Electrocatalytic Refinery for Sustainable Production of Fuels and Chemicals.

Compared to modern fossil fuel-based industrial refineries, the emerging electrocatalytic refinery (e-refinery) is a more sustainable and environmentally benign strategy to convert renewable feedstocks and energy sources to transportable fuels and value-added chemicals. E-refinery will promisingly lead to defossilization, decarbonization, and decentralization of chemical industry. A crucial step in conducting e-refinery processes is the selection and development of appropriate reactions and optimal electrocatalysts for efficient cleavage and formation of chemical bonds between H, O, C, and N. However, compared to well-studied primary reactions (e.g., O 2 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 concise and comprehensive fundamentals of heterogeneous electrocatalysis and some primary reactions, and then implement these foundations to establish the framework of e-refinery with greater complexity by electrocatalytic coupling in situ generated intermediates (integrated reactions) or products (tandem reactions). We will also present a set of materials design principles and strategies to efficiently manipulate the reaction intermediates and pathways, and conclude with a perspective section to accelerate the development of feasible electrochemical industrial processes.