Thomas Heine

Thomas Heine
Technische Universität Dresden | TUD · Faculty of Chemistry and Food Chemistry

Dr. rer. nat. habil.

About

451
Publications
112,925
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25,833
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Introduction
My group works in Theoretical Materials Science. We develop Density-Functional Theory based and topological methods. Our applications range from framework structures (MOFs, COFs etc.) over 2D inorganic materials and metal oxide nanoparticles to computational spectroscopy of organic and inorganic molecules.
Additional affiliations
July 2015 - March 2016
University of Leipzig
Position
  • Chair of Theoretical Chemistry
January 2012 - present

Publications

Publications (451)
Article
Single‐atom catalysts (SACs), as promising alternatives to Pt‐based catalysts, suffer from the limited choice of center metals and low single‐atom loading. Here, we report a pentacoordinated Zr‐based SAC with nontrivial axial O ligands (denoted O‐Zr‐N‐C) for oxygen reduction reaction (ORR). The O ligand downshifts the d‐band center of Zr and confer...
Article
Full-text available
Despite superb instrumental resolution in modern transmission electron microscopes (TEM), high-resolution imaging of organic two-dimensional (2D) materials is a formidable task. Here, we present that the appropriate selection of the incident electron energy plays a crucial role in reducing the gap between achievable resolution in the image and the...
Article
Full-text available
Two-dimensional (2D) membranes are emerging candidates for osmotic energy conversion. However, the trade-off between ion selectivity and conductivity remains the key bottleneck. Here we demonstrate a fully crystalline imine-based 2D polymer (2DPI) membrane capable of combining excellent ionic conductivity and high selectivity for osmotic energy con...
Preprint
The β-emitting 99Tc isotope is a high-yield fission product in 235U and 239Pu nuclear reactors, raising special concern in nuclear waste management due to its long half-life and the high mobility of pertechnetate (TcO4−). In the conditions of deep nuclear waste repositories, retention of Tc is achieved via biotic and abiotic reduction of TcO4− to c...
Article
The sixteen different high-symmetry stacking configurations in buckled honeycomb AsP bilayers were identified using block diagrams and studied through several high-level computations, including the adiabatic-connection fluctuation-dissipation theorem in the random phase approximation (ACFDT-RPA). The lowest-lying energy form is an AA-type stacking,...
Article
Solar-to-hydrogen conversion is one of the most promising avenues to provide emission-free fuels and long-term chemical energy storage. Wide-range application crucially requires high-performance photocatalysts that are environmentally benign and free of precious metals. With high robustness, controllable composition, tunable electronic structure, a...
Article
Single‐atom catalysts (SACs), as promising alternatives to Pt‐based catalysts, suffer from the limited choice of center metals and low single‐atom loading. Here, we report a pentacoordinated Zr‐based SAC with nontrivial axial O ligands (denoted O‐Zr‐N‐C) for oxygen reduction reaction (ORR). The O ligand downshifts the d‐band center of Zr and confer...
Article
Full-text available
We report an ion-exchanged zeolite as an excellent candidate for large-scale application in hydrogen isotope separation. Ag(I)-exchanged zeolite Y has been synthesized through a standard ion-exchange procedure. The D2/H2 separation performance has been systematically investigated via thermal desorption spectroscopy (TDS). Undercoordinated Ag+ in ze...
Article
Full-text available
PtSe2 is one of the most promising materials for the next generation of piezoresistive sensors. However, the large‐scale synthesis of homogeneous thin films with reproducible electromechanical properties is challenging due to polycrystallinity. It is shown that stacking phases other than the 1T phase become thermodynamically available at elevated t...
Preprint
Full-text available
In cove-edged zigzag graphene nanoribbons (ZGNR-C), one terminal CH group per length unit is removed on each zigzag edge, forming a regular pattern of coves which controls their electronic structure. Based on three structural parameters that unambiguously characterize the atomistic structure of ZGNR-C, we present a scheme that classifies their elec...
Article
Dithiine linkage formation via a dynamic and self-correcting nucleophilic aromatic substitution reaction enables the de novo synthesis of a porous thianthrene-based two-dimensional covalent organic framework (COF). For the first time, this organo-sulfur moiety is integrated as a structural building block into a crystalline layered COF. The structur...
Article
Most density functionals lack to correctly account for long‐range London dispersion interactions, and numerous a posteriori correction schemes have been proposed in recent years. In van der Waals structures, the interlayer distance controls the proximity effect on the electronic structure, and the interlayer interaction energy indicates the possibi...
