Edvin Lundgren

• PhD, Professor
• Professor (Full) at Lund University

In recent years, studies of surfaces at more realistic conditions has advanced significantly, leading to an increased understanding of surface dynamics under reaction conditions. The development has mainly been due to the development of new experimental techniques or new experimental approaches. Techniques such as High Pressure Scanning Tunneling/F...

We have used grazing incidence X‐ray absorption near edge spectroscopy (XANES) to investigate the behavior of monolayer FeO films on Pt(111) under near ambient pressure CO oxidation conditions with a total gas pressure of 1 bar. Spectra indicate reversible changes during oxidation and reduction by O and CO at 150 °C, attributed to a transformation...

Traditional methods to study electrochemical (EC) processes, although successful, are based on current/voltage measurements, providing information about performances rather than offering a direct observation of chemical and structural changes occurring at the electrode surface. These processes are localized at the electrode-electrolyte interface, t...

Corrosion results in large costs and environmental impact but can be controlled by thin oxide films that passivate the metal surfaces and hinder further oxidation or dissolution in an aqueous environment. The structure, chemistry, and thickness of these oxide films play a significant role in determining their anti-corrosion properties and the early...

Traditional operando methods to study electrochemical (EC) processes, although successful, are based on EC measurements, lacking in direct sensitivity of chemical and structural changes. A fundamental understanding of the underlying mechanism occurring during an EC reaction could allow to improve performances and properties of applied material syst...

Nanometer-thin and spontaneously formed oxide films, or passive films, govern the corrosion resistance of many advanced alloys [1]. Our current understanding of the structure and chemistry of the passive film is primarily based on ex situ surface analysis using X-ray Photoelectron Spectroscopy (XPS) [2] and Scanning Tunneling Microscopy (STM) [3]....

Industrial catalysts are complex materials systems operating in harsh environments. The active parts of the catalysts are nanoparticles that expose different facets with different surface orientations at which the catalytic reactions occur. However, these facets are close to impossible to study in detail under industrially relevant operating condit...

We investigated the structural evolution of electrochemically fabricated Pd nanowires in situ by means of grazing-incidence transmission small- and wide-angle x-ray scattering (GTSAXS and GTWAXS), x-ray fluorescence (XRF) and 2-dimensional surface optical reflectance (2D-SOR). This shows how electrodeposition and the hydrogen evolution reaction (HE...

In2O3-based catalysts have shown high activity and selectivity for CO2 hydrogenation to methanol; however, the origin of the high performance of In2O3 is still unclear. To elucidate the initial steps of CO2 hydrogenation over In2O3, we have combined X-ray photoelectron spectroscopy and density functional theory calculations to study the adsorption...

In$_2$O$_3$-based catalysts have shown high activity and selectivity for CO$_2$ hydrogenation to methanol, however the origin of the high performance of In$_2$O$_3$ is still unclear. To elucidate the initial steps of CO$_2$ hydrogenation over In$_2$O$_3$, we have combined X-ray Photoelectron Spectroscopy (XPS) and Density Functional Theory (DFT) ca...

Corrosion is the main factor limiting the lifetime of metallic materials, and a fundamental understanding of the governing mechanism and surface processes is difficult to achieve since the thin oxide films at the metal-liquid interface governing passivity are notoriously challenging to study. Here, a combination of synchrotron-based techniques and...

The catalytic oxidation of HCl by molecular oxygen (Deacon process) over ceria allows the recovery of molecular chlorine from omnipresent HCl waste produced in various industrial processes. Previous density functional theory (DFT) model-calculations1 proposed, that the most critical reaction step in this process is the displacement of tightly bound...

The electrochemical growth of Au nanowires in a template of nanoporous anodic aluminum oxide was investigated in situ by means of grazing-incidence transmission small- and wide-angle x-ray scattering (GTSAXS and GTWAXS), x-ray fluorescence (XRF), and two-dimensional surface optical reflectance. The XRF and the overall intensity of the GTWAXS patter...

Various mechanisms have been proposed for hydrogen embrittlement of duplex stainless steel, but the causation of hydrogen-induced material degradation has remained unclear. This work shows that phase instability (decomposition) of the austenite phase and ductile-to-brittle transition of the ferrite phase precedes hydrogen embrittlement. In-situ dif...

To investigate the aging effect on a passive film of Ni23Cr15Mo and Ni22Cr9Mo3Nb, synchrotron-based X-ray photoelectron spectroscopy (XPS) was used to analyze the structure and composition of the air-formed passive film on the alloys. The corrosion resistance of the two Ni alloys in 1M NaCl solution was evaluated with electrochemical cyclic polariz...

