Pieter C M M Magusin

Pieter C M M Magusin
University of Cambridge | Cam · Department of Chemistry

Dr.

About

153
Publications
18,194
Reads
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5,688
Citations
Citations since 2016
33 Research Items
3100 Citations
20162017201820192020202120220100200300400500
20162017201820192020202120220100200300400500
20162017201820192020202120220100200300400500
20162017201820192020202120220100200300400500
Additional affiliations
October 2017 - September 2020
Murray Edwards College
Position
  • Fellow
Description
  • Teaching Chem 1A (1st year Chemistry)
January 2015 - present
University of Cambridge
Position
  • Solid-state NMR specialist & lab manager
October 2014 - October 2014
Vrije Universiteit Brussel
Position
  • Guest Teacher
Description
  • Master course Bio-NMR (10 of 48 contact hours)

Publications

Publications (153)
Preprint
Full-text available
Lithium metal batteries with high energy densities can enable a revolution in energy storage and accelerate shifts in electric transportation and electricity generation. However, several morphological and electro-chemo-mechanical challenges impede their development. Solid state electrolytes such as those based on polymers show great promise in repl...
Preprint
Understanding electronic structure is a crucial component in the development of many functional materials including semiconductors, transparent-conducting oxides, and batteries, and is necessarily directly dependent on their underlying atomistic structure. The elucidation of atomistic structure is impeded, both experimentally and computationally, b...
Preprint
Full-text available
Advancing the next generation of materials for solid-state devices requires an understanding of their underlying electronic structure; yet the amorphous nature of many materials hinders progress in creating an atomic-level model. One such material is amorphous alumina, which is used to enhance performance in electronic devices from Li-ion batteries...
Preprint
Advancing the next generation of materials for solid-state devices requires an understanding of their underlying electronic structure; yet the amorphous nature of many materials hinders progress in creating an atomic-level model. One such material is amorphous alumina, which is used to enhance performance in electronic devices from Li-ion batteries...
Article
Full-text available
The enhancing effect of extraframework Al (EFAl) species on the acidity of bridging hydroxyl groups in a steam-calcined faujasite zeolite (ultrastabilized Y, USY) was investigated by in situ monitoring the H/D exchange reaction between benzene and deuterated zeolites by ¹H MAS NMR spectroscopy. This exchange reaction involves Brønsted acid sites (B...
Preprint
Full-text available
While organic mixed ionic/electronic conductors are widely studied for various applications in bioelectronics, energy generation/storage, and neuromorphic computing, a fundamental understanding of the interactions between the ionic and electronic carriers remains unclear, particularly in the wet state and on electrochemical cycling. Here, we show t...
Article
Full-text available
Li-O2 batteries offer a high theoretical discharge capacity due to the formation of light discharged species such as Li2O2, which fill the porous positive electrode. However, in practice, it is challenging to reach the theoretical capacity and completely utilize the full electrode pore volume during discharge. With the formation of discharge produc...
Article
Hydrous materials are ubiquitous in the natural environment and efforts have previously been made to investigate the structures and dynamics of hydrated surfaces for their key roles in various chemical and physical applications, with the help of theoretical modelling and microscopy techniques. However, an overall atomic-scale understanding of the w...
Article
Full-text available
Compared to nanomaterials exposing nonpolar facets, polar-faceted nanocrystals often exhibit unexpected and interesting properties. The electrostatic instability arising from the intrinsic dipole moments of polar facets, however, leads to different surface configurations in many cases, making it challenging to extract detailed structural informatio...
Article
Full-text available
The high theoretical capacity of Li-O2 batteries attracts a lot of attention and this field has expanded significantly in the last two decades. In a more general way, the large number of articles being published daily makes it difficult for researchers to keep track of the progress in science. Here we develop a text mining program in an attempt to...
Article
Silicon monoxide is a promising alternative anode material due to its much higher capacity than graphite, and improved cyclability over other Si anodes. An in-depth analysis of the lithium silicide (LixSi) phases that form during lithiation/delithiation of SiO is presented here and the results are compared with pure-Si anodes. A series of anode mat...
