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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Evaluation of bis-cyclometalated alkynylgold(III) sensitizers for water photoreduction to hydrogen
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Evaluation of bis-cyclometalated alkynylgold(III) sensitizers for water photoreduction to hydrogen

机译：双环金属化炔金（III）敏化剂对水光还原成氢的评价

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Well-defined gold sensitizers for hydrogen production from water remain extremely rare despite decades of interest, and are currently limited to systems based on ruthenium, iridium or platinum complexes. This report details the synthesis and characterization of a series of neutral cyclometalated gold(III) complexes of the type [(RC<^>N<^>CR)Au(C C R')] (R = H or tert-butyl group; R' = aryl groups) that have been found to be good candidates to function as harvesting materials in light-induced electron transfer reactions. We established the efficacy of systems with these gold(III) complexes as photosensitizers (PSs) in the production of renewable hydrogen in the presence of [Co(2,2'-bipyridine)(3)] Cl-2 or [Rh(4,4'-di-tert-butyl-2,2'-bipyridine) (3)](PF6)(3) as a H-2-evolved catalyst and triethanolamine (TEOA) as a sacrificial electron donor in acetone-water solution. All complexes are active, and there is a more than threefold increase over other candidates in photocatalytic H-2 generation activity. Under the optimal reaction conditions, hydrogen evolution took place through a photochemical route with the highest efficiency and with a turnover number (TON) of up to 1441.5 relative to the sensitizer over 24 hours. In the initial photochemical path, the reductive quenching of the excited gold(III) complex by TEOA due to the latter's greater concentration in the system followed by electron transfer to the catalyst species is proposed to be the dominant mechanism. A photo-to-H-2 quantum yield of approximately 13.7% was attained when illuminated with monochromatic light of 400 nm. Such gold(III) complexes have demonstrated significant utility in solar-to-hydrogen reactions and thus represent a new effective class of light-harvesting materials. These results open possibilities for pursuing more efficient photosensitizers featuring gold(III) complexes in photocatalytic solar energy conversion.
机译：尽管数十年来引起人们的关注，但用于水生产氢气的明确定义的金敏化剂仍然极为稀少，并且目前仅限于基于钌，铱或铂络合物的系统。该报告详细描述了[[RC ^ N ^ NCR] Au（CC R'）]（R = H或叔丁基; R = H或叔丁基）的一系列中性环金属化金（III）配合物的合成和表征。已发现R'=芳基）是在光诱导的电子转移反应中充当收集材料的良好候选者。我们建立了在[Co（2,2'-联吡啶）（3）] Cl-2或[Rh（4）存在下，将这些金（III）络合物作为光敏剂（PSs）在可再生氢生产中的功效。 ，4'-二叔丁基-2,2'-联吡啶）（3）]（PF6）（3）作为H-2-演化催化剂，三乙醇胺（TEOA）作为牺牲电子给体在丙酮水溶液中。所有复合物均具有活性，并且在光催化H-2生成活性方面比其他候选化合物增加三倍以上。在最佳反应条件下，相对于敏化剂，在24小时内通过光化学途径以最高的效率和高达1441.5的周转数（TON）析氢。在最初的光化学路径中，TEOA对激发的金（III）络合物的还原猝灭是主要机理，这是由于TEOA在系统中的浓度较高，随后电子转移至催化剂物质。当用400 nm的单色光照射时，H-2的光子量子产率约为13.7％。此类金（III）配合物在太阳能与氢的反应中已显示出显着的实用性，因此代表了一种新型的有效集光材料。这些结果为在光催化太阳能转化中追求更高效的以金（III）配合物为特征的光敏剂提供了可能性。

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