Towards a rational design of novel green catalysis: A computational perspective


Methane emissions now account for ~30 percent of current anthropogenic warming. Centralised methane capture and conversion, from methane rich sources such as waste processing and oil production, is an extremely promising technology for future green chemistry research. In silico studies at the UK Catalysis Hub focus on the issues holding back the industrialisation of catalytic routes for direct methane conversion. 

Materials and Methods 

High throughput QM/MM studies focus on improving the activity of metal exchange zeolites, polymers and oxygenase enzymes for the direct conversion of methane to hydrocarbons. The multiscale methods used have already shown to be extremely useful in rationalising the local and extended properties of both heme1 and non-heme dioxygenase enzymes.2

Results and Discussion 

First coordination sphere models of ([FeIV(O) (Por+) ̶ SH]),3 and (μ-nitrido-bridged diiron-oxo porphyrin),4 have proven sufficient for explaining reactivity. Collaboration with colleagues from both Cardiff Catalysis Institute and University College London have proven insightful in explaining the selectivity and reactivity of exemplar polymeric5 and microporous catalysts for methane hydroxylation, with ongoing work into the later class of material already demonstrating Au on ZSM-5 to be a powerful methane conversion catalyst.6


1. a) L. Ji, et al, Chem. Eur. J.,21, (2015) 9083–9092. b) A. S. Faponle, et al. Chemistry, 22, (2016) 5478–83.
2. a) R. Latifi, et al, Dalt. Trans.,49, (2020) 4266–4276. b) M. G. Quesne, et al. Chem. -A Eur. J., 20, (2014) 435–446. 
3. a) de Visser, et al, J. Am. Chem. Soc. 126, (2004) 8362–8363. b) K. Yoshizawa, J. Am. Chem. Soc. 123, (2001) 9806–9816. c) S. Shaik, et al, Chem. Rev. 105, (2005)2279–2328. 
4. M. G. Quesne, et al, ACS Catal. 6, (2016) 2230–2243.
5. Xie, J., Fu, C., Quesne, M.G., Guo, J., Wang, C., Xiong, L., Windle, C.D., Gadipelli, S., Guo, Z.X., Huang, W., Catlow, C.R.A., Tang, J., (2024) Nature, [in press].
6. G. Qi, et al, Nat. Catal. 5, (2022) 45–54.

M.G. Quesne 1,2 , C.R.A Catlow 1,2

1 Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Cardiff CF10 3AT, UK 
2 UK Catalysis Hub, Research Complex at Harwell, OX11 0FA, UK

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Matthew Quesne photo

Dr. Matthew Quesne undertook a PhD at the Manchester Institute of Biotechnology under the supervision of Dr Sam de Visser, in the fields of bio-mimetic and enzyme catalysis. He focused on modelling the catalytic activity of synthetic complexes of transition metal dependent homogeneous catalysts. Over the four years spent at Manchester he worked with dozens of different experimental groups and provided the in silico components to many joint computational/experimental studies. He joined the research group headed by Dr Tomasz Borowski at the Institute of Catalysis and Surface Chemistry Polish Academy of Science in Krakow (Poland) in November 2014, where he spent two years using MD, QM/MM and cluster model techniques to model enzyme catalysed reaction mechanisms. In 2016, he moved to Cardiff to work in Prof. Catlow’s group where he studied CO2 activation on a variety of transition metal carbides. This work formed a small part of a much larger EPSRC project that aimed to bring together several groups from across the UK in a multi-disciplinary fashion in order to develop integrated techniques for utilising CO2 as a feedstock for the production of fuels and fine chemicals. Matthew started his position with the UK Catalysis Hub in March of 2019 and is focused on the intersection of the modelling of heterogenously and homogenously catalysed reaction mechanisms.

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