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Marc Georg Willinger

Marc Georg Willinger
TU Munich · School of Natural Sciences

Professor

About

320
Publications
41,099
Reads
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8,922
Citations
Additional affiliations
February 2018 - present
ETH Zurich
Position
  • Group Leader
January 2014 - November 2017
Max Planck Institute for Chemical Energy Conversion
Position
  • Group Leader
January 2011 - January 2018
Fritz Haber Institute of the Max Planck Society
Position
  • Group Leader

Publications

Publications (320)
Article
Hydrogen production by electrocatalytic water splitting will play a key role in the realization of a sustainable energy supply. Owing to their relatively high stability and activity, iridium (hydr)oxides have been identified as most promising catalysts for the oxidation of water. Comprehensive spectroscopic and theoretical studies on the basis of R...
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Full-text available
Analytical methods that provide direct real-space information about the dynamics of catalysed reactions often require simplified model systems and operate under high-vacuum conditions. There is thus a strong need for the development of methods that enable observation of active catalysts under relevant working conditions. Here, in situ scanning elec...
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Dependent on the application or characterization method catalysts are exposed to different gas pressures, which results in different structures. The quantitative determination of the structure and composition of a catalyst as a function of its gas environment allows the establishment of structure–performance relationships. Herein, we determine the...
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Copper-zinc-alumina catalysts are used industrially for methanol synthesis from feedstock containing carbon monoxide and carbon dioxide. The high performance of the catalyst stems from synergies that develop between its components. This important catalytic system has been investigated with a myriad of approaches, however, no comprehensive agreement...
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One dimensional graphene nanostructures are one of the most promising materials for next generation electronics. Here, the chemical vapor depostion growth of graphene nanoribbons (GNRs) and graphene nanospears (GNSs) on a copper surface is reported. The growth of GNRs and GNSs is enabled by a vapor–liquid–solid (VLS) mechanism guided by on‐surface...
Article
The dynamic interactions between noble metal particles and reducible metal-oxide supports can depend on redox reactions with ambient gases. Transmission electron microscopy revealed that the strong metal-support interaction (SMSI)-induced encapsulation of platinum particles on titania observed under reducing conditions is lost once the system is ex...
Preprint
Direct growth of large-area vertically stacked two-dimensional (2D) van der Waal (vdW) materials is a prerequisite for their high-end applications in integrated electronics, optoelectronics and photovoltaics. Currently, centimetre- to even metre-scale monolayers of single-crystal graphene (MLG) and hexagonal boron nitride (h-BN) have been achieved...
Preprint
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The thermal carburization of MoO3 nanobelts (nb) and SiO2-supported MoO3 nanosheets under a 1 : 4 mixture of CH4 : H2 yields Mo2C-nb and Mo2C/SiO2. Following this process by in situ Mo K-edge X-ray absorption spectroscopy (XAS) reveals different carburization pathways for unsupported and supported MoO3. In particular, the carburization of α-MoO3-nb...
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Copper and zinc oxide are a dream team in transforming carbon dioxide and carbon monoxide together with hydrogen to the valuable base chemical methanol. Inspired by the cover art of the music masterpiece “Wish you were here” by Pink Floyd the picture featuring the Research Article (DOI: 10.1002/anie.202200301) by Jeroen A. van Bokhoven et al. highl...
Article
Kupfer und Zinkoxid sind ein Dreamteam bei der Umwandlung von Kohlendioxid und Kohlenmonoxid mit Wasserstoff in die wertvolle Basischemikalie Methanol. Inspiriert vom Cover von Pink Floyds Meisterwerk „Wish you were here“ illustriert das Titelbild, das zum Forschungsartikel (DOI: 10.1002/ange.202200301) von Jeroen A. van Bokhoven et al. gehört, das...
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Fossil-free ironmaking is indispensable for reducing massive anthropogenic CO2 emissions in the steel industry. Hydrogen-based direct reduction (HyDR) is among the most attractive solutions for green ironmaking, with high technology readiness. The underlying mechanisms governing this process are characterized by a complex interaction of several che...
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The copper-zinc-alumina (CZA) catalyst is one of the most important catalysts. Nevertheless, understanding of the complex CZA structure is still limited and hampers further optimization. Critical to the production of a highly active and stable catalyst are optimal start-up procedures in hydrogen. Here, by employing operando X-ray absorption spectro...