Article
Lithium-oxygen batteries are attractive for reversible energy storage because of their theoretically high capacities. Practically, high capacities are challenging to achieve due to key issues such as the transport and growth of the Li2O2 discharge product. Numerous carbon-based cathode mesostructures have been studied experimentally and computation...
Article
Fluoroethylene carbonate (FEC) and vinylene carbonate (VC) are widely used as electrolyte additives in lithium ion batteries. Here we analyze the solid electrolyte interphase (SEI) formed on binder-free silicon nanowires (SiNWs) electrodes in pure FEC or VC electrolytes containing 1 M LiPF6 by solid-state nuclear magnetic resonance (ssNMR) with and...
Article
The parasitic reactions associated with reduced oxygen species and the difficulty in achieving the high theoretical capacity have been major issues plaguing development of practical nonaqueous Li-O2 batteries. We hereby address the above issues by exploring the synergistic effect of 2,5-di-tert-butyl-1,4-benzoquinone and H2O on the oxygen chemistry...
Preprint
We report the exfoliation of layered Na2Ti3O7, a promising anode material for Na-ion batteries, and restacking using HNO3 and NaOH to form H-Ti3O7 and Na(x)-Ti3O7 compositions, respectively. The materials were characterised by a range of techniques (SEM, TEM, solid-state NMR, XRD, PDF). Although the formation of aggregated nanoparticles is favoured...
Preprint
The parasitic reactions associated with reduced oxygen species and the difficulty in achieving the high theoretical capacity have been major issues plaguing development of practical non-aqueous Li-O2 batteries. We hereby address the above issues by exploring the synergistic effect of 2,5-di-tert-butyl-1,4- benzoquinone and H2O on the oxygen chemist...
Preprint
To elucidate the role of fluoroethylene carbonate (FEC) as an additive in the standard carbonate-based electrolyte for Li-ion batteries, the solid electrolyte interphase (SEI) formed during electrochemical cycling on silicon anodes was analyzed with a combination of solution and solid-state NMR techniques, including dynamic nuclear polarization. To...
Article
We report the exfoliation of layered Na2Ti3O7, a promising anode material for Na-ion batteries, and restacking using HNO3and NaOH to form H-[Ti3O7] and Na(x)-[Ti3O7] compositions, respectively. The materials were characterized by a range of techniques (SEM, TEM, solid-state NMR, XRD, PDF). Although the formation of aggregated nanoparticles is favor...
Article
We report the exfoliation of layered Na2Ti3O7, a promising anode material for Na-ion batteries, and restacking using HNO3 and NaOH to form H-[Ti3O7] and Na(x)-[Ti3O7] compositions, respectively. The materials were characterised by a range of techniques (SEM, TEM, solid state NMR, XRD, PDF). Although the formation of aggregated nanoparticles is favo...
Article
The parasitic reactions associated with reduced oxygen species and the difficulty in achieving the high theoretical capacity have been major issues plaguing development of practical nonaqueous Li-O2 batteries. We hereby address the above issues by exploring the synergistic effect of 2,5-di-tert-butyl-1,4-benzoquinone and H2O on the oxygen chemistry...
Article
While large dispersions in electrochemical performance have been reported for lithium oxygen batteries in the literature, they have not been investigated in any depth. The variability in the results is often assumed to arise from differences in cell design, electrode structure, handling and cell preparation at different times. An accurate theoretic...
Chapter
This chapter describes the application of solid-state NMR spectroscopy for investigating battery electrode materials at controlled state of charge. Magic-angle spinning NMR gives the highest possible chemical resolution, but only allows these often metastable electrode materials to be studied in an ex situ manner, i.e., outside the electrochemical...
Article
To elucidate the role of fluoroethylene carbonate (FEC) as an additive in the standard carbonate-based electrolyte for Li-ion batteries, the solid electrolyte interphase (SEI) formed during electrochemical cycling on silicon anodes was analyzed with a combination of solution and solid-state NMR techniques, including dynamic nuclear polarization. To...
