) Of Engagement Activity | 2024 |
| URL | https://mcc.hec.ac.uk/events/mcc-workshop-on-the-modelling-of-point-defects/ |