Article
Flexible metal-organic frameworks that show reversible guest-induced phase transitions between closed and open pore phases have enormous potential for highly selective, energy-efficient gas separations. Here, we present the gate-opening process of DUT-8(Ni) that selectively responds to D2, whereas no response is observed for H2 and HD. In situ neut...
Article
Exotic oxidation states of the first row transition metals have recently attracted much interest. In order to investigate the oxidation states of a series of iron‐oxalate complexes, an aqueous solution of iron(III) nitrate and oxalic acid was studied by infrared free liquid matrix‐assisted laser desorption/ionization and ionspray mass spectrometry....
Article
Full-text available
Exotic oxidation states of the first row transition metals have recently attracted much interest. In order to investigate the oxidation states of a series of iron-oxalate complexes, an aqueous solution of iron(III) nitrate and oxalic acid was studied by infrared free liquid matrix-assisted laser desorption/ionization and ionspray mass spectrometry....
Article
Single iron atom and nitrogen-codoped carbon (Fe-N-C) electrocatalysts, which have great potential to catalyze the kinetically sluggish oxygen reduction reaction (ORR), have been recognized to be the most promising replacements...
Article
At present, the efficiency of high energy density Li-sulfur (Li-S) batteries is being narrowed by the limited strategies to deal with the shuttling effect, sluggish redox kinetics and poor ionic...
Preprint
Full-text available
PtSe$_2$ is one of the most promising materials for the next generation of piezoresistive sensors. However, the large-scale synthesis of homogeneous thin films with reproducible electromechanical properties is challenging due to polycrystallinity. We show that stacking phases other than the AA-stacking in the 1T phase become thermodynamically avail...
Article
Full-text available
The difficulties in designing high-performance hydrogen evolution reaction (HER) catalysts lie in the manipulation of adsorption behaviors of transition metals (TMs). Topological chiral semimetals with super-long Fermi arc surface states provide an ideal platform for engineering the catalytic performance of TMs through the metal-support interaction...
Article
The electronic properties of π-conjugated two-dimensional (2D) polymers near the Fermi level are determined by structural topology and chemical composition. Thus tight-binding (TB) calculations of the corresponding fundamental network can be used to explore the parameter space to find configurations with intriguing properties before designing the a...
Preprint
Interest in single-atom catalysts (SACs) has grown rapidly across multiple electrocatalytic disciplines in recent years. Current research efforts exclusively focus on nonmetal or transition-metal atoms as active centers, while employing main-group metal elements is seemingly excluded because their delocalized s/p-bands are prone to yield a broadene...
Article
Full-text available
The rapid development of on‐surface synthesis provides a unique approach toward the formation of carbon‐based nanostructures with designed properties. Herein, we present the on‐surface formation of CN‐substituted phenylene vinylene chains on the Au(111) surface, thermally induced by annealing the substrate stepwise at temperatures between 220°C and...
Preprint
Full-text available
Two-dimensional (2D) materials may exhibit intriguing band structure features (e.g., Dirac points), that lay far away from the Fermi level. They are, thus, not usable in applications. The semiconducting 2D material PC6 has two Dirac cones above and below the Fermi level. Therefore, it is an ideal playground to demonstrate chemical functionalization...
Article
Full-text available
We study the isotopologue-selective binding of dihydrogen at the undercoordinated boron site of B12X11 - (X = H, F, Cl, Br, I, CN) using ab initio quantum chemistry. With a Gibbs free energy of H2 attachment reaching up to 80 kJ mol-1 (ΔG at 300 K for X = CN), these sites are even more attractive than most undercoordinated metal centers studied so...
Preprint
Based on first principles calculations, we report the design of three two-dimensional (2D) binary honeycomb-kagome polymers composed of B- and N-centered heterotriangulenes with a periodically alternate arrangement as in hexagonal boron nitride. The 2D binary polymers with donor-acceptor characteristics, are semiconductors with a direct band gap of...
Preprint
Based on first principles calculations, we report the design of three two-dimensional (2D) binary honeycomb-kagome polymers composed of B- and N-centered heterotriangulenes with a periodically alternate arrangement as in hexagonal boron nitride. The 2D binary polymers with donor-acceptor characteristics, are semiconductors with a direct band gap of...
Article
We systematically explore the stability and properties of [B12X11NG]- adducts resulting from the binding of noble gas atoms to anionic [B12X11]- clusters in the gas phase of mass spectrometers. [B12X11]- can be obtained by stripping one X- off the icosahedral closo-dodecaborate dianion [B12X12]2-. We study the binding of the noble gas atoms He, Ne,...
