Electrocatalytic Refinery for Sustainable Production of Fuels and Chemicals

Abstract

Compared to modern fossil‐fuel‐based refineries, the emerging electrocatalytic refinery (e‐refinery) is a more sustainable and environmentally benign strategy to convert renewable feedstocks and energy sources into transportable fuels and value‐added chemicals. A crucial step in conducting e‐refinery processes is the development of appropriate reactions and optimal electrocatalysts for efficient cleavage and formation of chemical bonds. However, compared to well‐studied primary reactions (e.g., O2 reduction, water splitting), the mechanistic aspects and materials design for emerging complex reactions are yet to be settled. To address this challenge, herein, we first present fundamentals of heterogeneous electrocatalysis and some primary reactions, and then implement these to establish the framework of e‐refinery by coupling in situ generated intermediates (integrated reactions) or products (tandem reactions). We also present a set of materials design principles and strategies to efficiently manipulate the reaction intermediates and pathways.

Molecular Cleavage of Metal‐Organic Frameworks and Application to Energy Storage and Conversion

“…Electrocatalytic refinery is an emerging method to obtain fuel and chemical products from fossil fuels to renewable energy sources. [53] A critical step in practically realizing this method is the need to develop suitable electrocatalysts with high activity and selectivity for targeted chemical conversions. There are three main steps in typical heterogeneous electrocatalysis:…”

Electrocatalytic Reactions for Converting CO2 to Value‐Added Products

“…The combination of CO 2 and other heteroatoms, such as N, S, and Br from small-molecule reactants, can produce higher valuable products. [22] For example, combining CO 2 with Br elements can lead to the product of bromohydrins and 2-bromoethanol, whereas combining CO 2 with N elements may lead to N-ethylacetamide, N,N-dimethylacetamide, and so on. [24,59] As aforementioned, the formation of *OCCO dimerization intermediate is the limited step toward C 2þ products, in which the key factors include the adsorption capability of catalysts to CO and local concentrations of CO or *CO. To increase the proportion of *OCCO dimerization, Wang and coworkers introduced mixed CO 2 /CO feeds to enhance the *CO surface coverage (Figure 5a).…”

“…[3] Thus, coupling intermediates obtained by CO 2 reduction with small molecules and organic substrates has also attracted more attention from researchers, which may allow to obtain target products with higher economic benefits through electrocatalytic reactions. [22] The small molecules and organic substrates reactants can be derived from anode products or electrolyte additives. High selectivity and activity toward C 1 products have been widely reported in CO 2 RR.…”

Computational Studies on Carbon Dots Electrocatalysis: A Review

“…Therefore, researchers are continuing to pursue clean, efficient, low-cost, and environmentally benign sustainable energy. [1][2][3] In the recent past years, energy conversion devices such as fuel cells and rechargeable metal-air batteries have been extensively studied. [4][5] Electrocatalytic reactions play an essential role in these devices.…”