domino4chem: Semi-biological Domino Catalysis for Solar Chemical Synthesis

减少二氧化碳排放和向循环经济过渡是保护我们繁荣未来的紧急行动。碳捕获和利用是一种碳中性的过程，通过回收二氧化碳来合成有价值的分子和由可再生能源提供动力的材料。利用太阳光从二氧化碳合成燃料已取得重大进展，但主要挑战仍然存在：(i)利用半导体的合成方法在光能利用方面效率很高，但只能从二氧化碳中生产最简单的产品；生物方法可以产生更复杂的产品，但吸收二氧化碳的速度较慢，利用太阳能的效率也较低。这一提议将开创利用阳光，结合合成技术和生物技术的优势，以高效率控制复杂化学物质的合成。将开发一个集成平台，该平台结合了半导体的高效光收集，以驱动合成和生物催化剂网络，将二氧化碳转化为定制的复杂化学产品。具体来说，光电化学串联装置和光触媒粉末片将被用作光收集组件。这将驱动一系列集成在定制多孔结构中的（生物）催化剂，以催化顺序划分的反应（“多米诺骨牌催化”）。合成催化剂首先利用水氧化生成的电子将CO2还原为甲酸盐和CO等载体。载体随后将在同一设备中用作微生物或酶/合成级联的原料，以生产目标化学品。这种载体方法能够有效地利用各种催化剂，包括工程代谢途径，以高度控制的方式合成所需产品。提出的直接光子到化学转化技术将提供一个通用的生物混合平台，在未来从阳光中可持续地合成高价值的化学品。

Mitigating CO2 emissions and transitioning to a circular economy are urgent actions to safeguard our prosperous future. Carbon capture and utilisation is a carbon-neutral process to recycle CO2 for the synthesis of valuable molecules and materials powered by renewable energy. The synthesis of fuels from CO2 using sunlight has made significant advances, but major challenges remain: (i) Synthetic approaches using semiconductors are highly efficient in light utilisation but can only produce the simplest of products from CO2; (ii) biological approaches can generate more complex products but are slow in CO2 uptake and inefficient in their use of solar energy.This proposal will pioneer the controlled synthesis of complex chemicals at high efficiency using sunlight by combining the strength of synthetic and biological technologies. An integrated platform will be developed that incorporates efficient light harvesting by semiconductors to drive a network of synthetic and biological catalysts to convert CO2 to bespoke complex chemical products. Specifically, photoelectrochemical tandem devices and photocatalyst powder sheets will be employed as the light harvesting component. These will drive a series of (bio)catalysts integrated in a bespoke porous architecture to catalyse compartmentalised reactions in sequence ('domino catalysis'). Synthetic catalysts will first reduce CO2 to vectors such as formate and CO with electrons being sourced from the oxidation of water to O2. The vectors will subsequently be used in the same device as feedstocks for microorganisms or enzyme/synthetic cascades to produce the target chemical. This vector-approach enables the efficient use of a wide range of catalysts, including engineered metabolic pathways, to synthesise desired products with a high degree of control.The proposed direct photon-to-chemical conversion technology will provide a general biohybrid platform to synthesise high value chemicals sustainably from sunlight in the future.