Dye-Sensitized Photocathodes Assembly and Tandem Photoelectrochemical Cells for CO2 Reduction,Accounts of Materials Research

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Dye-Sensitized Photocathodes Assembly and Tandem Photoelectrochemical Cells for CO2 Reduction
Accounts of Materials Research ( IF 14.0 ) Pub Date : 2024-01-22 , DOI: 10.1021/accountsmr.3c00183
Ling Fei _{1,

2} , Lei Lei _{1,

2} , Thomas J. Meyer ₃ , Degao Wang _{1,

2,

4}

Affiliation

Increasing concentrations of atmospheric CO₂ are a worldwide problem that have triggered considerable environmental concerns, such as global warming, glacier melting, and a loss of biodiversity. Therefore, the conversion and utilization of CO₂ have become increasingly urgent. CO₂ photoreduction mimics natural photosynthesis and performs CO₂ reduction by using solar energy to drive the formation of renewable fuels, which has been documented as a potential solution for energy shortage and global warming. CO₂ photoreduction is a promising approach for achieving energy sustainability by forming and utilizing C-based reduction products. The traditional thermocatalytic CO₂ reduction technique requires high temperature and high-pressure conditions, which consumes huge energy amounts; by contrast, CO₂ photoreduction employs solar energy and electrical energy as the activation energy for catalytic reaction, resulting in faster reaction rates and minimal environmental impact. Although semiconductor-based photocatalysts are advantageous, given their low cost and easy modification, their slow carrier transfer rates and poor photostabilities limit their use in practical applications. Homogenous catalysts consisting of integrated photosensitizers and catalyst units on the surface of semiconductor electrodes can provide more appropriate photocatalytic capabilities for simultaneous CO₂ photoreduction and water oxidation. However, differences in reaction conditions for the two half reactions, with the integration of water oxidation and CO₂ reduction in single one-catalyst systems, may be inaccessible. To overcome these bottlenecks, a variety of approaches for artificial photosynthesis have been investigated to achieve more highly efficient CO₂ photoreduction, and these strategies primarily focused on the optimization of the surface structures of semiconductor electrodes and the development of novel catalysts. When the basic principles of the molecular chemical reaction are combined with surface construction preparations, the photocatalytic activity can be efficiently enhanced. This Account summarizes the mechanisms for CO₂ photoreduction in a Dye-Sensitized PhotoElectrochemical Cell (DSPEC), and it outlines the progress made in this area based on the design and assembly of molecular-based DSPEC and the role of chromophore–catalyst assemblies in these applications. By optimizing surface film internal structures, surface molecular assemblies have been prepared that open a door for preparing durable, efficient integrated assemblies for CO₂ photoreduction. In addition, this Account also briefly summarizes the research progress of a typical tandem DSPEC cell for coupling CO₂ reduction with water oxidation. Based on the research progress and challenges of semiconductor-surface molecular catalyst design, prospects are outlined at the end of the Account, including enhancement of catalytic behaviors and long-term stability, optimization of the surface assembly structures, and novel design of efficient bias-free tandem cells.

中文翻译：

用于二氧化碳减排的染料敏化光电阴极组件和串联光电化学电池

_{大气中CO 2}浓度不断增加是一个世界性问题，引发了相当大的环境问题，例如全球变暖、冰川融化和生物多样性丧失。_{因此，CO 2}的转化和利用变得越来越紧迫。CO ₂光还原模仿自然光合作用，通过利用太阳能驱动可再生燃料的形成来还原CO _{2 ，这已被记录为能源短缺和全球变暖的潜在解决方案。}CO ₂光还原是通过形成和利用基于碳的还原产物来实现能源可持续性的有前途的方法。传统的热催化CO ₂还原技术需要高温高压条件，消耗大量能源。相比之下，CO ₂光还原利用太阳能和电能作为催化反应的活化能，反应速率更快，对环境的影响最小。尽管半导体光催化剂具有优势，但由于其成本低且易于改性，但其载流子传输速率慢和光稳定性差限制了其在实际应用中的使用。由半导体电极表面集成光敏剂和催化剂单元组成的均质催化剂可以为同时进行CO ₂光还原和水氧化提供更合适的光催化能力。然而，两个半反应的反应条件的差异，以及在单个单催化剂系统中水氧化和CO _{2还原的整合，可能是难以接近的。}为了克服这些瓶颈，人们研究了多种人工光合作用方法来实现更高效的CO ₂光还原，这些策略主要集中在半导体电极表面结构的优化和新型催化剂的开发上。当分子化学反应的基本原理与表面构建制剂相结合时，可以有效增强光催化活性。本报告总结了染料敏化光电化学电池 (DSPEC) 中CO ₂光还原的机制，并概述了基于分子 DSPEC 的设计和组装以及发色团 - 催化剂组件在这些中的作用在该领域取得的进展。应用程序。通过优化表面膜内部结构，制备了表面分子组装体，为制备耐用、高效的 CO _{2集成组装体打开了大门}光还原。此外，本文还简要总结了典型串联DSPEC电池耦合CO ₂还原与水氧化的研究进展。基于半导体表面分子催化剂设计的研究进展和挑战，在报告的最后概述了前景，包括催化行为和长期稳定性的增强、表面组装结构的优化以及高效偏压的新颖设计。游离串联细胞。

更新日期：2024-01-22

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