An Daehyeon, Nishioka Shunta, Yasuda Shuhei, Kanazawa Tomoki, Kamakura Yoshinobu, Yokoi Toshiyuki, Nozawa Shunsuke, Maeda Kazuhiko
Department of Chemistry, School of Science, Tokyo Institute of Technology, 2-12-1-NE-2 Ookayama, Meguro-ku, Tokyo, 152-8550, Japan.
Nanospace Catalysis Unit, Institute of Innovative Research, Tokyo Institute of Technology, 4259 Nagatsuta-cho, Midori-ku, Yokohama, 226-8503, Japan.
Angew Chem Int Ed Engl. 2022 Jun 27;61(26):e202204948. doi: 10.1002/anie.202204948. Epub 2022 May 12.
Photocatalytic conversion of CO into transportable fuels such as formic acid (HCOOH) under sunlight is an attractive solution to the shortage of energy and carbon resources as well as to the increase in Earth's atmospheric CO concentration. The use of abundant elements as the components of a photocatalytic CO reduction system is important, and a solid catalyst that is active, recyclable, nontoxic, and inexpensive is strongly demanded. Here, we show that a widespread soil mineral, alpha-iron(III) oxyhydroxide (α-FeOOH; goethite), loaded onto an Al O support, functions as a recyclable catalyst for a photocatalytic CO reduction system under visible light (λ>400 nm) in the presence of a Ru photosensitizer and an electron donor. This system gave HCOOH as the main product with 80-90 % selectivity and an apparent quantum yield of 4.3 % at 460 nm, as confirmed by isotope tracer experiments with CO . The present work shows that the use of a proper support material is another method of catalyst activation toward the selective reduction of CO .
在阳光照射下，将CO光催化转化为可运输燃料（如甲酸，HCOOH），是解决能源和碳资源短缺以及地球大气中CO浓度增加问题的一种有吸引力的方法。使用丰富的元素作为光催化CO还原系统的组分很重要，并且强烈需要一种活性高、可回收、无毒且廉价的固体催化剂。在此，我们表明，负载在AlO载体上的一种广泛存在的土壤矿物α-氢氧化铁（α-FeOOH；针铁矿），在Ru光敏剂和电子供体存在下，在可见光（λ>400 nm）下作为光催化CO还原系统的可回收催化剂发挥作用。通过用CO进行同位素示踪实验证实，该系统以HCOOH作为主要产物，选择性为80-90%，在460 nm处的表观量子产率为4.3%。目前的工作表明，使用合适的载体材料是使催化剂活化以选择性还原CO的另一种方法。