Article
The use of a wide variety of NMR spectroscopy techniques to characterise the SEI that is formed on silicon on cycling will be described. We have synthesized ¹³ C enriched forms of additives such as FEC, which have allowed detailed structural studies to be performed. The results have been compared to the species identified in prior work on products...
Article
We are grateful for financial support by the Oppenheimer Foundation (M. A. H.), the Cambridge Commonwealth Trusts (D. M. H.), the National Natural Science Foundation of China (NSFC) (21573103 and 21661130149) and the Royal Society Newton Fund (L. P.). The DNP experiments were performed at the DNP MAS NMR Facility at the University of Nottingham, wi...
Article
Full-text available
Surface-selective direct (17)O DNP has been demonstrated for the first time on CeO2 nanoparticles, for which the first three layers can be distinguished with high selectivity. Polarisation build-up curves show that the polarisation of the (sub-)surface sites builds up faster than the bulk, accounting for the remarkable surface selectivity.
Article
The pyrolysis of 1,2-diphosphinobenzene at 800 °C gives a phosphorus-doped graphite (P-DG) with an unprecedented high phosphorus content, ca. 20 at%. In contrast with previously studied boron and nitrogen doped graphite materials, thorough characterisation and analysis of this material demonstrates that it is extensively disordered and contains sub...
Article
Desilication of ZSM-5 zeolite in basic medium creates intracrystalline mesoporosity advantageous to catalysis, but decrease of acidity often limits the gain by improved accessibility of sites. Atomic layer deposition of aluminum (Al-ALD) using cycles of reaction and hydrolysis of trimethylaluminum was applied to desilicated ZSM-5 samples to enhance...
Article
The novel ternary Zintl phase Li3NaGe2 is prepared by heating a stoichiometric mixture of the elements (Ta ampoule in evacuated silica tubes, 400 °C, 7 d; cooling at a rate of 0.5 °C/min).
Article
The reaction mechanism of etherification of ?-citronellene with ethanol in liquid phase over acid zeolite beta is revealed by in situ solid-state 13C NMR spectroscopy. Comparison of 13C Hahn-echo and 1H ? 13C cross polarization NMR characteristics are used to discriminate between molecules freely moving in liquid phase outside the zeolite and molec...
Article
The novel ternary Zintl phase Li3 NaGe2 comprises alkali-metal cations and [Ge2 ](4-) dumbbells. The diatomic [Ge2 ](4-) unit is characterized by the shortest GeGe distance (2.390(1) Å) ever observed in a Zintl phase and thus represents the first GeGe double bond under such conditions, as also suggested by the (8-N) rule. Raman measurements suppo...
Article
Supramolecular polymers based on ureido-pyrimidinone (UPy) represent a promising class of biocompatible materials for medical applications. Here, the chemical modification effect of UV irradiation, used to sterilize these materials, is studied. Besides anticipated crosslinking effects, UV irradiation causes telechelic UPy-polymers to become fluores...
Article
The wide range of liquid-phase reactions required for the catalytic conversion of biomass compounds into new bioplatform molecules defines a new set of challenges for the development of active, selective, and stable catalysts. The potential of bifunctional Ru/H-USY catalysts for conversions in hot liquid water (HLW) is assessed in terms of physicoc...
Article
Lewis acid Snβ-type zeolites with varying amounts of Brønsted acid Al in the framework were synthesized using a simple two-step procedure comprising partial dealumination of β zeolite under action of acid, followed by grafting with SnCl4·5H2O in dry isopropanol. Characterization of the thus-prepared Al-containing Snβ (Sn/pDeAlβ) zeolites with ICP,...
Article
The influence of mesoporosity and silylation on the physico-chemical and catalytic properties of Mo/HZSM-5 in methane dehydroaromatization was investigated. The zeolites were characterized by XRD, 27Al and 95Mo NMR, UV-Vis, UV Raman and pyridine IR spectroscopy and TEM. Base-desilicated mesoporous and bulk HZSM-5 zeolites with comparable Brønsted a...
Article
Solution processing of Al-doped ZnO (AZO) is interesting from an economical point of view for reducing synthesis and deposition costs in comparison to that for vacuum methods. Several (aqueous) chemical solution deposition routes have been explored for AZO, but the question that has never been answered is how state-of-the-art conductivity is achiev...
