Journal
JOURNAL OF MATERIALS CHEMISTRY A
Volume 10, Issue 35, Pages 18354-18362Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/d2ta03690h
Keywords
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Funding
- Jawaharlal Nehru Centre for Advanced Scientific Research (JNCASR)
- Department of Science and Technology, India (DST) [DST/TM/EWO/MI/CCUS/13(G), DST/TMDEWO/CCUS/CoE/2020/JNCASR (C)]
- DST [DST/SJF/CSA-02/2017-18]
- University Grants Commission
- Council of Scientific and Industrial Research (CSIR)
- Department of Science and Technology (Government of India)
- SERB, India [CRG/2021/001420]
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Different Schiff base functionalized SBA-15 materials were synthesized for efficient CO2 capture. These materials were also used as supports for Pd-Ag and Pd-Ni bimetallic systems, with the Pd-Ni system showing enhanced CO2 to formic acid conversion activity.
Different Schiff base functionalized SBA-15 materials were synthesized through condensation reactions between 3-aminopropyltriethoxysilane (APTES) and different aldehydes (glutaraldehyde and butyraldehyde) over a mesoporous silica, SBA-15 (APTES-GLU/SBA-15 and APTES-BUT/SBA-15). Both static and dynamic experiments have been used for testing the CO2 capture efficiency of these materials. The hybridization of the N atom in APTES has been tuned from sp(3) to sp(2) upon condensation facilitating optimum CO2 capture in the direct synthesis of APTES-GLU/SBA-15. The undesirable oxides of nitrogen have been removed during the synthesis process to improve the CO2 capture efficiency. These materials were employed as supports for Pd-Ag and Pd-Ni bimetallic systems for the selective conversion of the captured CO2 to formic acid (FA) in 0.5 M KHCO3 solution. The Pd-Ni catalyst system exhibited enhanced CO2 to FA conversion activity compared to other heterogeneous systems, which is similar to 4 times better than that of the Pd-Ag system in this study. The X-ray absorption studies over the catalyst material confirmed that the relatively electron-deficient Ni in Pd-Ni compared to Ag in Pd-Ag favoured higher charge polarization between the metals in the Pd-Ni system enhancing the CO2 to FA conversion. The experimental observations are well supported by the DFT calculations.
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