Citation: Jinhua Zhang, Yuanbin She. Unveiling the decomposition mechanism of formic acid on Pd/WC(0001) surface by using density function theory[J]. Chinese Journal of Catalysis, ;2020, 41(3): 415-425. doi: S1872-2067(19)63463-7 shu

Unveiling the decomposition mechanism of formic acid on Pd/WC(0001) surface by using density function theory

Jinhua Zhang ^a,b, ,
Yuanbin She ^a

a College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310014, Zhejiang, China;
b School of Materials and Environmental Engineering, Chizhou University, Chizhou 247000, Anhui, China

Received Date: 18 June 2019
Revised Date: 26 July 2019

Fund Project: This work was supported by the National Natural Science Foundation of China (21776259) and Key Laboratory of Micro-Nano Powder and Advanced Energy Materials of Anhui Higher Education Institutes, Chizhou University.

In pursuit of low-cost direct formic acid fuel cells, tungsten carbide (WC) supported Pd catalyst is considered as an ideal candidate for efficient decomposition of formic acid due to low Pd utilization and excellent performance. Herein, different adsorption configurations and active sites of the intermediates, involved in the HCOOH decomposition, on WC(0001)-supported Pd monolayer (Pd/WC(0001)) surface investigated by using density functional theory. The results reveal that trans-HCOOH, HCOO, cis-COOH, trans-COOH, HCO, CO, H₂O, OH and H exhibit chemisorption on Pd/WC(0001) surface, whereas cis-HCOOH and CO₂ exhibit weak interactions with Pd/WC(0001) surface. In addition, the minimum energy pathways of HCOOH decomposition are analyzed to generate CO and CO₂ due to the fracture of C-H, H-O and C-O bonds. The adsorbed HCOOH, HCOO, mHCOO, cis-COOH and trans-COOH configurations exhibit dissociation rather than desorption. CO formation occurs through the decomposition of cis-COOH, trans-COOH and HCO, whereas the CO₂ formation happens due to the decomposition of HCOO. It is found that the most favorable pathway for HCOOH decomposition on Pd/WC(0001) surface is HCOOH→HCOO→CO₂, where the formation of CO₂ from HCOO dehydrogenation determines the reaction rate. Overall, CO₂ is the most dominant product of HCOOH decomposition on Pd/WC(0001) surface. The presence of WC, as monolayer Pd carrier, does not alter the catalytic behavior of Pd and significantly reduces the Pd utilization.
- Density functional theory,
- Formic acid,
- Direct formic acid fuel cells,
- WC(0001)-supported Pd monolayer,
- Decomposition mechanism
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