Article
Full-text available
A new, single-step protocol for wrapping individual nanosized b-casein micelles with silica is presented. This biomolecule-friendly synthesis proceeds at low protein concentration at almost neutral pH, and makes use of sodium silicate instead of the common silicon alkoxides. This way, formation of potentially protein-denaturizing alcohols can be av...
Article
MgH2 is a promising material for reversible solid-state hydrogen storage. It is known that particle size can have a strong impact on hydrogen dynamics and sorption characteristics, but more detailed insight has been hampered by the great challenge to prepare small and well-defined particles and study their hydrogen storage properties upon cycling....
Article
Fluorite-structured Mg-Ti hydrides are interesting for hydrogen storage applications because of their high gravimetric hydrogen storage capacity, and improved (de)hydrogenation kinetics compared to MgH2. In the present study we have investigated the potential catalytic effect of Ni and Si as third element on the siting and mobility of electrochemic...
Article
Advanced solid-state 2D NMR spectroscopy and molecular dynamics computation are employed to investigate the interaction between adsorbed ferrocene molecules and the MOF-5 lattice. Relayed 13C–1H heteronuclear correlation (HETCOR) 2D NMR spectra clearly indicate short-distance contacts between the ferrocene guests and the benzene-1,4-dicarboxylic-ac...
Article
Although monodisperse amorphous silica nanoparticles have been widely investigated, their formation mechanism is still a topic of debate. Here, we demonstrate the formation of monodisperse nanoparticles from colloidally stabilized primary particles, which at a critical concentration, undergo a concerted association process, concomitant with a morph...
Article
In situ NMR and DFT modeling demonstrate that N,N-dimethylformamide (DMF) promotes the formation of metal-organic framework NH2-MIL-101(Al). In situ NMR studies show that upon dissociation of an aluminum-coordinated aqua ligand in NH2-MOF-235(Al), DMF forms a H-Cl-DMF complex during synthesis. This reaction induces a transformation from the MOF-235...
Article
Electrochemical deuteration of metastable Mg-Ti alloys is studied. To investigate the dynamics of deuterium atoms in the crystal host, the as-prepared hydrides are examined by means of NMR spectroscopy. Remarkably the host compound, which phase segregates upon gas phase deuteration at high temperatures, preserves its original structure during low t...
Article
A layered zirconosilicate composed of SiO4 tetrahedra and ZrO6 octahedra was hydrothermally synthesized in the presence of tetramethylammonium hydroxide. The layered material with a nominal composition Na2ZrSi4O11•xH2O was further characterized by XRD, SEM, thermogravimetric analysis, UV-Raman spectroscopy and single- and triple-quantum 23Na and 29...
Article
The influence of steaming at varying temperatures on the physicochemical properties of a HZSM-5 zeolite (Si/Al = 27) was investigated by X-ray diffraction, 27Al MAS NMR, Ar physisorption and IR spectroscopy of adsorbed pyridine, 2,4,6-trimethylpyridine and CO. The catalytic activity of the zeolites was evaluated in propane and methanol conversion r...
Article
The acidic properties of nanolayered ZSM-5 zeolites synthesized with the aid of multiquaternary ammonium surfactants were investigated in detail. A substantial fraction of Al is present in highly dispersed form at extraframework positions indicative of the defective nature of the calcined nanolayered zeolites. Acidity characterization reveals that...
Article
Chemical vapor deposition of trimethylaluminum (TMA) was explored as an approach for the preparation of model faujasite-type catalysts containing extraframework aluminum. The decomposition of the grafted organoaluminum species was investigated in hydrogen and oxygen atmosphere. The process of grafting Al-containing species and the associated change...
Article
Hierarchical SSZ-13 zeolites were synthesized by combining N,N,N-trimethyl-1-adamantanammonium hydroxide (TMAdOH) as the structure-directing agent for chabazite formation with mono- and diquaternary ammonium-type and organosilane mesoporogens and extensively characterized for their structural, textural, and catalytic properties. Mesoporous SSZ-13 z...
