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Synthesis of Ni-Doped Hydrotalcite Catalyst Through Hydrothermal Process for the Selective Reduction of α,β-Unsaturated Aldehyde (Citral) to Enantiospecific (+)-Citronellal

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Abstract

Citral is an oxygenated–monoterpenoid found as a major component in lemongrass essential oil (> 68%) in its isomeric forms of geranial (E−) and neral (Z−). For the value addition of this low-value essential oil, a novel catalytic process has been developed for transformation of citral to enantiospecific (+)-citronellal using 12% Ni–HT-530. The different amounts of Ni were doped through hydrothermal process and calcined at varying temperatures (490, 530, and 570 °C). The performance of composite prepared through hydrothermal process was compared with the wet impregnation method. The composite of hydrothermal process followed by calcination at 530 °C was highly potential for selective conversion of citral to (+)-citronellal. The effects of variables such as reaction time, temperature, hydrogen-pressure, and catalyst-dosage on citral conversion to (+)-citronellal were examined. The citral conversion (99%) was attained with 95% selectivity to citronellal in a ratio of catalyst to citral (1:6) under 110 psi H2 pressure at 90 °C for 90 min using 12% Ni–HT-530. Furthermore, the direct conversion of citral in lemongrass oil was studied at above optimized condition. The result indicated that the synthesized catalyst is equally effective in transforming citral in lemongrass oil to organoleptically superior (+)-citronellal with 93% selectivity. The selective conversion of citral to (+)-citronellal not only increases the fragrance value of the essential oil, but also increases the scope for various industrial applications like fine chemical synthesis and pharmaceutical applications.

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Acknowledgements

The authors are thankful to Science and Engineering Research Board (SERB), DST, India (CRG/2021/002525) for research funding. We are grateful to Director, CSIR-CIMAP, Lucknow for providing the necessary facility under Aroma Mission, Phase-II (HCP 0007, PE-II). Dr. S Chaturvedi is thankful to DST for WOS-A fellowship (DST/WOS-A/CS-94/2021).

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PK: methodology, validation, investigation, writing—original draft; PKS: methodology, writing—draft and investigation; SC: conceptualization, validation, reviewing; CSC: conceptualization, validation, visualization; PRR: methodology, validation; PM: methodology, validation, visualization; PKR: methodology, validation, investigation, funding acquisition, writing—review & editing

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Correspondence to Priyabrat Mohapatra or Prasant Kumar Rout.

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Kumar, P., Sharma, P.K., Chaturvedi, S. et al. Synthesis of Ni-Doped Hydrotalcite Catalyst Through Hydrothermal Process for the Selective Reduction of α,β-Unsaturated Aldehyde (Citral) to Enantiospecific (+)-Citronellal. Catal Lett 153, 3019–3030 (2023). https://doi.org/10.1007/s10562-022-04195-w

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