Xiao Changlong, Zhang Jie
School of Chemistry, Monash University, Clayton, VIC 3800, Australia.
ARC Centre of Excellence for Electromaterials Science, Monash University, Clayton, VIC 3800, Australia.
ACS Nano. 2021 May 25;15(5):7975-8000. doi: 10.1021/acsnano.0c10697. Epub 2021 May 6.
Electrochemical CO reduction to value-added chemicals and fuels is a promising approach to mitigate the greenhouse effect arising from anthropogenic CO emission and energy shortage caused by the depletion of nonrenewable fossil fuels. The generation of multicarbon (C) products, especially hydrocarbons and oxygenates, is of great interest for industrial applications. To date, Cu is the only metal known to catalyze the C-C coupling in the electrochemical CO reduction reaction (eCORR) with appreciable efficiency and kinetic viability to produce a wide range of C products in aqueous solutions. Nonetheless, poor product selectivity associated with Cu is the main technical problem for the application of the eCORR technology on a global scale. Based on extensive research efforts, a delicate and rational design of electrocatalyst architecture using the principles of nanotechnology is likely to significantly affect the adsorption energetics of some key intermediates and hence the inherent reaction pathways. In this review, we summarize recent progress that has been achieved by tailoring the electrocatalyst architecture for efficient electrochemical CO conversion to the target C products. By considering the experimental and computational results, we further analyze the underlying correlations between the architecture of a catalyst and its selectivity toward C products. Finally, the major challenges are outlined, and directions for future development are suggested.
将电化学CO还原为增值化学品和燃料是一种很有前景的方法，可减轻人为CO排放引起的温室效应以及不可再生化石燃料枯竭导致的能源短缺问题。多碳（C）产物的生成，尤其是碳氢化合物和含氧化合物，对于工业应用具有重大意义。迄今为止，Cu是唯一已知的能在电化学CO还原反应（eCORR）中以可观的效率和动力学可行性催化C-C偶联，从而在水溶液中生成多种C产物的金属。尽管如此，与Cu相关的产物选择性较差是eCORR技术在全球范围内应用的主要技术问题。基于广泛的研究工作，利用纳米技术原理对电催化剂结构进行精细且合理的设计可能会显著影响某些关键中间体的吸附能，进而影响固有的反应途径。在本综述中，我们总结了通过调整电催化剂结构以实现高效电化学CO转化为目标C产物所取得的最新进展。通过综合考虑实验和计算结果，我们进一步分析了催化剂结构与其对C产物选择性之间的潜在关联。最后，概述了主要挑战，并提出了未来的发展方向。
