My research program is focused on developing new ways to understand how to control structure, properties, and reactivity of molecular and supramolecular metal complexes, by harnessing coordination chemistry to explore a range of fundamental properties and applications of metal-organic ligand systems. We are particularly interested in the areas of coordination polymer materials and their uses, and new phthalocyanine-based compounds, with a special emphasis on emissive materials and paramagnetic organometallic complexes, as outlined below.
Coordination polymers are multi-dimensional materials that are held together with metal-ligand bonds, which can be self-assembled — like lego pieces - from judiciously chosen building blocks, and their structures and properties tuned to target a range of applications. The need to understand how to control structure, properties and reactivity of these coordination polymers via the choice of metals and the design of appropriate building blocks and ligands fundamentally lies at the heart of this research.
Phthalocyanines Pc are intensely coloured, chemically inert, redox-active compounds that are ubiquitous in industry, with uses from dyes to photodynamic therapy of cancer. However, despite their useful attributes, the synthesis and reactivity of metal-phthalocyanine PcM complexes for many metals remains barely unexplored and their organometallic chemistry is sparse. We explore PcM complexes with non-traditional metals and ring-oxidation states, uncovering new classes of compounds with unusual properties and reactivity. We are also active in the area of actinide chemistry, studying the unique coordination chemistry, properties and reactivity of complexes of the very large elements uranium and thorium.
Using combinations of transition metals, lanthanides, actinides and appropriate bridging ligands, we are pursuing novel coordination polymer materials. Bridging ligands include metal cyanides and thiocyanates, heterocyclic amines and sulfur-based ligands. In particular, the use of linear d 10 and square-planar d 8 metal cyanides such as [Au CN 2 ] - and [Pt CN 4 ] 2- that display strongly attractive metal-metal aurophilic, platinophilic etc.
We are targeting emissive and vapochromic materials for toxic small-molecule sensing, highly birefringent materials, molecule-based magnetic and multifunctional materials, systems with unusual thermal-expansion properties, crystalline Non-Linear Optical NLO materials, supramolecular systems that emit white or other-coloured light, and coordination polymer materials with other exciting properties.
A large majority of PcM complexes incorporate late first-row transition-metals.
The earlier text is concise pages , and contains only three chapters, appropriately entitled: Scandium, The Lanthanides, and The Actinides. The new text takes the original three chapters and separates the subsections into independent chapters. Each of the independent chapters has been updated with current examples from the literature and expanded data tables and figures.
A completely new chapter Chapter 8 has been added www. Other new features include a list of objectives and learning goals for students at the beginning of each chapter. These lists make the text more studentfriendly by providing an outline of the topics to be covered and by focusing attention on the important concepts in each chapter.
Organometallic chemistry: 18e rule and its exceptions, isolobal and isoelectronic analogies. Here the authors show that electrolyte cations unexpectedly stabilize higher-oxidation-state neptunium dioxocations in water through extended-coordination sphere interactions. Here the authors demonstrate that electron self-exchange through hydrogen bonds is highly efficient and can proceed either via the known proton-coupled pathway or an overlooked proton-uncoupled pathway. A current challenge in the development of molecular water oxidation catalysts is to overcome their inherent susceptibilities to oxidative or hydrolytic degradation under turnover conditions in water. Lists What are lists? Department of
In addition, a limited number of questions with answers has been added to the end of each chapter. The majority of the questions are very well-constructed and should help advanced students check their understanding of the material in the chapter. The bibliography is loaded with additional reading selections, with a good mix of current literature and classic references. The only omissions from the original text are a few specific chemical reactions detailing the production of various lanthanide halides and an interesting outline for the production of uranium metal from the ore concentrates.
On a negative note, the first few chapters have several typos, ranging from incorrect chemical symbols and equations to data in the text not matching data in tables. While I found the typos only annoying, students will find them confusing. Here, the authors explore a series of dilanthanide-encapsulated fullerenes where the radical bridge is taken to its limit and the role is played by a single unpaired electron.
Article 21 January Open Access. Understanding the structural dynamics of flexible metal-organic frameworks at a thin-film level is key if they are to be implemented in devices. Here, Fischer and colleagues anchor flexible MOF crystallites onto substrates and identify a structural responsiveness that is distinct to that of the bulk. Article 04 January Open Access.
Here the authors show that electrolyte cations unexpectedly stabilize higher-oxidation-state neptunium dioxocations in water through extended-coordination sphere interactions. Article 27 November Open Access.
While chemical bonding between carbon and the d - and p -block elements is relatively well-studied, that between carbon and the f -block elements remains comparatively poorly understood. Article 22 November Open Access. Adapting the cavity of a coordination capsule generally involves the addition or removal of subcomponents.
Here, the authors report two vanadium-organic coordination nanocapsules with the same number of components but variable cavity sizes—an expanded ball and contracted octahedron—whose solvent-controlled interconversion is attributed to the versatile coordination geometry of the vanadium centers. Article 20 November Open Access. A current challenge in the development of molecular water oxidation catalysts is to overcome their inherent susceptibilities to oxidative or hydrolytic degradation under turnover conditions in water.
