Surface oxidation-induced restructuring of liquid Pd-Ga SCALMS model catalysts

Author(s):  
Haiko Wittkaemper ◽  
Sven Maisel ◽  
Michael Moritz ◽  
Mathias Grabau ◽  
Andreas Görling ◽  
...  

We have examined model systems for the recently reported Pd-Ga Supported Catalytically Active Liquid Metal Solutions (SCALMS) catalysts using near-ambient pressure x-ray photoelectron spectroscopy (NAP-XPS) under oxidizing conditions. Gallium is...


2011 ◽  
Vol 2 ◽  
pp. 593-606 ◽  
Author(s):  
Matthias Roos ◽  
Dominique Böcking ◽  
Kwabena Offeh Gyimah ◽  
Gabriela Kucerova ◽  
Joachim Bansmann ◽  
...  

Aiming at model systems with close-to-realistic transport properties, we have prepared and studied planar Au/TiO2 thin-film model catalysts consisting of a thin mesoporous TiO2 film of 200–400 nm thickness with Au nanoparticles, with a mean particle size of ~2 nm diameter, homogeneously distributed therein. The systems were prepared by spin-coating of a mesoporous TiO2 film from solutions of ethanolic titanium tetraisopropoxide and Pluronic P123 on planar Si(100) substrates, calcination at 350 °C and subsequent Au loading by a deposition–precipitation procedure, followed by a final calcination step for catalyst activation. The structural and chemical properties of these model systems were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), N2 adsorption, inductively coupled plasma ionization spectroscopy (ICP–OES) and X-ray photoelectron spectroscopy (XPS). The catalytic properties were evaluated through the oxidation of CO as a test reaction, and reactivities were measured directly above the film with a scanning mass spectrometer. We can demonstrate that the thin-film model catalysts closely resemble dispersed Au/TiO2 supported catalysts in their characteristic structural and catalytic properties, and hence can be considered as suitable for catalytic model studies. The linear increase of the catalytic activity with film thickness indicates that transport limitations inside the Au/TiO2 film catalyst are negligible, i.e., below the detection limit.





ACS Catalysis ◽  
2014 ◽  
Vol 4 (9) ◽  
pp. 3160-3168 ◽  
Author(s):  
Luis M. Martínez-Prieto ◽  
Sophie Carenco ◽  
Cheng H. Wu ◽  
Eric Bonnefille ◽  
Stephanus Axnanda ◽  
...  


Crystals ◽  
2020 ◽  
Vol 10 (10) ◽  
pp. 947
Author(s):  
Raffael Rameshan ◽  
Andreas Nenning ◽  
Johannes Raschhofer ◽  
Lorenz Lindenthal ◽  
Thomas Ruh ◽  
...  

For an in-depth characterization of catalytic materials and their properties, spectroscopic in-situ (operando) investigations are indispensable. With the rapid development of advanced commercial spectroscopic equipment, it is possible to combine complementary methods in a single system. This allows for simultaneously gaining insights into surface and bulk properties of functional oxides, such as defect chemistry, catalytic characteristics, electronic structure, etc., enabling a direct correlation of structure and reactivity of catalyst materials, thus facilitating effective catalyst development. Here, we present a novel sample-stage, which was specifically developed to pave the way to a lab–based combination of near ambient pressure X-ray photoelectron spectroscopy and electrochemical impedance spectroscopy with simultaneous catalytic operando measurements. This setup is designed to probe different (model) systems under conditions close to real heterogeneous catalysis, with a focus on solid oxide electrochemical cells. In a proof of concept experiment using an electrochemical model cell with the doped perovskite Nd0.6Ca0.4Fe0.9Co0.1O3-δ as working electrode, the precise control of the surface chemistry that is possible with this setup is demonstrated. The exsolution behavior of the material was studied, showing that at a lower temperature (500 °C) with lower reducing potential of the gas phase, only cobalt was exsolved, forming metallic particles on the surface of the perovskite-type oxide. Only when the temperature was increased to 600 °C and a cathodic potential was applied (−250 mV) Fe also started to be released from the perovskite lattice.



2016 ◽  
Vol 8 (1) ◽  
pp. 102-108 ◽  
Author(s):  
Luca Artiglia ◽  
Fabrizio Orlando ◽  
Kanak Roy ◽  
René Kopelent ◽  
Olga Safonova ◽  
...  


Catalysts ◽  
2020 ◽  
Vol 10 (12) ◽  
pp. 1456
Author(s):  
Yujie Fu ◽  
You Zhang ◽  
Qi Xin ◽  
Zhong Zheng ◽  
Yu Zhang ◽  
...  

Chlorinated volatile organic compounds (CVOCs) are vital environmental concerns due to their low biodegradability and long-term persistence. Catalytic combustion technology is one of the more commonly used technologies for the treatment of CVOCs. Catalysts with high low-temperature activity, superior selectivity of non-toxic products, and resistance to chlorine poisoning are desirable. Here we adopted a plasma treatment method to synthesize a tin-doped titania loaded with ruthenium dioxide (RuO2) catalyst, possessing enhanced activity (T90%, the temperature at which 90% of dichloromethane (DCM) is decomposed, is 262 °C) compared to the catalyst prepared by the conventional calcination method. As revealed by transmission electron microscopy, X-ray diffraction, N2 adsorption, X-ray photoelectron spectroscopy, and hydrogen temperature-programmed reduction, the high surface area of the tin-doped titania catalyst and the enhanced dispersion and surface oxidation of RuO2 induced by plasma treatment were found to be the main factors determining excellent catalytic activities.



Nano Energy ◽  
2021 ◽  
Vol 83 ◽  
pp. 105830
Author(s):  
Yu Wang ◽  
Wanwan Wang ◽  
Jing Xie ◽  
Chia-Hsin Wang ◽  
Yaw-Wen Yang ◽  
...  


2021 ◽  
Vol 4 (1) ◽  
Author(s):  
Marc Benjamin Hahn ◽  
Paul M. Dietrich ◽  
Jörg Radnik

AbstractIonizing radiation damage to DNA plays a fundamental role in cancer therapy. X-ray photoelectron-spectroscopy (XPS) allows simultaneous irradiation and damage monitoring. Although water radiolysis is essential for radiation damage, all previous XPS studies were performed in vacuum. Here we present near-ambient-pressure XPS experiments to directly measure DNA damage under water atmosphere. They permit in-situ monitoring of the effects of radicals on fully hydrated double-stranded DNA. The results allow us to distinguish direct damage, by photons and secondary low-energy electrons (LEE), from damage by hydroxyl radicals or hydration induced modifications of damage pathways. The exposure of dry DNA to x-rays leads to strand-breaks at the sugar-phosphate backbone, while deoxyribose and nucleobases are less affected. In contrast, a strong increase of DNA damage is observed in water, where OH-radicals are produced. In consequence, base damage and base release become predominant, even though the number of strand-breaks increases further.



2019 ◽  
Author(s):  
Chia-Hsin Wang ◽  
Sun-Tang Chang ◽  
Sheng-Yuan Chen ◽  
Yaw-Wen Yang


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