3 years ago

Facile CO2 Electro-Reduction to Formate via Oxygen Bidentate Intermediate Stabilized by High-Index Planes of Bi Dendrite Catalyst

Facile CO2 Electro-Reduction to Formate via Oxygen Bidentate Intermediate Stabilized by High-Index Planes of Bi Dendrite Catalyst
Jai Hyun Koh, Kwang Deog Jung, Taedaehyeong Eom, Da Hye Won, Yun Jeong Hwang, Byoung Koun Min, Hyungjun Kim, Nak-Kyoon Kim
Electrochemical CO2 conversion to chemical products is a promising strategy for sustainable industrial development. However, the success of this approach requires an in-depth understanding of catalysis because it involves highly complex multistep reactions. Herein, we suggest a rational design of a hierarchical Bi dendrite catalyst for an efficient conversion of CO2 to formate. A high selectivity (∼89% at −0.74 VRHE) and, more importantly, a stable performance during long-term operation (∼12 h) were achieved with the Bi dendrite. Density functional theory (DFT) is used to investigate three possible reaction pathways in terms of surface intermediate, and the one via *OCOH surface intermediate is calculated to be the most energetically feasible. DFT calculations further elucidate the plane-dependent catalytic activity and conclude that the high-index planes developed on the Bi dendrite are responsible for the sustainable performance of Bi dendrite. We expect that our experimental and theoretical study will provide a fundamental guideline for the CO2-to-formate conversion pathway as well as design principles for enhancing the catalytic performance.

Publisher URL: http://dx.doi.org/10.1021/acscatal.7b00707

DOI: 10.1021/acscatal.7b00707

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