Journal
CHEMICAL ENGINEERING JOURNAL
Volume 446, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.137131
Keywords
CO reduction; Formaldehyde synthesis; Pt alloys; CO coverage; DFT calculations
Categories
Funding
- National Science Foundation [1955452]
- Ohio Research Scholars Program Research Cluster on Surfaces in Advanced Materials
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [1955452] Funding Source: National Science Foundation
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A new mechanism for direct CO reduction to formaldehyde (CORTF) is reported, which utilizes hydrogen underpotential deposition to balance the species coverage on the catalyst surface. By tuning the composition of Pt alloy catalyst and the potential of hydrogen underpotential deposition, the formaldehyde production rate is significantly increased.
Direct CO reduction to formaldehyde (CORTF) provides an alternative, energy-efficient route for production of formaldehyde, a critical chemical commodity as well as promising hydrogen carrier. However, the conventional thermal catalysis approach is challenged with slow reaction kinetics, which can be attributed to imbalanced CO and hydrogen competitive chemisorption to catalyst, with stronger CO adsorption significantly inhibiting hydrogen adsorption that suppresses their reaction towards formaldehyde generation. We report a new, innovative CORTF mechanism to promote the reaction by utilizing hydrogen underpotential deposition to balance the species coverage on catalyst surface. Our study shows that, by separately tuning Pt alloy nanoparticle catalyst composition to control CO chemical adsorption favorability and tuning hydrogen underpotential deposition potential to control hydrogen electrochemical adsorption favorability, the formaldehyde production rate with Pt alloys (866 mg/gcat/h) is 300 times higher compared to conventional thermal catalysis method (2.6 mg/gcat/h) and 50 time higher than previously reported molybdenum phosphide (MoP, 16.3 mg/gcat/h) electrocatalyst. DFT simulations show reduced energy barriers for the rate-limiting steps by means of balancing hydrogen and CO adsorption, thus supporting this new mechanism to achieve more dramatically improved CORTF kinetics. This CORTF mechanism provides a new strategy towards efficient formaldehyde production.
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