Publication date: 7th February 2022
Increase in the concentration of atmospheric CO2 happens to be one of the major driving factor towards global warming. The main reason for the increase in the amount of CO2 emissions is due to the dependency on fossil fuels to meet the energy requirements [1]. Developing an alternate form of fuel or converting CO2 back to the fuel forms would balance the level of CO2 in the atmosphere.
For sustainable development, it becomes essential to capture CO2 from the atmosphere and convert it into a product of high economic value. Among different strategies available, photocatalytic reduction of CO2 to usable fuels is an attractive option. TiO2 is widely used as photocatalyst due to its excellent properties like high photocatalytic activity, stability and availability [2]. Among the different crystalline forms of TiO2, anatase and rutile are the stable ones and studies have confirmed that anatase structure is the one which is easier to form at a nanoscale level [3]. Anatase (101) surface is the most stable and easily exposed among the other surfaces [4].Further, doping of TiO2 with a high valence dopants like Ta enhances its photocatalytic performance by reducing band gap, suppressing electron-hole recombination rate, and increasing the absorption of light irradiation.
Since CO2 is a thermodynamic stable molecule, activation becomes an important step in photocatalytic reduction of CO2. Activation involves geometric and electronic changes in CO2 molecule when it is adsorbed on the TiO2 catalyst surface. In this work, DFT calculations coupled with nudged elastic band (NEB) method have been performed to understand the adsorption behavior and calculate the activation barrier of CO2 in Ta-doped TiO2 , and water assisted Ta-doped TiO2 (101) surface. It was found that presence of water and high valence dopant (Ta) activates the CO2 molecule and water helps in reducing the barrier for CO2 activation.
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