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，人工系统的挑战在于将光收集和转化与催化多电子氧化还原过程结合起来，并引入自然系统中存在的（自动）再生和保护机制，而人工系统则缺乏这些机制。此外，人工光合系统的各个组成部分（光敏剂（ps），催化剂，牺牲电子供体（sed））仍然有重要的缺点。迄今为止，太阳能到燃料的转换效率和/或人工光合系统的寿命（稳定性/鲁棒性）不符合允许其大规模应用的参数。此外，这些系统通常是有效的，但不是有选择性的，或者有选择性的，但不是很有效。在保持高选择性的同时实现高活性是另一个重要的挑战。我的研究计划在三个主要方向上发展：1)改进的分子光敏剂（PS）和人工光合作用的催化剂（例如，稳定的水溶性PS与改进的太阳光子转换；稳定的水溶性选择性催化剂）-这是分子方法的一个例子-“智能化学工具和策略”（SCTS）用于改善单个化合物的性质；II)用于二氧化碳还原和水分解的混合光催化系统，具有预先设计的再生/保护功能-预先设计的智能化合物集成（例如，分子光敏剂/催化剂+智能聚合物）-这是一种专注于化合物或过程的系统集成的方法- SCTS被用作在给定系统中组合/集成化合物或过程的方法；III)集成自动化和原位测量技术的“智能”光反应器的发展。拟议的研究计划具有科学影响，以及教育/学术影响。研究结果将使整个参与能源转换和有关领域的科学界感兴趣，同时将协助培训这些部门的人员。实现这一研究计划的目标将带来从协调复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在促进可持续发展和解决当今社会面临的主要挑战所需的全球解决方案方面的强大能力，符合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。

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.