Article
The copper‐zinc‐alumina (CZA) catalyst is one of the most important catalysts. Nevertheless, the still limited understanding of the complex CZA structure hampers further optimization. Critical to the production of a highly active and stable catalyst are optimal start‐up procedures in hydrogen. Here, by employing operando X‐ray absorption spectrosco...
Preprint
Full-text available
Fossil-free ironmaking is indispensable for reducing massive anthropogenic CO2 emissions in the steel industry. Hydrogen-based direct reduction (HyDR) is among the most attractive solutions for green ironmaking, with high technology readiness. The underlying mechanisms governing this process are characterized by a complex interaction of several che...
Preprint
The properties of two-dimensional (2D) van der Waals (vdW) materials can be tuned through nanostructuring or controlled layer stacking, where interlayer hybridization induces exotic electronic states and transport phenomena. Here, we describe an assisted self-assembly of twisted layer graphene. The process, which can be implemented in standard chem...
Preprint
Full-text available
Graphene nanoribbons (GNRs) are considered one of the most promising materials for next generation electronics, however a reliable and controllable synthesis method is still lacking. Here, we report the CVD growth of GNRs on a copper surface and the corresponding mechanisms of growth. One-dimensional GNR growth is enabled by a vapor-liquid-solid (V...
Article
The thermal carburization of MoO 3 nanobelts (nb) and SiO 2 -supported MoO 3 nanosheets under a 1 : 4 mixture of CH 4 : H 2 yields Mo 2 C-nb and Mo 2 C/SiO 2 . Following this process by in...
Article
Water splitting will become important to store excess renewable electrical energy into hydrogen. Although the oxygen-evolution reaction (OER) by water oxidation is a critical reaction for water splitting, further investigations are needed to find the details of the OER mechanism for various electrocatalysts. More in particular for homogeneous elect...
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Full-text available
Metal catalysts play an important role in industrial redox reactions. Although extensively studied, the state of these catalysts under operating conditions is largely unknown, and assignments of active sites remain speculative. Herein, an operando transmission electron microscopy study is presented, which interrelates the structural dynamics of red...
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Full-text available
The active state of heterogeneous catalysts is typically metastable and can only be generated under actual reaction conditions. In article number 2101772, Xing Huang, Marc‐Georg Willinger, and co‐workers report an operando transmission electron microscopy study to characterize chemical dynamics and surface sites of metal catalysts, as well as their...
Article
We explore three different potential mechanisms to introduce 4 mol% ZnO sintering additive to the promising yttrium-doped barium zirconate (Ba(Zr,Y)O3-δ, BZY) proton conductor. The mechanisms involve Zn substitution for Y, Zr, or B-site cation excess. The addition of ZnO promotes high densification levels (up to 98% of the theoretical value) at 130...
Preprint
Full-text available
div>Metal catalysts play an important role in industrial redox reactions. Although extensively studied, the state of these catalysts under operating conditions is largely unknown and assignments of active sites remain speculative. Herein, we present an operando transmission electron microscopy study that interrelates structural dynamics of redox me...
Article
Multiferroic materials demonstrating coexistence of magnetic and ferroelectric orders are promising candidates for magnetoelectric devices. While understanding the underlying mechanism of interplaying of ferroic properties is important, tailoring their properties to make them potential candidates for magnetoelectric devices is challenging. Here, th...
Article
Synthesizing high‐quality two‐dimensional nanomaterials of non‐layered metal oxide is a grand challenge, especially when long range single‐crystallinity and clean high‐energy surfaces are required. Here, we report the synthesis of single‐crystalline MgO(111) nanosheets via a two‐step process involving the formation of ultrathin Mg(OH) 2 nanosheets...
Article
Ultrathin single crystalline MgO nanosheets that are preferentially oriented in the [111] direction are prepared through topotactic decomposition of Mg(OH)2 nanosheets under dynamic vacuum. The surface is highly defect‐rich with under‐coordinated O and Mg ions and F‐centers, which makes the MgO nanosheets highly active in interacting with CO probe...
Preprint
Synthesizing high-quality two-dimensional nanomaterials of non-layered metal oxide is a grand challenge because it requires long range single-crystallinity and clean high-energy surfaces. Here, we report the synthesis of single-crystalline MgO(111) nanosheets via a two-step process involving the formation of ultrathin Mg(OH)<sub>2</sub> nanosheets...