Article
Full-text available
The potential of metal–organic frameworks (MOFs) for applications in optoelectronics results from a unique combination of interesting photophysical properties and straightforward tunability of organic and inorganic units. Here, it is demonstrated that using MOF approach chromophores can be assembled into well‐ordered 1D arrays using metal‐oxo stran...
Article
Full-text available
Surface-modification of phthalocyanine-based two-dimensional conjugated metal-organic framework (2D c-MOF) films by grafting aliphatic alkyl chains is developed for achieving high-performance polarity-selective chemiresitive sensing toward humidity and polar alcohols. Abstract 2D conjugated metal–organic frameworks (2D c-MOFs) are emerging as elec...
Article
Full-text available
Two‐dimensional conjugated metal‐organic frameworks (2D c ‐MOFs) are emerging as new‐generation electroactive materials for chemiresistive sensors. However, selective sensing with fast response/recovery remains a challenge. Here, we report for the first time phthalocyanine‐based Ni 2 [MPc(NH) 8 ] 2D c ‐MOF films as active layers for polarity‐select...
Article
The ability to dynamically control chirality remains a grand challenge in chemistry. Although many molecules possess chiral isomers, lacking their isolation, for instance during photoisomerization, results in racemic mixtures with suppressed enantiospecific chiral properties. Here, we present a nanoporous solid in which chirality and enantioselecti...
Article
Full-text available
Two‐dimensional polymers (2DPs) are a class of atomically/molecularly thin crystalline organic 2D materials. They are intriguing candidates for the development of unprecedented organic‐inorganic 2D van der Waals heterostructures (vdWHs) with exotic physicochemical properties. In this work, we demonstrate the on‐water surface synthesis of large‐area...
Article
Two‐dimensional polymers (2DPs) are a class of atomically/molecularly thin crystalline organic 2D materials. They are intriguing candidates for the development of unprecedented organic‐inorganic 2D van der Waals heterostructures (vdWHs) with exotic physicochemical properties. In this work, we demonstrate the on‐water surface synthesis of large‐area...
Article
Full-text available
Transition metal dichalcogenide semiconductors, particularly MoS2, are known as promising alternative non-precious hydrogen evolution reaction (HER) electrocatalysts to high-cost Pt. However, their performance is strongly limited by the poor conductivity and lack of active sites in the basal plane. Therefore, it is desirable to find alternatives wi...
Preprint
We show that the topological states inherent in the two-dimensional vertex transitive fes lattice, also referred to as square-octagon lattice, can be tailored by modifying the interactions between the knots. Contrary to other lattices formed of light-weight atoms, such as in graphene, where the spin-orbit interactions are too weak for opening a ban...
Article
Two-dimensional conjugated covalent organic frameworks (2D c-COFs) are emerging as a unique class of semiconducting 2D conjugated polymers for (opto)electronics and energy storage. Doping is one of the common, reliable strategies to control the charge carrier transport properties, but the precise mechanism underlying COF doping has remained largely...
Article
High-level first-principles computations predict blue phosphorene bilayer to be a two-dimensional metal. This structure has not been considered before and was identified by employing a block-diagram scheme that yields the complete set of five high-symmetry stacking configurations of buckled honeycomb layers, and allows their unambiguous classificat...
Article
Full-text available
Metal–organic frameworks (MOFs) and covalent organic frameworks (COFs) consist of molecular building blocks being stitched together by strong bonds. They are well known for their porosity, large surface area, and related properties. The electronic properties of most MOFs and COFs are the superposition of those of their constituting building blocks....
Article
Full-text available
While the isotope‐dependent hydrogen permeability of graphene membranes at ambient condition has been demonstrated, the underlying mechanism has been controversially discussed during the past 5 years. The reported room‐temperature proton‐over‐deuteron (H⁺‐over‐D⁺) selectivity is 10, much higher than in any competing method. Yet, it has not been und...
Article
Full-text available
Two-dimensional (2D) polymers hold great promise in the rational materials design tailored for next-generation applications. However, little is known about the grain boundaries in 2D polymers, not to mention their formation mechanisms and potential influences on the material’s functionalities. Using aberration-corrected high-resolution transmission...
Preprint
Full-text available
High-level first-principles computations predict blue phosphorene bilayer to be a two-dimensional metal. This structure has not been considered before and was identified by employing a block-diagram scheme that yields the complete set of five high-symmetry stacking configurations of buckled honeycomb layers, and allows their unambiguous classificat...
Article
First-principles calculations predicted electronic topological properties for 2D honeycomb–kagome polymers, which have been now confirmed experimentally thanks to improvements in on-surface synthesis.
