Syngas production from phenolic pollutants <i>via</i> a series of hydroxylation, ring cleavage, and aqueous-phase reforming catalyzed by a hydrotalcite-supported Fe-Mn-Ni alloy
dc.contributor.author | Sudibyo, Hanifrahmawan | |
dc.contributor.author | Cabrera, Daniela V. | |
dc.contributor.author | Labatut, Rodrigo | |
dc.contributor.author | Supriyanto, Calvin J. | |
dc.contributor.author | Budhijanto, Budhijanto | |
dc.contributor.author | Widyaparaga, Adhika | |
dc.date.accessioned | 2025-01-20T16:07:10Z | |
dc.date.available | 2025-01-20T16:07:10Z | |
dc.date.issued | 2024 | |
dc.description.abstract | A trifunctional catalyst facilitating a series of hydroxylation, oxidative ring opening, and aqueous-phase reforming reactions was developed to convert phenolic wastewater into syngas. The definitive screening design experiment at 250 degrees C for 5 h with 1.75% H(2)O(2 )and 2 wt% catalyst loading demonstrated the importance of Fe, Mn, and Ni among the first-row transition metals to be impregnated into hydrotalcite to acquire the trifunctional feature. The surface chemistry characterization revealed that they improved the amount of strong and weak Br & oslash;nsted (SBrA and WBrA) and Lewis (SLA and WLA) acidic active sites. The mechanistic roles of these sites via semi-continuous kinetic investigation at 200-300 degrees C for 1-5 h with 1.75% H2O2 and 2 wt% catalyst loading were unraveled: (1) SBrA (surface metal oxyhydroxides) facilitated hydroxylation and homolytic cleavage producing hydroxyphenols; (2) WBrA (surface metal hydroxides) promoted ring opening of hydroxyphenols yielding oxo- and di-carboxylic acids; (3) WLA (mineral phase with a tetrahedral coordination) catalyzed reforming of acids into syngas; and (4) SLA (mineral phase with an octahedral coordination) improved the H2 yield by promoting the water-gas shift reaction. The optimal content of Fe, Mn, and Ni was 49.4, 21.2, and 29.4 wt%, respectively, from 20 wt% of active metals on the support to achieve the maximal organic carbon removal (similar to 82%) and H2 yield (similar to 80%) with a CO-to-H2 ratio of 0.6, useful for chemical building block synthesis. The optimized catalyst demonstrated high activity and reusability, with a turnover number and frequency of similar to 1 x 106 and similar to 6 x 104 s-1, respectively, marking a breakthrough in sustainable syngas production. | |
dc.fuente.origen | WOS | |
dc.identifier.doi | 10.1039/d4re00348a | |
dc.identifier.issn | 2058-9883 | |
dc.identifier.uri | https://doi.org/10.1039/d4re00348a | |
dc.identifier.uri | https://repositorio.uc.cl/handle/11534/89983 | |
dc.identifier.wosid | WOS:001326771100001 | |
dc.issue.numero | 12 | |
dc.language.iso | en | |
dc.pagina.final | 3298 | |
dc.pagina.inicio | 3285 | |
dc.revista | Reaction chemistry & engineering | |
dc.rights | acceso restringido | |
dc.title | Syngas production from phenolic pollutants <i>via</i> a series of hydroxylation, ring cleavage, and aqueous-phase reforming catalyzed by a hydrotalcite-supported Fe-Mn-Ni alloy | |
dc.type | artículo | |
dc.volumen | 9 | |
sipa.index | WOS | |
sipa.trazabilidad | WOS;2025-01-12 |