Aqueous phase reforming of xylose using bimetallic Pt3-Rex/SiO2 catalysts for H2 production: Experimental and computational study

Chan Hyun Lee, Min Kyeong Kim, Seung hoon Kim, Seong Wan Choi, Hyun Wook Kim, Jungho Jae, Hyuntae Sohn, Sun Hee Choi, Sung Pil Yoon, Ki Bong Lee, Hyung Chul Ham

Research output: Contribution to journalArticlepeer-review

Abstract

In recent years, the aqueous phase reforming (APR) reaction using heterogeneous catalysts has been highlighted as one of possible approaches for converting nonedible biomass into hydrogen for fuel cell application. In this study, we have synthesized the rhenium (Re)-doped Pt/SiO2 (Pt3Rex/SiO2) (based on weight; x = 1, 3, 5) catalysts for enhancing the APR of organic liquid C5 sugar xylose. Our study showed that the activity of bimetallic Pt-Re catalysts toward the APR of xylose strongly depends on the level of Re dopant. In particular, the Pt3-Re1/SiO2 catalyst exhibited the higher H2 selectivity compared to the catalysts having the higher amount of Re dopant (Pt3-Re2/SiO2 and Pt3-Re3/SiO2). Furthermore, the oxygen state of ReOx could be modified by changing reduction temperature. The measured hydrogen selectivity and reaction rate could be enhanced when the catalyst was reduced at higher temperature. Especially, the Pt3-Re1/SiO2 catalyst reduced at 500°C under 10 vol% H2 flow exhibited high catalytic performances close to the theoretical values in the initial stage of the reaction, but its activity was gradually reduced by re-oxidation of ReOx. From the various analysis results, we can figure out that the presence of metallic state Pt and Re in Pt3Re alloy phase and low oxidation state Re (Re3+) element is responsible for the improved H2 selectivity in Pt3-Re1/SiO2 catalyst reduced at 500°C. In addition, the density functional theory calculation also predicted that the surface exposure of Pt and Re atoms (rather than oxidized ReOx) can boost the first dehydrogenation of xylose, which is in a good agreement with the experimental observation. This study can provide the optimal oxidation level of Re and Pt in the bimetallic Pt-Re catalyst to efficiently obtain hydrogen from xylose via APR reaction.

Original languageEnglish
Pages (from-to)14478-14490
Number of pages13
JournalInternational Journal of Energy Research
Volume46
Issue number10
DOIs
Publication statusPublished - 2022 Aug

Bibliographical note

Funding Information:
This research was supported by the Hydrogen Energy Innovation Technology Development Program of the National Research Foundation of Korea (NRF) funded by the Korean government (Ministry of Science and ICT[MSIT]) (NRF‐2020M3E6A1043955, NRF‐2019M3E6A1104113).

Publisher Copyright:
© 2022 John Wiley & Sons Ltd.

Keywords

  • DFT calculation
  • aqueous phase reforming
  • heterogeneous catalyst
  • hydrogen production
  • xylose conversion

ASJC Scopus subject areas

  • Renewable Energy, Sustainability and the Environment
  • Nuclear Energy and Engineering
  • Fuel Technology
  • Energy Engineering and Power Technology

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