Smart Compounds, Systems and Research Methods in Artificial Photosynthesis

开发与自然光合作用原理相同的人工设备被认为是解决我们社会面临的能源和环境问题的可行方案。然而，人工系统中的挑战是将光收集和转化与催化多电子氧化还原过程相结合，以及引入自然系统中存在的(自动)再生和保护机制，而人工系统中缺乏这种机制。此外，人工光合作用系统的各个组成部分(光敏剂(PSS)、催化剂、牺牲电子供体(SED))仍然存在重大缺陷。到目前为止，人工光合作用系统的太阳能到燃料的转换效率和/或寿命(稳定性/稳健性)还不能满足大规模应用的参数。此外，这些系统通常是有效的，但不是选择性的或选择性的，但不是非常有效。在保持高选择性的同时实现高活性是另一个重要的挑战。我的研究计划的发展主要有三个方向：i)改进的分子光敏剂(PS)和用于人工光合作用的催化剂(例如，具有改进的太阳光子转化的稳定的水溶PS；稳定的水溶选择性催化剂)-这是分子方法的一个例子-‘智能化学工具和策略’(SCTS)被用于改善单个化合物的性质；二)具有预先设计的再生成/保护功能的二氧化碳还原和水分解的混合光催化系统--预先设计的智能化合物的集成(例如，分子光敏剂/催化剂+智能聚合物)--这是一种侧重于化合物或过程的系统集成的方法--SCT用作在特定系统中组合/集成化合物或过程的方法；三)开发集成自动化和现场测量技术的“智能”光反应堆。拟议的研究计划产生了科学影响，也产生了教育/学术影响。研究结果将对整个涉及能源转换和相关领域的科学界产生兴趣，同时将有助于这些领域的人员培训。实现这一研究计划的目标将带来从配位络合物的基础研究和学术研究中的原理证明，一直到原型，甚至可能到全面应用的进步。最后，拟议项目的实现将证明学术研究的强大能力，有助于根据加拿大和全球在教育、研究、环境和能源政策方面的优先事项，促进可持续发展和解决当今社会面临的重大挑战所需的全球解决办法。

The development of artificial devices working on the same principles as natural photosynthesis is considered a viable solution to the energy and environmental problems our society faces. However, the challenge in an artificial system is to integrate light harvesting and conversion with catalytic multi-electron redox processes, as well as to introduce the (auto)regeneration and protection mechanisms present in natural systems, but lacking in the artificial ones. In addition, the individual components of artificial photosynthetic systems (photosensitizers (PSs), catalysts, sacrificial electron donors (SEDs)) continue to have important drawbacks. To date, the solar to fuel conversion efficiency and/ or the life-time (stability/ robustness) of the artificial photosynthetic systems do not meet the parameters that allow their large-scale application. In addition, these systems are usually efficient but not selective or selective but not very efficient. Achieving high activities while retaining high selectivity is another important challenge. The development of my research program is proposed in three major directions: I) improved molecular photosensitizers (PS) and catalysts for artificial photosynthesis (e.g., stable water soluble PS with improved solar photon conversion; stable water soluble selective catalysts) - this represents an example of molecular approach - `Smart Chemistry Tools and Strategies' (SCTS) are used to improve the properties of individual compounds; II) hybrid photocatalytic systems for CO2 reduction and water splitting with pre-designed re-generation/protection features - pre-designed integration of smart compounds (e.g., molecular photosensitizers/ catalysts + smart polymers) - this is an approach focusing on system integration of compounds or processes - the SCTS are used as methods of combining/integration of the compounds or processes in a given system; III) development of `smart' photoreactors integrating automated and in situ measurement techniques. The proposed research program has a scientific impact, as well as an educational/academic one. The results will be of interest for the whole scientific community involved in energy conversion and related fields while the training of personnel in these sectors will be assisted. Realizing the objectives of this research program would bring advancements from the fundamental study of coordination complexes and proofs-of-principle in academic research, all the way to prototypes, and possibly to full-scale applications. Finally, the realization of the proposed project will prove the powerful capacity of academic research to contribute to sustainable development and to the global solutions needed to solve the major challenges society faces today, in line with Canadian and global priorities in term of education, research, environment and energy policies.