This work introduces the high-energy surface X-ray diffraction analysis toolkit (HAT), an open-source cross-platform software package written in Python to allow the extraction and processing of high-energy surface X-ray diffraction (HESXRD) data sets. Thousands of large-area detector images are collected in a single HESXRD scan, corresponding to bi...

The passive film stability on stainless steel can be affected by hydrogen absorption and lead to microstructure embrittlement. This work shows that the absorption of hydrogen results in surface degradation due to oxide reduction and ionic defect generation within the passive film, which decomposes and eventually vanishes. The passive film provides...

The electrochemical growth of Au nanowires in a template of nano-porous anodic aluminum oxide was investigated in situ by means of grazing-incidence transmission small- and wide-angle x-ray scattering (GTSAXS and GTWAXS), x-ray fluorescence (XRF) and 2-dimensional surface optical reflectance (2D-SOR). The XRF and the overall intensity of the GTWAXS...

We investigated the structural evolution of electrochemically fabricated Pd nanowires in situ by means of grazing-incidence transmission small- and wide-angle x-ray scattering (GTSAXS and GTWAXS), x-ray fluorescence (XRF) and 2-dimensional surface optical reflectance (2D-SOR). This shows how electrodeposition and the hydrogen evolution reaction (HE...

Ambient Pressure X-ray Photoelectron Spectroscopy combined with an electrochemical setup is used to study, in situ, the electrochemical oxide growth on an industrial Ni-Cr-Mo alloy. The native oxide film was characterized in vacuum and in water vapor at 17 mbar, and was found to be 11.4 Å thick and rich in Cr³⁺. In 0.1M NaCl electrolyte, anodic gro...

Various mechanisms have been proposed for hydrogen embrittlement, but the causation of hydrogen-induced material degradation has remained unclear. This work shows hydrogen embrittlement due to phase instability (decomposition). In-situ diffraction measurements revealed metastable hydrides formed in stainless steel, typically declared as a non-hydri...

Curved crystals are a simple but powerful approach to bridge the gap between single crystal surfaces and nanoparticle catalysts, by allowing a rational assessment of the role of active step sites in gas-surface reactions. Using a curved Rh(111) crystal, here, we investigate the effect of A-type (square geometry) and B-type (triangular geometry) ato...

Many surface science experiments within heterogeneous catalysis are now conducted in realistic conditions at higher pressures. At these pressures, localized gas conditions will form throughout the reactor. Understanding these gas conditions and their interaction with the catalyst surface at relevant time scales and with spatial resolution is import...

A high-throughput method for the fabrication of ordered arrays of Au nanoparticles is presented. It is based on pulsed electrodeposition into porous anodic alumina templates. In contrast to many synthesis routes, it is cyanide-free, prior separation of the alumina template from the aluminium substrate is not required, and the use of contaminating s...

Determination of the atomic structure of solid surfaces typically depends on comparison of measured properties with simulations based on hypothesized structural models. For simple structures, the models may be guessed, but for more complex structures there is a need for reliable theory‐based search algorithms. So far, such methods have been limited...

Determination of the atomic structure of solid surfaces typically depends on comparison of measured properties with simulations based on hypothesized structural models. For simple structures, the models may be guessed, but for more complex structures there is a need for reliable theory‐based search algorithms. So far, such methods have been limited...

We have used grazing incidence X-ray absorption fine structure spectroscopy at the cobalt K-edge to characterize monolayer CoO films on Pt(111) under ambient pressure exposure to CO and O2, with the aim of identifying the Co phases present and their transformations under oxidizing and reducing conditions. X-ray absorption near edge structure (XANES...

The local lattice strain evolution during electrochemical hydrogen charging and mechanical loading in 25Cr-7Ni super duplex stainless steel were measured in-situ using synchrotron high-energy x-ray diffraction. Post-mortem electron backscattered diffraction analysis showed that the austenite phase underwent plastic deformation in the near-surface d...

Determination of the atomic structure of solid surfaces is a challenge that has resisted solution despite advancements in experimental methods. Theory-based global optimization has the potential to revolutionize the field by providing reliable structure models as the basis for interpretation of experiments and for prediction of material properties....

The surface chemistry and thickness of the native oxide, hydroxide, and modified sub-surface layer of three Ni superalloys (alloy 59, 625, and 718) were determined by synchrotron X-ray Photoelectron Spectroscopy (XPS) and X-ray Reflectivity (XRR). Taking advantage of the synchrotron radiation techniques, a procedure for normalizing the photoelectro...