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Full-text available
Starting from subsurface Zr0-doped “inverse” Pd and bulk-intermetallic Pd0Zr0 model catalyst precursors, we investigated the dry reforming reaction of methane (DRM) using synchrotron-based near ambient pressure in-situ X-ray photoelectron spectroscopy (NAP-XPS), in-situ X-ray diffraction and catalytic testing in an ultrahigh-vacuum-compatible recir...
Article
The fabrication of power semiconductor devices based on 4H-silicon carbide (SiC) typically includes doping by ion implantation and postimplantation annealing to activate the implanted dopants. The high-temperature annealing process can initiate various diffusion mechanisms that alter the initial implantation profile in terms of spatial distribution...
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How a catalyst behaves microscopically under reaction conditions, and what kinds of active sites transiently exist on its surface, is still very much a mystery to the scientific community. Here we present an in situ study on the red-ox behaviour of copper in the model reaction of hydrogen oxidation. Direct imaging combined with on-line mass spectro...
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Full-text available
Ag doped TiO2 photocatalysts (Ag@TiO2) were prepared with an aim to extend the absorption range of TiO2 into the visible region, for tentative application under solar irradiation. Photocatalyst synthesized by the novel method using chitosan for reduction of Ag+ to Ag0 nanoparticles was compared to similar catalysts previously reported. The photocat...
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Full-text available
Light elements in the interstitial site of transition metals have strong influence on heterogeneous catalysis via either expression of surface structures or even direct participation into reaction. Interstitial atoms are generally metastable with a strong environmental dependence, setting up giant challenges in controlling of heterogeneous catalysi...
Article
Heterogeneous catalysts in the form of atomically dispersed metals on a support provide the most efficient utilization of the active component, which is especially important for scarce and expensive late transition metals. These catalysts also enable unique opportunities to understand reaction pathways through detailed spectroscopic and computation...
Article
Full-text available
Heterogeneous catalysts play a pivotal role in the chemical industry. The strong metal-support interaction (SMSI), which affects the catalytic activity, is a phenomenon researched for decades. However, detailed mechanistic understanding on real catalytic systems is lacking. Here, this surface phenomenon was studied on an actual platinum-titania cat...
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Full-text available
Common methods to produce supported catalysts include impregnation, precipitation, and thermal spray techniques. Supported electrocatalysts produced by a novel method for thermal spray deposition were investigated with respect to their structural properties, elemental composition, and electrochemical performance. This was done using electron micros...
Article
Herein, we report TiC as precursor of a highly active and novel TiO2-TiC composite for the catalytic oxidation of HBr into Br2, which is a key technology for bromine looping in the halogen-mediated process for natural gas valorisation. In addition, we investigate the mechanism of TiO2 formation that is pivotal in deriving synthesis-structure-perfor...
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Full-text available
The effect of NaNO3 and its physical state on the thermal decomposition pathways of hydrated magnesium hydroxycarbonate (hydromagnesite, HM) towards MgO was examined by in situ total scattering. Pair distribution function (PDF) analysis of these data allowed us to probe the structural evolution of pristine and NaNO3-promoted HM. A multivariate curv...
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Plasma nitriding was applied to ferritic stainless steel substrates to improve their performances as interconnects for solid oxide fuel cell devices. The samples underwent electrical conductivity test and SEM/EDS, TEM/EDS, environmental-SEM analyses. The first stages of corrosion were recorded in-situ with the e-SEM. Nitriding is effective in limit...
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Full-text available
High-quality AB-stacked bilayer or multilayer graphene larger than a centimetre has not been reported. Here, we report the fabrication and use of single-crystal Cu/Ni(111) alloy foils with controllable concentrations of Ni for the growth of large-area, high-quality AB-stacked bilayer and ABA-stacked trilayer graphene films by chemical vapour deposi...
Article
Full-text available
Understanding how catalysts work during chemical reactions is crucial when developing efficient catalytic materials. The dynamic processes involved are extremely sensitive to changes in pressure, gas environment and temperature. Hence, there is a need for spatially resolved operando techniques to investigate catalysts under working conditions and o...
Preprint
Full-text available
Heterogeneous catalysts in the form of atomically dispersed metals on a support provide the most efficient utilization of the active component, which is especially important for scarce and expensive late transition metals. These catalysts also enable unique opportunities to understand reaction pathways through detailed spectroscopic and computation...
Preprint
Heterogeneous catalysts in the form of atomically dispersed metals on a support provide the most efficient utilization of the active component, which is especially important for scarce and expensive late transition metals. These catalysts also enable unique opportunities to understand reaction pathways through detailed spectroscopic and computation...
