CO2 hydrogenation to formic acid over heterogenized ruthenium catalysts using a fixed bed reactor with separation units

Authors
Park, KwanghoGunasekar, Gunniya HariyanandamKim, Seong-HoonPark, HongjinKim, SamhwanPark, KiyoungJung, Kwang-DeogYoon, Sungho
Issue Date
2020-03-07
Publisher
ROYAL SOC CHEMISTRY
Citation
GREEN CHEMISTRY, v.22, no.5, pp.1639 - 1649
Abstract
Along with the mitigation of CO2 emission, recently, the CO2-derived formic acid process has drawn attention as a promising platform for the renewable-energy-derived hydrogen storage cycle by using formic acid as a liquid organic hydrogen carrier (LOHC). Here, a heterogenized Ru molecular catalyst on a bpyTN-30-CTF support is prepared and successfully implemented in an integrated trickle-bed reactor system for continuous CO2 hydrogenation to produce formic acid. The bpyTN-30-CTF support with an alternative structure of the bpy and TN motif increases the porosity and metal anchoring sites. The Ru/bpyTN-30-CTF catalyst prepared using the bpyTN-30-CTF support displays sufficient catalytic activity for commercialization. Under the continuous process, the catalyst exhibits substantial catalytic performance with the highest productivity of 669.0 g(form.) g(cat)(-1) d(-1) with CO2 conversion of 44.8% for a superficial gas velocity of 72 cm s(-1). Furthermore, the catalyst shows excellent stability in the continuous hydrogenation process with a trickle-bed reactor over 30 days of operation, reaching a total turnover number of 524 000 without any significant deactivation. Based on kinetic data, a new process to produce formic acid by CO2 hydrogenation has thus been proposed here.
Keywords
COVALENT TRIAZINE FRAMEWORKS; CARBON-DIOXIDE; CAPTURE; FORMATE; EQUILIBRIUM; CONVERSION; METHANOL; COVALENT TRIAZINE FRAMEWORKS; CARBON-DIOXIDE; CAPTURE; FORMATE; EQUILIBRIUM; CONVERSION; METHANOL; 이산화탄소; 수소화; 포름산
ISSN
1463-9262
URI
https://pubs.kist.re.kr/handle/201004/118859
DOI
10.1039/c9gc03685g
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KIST Article > 2020
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