<p>This work investigates the post-plasma catalytic hydrogenation of C<sub>2</sub>H<sub>2</sub> into C<sub>2</sub>H<sub>4</sub> from CH<sub>4</sub>, H<sub>2</sub>, and C<sub>2</sub>H<sub>2</sub> mixtures designed to emulate effluents from plasma reactors used for non-oxidative CH<sub>4</sub> coupling. Four noble and non-noble metal catalysts supported on γ-Al<sub>2</sub>O<sub>3</sub> were tested across a controlled temperature range, representative of plasma reactor outflows. Supported by a temperature-dependent surface micro-kinetic model, our study aids to understand the interplay between plasma-derived gas compositions and catalyst surface chemistry, confirming how temperature influences the reaction mechanisms, selectivity and by-product formation in the post-plasma zone. In line with previous research, Pd exhibits the highest C<sub>2</sub>H<sub>4</sub> selectivity (up to 63%), while Pt favours over-hydrogenation to C<sub>2</sub>H<sub>6</sub> and non-noble Cu and Ni catalysts show limited C<sub>2</sub>H<sub>4</sub> selectivity due to oligomerisation and coking, respectively. Interestingly, our model provides novel mechanistic insights into CH<sub>4</sub> formation and catalyst deactivation by carbon deposition on the Ni catalyst. These findings offer new practical guidance relevant to further development and implementation of post-plasma hydrogenation for plasma-based valorisation of CH<sub>4</sub> towards C<sub>2</sub>H<sub>4</sub>.</p>

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C2H4 Synthesis Through Catalytic C2H2 Hydrogenation in post-CH4 Plasma Streams: Performance of Noble and non-noble Catalysts

  • Eduardo Morais,
  • Qian Chen,
  • Rui Liu,
  • Yanhui Yi,
  • Annemie Bogaerts

摘要

This work investigates the post-plasma catalytic hydrogenation of C2H2 into C2H4 from CH4, H2, and C2H2 mixtures designed to emulate effluents from plasma reactors used for non-oxidative CH4 coupling. Four noble and non-noble metal catalysts supported on γ-Al2O3 were tested across a controlled temperature range, representative of plasma reactor outflows. Supported by a temperature-dependent surface micro-kinetic model, our study aids to understand the interplay between plasma-derived gas compositions and catalyst surface chemistry, confirming how temperature influences the reaction mechanisms, selectivity and by-product formation in the post-plasma zone. In line with previous research, Pd exhibits the highest C2H4 selectivity (up to 63%), while Pt favours over-hydrogenation to C2H6 and non-noble Cu and Ni catalysts show limited C2H4 selectivity due to oligomerisation and coking, respectively. Interestingly, our model provides novel mechanistic insights into CH4 formation and catalyst deactivation by carbon deposition on the Ni catalyst. These findings offer new practical guidance relevant to further development and implementation of post-plasma hydrogenation for plasma-based valorisation of CH4 towards C2H4.