open access publication

Article, 2021

LED-driven controlled deposition of Ni onto TiO 2 for visible-light expanded conversion of carbon dioxide into C 1 –C 2 alkanes

Nanoscale Advances, ISSN 2516-0230, Volume 3, 13, Pages 3788-3798, 10.1039/d1na00021g

Contributors

Sanz-Marco, Arturo [1] [2] Hueso, José Luis [1] [2] [3] Sebastian, Victor [1] [2] [3] Nielsen, David 0000-0002-7764-1151 [4] Mossin, Susanne Lis 0000-0001-7763-9660 [4] Holgado, Juan Pedro 0000-0003-4551-5094 [5] Bueno-Alejo, Carlos J 0000-0002-8762-6203 [1] [2] Balas, Francisco 0000-0001-5512-0075 (Corresponding author) [1] [2] [3] Santamaría, Jesús Alberto 0000-0003-4594-2686 (Corresponding author) [1] [2] [3]

Affiliations

  1. [1] Department of Chemical and Environmental Engineering, University of Zaragoza, c/Mariano Esquillor, s/n; Campus Rio Ebro, Edificio I+D, Zaragoza, 50018, Spain, fbalas@unizar.es
    2. [NORA names: Spain; Europe, EU; OECD];
  2. [2] University of Zaragoza
    3. [NORA names: Spain; Europe, EU; OECD];
  3. [3] Centro de Investigación Biomédica en Red
    4. [NORA names: Spain; Europe, EU; OECD];
  4. [4] Technical University of Denmark
    5. [NORA names: DTU Technical University of Denmark; University; Denmark; Europe, EU; Nordic; OECD];
  5. [5] University of Seville
    6. [NORA names: Spain; Europe, EU; OECD]

Abstract

Photocatalytic gas-phase hydrogenation of CO2 into alkanes was achieved over TiO2-supported Ni nanoparticles under LED irradiation at 365 nm, 460 nm and white light. The photocatalysts were prepared using photo-assisted deposition of Ni salts under LED irradiation at 365 nm onto TiO2 P25 nanoparticles in methanol as a hole scavenger. This procedure yielded 2 nm Ni particles decorating the surface of TiO2 with a nickel mass content of about 2%. Before the photocatalytic runs, Ni/TiO2 was submitted to thermal reduction at 400 °C in a 10% H2 atmosphere which induced O-defective TiO2-x substrates. The formation of oxygen vacancies, Ti3+ centers and metallic Ni sites upon photocatalytic CO2 hydrogenation was confirmed by operando EPR analysis. In situ XPS under reaction conditions suggested a strong metal-support interaction and the co-existence of zero and divalent Ni states. These photoactive species enhanced the photo-assisted reduction of CO2 below 300 °C to yield CO, CH4 and C2H6 as final products.

Keywords

CO, EPR, EPR analysis, LED, LED irradiation, Ni nanoparticles, Ni particles, Ni salts, Ni sites, Ni states, P25, P25 nanoparticles, TiO, TiO 2, XPS, alkanes, analysis, atmosphere, carbon dioxide, center, co-existence, conditions, content, conversion, conversion of carbon dioxide, deposition of Ni, dioxide, formation, formation of oxygen vacancies, gas-phase hydrogenation, hole scavenger, holes, hydrogen, interaction, irradiation, light, mass content, metal-support interaction, metallic Ni sites, methanol, nanoparticles, nickel, oxygen vacancies, particles, photo-assisted deposition, photoactive species, photocatalyst, photocatalytic runs, procedure, production, reaction, reaction conditions, reduction, reduction of CO<sub>2</sub>, running, salt, scavenging, sites, species, state, substrate, surface, surface of TiO<sub>2</sub> an, thermal reduction, vacancies, visible-light, white light, zero

Funders

  • Carlsberg Foundation
  • Ministry of Economy, Industry and Competitiveness
  • Centro de Investigación Biomédica en Red en Bioingeniería, Biomateriales y Nanomedicina

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