4.6 Article

A nitrogen-doped carbon-coated silicon carbide as a robust and highly efficient metal-free catalyst for sour gas desulfurization in the presence of aromatics as contaminants

Journal

CATALYSIS SCIENCE & TECHNOLOGY
Volume 10, Issue 16, Pages 5487-5500

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/d0cy00945h

Keywords

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Funding

  1. TRAINER project (Catalysts for Transition to Renewable Energy Future) of the Make our Planet Great Again program [ANR-17-MPGA-0017]
  2. Italian MIUR through the PRIN 2017 Project MULTI-e Multielectron transfer for the conversion of small molecules: an enabling technology for the chemical use of renewable energy [20179337R7]
  3. SATT-Conectus through the DECORATE project
  4. Vietnam National Foundation for Science and Technology Development (NAFOSTED) [104.052017.336]
  5. National Natural Science Foundation of China [21606243, 91645117]
  6. Liao Ning Revitalization Talents Program [XLYC1907053]
  7. CAS Youth Innovation Promotion Association [2018220]

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As far as environmental chemistry is concerned, N-doped nanocarbons have been employed as efficient, selective and robust metal-free systems for the selective oxidation of H2S to elemental sulfur in tail gas treatment units. Modified Claus units that include tail gas treatments can reach up to 99.9% conversion of H2S into elemental sulfur, a technology that matches well with the more and more challenging environmental concerns. Contaminants in the feed stream include hydrocarbons whose incomplete upstream removal may pose several problems to the catalytic units of a modified Claus reactor. Indeed, when hydrocarbons meet catalysts, they may undergo degradation processes that typically cause catalyst poisoning and make necessary its frequent regeneration if not its complete substitution. This contribution describes a straightforwardly prepared mesoporous N-doped carbon coating for SiC extrudates, offering the excellent desulfurization performance of the corresponding composite (N-C/SiC) along with its remarkably high resistance towards deactivation/fouling in the presence of relatively high concentrations of toluene [1000 ppm <= [tol] <= 20 000 ppm] as aromatic contaminant. The study has unveiled the existence of a positive solvent effect played by toluene on the process selectivity when N-C/SiC is used as a catalyst while confirming at the same time the remarkably high H2S conversion rates and resistance to deactivation of the metal-free system under harsh reaction conditions.

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