@article{novotny_lamb_2021, title={MoO3 films grown on stepped sapphire (0001) by molecular beam epitaxy}, volume={39}, ISSN={["1520-8559"]}, DOI={10.1116/6.0000962}, abstractNote={MoO3 films were grown on stepped c-plane sapphire substrates by molecular beam epitaxy using MoO3 vapor from a conventional Knudsen cell. Stepped sapphire (0001) substrates were prepared by ex situ annealing at 1100–1300 °C in dry air. Step bunching typically resulted in multistepped surfaces with wide atomically smooth terraces. Ex situ annealing at 1100 °C followed by in vacuo annealing at 700 °C provided clean substrates for growth. Ultrathin films were grown at 450 °C via a self-limiting process that represents a balance between the incident MoO3 flux and the desorption flux. Elongated bilayer islands (0.7-nm thick) were formed on sapphire (0001) terraces. Monocrystalline α-MoO3 (010) thin films [(010)α-MoO3∥(0001)sapphire] were grown at 450 °C using a higher incident MoO3 flux and characterized by atomic force microscopy, x-ray photoelectron spectroscopy, x-ray diffraction, and cross-sectional transmission electron microscopy. The step-terrace surface morphology of the monocrystalline films strongly suggests multilayer growth.}, number={4}, journal={JOURNAL OF VACUUM SCIENCE & TECHNOLOGY A}, author={Novotny, Petr and Lamb, H. Henry}, year={2021}, month={Jul} } @article{novotny_yusuf_li_lamb_2020, title={MoO3/Al2O3 catalysts for chemical-looping oxidative dehydrogenation of ethane}, volume={152}, ISSN={["1089-7690"]}, url={http://www.scopus.com/inward/record.url?eid=2-s2.0-85078845301&partnerID=MN8TOARS}, DOI={10.1063/1.5135920}, abstractNote={MoO3/γ-Al2O3 catalysts containing 0.3–3 monolayer (ML) equivalents of MoO3 were prepared, characterized, and tested for ethane oxidative dehydrogenation (ODH) in cyclic redox and co-feed modes. Submonolayer catalysts contain highly dispersed (2D) polymolybdate structures; a complete monolayer and bulk Al2(MoO4)3 are present at >1ML loadings. High ethylene selectivity (>90%) in chemical looping (CL) ODH correlates with Mo+VI to Mo+V reduction; COx selectivity is <10% under these conditions. Mo+V and Mo+IV species trigger CH4 production resulting in much higher conversion albeit with <20% selectivity. In CL-ODH, submonolayer catalysts exhibit ethylene selectivities that decrease linearly from 96% at near-zero conversion to 70% at 45% conversion. >1ML catalysts provide higher conversions albeit with 10%–18% lower selectivity and greater selectivity loss with increasing conversion. In co-feed mode, ethylene selectivity drops to <50% at 46% conversion for a 0.6ML catalyst, but selectivity is virtually unaltered for a 3ML catalyst. We infer that at <1ML loadings, small domain size and strong Mo—O—Al bonds decrease 2D polymolybdate reducibility and enhance ethylene selectivity in CL-ODH.}, number={4}, journal={JOURNAL OF CHEMICAL PHYSICS}, author={Novotny, Petr and Yusuf, Seif and Li, Fanxing and Lamb, H. Henry}, year={2020}, month={Jan} } @article{novotny_lamb_2019, title={Nanostructured MoOx films deposited on c-plane sapphire}, volume={37}, ISSN={["1520-8559"]}, DOI={10.1116/1.5100752}, abstractNote={Molybdenum oxide films were deposited on α-Al2O3 (0001) at 580 °C using MoO3 from a conventional molecular beam epitaxy Knudsen cell. A relatively smooth film (RMS roughness 1.1 nm) was deposited in 1 min at 580 °C using a Knudsen cell temperature of 620 °C; however, after 15 min deposition under these conditions, isolated islands (30–50 nm wide × 10–20 nm tall) develop that are stable to annealing at 600 °C for 60 min. XPS evidenced that the films are oxygen deficient with an average formula of MoO2.7. The authors infer that this oxygen deficiency is responsible for their thermal stability and may have significant effects on their catalytic and electronic properties. In contrast, stoichiometric MoO3 films deposited at 400 °C sublime completely during annealing at 600 °C.}, number={5}, journal={JOURNAL OF VACUUM SCIENCE & TECHNOLOGY A}, author={Novotny, Petr and Lamb, H. Henry}, year={2019}, month={Sep} } @article{novotny_yusuf_li_lamb_2018, title={Oxidative dehydrogenation of ethane using MoO3/Fe2O3 catalysts in a cyclic redox mode}, volume={317}, ISSN={["1873-4308"]}, url={http://www.scopus.com/inward/record.url?eid=2-s2.0-85042634041&partnerID=MN8TOARS}, DOI={10.1016/j.cattod.2018.02.046}, abstractNote={Oxidative dehydrogenation (ODH) of ethane offers large reductions in energy consumption and associated greenhouse gas emissions when compared to conventional steam cracking for ethylene production; however, catalytic ODH of ethane using co-fed O2 requires expensive air separation. As an alternative, we are investigating novel core-shell catalysts that utilize lattice oxygen (O2−) as the sole oxidant and operate in a cyclic redox mode. In this work, redox catalysts having 1, 3 and 6 monolayer (ML) equivalents of MoO3 on α-Fe2O3 and a stoichiometric ferric molybdate, Fe2(MoO4)3, were prepared, characterized by powder x-ray diffraction (XRD), x-ray photoelectron spectroscopy (XPS), diffuse-reflectance infrared Fourier transform spectroscopy (DRIFTS), and temperature-programmed reduction (TPR) and evaluated for ethane ODH in a cyclic redox mode at 600 °C. The characterization data are consistent with a core-shell structure for the calcined MoO3/Fe2O3 catalysts with a mixed Mo-Fe oxide surface layer. H2 and ethane TPR evidence that the shell inhibits Fe2O3 reduction and decreases the ethane combustion activity of the fully oxidized catalyst. Covering the Fe2O3 core with MoO3 also increases ODH activity and ethylene selectivity. In cyclic redox mode at 600 °C, ethylene selectivity was 57–62% for catalysts with 3 and 6 ML equivalents of MoO3.}, journal={CATALYSIS TODAY}, author={Novotny, Petr and Yusuf, Seif and Li, Fanxing and Lamb, H. Henry}, year={2018}, month={Nov}, pages={50–55} }