Department of Chemistry, Graduate School of Science, Kobe University, Kobe, Japan.
Molecular Photoscience Research Center, Kobe University, Kobe, Japan.
Nat Chem. 2023 Jun;15(6):794-802. doi: 10.1038/s41557-023-01157-6. Epub 2023 Mar 23.
Increasing levels of CO in the atmosphere is a problem that must be urgently resolved if the rise in current global temperatures is to be slowed. Chemically reducing CO into compounds that are useful as energy sources and carbon-based materials could be helpful in this regard. However, for the CO reduction reaction (CORR) to be operational on a global scale, the catalyst system must: use only renewable energy, be built from abundantly available elements and not require high-energy reactants. Although light is an attractive renewable energy source, most existing CORR methods use electricity and many of the catalysts used are based on rare heavy metals. Here we present a transition-metal-free catalyst system that uses an organohydride catalyst based on benzimidazoline for the CORR that can be regenerated using a carbazole photosensitizer and visible light. The system is capable of producing formate with a turnover number exceeding 8,000 and generates no other reduced products (such as H and CO).
大气中 CO 含量的增加是一个必须紧急解决的问题，如果要减缓当前全球气温的上升。将 CO 通过化学反应转化为有用的能源化合物和碳基材料，可能对此有所帮助。然而，为了使 CO 还原反应（CORR）在全球范围内运行，催化剂系统必须：仅使用可再生能源、由丰富的元素构建，且不需要高能反应物。尽管光作为一种有吸引力的可再生能源，但大多数现有的 CORR 方法都使用电力，并且许多使用的催化剂都是基于稀有重金属。在这里，我们提出了一种无过渡金属的催化剂系统，该系统使用基于苯并咪唑啉的有机氢化物催化剂进行 CORR，可使用咔唑敏化剂和可见光进行再生。该系统能够以超过 8000 的转化率生成甲酸盐，且不会生成其他还原产物（如 H 和 CO）。
