4.8 Article

Synergistic Hybrid Support Comprising TiO2-Carbon and Ordered PdNi Alloy for Direct Hydrogen Peroxide Synthesis

Journal

ACS CATALYSIS
Volume 11, Issue 14, Pages 8407-8416

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c05485

Keywords

Direct synthesis of H2O2; ordered structure; PdNi alloy; hybrid support; defect support

Funding

  1. Ministry of Science and Technology of Taiwan [109-2639-E-011-001-ASP, 109-2923-E-011-009, 109-2923-E-011-008, 109-2221-E-011-063-MY3, 109-3116-F-011-002-CC1, 108-3116-F-011-001-CC1, 108-2627-M-011-001-, 107-2923-E-011-002, 107-2119-M-002-033-, 106-2923-E-011-005, 106-2221-E-011-125-MY3]
  2. Ministry of Education of Taiwan (U2RSC program) [MOE 1080059]
  3. Taiwan's Deep Decarbonization Pathways toward a Sustainable Society Project from Academia Sinica [AS-KPQ-106-DDPP]
  4. Instrumentation Center at National Taiwan Normal University [MOST 110-2731-M-NMR000400]

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A new catalyst design utilizing the synergistic effects of TiO2-C supports and PdNi alloy nanoparticles was developed for the direct synthesis of hydrogen peroxide in a neutral reaction solution. The ordered structure of the alloyed PdNi nanocatalysts was transformed through thermal hydrogen treatment, leading to excellent performance with high productivity and selectivity. This work provides a promising economically viable alternative to existing Pd-based heterogeneous catalysts for the direct synthesis of hydrogen peroxide.
The development of high-activity catalysts with good selectivity for the direct synthesis of H2O2 from H-2 and O-2 remains challenging. TiO2-C used as a support material is able to facilitate strong metal-support interactions. We designed catalysts for the direct synthesis of hydrogen peroxide that utilized the synergistic effects of hybrid TiO2-C supports and ordered alloyed PdNi nanoparticles in a neutral reaction solution. Through thermal hydrogen treatment, the ordered structure of the alloyed PdNi nanocatalysts was transformed. H-1 NMR was used to measure the amount of water formed as an estimate of selectivity. High-resolution transmission electron microscopy and X-ray photoelectron spectroscopy studies showed an excellent dispersion of the bimetallic PdNi nanocatalyst on the hybrid support. X-ray absorption spectroscopy gave clear evidence of metal-support interactions with electron transfer from the ordered alloyed PdNi nanocatalysts to the defect TiO2-C support, resulting in a noteworthy performance with high H2O2 productivity and selectivity under ambient conditions. This work provides a route to an economically viable alternative to existing Pd-based heterogeneous catalysts for the direct synthesis of hydrogen peroxide.

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