Article
A series of faujasite zeolites was modified by extraframework Al (AlEF) with the goal to investigate the influence of such species on the intrinsic Brønsted acidity and catalytic activity towards paraffin cracking. The chemical state of AlEF and zeolite acidity were investigated by 27Al MAS NMR and COads IR spectroscopy, H/D exchange reaction, and...
Article
To understand the catalytic influence of TiF3 on the de- and rehydrogenation of ball milled MgH2–TiF3, a detailed study has been performed of the different crystallographic phases of the de- and rehydrogenated materials. Rietveld-refined XRD analysis of the dehydrogenated material indicates the presence of a rutile, nonstoichiometric MgF2–x phase a...
Article
The mechanism of crystallization of microporous titanosilicate ETS-10 was investigated by Raman spectroscopy combined with (29) Si magic-angle spinning (MAS) NMR spectroscopy, DFT calculations, and SEM imaging. The formation of three-membered ring species is shown to be the key step in the hydrothermal synthesis of ETS-10. They are formed by means...
Article
The dual template synthesis of zeolite SSZ-13 by use of trimethyl-adamantanammonium hydroxide and a diquaternary-ammonium mesoporogen induces considerable mesoporosity without impeding zeolite microporosity. The strongly improved accessibility of Brønsted sites in mesoporous SSZ-13 increases its stability during application as an acid catalyst in t...
Article
To increase the content of well-dispersed aluminum in Al/SBA-15 and its Bronsted acidity, a water-free synthesis method involving a Si-O-Al precursor was employed to prepare a series of Al/SBA-15 of widely varying composition. The materials were characterized with ICP, BET, TEM, Al-27 MAS NMR and IR spectroscopy and compared to conventionally prepa...
Article
The hydrogen-bonded hexagonal columnar LC (Col(hd)) phases formed by benzene-1,3,5-tricarboxamide (BTA) derivatives can be aligned uniformly by an electric field and display switching behavior with a high remnant polarization. The polar switching in three symmetrically substituted BTAs with alkyl chains varying in length between 6 and 18 carbon ato...
Article
Para hydrogen induced polarization (PHIP) is a powerful hyperpolarization technique, which increases the NMR sensitivity by several orders of magnitude. However the hyperpolarized signal is created as an anti-phase signal, which necessitates high magnetic field homogeneity and spectral resolution in the conventional PHIP schemes. This hampers the a...
Article
New routes for the preparation of highly active TiO(2)-supported Cu and CuZn catalysts have been developed for C-O coupling reactions. Slurries of a titania precursor were dip-coated onto glass beads to obtain either structured mesoporous or non-porous titania thin films. The Cu and CuZn nanoparticles, synthesized using a reduction by solvent metho...
Article
A novel route for the introduction of well-defined zinc species into ZSM-5 zeolite via chemical vapor deposition of dimethylzinc (CVD(DMZ)) is explored. The structural properties and catalytic reactivity of the synthesized material (Zn/ZSM-5-CVD(DMZ)) are investigated against a set of Zn/ZSM-5 catalysts prepared by incipient wetness impregnation (I...
Article
Unsaturated metal coordination sites in metal organic frameworks (MOFs) offer preferential hydrogen adsorption sites. In addition, MOFs can be applied as scaffolds for nano metal hydrides operating at elevated temvratures. For these reasons, the thermal stability of the framework with unsaturated Cu2+. coordination sites in a hydrogen atmosphere ha...
Article
Small pore size and hydrophobic nature of DD3R make this material a unique zeolite with high potential in industrial separation applications. However, the reproducible rapid synthesis of this zeolite is still a problem. In this work, a thorough assessment of different synthetic methods revealed that synthesis reproducibility relies on two main pill...
Chapter
Full-text available
1H NMR transverse relaxation and double-quantum (DQ) build up have been compared for a series of EPDM grades crosslinked with different amounts of sulfur or peroxide. The modulus at 100% elongation of the same EPDM samples correlates linearly to the effective transverse-relaxation and DQ build-up rate, suggesting that both rates are proportional to...