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RESEARCH SUMMARY

My goal is to apply sustainable synthesis and advanced manufacturing techniques in the development of a new, cost-effective catalyst with superior performance for environmental remediation, utilising nanoporous materials. Through this work, I aim to address pressing global challenges and support the United Nations' Sustainable Development Goals, with a focus on achieving clean energy (Goal 7), reducing plastic waste (Goal 12), and mitigating global warming (Goal 13).

Main Research Areas:

  • Porous materials synthesis and characterisation

  • Synthesis of hierarchical porous materials using green and scalable synthetic approaches

  • Innovative catalyst technologies using functional porous materials 

  • Energy conversion and storage using hierarchical porous materials

research summary

One of my key scientific contributions was the development of a low-solvent, more environmentally-friendly synthesis route for the production of copper-based MOF catalysts with hierarchical porosity. I have developed a new method using supercritical CO2 (scCO2) as a time- and material-efficient route to MOF synthesis with a high level of control over the crystallization process for accessing tailored material properties. I also made significant intellectual contributions to the development of intelligent scalable synthetic methods to produce additional large pores in defective MOF structures which were shown to be highly beneficial for their catalytic activity. The impact of this approach on heterogeneous catalysis was that these new MOFs with hierarchical porosity delivered an enhanced performance with fast intercalation of reactants into active sites. 

Furthermore, my experience in using sustainable synthetic approaches has allowed me to achieve the economical production of nanomaterials. For instance, I have demonstrated the development of nanocomposites with novel heterostructures using cheap resources such as plastic waste and natural halloysite, for example, producing multifunctional AgInS2@MIL-101(Cr) and O-g-C3N4@MIL-53(Fe) materials with enhanced porosity via a facile preparation, Co-Fe-BTC/CN nanocomposite with bimetallic structures via a microwave-assisted hydrothermal method and Ag@AgBr/Al-SBA-15, Ag-g-C3N4@HNT and V2O5/Al-SBA-15 with semiconductor-containing porous structures via a one-pot and green synthetic approach. The novel nanocomposites were shown to improve the activity of visible-light-driven catalysts for the efficient treatment of multiple toxic pollutants in water. This could allow wastes to be transformed into economically valuable materials again and protect wildlife and the environment from further pollution. 

RESEARCH BLOGS


MOF formation in scCO2

In this report, we explore the use of supercritical CO2 (scCO2) in the synthesis of well-known metal-organic frameworks (MOFs) including Zn-MOF-74 and UiO-66, as well as on the preparation of [Cu24(OH-mBDC)24]n metal-organic polyhedra (MOPs) and two new MOF structures {[Zn2(L1)(DPE)]∙4H2O}n and {[Zn3(L1)3(4,4/-azopy)]∙7.5H2O}n, where BTC = benzene-1,3,5-tricarboxylate, BDC = benzene-1,4-dicarboxylate, L1 = 4-carboxy-phenylene-methyleneamino-4-benzoate, DPE = 1,2-di(4-pyridyl)ethylene, 4.4/-azopy = 4,4/- azopyridine, and compare the results versus traditional solvothermal preparations at low temperatures (i.e., 40 °Ϲ). The objective of the work was to see if the same or different products would result from the ssCO2 route versus the solvothermal method. We were interested to see which method produced the highest yield, the cleanest product and what types of morphology resulted. While there was no evidence of additional meso- or macroporosity in these MOFs/MOPs nor any significant improvements in product yields through the addition of scCO2 to these systems, it was shown that the use of scCO2 can have an effect on crystallinity, crystal size and morphology.

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MOF for pesticide delivery

Controlled-release technologies are considered a key solution to deliver both pheromones and pesticides for better environmental and economical benefits. Metal-organic frameworks (MOFs) have gained a certain success in this area to deliver drug molecules. In this study, three different zirconium-based MOFs with different linkers (benzene-1,4-dicarboxylate, 2-aminobenzene-1,4-dicarboxylate and 2-(propylamino)benzene-1,4-dicarboxylate) were synthesised via a solvothermal method and examined for their possible use in pheromone delivery. The powder X-ray diffraction (PXRD) and nuclear magnetic resonance (NMR) results showed that these MOFs were produced successfully. 3-octanone, an archetypal pheromone used in this study, was loaded into the MOFs and the loading examined by NMR spectroscopy, showing that these MOFs are capable of accommodating pheromones in different quantities. Physical properties (e.g. surface area, pore volume and crystal density), nitrogen adsorption and pheromone diffusion of MOFs were studied in depth using simulation methods. The higher electrostatic contribution of UiO-66-NH2 leads to higher guest-host interaction energies than UiO-66. These findings suggest a promising porous material for use in sustainable agriculture.

MOF molecular simulation

Figure. a) Simulated nitrogen isotherm of MOFs at 77 K (logarithmic pressure axis) generated from Monte Carlo simulation. b) Mean square displacement of 3-octanone in MOFs generated from Molecular Dynamics simulation

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chabazite ion exchange

Chabazite (CHA), one of the most common zeolite framework types, has been studied extensively in selective gas sorption. This is due to the remarkable capacity of this zeolite to accommodate cations within the unique CHA framework. Here, we report a systematic study on a series of chabazite zeolites exchanged by divergent extra-framework cations with valence and atomic radius difference. The results showed that chabazite (KNa-CHA) was synthesised successfully from zeolite Y, and six chabazite zeolites including K-CHA, Cs-CHA, Ca-CHA, Ba-CHA, Sr-CHA and Zn-CHA were prepared from the parent chabazite by ion exchange. These samples were examined by numerous techniques and it was found that the difference in valence and size between extra-framework cations exert a significant effect on the abundance of these cations positioned in the framework, resulting in differing nitrogen sorption ability measured in the synthesised chabazite zeolites. These findings will help to understand the molecular sieve of the zeolite countercation which is a promising mechanism to selectively sequester and separate gases.

chabazite NMR

Figure. a) 27Al NMR spectrum of all chabazite zeolites. b) Nitrogen isotherms at 77 K of all chabazite zeolites


This work has been published in CrystEngComm

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