Study of catalytic performance of CO2 hydrogenation over Copper and Ruthenium loaded on N-doped modified PBZ-Derived carbons

Name: Nattanida Thepphankulngarm

LCSH: Kasetsart University -- Dissertations. Ph.D. (Chemical Engineering) 2022

LCSH: Kasetsart University. -- Department of Chemical Engineering -- Dissertations

LCSH: Hydrogenation

LCSH: Carbon dioxide

LCSH: Global warming

LCSH: Methanol

LCSH: Catalysts

LCSH: Porous materials

LCSH: Surface active agents

LCSH: Copper

LCSH: Ruthenium

Abstract: Carbon Dioxide (CO2) hydrogenation to methanol (MeOH) has been a promising method for transforming renewable energy into useful fuels and chemicals. It also could reduce the greenhouse gas emissions, which cause global warming. As a result, many researchers have been increasingly attracted to enhancing catalytic activity and product selectivity in CO2 hydrogenation. In this thesis, a novel copper (Cu) and ruthenium (Ru) loaded on nitrogen-doped polybenzoxazine (PBZ) derived carbons modified with surfactants were successfully synthesized. The system consisted of PBZ, high performance thermosetting carbon porous, improving the physical properties by the surfactants as an adsorbent. Then, enhancing the basicity for CO2 capturing by doping nitrogen species. Cu and Ru metals are used as MeOH synthesis’s catalyst, and activate the potential by loading metal oxides (i.e., CeO2 and ZrO2) as supporters. The obtained catalysts were characterized by various techniques. SEM and TEM showed the smooth continuous 3D polymer network with the size of approximately 20 nm, and a more spherical shape exhibited after modifying with surfactants. The Cu and Ru metals displayed well-dispersed on the surface. The best catalyst appeared on CuRu-Zr/Am-P123, with pore size, pore volume, and specific surface area of 3.5–4.1 nm, 0.51 mL g−1, and 207 m2 g−1,respectively. CO2-TPD manifested the total adsorption of Cu-Ru-Zr/Am-P123 at high value of 6.72 mmol CO2 g–1, which dramatically increased upto 322% compared to previous work. XRD confirmed that Cu0 and Ru0 particles and alloy structures apparently dispersed on the interface and partially incorporated into ZrO2 structure.TGA certified the superior thermal stability of Cu-Ru-Zr/Am-P123 with Char yield (1000 °C) of 83.8%. Cu-RuZr/Am-P123 illustrated the remarkable catalytic performance at mild conditions (T = 210 °C, P = 15 bar of CO2:H2 (1:3), GHSV of 2000 h−1. ) with the STYMeOH and CO2 conversion of 642 mgMeOHgcat−1h−1 and 37 %, respectively. Similar trends of results appear on Cu-Ru-Zr/U-P123. Interestingly, after switching ZrO2 into CeO2, the selectivity of MeOH increased from 75 % to 91 %. The results approved that these catalysts expose the superiority in both physical and chemical properties for CO2 hydrogenation to MeOH.

Kasetsart University. Office of the University Library

Address: Bangkok

Email: tdckulib@ku.ac.th

Name: Paisan Kongkachuichay

Role: Thesis Advisor

Created: 2022

Modified: 2025-07-27

Issued: 2025-07-27

วิทยานิพนธ์/Thesis

application/pdf

URL: https://www.lib.ku.ac.th/KUthesis/2565/nattanida-the-all.pdf

CallNumber: TP156.H8 .N38

eng

DegreeName: Doctor of Philosophy

Level: Doctoral Degraee

Descipline: Chemical Engineering

Grantor: Kasetsart University

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