Zhou Guosheng, Wang Zhenzhen, Gong Junjie, Shen Shijie, Zhong Wenwu
Zhejiang Key Laboratory for Island Green Energy and New Materials, Taizhou University Jiaojiang 318000 Zhejiang P. R. China
School of Chemistry and Chemical Engineering, Shaoxing University Shaoxing 312000 P. R. China.
Chem Sci. 2025 Jun 12. doi: 10.1039/d5sc02284c.
Photoelectrochemical carbon dioxide reduction reaction (PEC CORR) is a promising strategy for converting CO into high-value chemicals that contribute to carbon neutrality. However, CO reduction is often accompanied by various competitive reaction pathways in the actual reaction process, which may generate a variety of products. The selective regulation of different products not only directly affects the yield and separation cost of the target product, but also influences the energy efficiency and economic feasibility of the whole process. Improving product selectivity is essential for increasing product yield and understanding the reaction mechanism. This review systematically summarizes recent advances and challenges in achieving high selectivity in PEC CORR. First, the basic concept and principle of the PEC CORR are summarized. Next, the key factors affecting product selectivity are discussed, including catalyst design (catalyst type, modification, composition, and morphology), reaction conditions (applied voltage, light intensity and wavelength, reaction temperature, and electrolyte type) and reactor design (photoelectrode area, synergistic oxidation effect, geometric structure, and gas diffusion electrode). In addition, kinetic and thermodynamic aspects such as the CO adsorption model, band gap structure, and reaction free energy are also explored. Then, the research progress over the past five years on different products is described in detail, focusing on the current status and challenges in the study of C products and C products. Subsequently, the primary factors leading to the failure of PEC CORR are summarized, and various cooperative strategies are introduced to achieve long-term stability in product selectivity. Finally, the challenges and future directions for developing PEC CORR systems with enhanced selectivity are introduced. In particular, the importance of innovative catalyst design, reaction stability, reaction environment optimization, advanced equipment structure and reaction mechanism analysis for promoting PEC CORR in industrial applications is emphasized.
光电化学二氧化碳还原反应（PEC CORR）是一种将CO转化为有助于实现碳中和的高价值化学品的有前景的策略。然而，在实际反应过程中，CO还原通常伴随着各种竞争反应途径，这可能会产生多种产物。对不同产物的选择性调控不仅直接影响目标产物的产率和分离成本，还会影响整个过程的能源效率和经济可行性。提高产物选择性对于提高产物产率和理解反应机理至关重要。本文综述系统地总结了在PEC CORR中实现高选择性方面的最新进展和挑战。首先，总结了PEC CORR的基本概念和原理。接下来，讨论了影响产物选择性的关键因素，包括催化剂设计（催化剂类型、改性、组成和形态）、反应条件（施加电压、光强和波长、反应温度和电解质类型）以及反应器设计（光电极面积、协同氧化效应、几何结构和气体扩散电极）。此外，还探讨了诸如CO吸附模型、带隙结构和反应自由能等动力学和热力学方面。然后，详细描述了过去五年中不同产物的研究进展，重点关注C产物和C产物研究的现状和挑战。随后，总结了导致PEC CORR失败的主要因素，并介绍了各种协同策略以实现产物选择性的长期稳定性。最后，介绍了开发具有更高选择性的PEC CORR系统面临的挑战和未来方向。特别强调了创新催化剂设计、反应稳定性、反应环境优化、先进设备结构和反应机理分析对于推动PEC CORR在工业应用中的重要性。
