Browsing by Subject "CO"

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  • Väyrynen, Katja; Hatanpää, Timo; Mattinen, Miika; Heikkilä, Mikko; Mizohata, Kenichiro; Meinander, Kristoffer; Räisänen, Jyrki; Ritala, Mikko; Leskelä, Markku (2018)
    In this paper, we introduce a new Co precursor for the atomic layer deposition (ALD) of Co metal and other Co containing materials. CoCl2(TMEDA) (TMEDA = N,N,N ',N '-tetramethylethylenediamine) is a diamine adduct of cobalt(II) chloride that is inexpensive and easy to synthesize, making it an industrially viable precursor. Furthermore, CoCl2(TMEDA) shows good volatility at reasonably low temperatures and is thermally stable up to a temperature of, similar to 300 degrees C. We also present a full ALD study for the deposition of CoO thin films using CoCl2(TMEDA) and water as precursors. The process was investigated within a temperature range of 225-300 degrees C. Saturation of the film growth with respect to both precursor pulse lengths was verified. According to X-ray diffraction, the films were a mixture of hexagonal and cubic CoO. No reflections corresponding to Co3O4 were detected. The hexagonal phase is characteristic to nanomaterials only and is not seen in bulk CoO. The crystal structure of the films could be tuned by temperature, water pulse lengths, and type of substrate material. The films deposited at 275 degrees C exhibited 1:1 Co:O stoichiometry and very high purity. The CoO films could be reduced to Co metal at an exceptionally low temperature of 250 degrees C in 10% forming gas. Continuity of the reduced Co films was improved when the CoO film was deposited on TiN instead of native oxide terminated Si. The Co content of a 50 nm reduced metal film was as high as 95 at. %, with negligible amounts of oxygen and hydrogen.
  • Mattinen, Miika; Hatanpaa, Timo; Mizohata, Kenichiro; Raisanen, Jyrki; Leskela, Markku; Ritala, Mikko (2021)
    Co9S8 is an interesting sulfide material with metallic conductivity that has shown promise for various energy applications. Herein, we report a new atomic layer deposition process producing crystalline, pure, and highly conductive Co9S8 thin films using CoCl2(TMEDA) (TMEDA = N,N,N ',N '-tetramethylethylenediamine) and H2S as precursors at 180-300 degrees C. The lowest resistivity of 80 mu omega cm, best uniformity, and highest growth rate are achieved at 275 degrees C. Area-selective deposition is enabled by inherent substrate-dependency of film nucleation. We show that a continuous and conductive Co9S8 film can be prepared on oxide-covered silicon without any growth on Si-H. Besides silicon, Co9S8 films can be grown on a variety of substrates. The first example of an epitaxial Co9S8 film is shown using a GaN substrate. The Co9S8 films are stable up to 750 degrees C in N-2, 400 degrees C in forming gas, and 225 degrees C in O-2 atmosphere. The reported ALD process offers a scalable and cost-effective route to high-quality Co9S8 films, which are of interest for applications ranging from electrocatalysis and rechargeable batteries to metal barrier and liner layers in microelectronics and beyond.