Using a new sample environment, the two operando surface diagnostic techniques two-dimensional surface optical reflection (2D-SOR) and polarization-modulated infrared reflection-absorption spectroscopy (PM-IRRAS) have been combined with mass spectrometry (MS) to characterize a catalytic reaction. With both techniques integrated in a custom-built se...

Steps at metal surfaces may influence energetics and kinetics of catalytic reactions in unexpected ways. Here, we report a significant reduction of the CO saturation coverage in Pd vicinal surfaces, which in turn is relevant for the light-off of the CO oxidation reaction. The study is based on a systematic investigation of CO adsorption on vicinal...

We have combined high-energy surface x-ray diffraction (HESXRD) with 2D surface optical reflectance (2D-SOR) to perform in situ electrochemical measurements of a Au(111) electrode in 0.1 M HClO4 electrolyte. We show that electrochemically induced changes to Au(111) surface during cyclic voltammetry can be simultaneously observed with 2D-SOR and HES...

Industrial catalysts are often comprised of nanoparticles supported on high-surface-area oxides, in order to maximise the catalytically active surface area and thereby utilise the active material better. These nanoparticles expose steps and corners that, due to low coordination to neighboring atoms, are more reactive and, as a consequence, are ofte...

X-ray diffractometers primarily designed for surface X-ray diffraction are often used to measure the diffraction from powders, textured materials and fiber-texture samples in 2θ scans. Unlike in high-energy powder diffraction, only a fraction of the powder rings is typically measured, and the data consist of many detector images across the 2θ range...

Performing fundamental operando catalysis studies under realistic conditions is a key to further develop and increase the efficiency of industrial catalysts. Operando X-ray photoelectron spectroscopy (XPS) experiments have been limited to pressures, and the relevance for industrial applications has been questioned. Herein, we report on the CO oxida...

Using grazing incidence X-rays and X-ray photoelectron spectroscopy during the mass transfer limited catalytic oxidation of CO, the long-range surface structure of Pd(100) was investigated. Under the reaction conditions of 50:4 O2 to CO, 300 mbar pressure, and temperatures between 200 and 450 °C, the surface structure resulting from oxidation and t...

We have developed a microscope with a spatial resolution of 5 μm, which can be used to image the two-dimensional surface optical reflectance (2D-SOR) of polycrystalline samples in operando conditions. Within the field of surface science, operando tools that give information about the surface structure or chemistry of a sample under realistic experi...

Templated electrochemical growth in nanoporous alumina can be used to fabricate nanowires with applications in magnetic storage devices, hydrogen sensors, and electrocatalysis. It is known that nanowires, grown in such templates, are strained. The strain in nanoscale materials can influence their performance in applications such as catalysts and el...

X-ray diffractometers primarily designed for surface x-ray diffraction are often used to measure the diffraction from powders, textured materials, and fiber-texture samples in so-called 2θ scans. There are, however, very few examples where the measured intensity is directly used, such as for Rietveld refinement, as is common with other powder diffr...

To bridge the pressure gap in heterogeneous catalysis and maximize the gain of operando information, we have combined PM-IRRAS with the imaging techniques SOR and PLIF and measured CO oxidation on a Pd(100) crystal.

Catalysts are materials that accelerate the rate of a desired chemical reaction. As such, they constitute an integral part in many applications ranging from the production of fine chemicals in chemical industry to exhaust gas treatment in vehicles. Accordingly, it is of utmost economic interest to improve catalyst efficiency and performance, which...

p> Templated electrochemical growth in nanoporous alumina can be used to fabricate nanowires with applications in magnetic storage devices, hydrogen sensors, and electrocatalysis. It is known that nanowires, grown in such templates, are strained. The strain in nanoscale materials can influence their performance in applications such as catalysts and...

Down to a cathodic potentials of -1.20 V versus the reversible hydrogen electrode, the structure of IrO2(110) electrodes supported by TiO2(110) is found to be stable by in situ synchrotron-based X-ray diffraction. Such high cathodic potentials should lead to reduction to metallic Ir (Pourbaix diagram). From the IrO2 lattice parameters, determined d...

We investigate with in situ surface X-ray diffraction (SXRD) and X-ray reflectivity (XRR) experiments the cathodic stability of an ultrathin single-crystalline IrO2(110) film with a regular array of mesoscopic rooflike structures that is supported on a RuO2(110)/Ru(0001) template. It turns out that the planarity of the single-crystalline IrO2(110)...

