In Situ Generation of Flash Graphene Supported Spherical Bismuth Nanoparticles in Less than 200 ms for Highly Selective Carbon Dioxide Electroreduction

Abstract

Flash Joule heating (FJH) method is an emerging and powerful technique that has exhibited great potential in various domains. Herein, we successfully prepared flash graphene (FG)-supported Bi nanoparticles (Bi-NPs/FG) via the ultrafast and ecofriendly FJH method in less than 200 ms for the first time. Benefited from the synergistic effect of highly conductive FG and active Bi nanocrystals, the Bi-NPs/FG hybrid shows a highly selective CO 2 electroreduction with an ultrahigh Faradaic efficiency of 93.8% toward C1 product (i.e., formate). Furthermore, the findings from Density Functional Theory (DFT) calculations unveil that the reconstruction process not only enhances the bonding strength of the surface Bi-OCHO*, but also optimizes the adsorption energy of the key intermediate (OCHO*), thus benefiting the production of formate. In addition, we conducted an extension study of the FJH route to demonstrate its versatility in preparing a range of other metal/alloy NPs encased in FG. This work presents a feasible pathway to the superfast and massive production of highly efficient electrocatalyst for CO 2 conversion, and it can be extended to other application scenarios with great potential.

Review on strategies for improving the added value and expanding the scope of CO2 electroreduction products

“…Currently, various Bi-based nano-materials with different morphologies (Fig. 7(a)–(d)), including nanoparticles, 118,124 nanosheets, 82,123,125,126 nanorods, 8 and nanoflowers, 119 have been reported to exhibit high selectivity (FE formate is approximately 90%) for electrocatalytic CO 2 reduction to formic acid in aqueous solutions. Moreover, through the utilization of molecular or ionic modifications, it becomes possible to efficiently regulate the distribution of electrons on the surface of Bi-based materials.…”

“…123 This doping strategy enables the construction of multi-component active sites, leading to improved catalytic performance. Integrating Bi-based nanostructures with conductive carbonaceous supports including carbon black, 130 carbon fiber, 125 graphene, 118,131 nitrogen-doped carbon, 8,132 aerogel, 121 and polymer polypyrrole 133 represents another effective approach to enhance the electrochemical performance. These conductive support materials not only accelerate the electron transfer process but also enhance the binding of key reactive intermediates (such as *OCHO) on the catalyst surface through their synergistic effect.…”

Graphene Materials from Coke-like Wastes as Proactive Support of Nickel–Iron Electro-Catalysts for Water Splitting

“…A more environmentally friendly approach to graphene production consists of using, as a carbon source, a carbonaceous residue, like plastic waste [ 35 ], or other carbonaceous sources [ 36 , 37 ]. In line with these ideas, we have recently reported the preparation of graphene oxides from industrial waste which consists of a residue of the production of coke in a coke oven battery (which is deposited at the top inner section of the coking oven) [ 38 ].…”