Here, the authors design an inherently-stable water oxidation catalyst using oxidatively-inert ligands to harness a reactive metal oxide. Article 12 November Open Access. Controlled switching of the spin state of transition metal ions is key in many enzymatic reactions, but difficult to replicate in synthetic systems. Here the authors report on an iron III porphyrin with a photochromic axial ligand that, in solution, reversibly switches between low-spin and high-spin upon irradiation with two different wavelengths.
Article 01 November Open Access. Coordination-driven supramolecular assembly provides the ability to build molecular architectures of impressive complexity. Here, the authors use a series of linear metal-organic ligands with specific sequences to construct multiple generations of precisely-controlled, 2D fractal polycyclic supramolecules. Article 24 October Open Access.
Supramolecular containers are promising enzyme mimics, but they currently accommodate only a limited range of chemical transformations. Here, the authors describe coordination cages that catalyze two-component cascade reactions without relying on an external or encapsulated catalytic species. Article 23 October Open Access. Understanding how one metal nanocluster transforms into another is of synthetic and fundamental importance.
Here, the authors use mass spectrometry to reveal an acid-induced structural transformation between two Ag clusters that proceeds via a breakage-growth-reassembly mechanism. Article 12 October Open Access. Hyperpolarization methods play a crucial role in the in vivo observation of molecular metabolism by MRI techniques. Here, the authors develop NHC-containing iridium complexes which improve the NMR detectability of 1 H, 13 C and 15 N nuclei via transfer of latent magnetism of para-hydrogen into a substrate.
Article 24 September Open Access. Article 21 September Open Access. Configuring surfaces on-demand for desired functionalities is an ongoing challenge. Here, diverse and tailorable modifications of quartz and porous silica surfaces that are rapidly and reversibly switchable by the use of visible light are achieved via ruthenium-thioether coordination. Article 14 September Open Access. Metal-mediated activation of CO for C-C coupling reactions is a valuable approach to carbon monoxide valorization.
Here, the authors use low-coordinate iron II complexes for the selective scission and homologation of CO affording unusual squaraines and iron carboxylates under mild conditions. Article 10 August Open Access. Polynuclear metal-organic coordination complexes are often inaccessible by traditional synthetic chemistry methods. Here, the authors use on-surface supramolecular chemistry to form a planar trinuclear Fe complex, in which an accumulation of electrons around the positive mixed-valence polynuclear centre suggests a catalytically active core.
Nitrogenase—whose cofactor consists of a metal—sulfur cluster—catalyzes the production of NH 3 from N 2 , but designing metal—sulfur complexes capable of promoting this conversion remains challenging. Article 07 August Open Access. Understanding quantum tunnelling of the magnetisation in single-molecule magnets is crucial for their potential application in information storage. Here the authors conduct a field- and temperature-dependent study of the magnetisation dynamics of a dysprosium-based SMM, finding four distinct relaxation processes that dominate in different regimes.
Article 06 August Open Access. Stimuli-responsive porous materials are attractive for a range of applications, but each material typically exhibits only one type of transformation. Here, the authors report on a metal—organic material that exhibits six distinct phases as a result of four types of structural transformation in response to different stimuli.
While polyhedral boron hydride complexes have found application in a number of diverse fields, the isolation of stable aluminium analogues remains highly challenging. Here, Jones and colleagues demonstrate that reduction of an amidinato-aluminum III hydride complex with magnesium I dimers affords stable aluminium I hydride compounds. Article 16 July Open Access. Owing to the energetic nature of N—N bonds, poly-nitrogen compounds are considered promising high energy density materials. While metal—carbon double bonds are common in transition metal chemistry and catalysis, unsupported uranium—carbon double bonds remain highly challenging to prepare.
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Article 19 September Open Access Switchable organoplatinum metallacycles with high quantum yields and tunable fluorescence wavelengths Fluorescent supramolecular coordination complexes are of interest for chemical sensing and optical devices. Article 13 September Open Access Thorium-nitrogen multiple bonds provide evidence for pushing-from-below for early actinides Despite the burgeoning nature of uranium—ligand multiple bonding, analogous thorium complexes remain incredibly rare.
Organometallic and Coordination Chemistry of the Actinides. Editors: Albrecht- Schmitt, Thomas E. (Ed.) Free Preview. Presents critical reviews of the present. Organometallic and Coordination Chemistry of the Actinides.
Article 06 September Open Access Solvent-triggered reversible interconversion of all-nitrogen-donor-protected silver nanoclusters and their responsive optical properties Noble metal nanoclusters are commonly protected by thiolate, phosphine, or alkynyl ligands. Article 27 August Open Access A stable zirconium based metal-organic framework for specific recognition of representative polychlorinated dibenzo- p -dioxin molecules The sensing of polychlorinated dibenzo- p -dioxins PCDDs is important for the environment and public health but challenging to achieve.
Article 27 August Open Access Molecular cobalt corrole complex for the heterogeneous electrocatalytic reduction of carbon dioxide Electrochemical conversion of carbon dioxide to ethanol is one of the most challenging energy conversion reactions. Article 23 August Open Access Atomistic structures and dynamics of prenucleation clusters in MOF-2 and MOF-5 syntheses Numerous techniques have been used to study the crystallization process of metal-organic frameworks, but little is known about their prenucleation clusters. Article 09 August Open Access Computer-aided discovery of connected metal-organic frameworks Composite metal-organic framework materials can display useful synergetic properties, but typically suffer from disordered interfaces.