Article
Wafer-scale monocrystalline two-dimensional (2D) materials can theoretically be grown by seamless coalescence of individual domains into a large single-crystal. Here we present a concise study of the coalescence behavior of crystalline 2D films using a combination of complementary in situ methods. Direct observation of overlayer growth from the ato...
Article
Full-text available
ZnO has prominent electron transport and optical properties, beneficial for photovoltaic application, but its surface is prone to the formation of defects. To overcome this problem, we deposited nanostructured TiO2 thin film on ZnO nanorods to form a stable shell. ZnO nanorods synthesized by wet-chemistry are single crystals. Three different proced...
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Full-text available
Understanding the growth mechanism of carbon nanotubes (CNTs) has been long pursued since its discovery. With recent integration of in situ techniques into the study of CNT growth, important insights about the growth mechanism of CNT have been generated, which have improved our understanding significantly. However, previous in situ experiments were...
Article
Imaging Reaction Dynamics on Inverse Model Catalyst Surfaces by In Situ Environmental SEM - Volume 25 Supplement - Cédric Barroo, Zhu-Jun Wang, Marc Georg Willinger
Article
We report an operando examination of a model nanocrystalline In2O3 catalyst for methanol synthesis via CO2 hydrogenation (300 oC, 20 bar) by combing X-ray absorption spectroscopy (XAS), X-ray powder diffraction (XRD) and in situ TEM. Three distinct catalytic regimes are identified during CO2 hydrogenation: activation, stable performance, and deacti...
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Full-text available
The development of two-dimensional (2D) materials has opened up possibilities for their application in electronics, optoelectronics and photovoltaics, because they can provide devices with smaller size, higher speed and additional functionalities compared with conventional silicon-based devices¹. The ability to grow large, high-quality single cryst...
Article
Atomistische Einblicke in die Metall‐Promotor‐Wechselwirkung in Rhodium‐Katalysatoren für die Umwandlung von Syngas in Ethanol liefern X. Huang, M. G. Willinger, A. Trunschke und Mitarbeiter in ihrer Zuschrift (DOI: 10.1002/ange.201902750). Beim besten Katalysator (zweifach Mn‐ und Fe‐promotiertes Rh auf Silica) führt die Metall‐Promotor‐Wechselwir...
Article
Atomic‐level insight about the metal–promoter interaction in Rh‐based catalysts for the conversion of syngas to ethanol is provided by X. Huang, M. G. Willinger, A. Trunschke and co‐workers in their Communication (DOI: 10.1002/anie.201902750). In the best performing catalyst (Mn and Fe bi‐promoted Rh on silica), the metal–promoter interaction leads...
Article
The direct conversion of syngas to ethanol is a cornerstone reaction in evolving technologies of CO2 utilization and hydrogen storage, which is typically performed using promoted Rh catalysts. A rational catalyst development requires a detailed structural understanding of the activated catalyst and in particular, the specific roles that promoters p...
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Full-text available
Grazing incidence X-ray diffractometry (GIXRD) can deliver integral information of the structure and chemistry of surface near regions, which can be beneficial for functional materials related to interfacial reactions. Here, we present an in situ laboratory GIXRD setup for electrochemical experiments. The method is capable to directly correlate cha...
Article
The direct conversion of syngas to ethanol is a cornerstone reaction in evolving technologies of CO2 utilization and hydrogen storage, which is typically performed using promoted Rh catalysts. A rational catalyst development requires a detailed structural understanding of the activated catalyst and in particular, the specific roles that promoters p...
Article
Full-text available
Near-field spectral response of metallic nanocavities is a key characteristic in plasmon-assisted photophysical and photochemical processes. Here we show that the near-field spectral response of an optically-excited plasmonic scanning tunneling microscope (STM) junction can be probed by single-molecule reactions which serve as a nanoscale sensor de...
Article
The dynamics of solid state dewetting phenomena of a 50 nm thick, mazed bicrystalline Al film on single crystalline α-Al2O3 (sapphire) substrates was studied in-situ using an environmental scanning electron microscope (ESEM). The bicrystalline Al thin films served as a model system where the influence of grain boundaries and texture effects are wel...
Article
Pattern Formation in Catalyzed Surface Reactions Studied by In Situ SEM - Volume 25 Issue S1 - Cédric Barroo, Zhu-Jun Wang, Marc Georg Willinger