Bismuth nanosheets with rich grain boundaries for efficient electroreduction of CO2 to formate under high pressures

doi:10.1016/S1872-2067(22)64131-7

Abstract

Abstract:

Electrochemical CO₂ reduction reaction (CO₂RR) driven by sustainable energy has emerged as an attractive route to achieve the target of carbon neutral. Formate is one of the most economically viable products, and electrocatalytic CO₂RR to formate is a promising technology. High-pressure H-cell electrolyzer is easy to operate and allows high CO₂ solubility for realizing high current density, but the design of highly efficient catalysts for working under high CO₂ pressures remains challenging. Bismuth-based catalysts exhibit high formate selectivity, but suffer from limited activity. Here, we report a high-performance catalyst, which is derived from BiPO₄ nanopolyhedrons during electrocatalytic CO₂RR to formate in neutral solution under high CO₂ pressures. A high partial current density of formate (534 mA cm^-2) and formate formation rate (9.9 mmol h^-1 cm^-2) with a formate Faradaic efficiency of 90% have been achieved over BiPO₄-derived catalyst at an applied potential of -0.81 V vs. RHE under 3.0 MPa CO₂ pressure. We discover that BiPO₄ nanopolyhedrons evolve into metallic Bi nanosheets with rich grain boundaries in electrocatalytic CO₂RR under high CO₂ pressures, and the grain boundaries of the BiPO₄-derived catalyst play a vital role in promoting electrocatalytic CO₂RR to formate. Our theoretical studies reveal that the charge redistribution occurs at the grain boundaries of Bi surface, and this promotes CO₂ activation and increases HCOO* intermediate stability, thus making the pathway for CO₂RR to formate more selective and energy-favorable. This work not only demonstrates a highly efficient catalyst for CO₂RR to formate but also discovers a unique feature of catalyst evolution under high CO₂ pressures.

Key words: Electrocatalytic CO₂ reduction, Formate, High-pressure H-cell, Bi nanosheet, Grain boundary

Sunhong Ruan, Biao Zhang, Jinhan Zou, Wanfu Zhong, Xiaoyang He, Jinhai Lu, Qinghong Zhang, Ye Wang, Shunji Xie. Bismuth nanosheets with rich grain boundaries for efficient electroreduction of CO₂ to formate under high pressures[J]. Chinese Journal of Catalysis, 2022, 43(12): 3161-3169.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(22)64131-7

https://www.cjcatal.com/EN/Y2022/V43/I12/3161

Figures/Tables 5

Fig. 1. (a) Schematic setup of high-pressure H-cell for electrocatalytic CO2RR. (b) Current densities and FEs of CO2RR products over the BiPO4-derived catalyst in 1.0 mol L-1 KHCO3 under 1.0 MPa CO2. (c) Partial current density of formate under different CO2 pressures in 1.0 mol L-1 KHCO3. (d) Partial current density of products and formate formation rate of CO2RR in 2.0 mol L-1 KHCO3 under 3.0 MPa CO2. The experiments in each case were performed at least for three times and the error bar represents the relative deviation.

Fig. 2. CO2RR performances of BiPO4 derived under 3.0 MPa CO2 (BiPO4-derived-3) and 0.1 MPa CO2 (BiPO4-derived-0.1) then evaluated under 0.1 MPa CO2 in 1.0 mol L-1 KHCO3. (a) BiPO4-derived-3. (b) BiPO4-derived-0.1. (c) Double-layer capacitance (Cdl) of BiPO4-derived-3 and BiPO4-derived-0.1; (d) ECSA-corrected partial current density of formate for BiPO4-derived-3 and BiPO4-derived-0.1. The experiments in each case were performed at least for three times and the error bar represents the relative deviation.

Fig. 3. XRD patterns (a) and cyclic voltammetry curves (b) of BiPO4-derived-3 and BiPO4-derived-0.1.

Fig. 4. SEM (a), TEM and SAED (inset) (b), and HRTEM (c) images of BiPO4-derived-0.1. SEM (d), TEM and SAED (inset) (e), and HRTEM (f) of BiPO4-derived-3; (g) Schematic diagram of the structure evolution of BiPO4-derived catalysts under different CO2 pressures.

Fig. 5. (a) Optimized configurations of *CO2, HCOO*, *HCOOH on (001) facet of Bi and Bi-GB respectively. (b,c) Gibbs free energy diagrams for electrocatalytic CO2RR to formate and CO on Bi and Bi-GB. (d) Charge density differences plots of *CO2 and HCOO* on Bi and Bi-GB. Yellow and cyan regions represent electron accumulation and depletion, respectively. The yellow and cyan regions represent 0.0002 e per Å3 isosurfaces for *CO2 and 0.0020 e per Å3 isosurfaces for HCOO*. The light pink, brown, red and purple represent H, C, O and Bi atoms, respectively, and especially lilac represents Bi atom on the grain boundaries.

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Bismuth nanosheets with rich grain boundaries for efficient electroreduction of CO₂ to formate under high pressures

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