Article
Full-text available
Visible light driven hydrogen (H2) production from water is a promising strategy to convert and store solar energy as chemical energy. Covalent organic frameworks (COFs) are front runners among different classes of organic photocatalysts. Photocatalytic activity of COFs depends on numerous factors such as electronic band gap, crystallinity, surface...
Cover Page
Full-text available
The structural topology of a 2D network defines its electronic structure. The strength of interacting lattice nodes affects the resulting band structure, in this example the relative position of flat band and Dirac point in the Lieb lattice. See Thomas Heine et al ., Chem. Soc. Rev ., 2020, 49 , 2007. DOI: 10.1039/c9cs00893d
Article
There are more than 200 two-dimensional (2D) networks with different topologies. The structural topology of a 2D network defines its electronic structure. Including the electronic topological properties, it gives rise to Dirac cones, topological flat bands and topological insulators. In this Tutorial Review, we show how electronic properties of 2D...
Article
Full-text available
Edel und stark: Edelmetalldichalkogenide und ‐phosphochalkogenide stellen eine neue Klasse der zweidimensionalen Materialien dar. Dieser Kurzaufsatz fasst die Entwicklungen in der Synthese, Charakterisierung und Anwendung dieser Materialien zusammen, wobei ein besonderer Fokus auf ihre einzigartigen Strukturen und deren Beziehungen zueinander geleg...
Article
Full-text available
Noble‐metal chalcogenides, dichalcogenides and phosphochalcogenides are an emerging class of two‐dimensional materials. Their properties can be broadly tuned via quantum confinement (number of layers) and defect engineering, including metal‐to‐semiconductor transitions, magnetic ordering, and topological surface states. They possess various polytyp...
Article
Full-text available
Despite the recent progress in the synthesis of crystalline boronate ester covalent organic frameworks (BECOFs) in powder and thin‐film through solvothermal method and on‐solid‐surface synthesis, respectively, their applications in electronics, remain less explored due to the challenges in thin‐film processability and device integration associated...
Article
Despite the recent progress in the synthesis of crystalline boronate ester covalent organic frameworks (BECOFs) in powder and thin‐film through solvothermal method and on‐solid‐surface synthesis, respectively, their applications in electronics, remain less explored due to the challenges in thin‐film processability and device integration associated...
Article
Full-text available
Single‐layer and multi‐layer 2D polyimine films have been achieved through interfacial synthesis methods. However, it remains a great challenge to achieve the maximum degree of crystallinity in the 2D polyimines, which largely limits the long‐range transport properties. Here we employ a surfactant‐monolayer‐assisted interfacial synthesis (SMAIS) me...
Article
Full-text available
Drei kristalline Imin‐basierte 2D‐Polymerfilme wurden durch tensidmonolagenunterstützte Grenzflächensynthese (SMAIS) hergestellt. Die synthetischen PI‐2DP‐Filme sind mit polykristallinen Mehrfachlagen mit abstimmbarer Dicke von 6–200 nm und großen kristallinen Domänen (100–150 nm) ausgestattet und weisen p‐Halbleiterverhalten mit einer Bandlücke vo...
Preprint
Noble-metal chalcogenides, dichalcogenides and phosphochalcogenides are an emerging class of two-dimensional materials. Their properties can be broadly tuned via quantum confinement (number of layers) and defect engineering, including metal-to-semiconductor transitions, magnetic ordering, and topological surface states. They possess various polytyp...
Article
Full-text available
Time‐dependent density functional theory is thoroughly benchmarked for the predictive calculation of UV–vis spectra of porphyrin derivatives. With the aim to provide an approach that is computationally feasible for large‐scale applications such as biological systems or molecular framework materials, albeit performing with high accuracy for the Q‐ba...
Article
Full-text available
Despite rapid progress in recent years, it has remained challenging to prepare crystalline two-dimensional polymers. Here, we report the controlled synthesis of few-layer two-dimensional polyimide crystals on the surface of water through reaction between amine and anhydride monomers, assisted by surfactant monolayers. We obtained polymers with high...
Preprint
div>Metal-organic frameworks (MOFs) and covalent organic frameworks (COFs) consist of molecular building blocks being stitched together by strong bonds. They are well known for their porosity, large surface area, and related properties. The electronic properties of most MOFs and COFs are the superposition of those of their constituting building blo...
Preprint
p>We thoroughly benchmark time-dependent density- functional theory for the predictive calculation of UV/Vis spectra of porphyrin derivatives. With the aim to provide an approach that is computationally feasible for large-scale applications such as biological systems or molecular framework materials, albeit performing with high accuracy for the Q-b...