Photocatalytic H2 Production with a Rhenium/Cobalt System in Water under Acidic Conditions
Photocatalytic H2 Production with a Rhenium/Cobalt System in Water under Acidic Conditions
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DOI：
10.1002/ejic.201100883
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发表时间：
2012-01-01
影响因子：
2.3
通讯作者：
Alberto, Roger
中科院分区：
文献类型：
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作者：
Guttentag, Miguel;Rodenberg, Alexander;Alberto, Roger
在光催化H-2形成中，叔胺通常用作牺牲电子供体，从而限制了水中研究的pH范围和游离质子的浓度。我们发现抗坏血酸能迅速还原淬灭[Re（CO）（3）（bipy）（py）]（+）（bpy = 2，2 '-bipyridine; py = pyridine）的激发态。与水还原催化剂（WRC）[Co{（DO）（DOH）pn}Br-2] [（DO）（DOH）pn =N-2，N-2 ′-丙二基双（2，3-丁二酮2-亚胺3-肟）]组合，该体系在酸性条件（pH范围2-6）下用光照射时产生H-2，并具有显著提高的转换数。此外，我们观察到，在与叔胺类似的系统，氧化的抗坏血酸（脱氢抗坏血酸）是缓慢的过程中，再还原的。
In photocatalytic H-2 formation, tertiary amines are commonly used as sacrificial electron donors, thereby limiting the pH range for studies in water and the concentration of free protons. We found that ascorbate rapidly reductively quenches the excited state of [Re(CO)(3)(bipy)(py)](+) (bpy = 2,2'- bipyridyl; py = pyridine). In combination with the water reduction catalyst (WRC) [Co{(DO)(DOH)pn}Br-2] [(DO)(DOH)pn =N-2,N-2'-propanediylbis(2,3-butanedione 2-imine 3-oxime)], this system produces H-2 upon irradiation with light under acidic conditions (pH range 2-6) and with significantly enhanced turnover numbers. Furthermore, we observed that, in contrast to similar systems with tertiary amines, oxidized ascorbate (dehydroascorbic acid) is slowly re-reduced during the course of photocatalysis.