CO2 activation and dissociation on In2O3(110) supported PdnPt(4−n) (n = 0–4) catalysts: a density functional theory study. Issue 19 (11th May 2021)

• Record Type: Journal Article
• Authors: Wang, Xiaowen; Pan, Jiaying; Wei, Haiqiao; Li, Wenjia; Zhao, Jun; Hu, Zhen
• Is Part Of: Physical chemistry chemical physics. Volume 23:Issue 19(2021)
• Page Start: 11557
• Page End: 11567
• Publication Date: 2021-05-11
• Subjects: Chemistry, Physical and theoretical -- Periodicals; 541.3
• DOI: 10.1039/d1cp01015h
• Languages: English
• ISSNs: 1463-9076

Abstract

Abstract : The CO2 adsorption and dissociation procedures on the Pd n Pt(4− n ) /In2 O3 ( n = 0–4) catalysts are studied. Compromised between the adsorption energies and dissociation barriers, Pd2 Pt2 /In2 O3 is regarded as the optimal component for CO2 reduction. Abstract : Converting CO2 into valuable chemicals via catalytic reactions can mitigate both the greenhouse effect and energy shortage problems, thus designing efficient catalysts have attracted considerable attention over the past decades. In this work, a density functional theory (DFT) calculation was carried out to investigate the CO2 activation and dissociation processes on various Pd n Pt(4− n ) /In2 O3 ( n = 0–4) catalysts. The Pd n Pt(4− n ) /In2 O3 models were initially built, and the interface sites of Pd n Pt(4− n ) /In2 O3 for CO2 adsorption were confirmed among cluster sites and substrate sites. The CO2 adsorption geometries, charger transfer, and projected density of states (PDOS) were analyzed to study the CO2 –Pd n Pt(4− n ) /In2 O3 interactions. From the adsorbed *CO2, the transition states (TSs) for CO2 dissociation to form *CO and *O were gained to reveal the characteristics of the activated CO 2 δ − . Overall, according to the adsorption energy E ads results, the bimetallic PdPt3 /In2 O3 and Pd3 Pt/In2 O3 catalysts showed the strongest and weakest CO2 adsorption stabilities, respectively, while the Pd element addition decreases the barriers for CO2 dissociation with the priority order of Pd4 > Pd3 Pt > Pd2 Pt2 > PdPt3 > Pt4 . The Brønsted–Evans–Polanyi (BEP) relation between activation barriers ( E b ) and reaction energies E was obtained for the CO2 dissociation mechanism on Pd n Pt(4− n ) /In2 O3 catalysts with the equation of E = 0.20 E b + 0.40. Finally, the optimal Pd2 Pt2 /In2 O3 catalyst for CO2 activation and dissociation was proposed. This study provides useful information for CO2 activation and conversation procedures on bimetal-oxide catalysts, and helps to take the optimal design of PdPt/In2 O3 catalysts for the CO2 reaction.