  • Kouki, Kerttu (Helsingfors universitet, 2017)
    Tutkimukseni tavoitteena oli selvittää, miten kasviperäisten hiukkasten määrä muuttuu Amazonilla ilmaston lämmetessä ja miten se vaikuttaa Amazonin ilmastoon. Hallitustenvälisen ilmastonmuutospaneelin (IPCC) mukaan merkittävimmät epävarmuudet ilmastonmuutoksessa liittyvät aerosoleihin, ja luonnolliset aerosolit aiheuttavat suuremman epävarmuuden ilmastoon kuin antropogeeniset aerosolit. Amazonin sademetsä on erityisen sopiva kasviperäisten hiukkasten tutkimiseen ja tutkimuskysymykseni kannalta kiinnostava, sillä etenkin sadekaudella valtaosa aerosoleista on kasviperäisiä. Tutkimusaineistona käytettiin satelliittien keräämiä havaintoja, joiden avulla määritettiin lämpötila (LST, engl. land surface temperature), aerosolien määrä ilmakehässä (AOD, engl. aerosol optical depth) sekä eri pienhiukkaslähteitä. Samat lähteet, jotka tuottavat pienhiukkasia ilmakehään, päästävät sinne myös hivenkaasuja. Erilaiset lähteet tuottavat erilaisia pienhiukkasia ja kaasuja, joten yhdistämällä havaintoja pienhiukkasista ja hivenkaasuista voidaan niiden lähteet selvittää luotettavammin. LST ja AOD määritettiin AATSR:n (Advanced Along-Track Scanning Radiometer) havaintojen avulla. Pienhiukkaslähteiden tunnistamiseen käytettiin OMI:n (Ozone Monitoring Instrument) keräämiä havaintoja typpidioksidista (NO2) ja formaldehydistä (HCHO) sekä AIRS:n (Atmospheric Infrared Sounder) havaintoja hiilimonoksidista (CO). Tulosteni mukaan pienhiukkasten määrä vaihtelee Amazonilla vuoden aikana varsin paljon: sadekaudella hiukkasten määrä on hyvin vähäinen, kun taas kuivalla kaudella määrä kasvaa moninkertaiseksi laajojen metsäpalojen seurauksena. Voisi olettaa, että lämpimämpinä aikoina myös metsäpalot lisääntyisivät, mutta tulosten mukaan palokaudella pienhiukkasten määrä pienenee lämpötilan noustessa. Suuri osa paloista on kuitenkin ihmisen sytyttämiä, joten myös ihmistoiminnalla on merkittävä vaikutus palokauden hiukkasiin. Hiilimonoksidia ja formaldehydiä muodostuu sadekaudella pääosin kasviperäisistä lähteistä, ja erityisesti hiilimonoksidin määrän havaittiin korreloivan positiivisesti lämpötilan kanssa, mikä viittaa kasviperäisten hiukkasten määrän kasvuun lämpötilan noustessa. Sadekaudella suurin osa hiukkasista on kasviperäisiä ja silloin AOD:n lämpötilariippuvuus on 0,008 ± 0,015 K-1, joten kasviperäisten hiukkasten suora säteilyvaikutus on siten –0,22 ± 0,40 Wm-2K-1 pilvettömälle taivaalla ja –0,08 ± 0,16 Wm-2K-1, kun pilvien osuus on 60 % koko taivaasta. Lämpötilan noustessa kasviperäiset hiukkaset siis todennäköisesti aiheuttavat negatiivisen säteilypakotteen ja siten hillitsevät ilmaston lämpenemistä. Toisaalta tulokseni kuitenkin osoittavat, että metsäpalot ovat hiukkasten merkittävin lähde Amazonilla, sillä metsäpalojen yhteydessä esiintyy merkittävästi luonnollista tasoa enemmän hiukkasia. Metsäpaloista syntyneet hiukkaset todennäköisesti määrittelevätkin AOD:n muutokset myös tulevaisuudessa.
  • Nieminen, Heta-Elisa; Kaipio, Mikko; Ritala, Mikko (2020)
    In this work, a growth mechanism of an intermetallic Co3Sn2 thin film is studied in situ with a quartz crystal microbalance (QCM) and quadrupole mass spectrometer (QMS). The film is deposited by atomic layer deposition (ALD) from CoCl2 (TMEDA) and Bu3SnH precursors (TMEDA = N,N,N' ,N' - tetramethylethylenediamine). Balanced reaction equations are resolved by fitting the QMS and QCM data, and a step-by-step growth mechanism is determined for the process. During the CoCl2 (TMEDA) pulse, only 1-chlorobutane is formed as a byproduct. However, during the Bu3SnH pulse, two byproducts, BuCl and Bu3SnCl, were clearly detected, indicating that two competing reaction pathways exist during that pulse. Preliminary studies on another intermetallic ALD process, Ni3Sn2, revealed that the reactions occur similarly as in the Co3Sn2 process.
  • Moya-Cancino, Jose G.; Honkanen, Ari-Pekka; van der Eerden, Ad M. J.; Oord, Ramon; Monai, Matteo; ten Have, Iris; Sahle, Christoph; Meirer, Florian; Weckhuysen, Bert M.; de Groot, Frank M. F.; Huotari, Simo (2021)
    We present in situ experiments to study the possible formation of cobalt carbides during Fischer–Tropsch synthesis (FTS) in a Co/TiO2 catalyst at relevant conditions of pressure and temperature. The experiments were performed by a combination of X-ray Raman scattering (XRS) spectroscopy and X-ray diffraction (XRD). Two different experiments were performed: (1) a Fischer–Tropsch Synthesis (FTS) reaction of an ∼14 wt % Co/TiO2 catalyst at 523 K and 5 bar under H2 lean conditions (i.e., a H2:CO ratio of 0.5) and (2) carburization of pure cobalt (as reference experiment). In both experiments, the Co L3-edge XRS spectra reveal a change in the oxidation state of the cobalt nanoparticles, which we assign to the formation of cobalt carbide (Co2C). The C K edge XRS spectra were used to quantify the formation of different carbon species in both experiments.