A method for the electrochemical synthesis of palladium nanowires, using porous alumina templates with diameters of 25 nm and 40 nm, is presented. Through an electrochemical barrier layer thinning step, pulsed electrodeposition can take place directly into the anodized aluminum; without need for extra removal, pore opening, and metal contact coatin...

The catalytic oxidation of CO on transition metals, such as Pt, is commonly viewed as a sharp transition from the CO‐inhibited surface to the active metal, covered with O. However, we find that minor amounts of O are present in the CO‐poisoned layer that explain why, surprisingly, CO desorbs at stepped and flat Pt crystal planes at once, regardless...

High resolution x-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) were used to characterize IrO2(110) films on Ir(100) with stoichiometric as well as OH-rich terminations. Core-level Ir 4f and O 1s peaks were identified for the undercoordinated Ir and O atoms and bridging and on-top OH groups at the IrO2(110) surfaces. Peak...

Determining how electrode structure governs the performance of an electrocatalyst requires techniques capable of probing structure at the atomic scale, often in situ and operando. In recent years, there have been numerous advances in the main experimental techniques for determining the structure of the electrochemical interface. In situ/operando sy...

The light‐off of the CO oxidation is simultaneous on all Pt crystal surfaces vicinal to the (111) plane, regardless of the reaction conditions, and in contrast with the structural dependence of Pd. Using ambient‐pressure XPS we find that, immediately prior to ignition, atomic oxygen incorporates to the subsurface plane, leading to buckling of the t...

Local strain development in the microstructure of a commercial 25Cr-7Ni super duplex stainless steel was mapped using high-energy x-ray diffraction during cathodic hydrogen charging under constant uniaxial load. The infusion of hydrogen resulted in tensile strains in austenite grains, one order of magnitude larger than those in the ferrite. Most st...

The interaction of ultrathin single crystalline IrO2(110) films with the gas phase proceeds via the coordinatively unsaturated sites (cus), in particular Ircus, the undercoodinated oxygen species on-top O (Oot) that are coordinated to Ircus, and bridging O (Obr). With the combination of different experimental techniques, such as thermal desorption...

Grazing-incidence x-ray diffraction was employed to measure, operando, during electrochemical hydrogen charging, the lattice strain development of the near-surface in super duplex stainless steel under applied tensile load. Hydrogen absorption led to the formation of tensile strains in both the austenite (γ) and ferrite (δ) phases perpendicular to...

A native passive film on 25Cr-7Ni super duplex stainless steel was analyzed using synchrotron hard X-ray photoemission electron microscopy, focusing on variations between individual grains of ferrite and austenite phases. The film consists of an oxide inner layer and an oxyhydroxide outer layer, in total 2.3 nm thick. The Cr content is higher in th...

We have developed an electrochemical cell for in situ 2-Dimensional Surface Optical Reflectance (2D-SOR) studies during anodization and cyclic voltammetry. The 2D-SOR signal was recorded from electrodes made of polycrystalline Al, Au(111), and Pt(100) single crystals. The changes can be followed at a video rate acquisition frequency of 200 Hz and d...

We have developed an electrochemical cell for in situ 2-Dimensional Surface Optical Reflectance (2D-SOR) studies during anodization and cyclic voltammetry. The 2D-SOR signal was recorded from electrodes made of polycrystalline Al, Au(111), and Pt(100) single crystals. The changes can be followed at a video rate acquisition frequency of 200 Hz and d...

High energy surface x-ray diffraction (HESXRD), x-ray reflectivity (XRR), mass spectrometry (MS) and surface optical reflectance (SOR) have been combined to simultaneously obtain sub-second information on the surface structure and morphology from a Pd(100) model catalyst during in situ oxidation at elevated temperatures and pressures resulting in P...

We have investigated the structure of an ultrathin iron oxide phase grown on Ag(100) using surface x-ray diffraction in combination with Hubbard-corrected density functional theory (DFT+U) calculations. The film exhibits a novel structure composed of one close-packed layer of octahedrally coordinated Fe²⁺ sandwiched between two close-packed layers...

We combine PLIF and NAP-XPS to investigate the CO oxidation reaction at vicinal Pt(111) surfaces in the millibar regime, using a curved sample. We find that the catalytic activation of Pt occurs in all vicinal planes simultaneously, irrespectively of the reaction parameters. The systematic analysis of chemical species across the entire curved surfa...