Department of Chemistry, University of Rochester, 120 Trustee Rd., Rochester, NY 14627-0216, USA.
Department of Chemical Sciences, University of Naples Federico II, Complesso Universitario Monte S. Angelo, via Cintia 45, 80126 Naples, Italy.
J Inorg Biochem. 2022 May;230:111753. doi: 10.1016/j.jinorgbio.2022.111753. Epub 2022 Feb 8.
A system for visible light-driven hydrogen production from water is reported. This system makes use of a synthetic mini-enzyme known as a mimochrome (CoMC6a) consisting of a cobalt deuteroporphyrin and two attached peptides as a catalyst, [Ru(bpy)] (bpy = 2,2'-bipyridine) as a photosensitizer, and ascorbic acid as a sacrificial electron donor. The system achieves turnover numbers (TONs) up to 10,000 with respect to catalyst and optimal activity at pH 7. Comparison with related systems shows that CoMC6a maintains the advantages of biomolecular catalysts, while exceeding other cobalt porphyrins in terms of total TON and longevity of catalysis. Herein, we lay groundwork for future study, where the synthetic nature of CoMC6*a will provide a unique opportunity to tailor proton reduction chemistry and expand to new reactivity.
本文报道了一种可见光驱动的水制氢系统。该系统利用一种名为拟色团（CoMC6a）的合成微型酶作为催化剂，其由钴原卟啉和两个附着的肽组成，[Ru(bpy)]（bpy=2,2'-联吡啶）作为光敏剂，抗坏血酸作为牺牲电子供体。该系统的催化剂转化率（TON）高达 10000，在 pH 7 时具有最佳活性。与相关系统的比较表明，CoMC6a 保持了生物分子催化剂的优势，同时在总 TON 和催化寿命方面超过了其他钴卟啉。本文为进一步研究奠定了基础，其中 CoMC6*a 的合成性质将为调整质子还原化学和拓展新反应性提供独特的机会。