  • Wlodarski, Maksymilian; Putkonen, Matti; Norek, Malgorzata (2020)
    Infrared (IR) spectroscopy is a powerful technique to characterize the chemical structure and dynamics of various types of samples. However, the signal-to-noise-ratio drops rapidly when the sample thickness gets much smaller than penetration depth, which is proportional to wavelength. This poses serious problems in analysis of thin films. In this work, an approach is demonstrated to overcome these problems. It is shown that a standard IR spectroscopy can be successfully employed to study the structure and composition of films as thin as 20 nm, when the layers were grown on porous substrates with a well-developed surface area. In contrast to IR spectra of the films deposited on flat Si substrates, the IR spectra of the same films but deposited on porous ceramic support show distinct bands that enabled reliable chemical analysis. The analysis of Zn-S ultrathin films synthesized by atomic layer deposition (ALD) from diethylzinc (DEZ) and 1,5-pentanedithiol (PDT) as precursors of Zn and S, respectively, served as proof of concept. However, the approach presented in this study can be applied to analysis of any ultrathin film deposited on target substrate and simultaneously on porous support, where the latter sample would be a reference sample dedicated for IR analysis of this film.
  • Debouk, Haifa; Altimir, Núria; Sebastià, Maria-Teresa (2018)
    Measurements of greenhouse gas (GHG) fluxes, particularly methane (CH4) and nitrous oxide (N2O) in mountain ecosystems are scarce due to the complexity and unpredictable behavior of these gases, in addition to the remoteness of these ecosystems. In this context, we measured CO2, CH4, and N2O fluxes in four semi-natural pastures in the Pyrenees to investigate their magnitude and range of variability. Our interest was to study GHG phenomena at the patch-level, therefore we chose to measure the gas-exchange using a combination of a gas analyzer and manual chambers. The analyzer used is a photoacoustic field gas-monitor that allows multi-gas instantaneous measurements. After implementing quality control and corrections, data was of variable quality. We tackled this by categorizing data as to providing quantitative or only qualitative information:•50% and 59% of all CH4 and N2O data, respectively, provided quantitative information above the detection limit.•We chose not to discard data providing only qualitative information, because they identify highest- and lowest-flux peak periods and indicate the variability of the fluxes, along different altitudes and under different climatic conditions.•We chose not to give fluxes below detection limit a quantitative value but to acknowledge them as values identifying periods with low fluxes.
  • Aminoff, S.Tatiana H. (University of Helsinki, 1992)
  • Shtepliuk, I.; Pliatsikas, N.; Jian, J.; Ben Sedrine, N.; Iakimov, T.; Sarakinos, K.; Ivanov, I. G.; Sun, Jianwu; Yakimova, R. (2021)
    The paucity of research on hydrogen evolution reaction (HER) under neutral conditions, which is a more sustainable way to produce H-2 compared to acidic and alkaline HER, encourages the development of efficient catalytic materials and devices and deeper investigation of the mechanisms behind neutral HER. We present an electrode concept for facilitating HER under neutral conditions. The concept entails the use of annealing-reshaped silver (Ag) nanoparticle array on monolayer epitaxial graphene (MEG) on 4H-SiC. Measurements of HER performance show more positive onset potential of the cathodic HER for Ag-decorated MEG compared to that for pristine MEG, indicating improved water dissociation at Ag/MEG electrodes. Complementary morphological characterization, absorption measurements, and Raman mapping analysis enable us to ascribe the enhanced catalytic performance of electrodes decorated with 2 nm thick annealed Ag on the synergetic effect originating from simultaneous water reduction on circular Ag nanoparticles of 31 nm in diameter and on compressively strained Ag-free graphene regions. The overall results pave the way toward development of stable van der Waals heterostructure electrodes with a tunable metal-carbon interaction for fast HER under neutral conditions. (C) 2021 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/).