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

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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 gform. gcat−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.

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

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Article information


Submitted
27 Oct 2019
Accepted
21 Jan 2020
First published
22 Jan 2020

Green Chem., 2020, Advance Article
Article type
Paper

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

K. Park, G. H. Gunasekar, S. Kim, H. Park, S. Kim, K. Park, K. Jung and S. Yoon, Green Chem., 2020, Advance Article , DOI: 10.1039/C9GC03685G

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