Tang Cheng, Zheng Yao, Jaroniec Mietek, Qiao Shi-Zhang
Centre for Materials in Energy and Catalysis, School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, SA, 5005, Australia.
Department of Chemistry and Biochemistry, Kent State University, Kent, OH, 44242, USA.
Angew Chem Int Ed Engl. 2021 Sep 1;60(36):19572-19590. doi: 10.1002/anie.202101522. Epub 2021 Mar 10.
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., O 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.
与基于现代化石燃料的炼油厂相比，新兴的电催化炼油厂（电子炼油厂）是一种更具可持续性且对环境更友好的策略，可将可再生原料和能源转化为可运输燃料和增值化学品。进行电子炼油厂工艺的关键一步是开发合适的反应和优化的电催化剂，以实现化学键的有效断裂和形成。然而，与研究充分的初级反应（如氧还原、水分解）相比，新兴复杂反应的机理方面和材料设计仍有待解决。为应对这一挑战，在此，我们首先介绍多相电催化的基本原理和一些初级反应，然后通过耦合原位生成的中间体（集成反应）或产物（串联反应）来应用这些原理，以建立电子炼油厂的框架。我们还提出了一套材料设计原则和策略，以有效控制反应中间体和反应途径。
