Regulating Pd-catalysis for electrocatalytic CO2 reduction to formate via intermetallic PdBi nanosheets

doi:10.1016/S1872-2067(21)63999-2

Abstract

Abstract:

Electrocatalytic CO₂ reduction plays an important role in the reduction of the CO₂ concentration in atmosphere and consequently the mitigation of greenhouse effects. Pd has been extensively investigated as an electrocatalyst for the CO₂ reduction to formate, which is an important raw material in the production of organic chemicals. However, the low selectivity and competitive reaction (hydrogen evolution reaction (HER)) have hindered the performance of monometallic Pd catalysts. In this paper, intermetallic PdBi nanosheets (NSs) are prepared for efficient CO₂ reduction to formate. The highest Faradaic efficiency (FE) of formate on fully ordered PdBi NSs reaches 91.9% at -1.0 V vs. RHE, which outperforms that of the disordered PdBi and pure Pd catalysts. Density functional theory calculations suggest that compared to disordered PdBi NSs, the ordered structure can decrease the free energy barrier of *OCHO (a key intermediate of formate formation) and inhibit H₂ evolution as well, thereby enhancing the activity and selectivity for formate production.

Key words: CO₂ reduction, Electrocatalysis, Formate, Palladium, Intermetallic compound, Nanosheet

Linfeng Xie, Xuan Liu, Fanyang Huang, Jiashun Liang, Jianyun Liu, Tanyuan Wang, Liming Yang, Ruiguo Cao, Qing Li. Regulating Pd-catalysis for electrocatalytic CO₂ reduction to formate via intermetallic PdBi nanosheets[J]. Chinese Journal of Catalysis, 2022, 43(7): 1680-1686.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63999-2

https://www.cjcatal.com/EN/Y2022/V43/I7/1680

Figures/Tables 5

Scheme 1. Schematic of the synthesis of fully ordered (o-), partially ordered (p-), and disordered (d-) PdBi NSs.

Fig. 1. TEM images of Pd (a) and o-PdBi NSs (b). (c) Height profile of o-PdBi NSs and the corresponding measuring AFM image. (d) HRTEM image of o-PdBi NSs. The inset illustrates the FFT patterns of the corresponding area, where (1) and (2) are the enlarged views of the corresponding regions in Fig. (d). (e) HAADF-STEM image of o-PdBi NSs.

Fig. 2. (a) XRD patterns of Pd, d-PdBi/C, p-PdBi/C, and o-PdBi/C NSs. (b) XPS spectra of the Pd 3d electrons of Pd/C and o-PdBi/C NSs.

Fig. 3. (a) LSV curves of Pd/C, d-PdBi/C, p-PdBi/C, and o-PdBi/C NSs and commercial Pd/C. (b) FE of formate on d-PdBi/C, p-PdBi/C, and o-PdBi/C NSs and (c) corresponding partial current density of formate at -0.8 V, -0.9 V, -1.0 V, -1.1 V vs. RHE. (d) FEs of formate, CO, and H2 on o-PdBi/C NSs in the potential range of -0.4 to -1.1 V. (e) Durability test of o-PdBi/C NSs at -0.9 V for 10 h. The inset diagram is corresponding formate FEs at -0.9 V for 10 h. All CO2RR tests were conducted in a CO2-saturated 0.5 mol/L KHCO3 solution.

Fig. 4. Free energy diagrams for the CO2 reduction to HCOOH on d-PdBi and o-PdBi with Pd (a) and Bi (b) surface exposed (the schematic corresponding to each step is shown below, where the blue, yellow, black, red, and green atoms are Pd, Bi, C, O, and H, respectively). The free energy diagrams for the CO2 reduction to HCOOH on the o-PdBi (0001) facets with Pd and Bi exposed at 0 V (c) and -0.9 V (d) vs. RHE.

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Regulating Pd-catalysis for electrocatalytic CO₂ reduction to formate via intermetallic PdBi nanosheets

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