School of Chemical Engineering & Materials Science, Chung-Ang University, 84 Heukseok-ro, Dongjak-gu, Seoul, 06974, Republic of Korea.
Chem Rec. 2022 Jan;22(1):e202100219. doi: 10.1002/tcr.202100219. Epub 2021 Sep 3.
Uncontrolled CO emission from various industrial and domestic sources is a considerable threat to environmental sustainability. Scientists are trying to develop multiple approaches to not only reduce CO emissions but also utilize this potent pollutant to get economically feasible products. The electrochemical reduction of CO (ERC) is one way to effectively convert CO to more useful products (ranging from C1 to C5). Nevertheless, this process is kinetically hindered and less selective towards a specific product and, consequently, requires an efficient electrocatalyst with characteristics like selectivity, stability, reusability, low cost, and environmentally benign. Owing to specified commercial features, copper (Cu)-based materials are highly anticipated and widely investigated for the last two decades. However, their non-modified polycrystalline Cu forms usually lack selectivity and lower overpotential of CO reduction. Therefore, extensive research is in progress to induce various alterations ranging from morphological and surface chemistry tuning to structural and optoelectrical characteristics modifications. This review provides an overview of those strategies to improve the CO conversion efficiency through Cu-based ERC into valuable C1, C2 and higher molecular weight hydrocarbons. The thermodynamics and kinetics of CO reduction via Cu-based electrocatalysts are discussed in detail with the support of the first principle DFT-based models. In the last portion of the review, the reported mechanisms for various products are summarized, with a short overview of the outlook. This review is expected to provide important basics as well as advanced information for experienced as well as new researchers to develop various strategies for Cu and related materials to achieve improved ERC.
从各种工业和家庭来源排放的不受控制的 CO 是对环境可持续性的重大威胁。科学家们正试图开发多种方法,不仅要减少 CO 排放,还要利用这种强效污染物来获得经济可行的产品。CO 的电化学还原(ERC)是一种将 CO 有效转化为更有用的产品(从 C1 到 C5)的方法。然而,这个过程在动力学上受到阻碍,对特定产品的选择性较低,因此需要具有选择性、稳定性、可重复使用性、低成本和环境友好等特点的高效电催化剂。由于具有特定的商业特征,铜(Cu)基材料在过去二十年中备受期待并得到了广泛研究。然而,它们未经修饰的多晶 Cu 形式通常缺乏选择性和较低的 CO 还原过电势。因此,正在进行广泛的研究,以诱导从形态和表面化学调谐到结构和光电特性修饰的各种改变。本综述提供了通过 Cu 基 ERC 将 CO 转化为有价值的 C1、C2 和更高分子量烃类来提高 CO 转化效率的那些策略的概述。通过基于第一性原理 DFT 的模型详细讨论了 Cu 基电催化剂还原 CO 的热力学和动力学。在综述的最后一部分,总结了各种产物的报道机制,并对展望进行了简短概述。本综述有望为有经验和新的研究人员提供重要的基础知识和高级信息,以开发各种用于 Cu 及相关材料的策略,从而实现改进的 ERC。