Electro- and Photocatalytic CO2 Reduction with [FeNi]-Chalcogenides

二氧化碳是一种主要的温室气体，被认为是造成当前气候变化的关键因素之一。尽管它的反应性很低，但利用二氧化碳是社会的最大兴趣，并将有助于降低其在空气中总浓度的增加。除了将其转化为有机碳酸盐之外，热力学上坡转化，减少二氧化碳以提供重要的工业化学品和燃料是在人工碳循环中回收二氧化碳的有希望的途径。特别是，光催化和电催化还原过程将是这些转化为各种产品的必要条件。与工业催化相反，大自然拥有高度复杂的机器，可以在温和的条件下选择性地减少二氧化碳。虽然这些酶活性位点是众所周知的，并且包含一个[NiFe]杂双金属反应中心，但尚未对该基元进行非均相催化还原CO2的研究。我们在此的目的是表征和推进[FeNi]-硫族化合物作为非均相光和电催化剂的CO2还原的原理证明研究。

Carbon dioxide is a major greenhouse gas and assumed to be one of the key factors responsible for the current climate change. Despite its low reactivity, utilization of CO2 is of utmost interest for society and will contribute to lowering the increase of its total concentration in air. Besides its conversion into organic carbonates, the thermodynamic uphill conversion, reduction of CO2 to afford industrial important chemicals and fuels is a promising pathway towards the recycling of CO2 in an artificial carbon cycle. Especially, photo- and electrocatalytic reduction processes will be essential for such conversions into various products. Contrary to industrial catalysis, nature possesses highly sophisticated machineries to allow for a selective reduction of CO2 under mild conditions. Although such enzymatic active sites are well-known and comprise a [NiFe] heterobimetallic reaction center, this motif was not yet investigated for heterogeneous catalytic reduction of CO2. We herein aim at the characterization and advancement of [FeNi]- chalcogenides as heterogeneous photo- and electrocatalysts for the reduction of CO2 in a proof-of-principle study.