Põldme Nils, O'Reilly Laura, Fletcher Ian, Portoles Jose, Sazanovich Igor V, Towrie Michael, Long Conor, Vos Johannes G, Pryce Mary T, Gibson Elizabeth A
School of Natural and Environmental Science , Newcastle University , Newcastle upon Tyne , NE1 7RU , UK . Email:
School of Chemical Sciences , Dublin City University , Dublin 9 , Ireland . Email:
Chem Sci. 2018 Oct 4;10(1):99-112. doi: 10.1039/c8sc02575d. eCollection 2019 Jan 7.
A new approach to increasing the faradaic efficiency of dye-sensitised photocathodes for H evolution from water, using integrated photocatalysts, furnished with ester groups on the peripheral ligands, Ru(decb)(bpt)PdCl(HO) () and Ru(decb)(2,5-bpp)PtI(CHCN) (), (decb = 4,4'-diethylcarboxy-2,2'-bipyridine, bpp = 2,2':5',2''-terpyridine, bpt = 3,5-bis(2-pyridyl)-1,2,4-triazole) is described. Overall, |NiO is superior to previously reported photocathodes, producing photocurrent densities of 30-35 μA cm at an applied bias of -0.2 V Ag/AgCl over 1 hour of continuous white light irradiation, resulting in the generation of 0.41 μmol h cm of H with faradaic efficiencies of up to 90%. Furthermore, surface analysis of the photocathodes before and after photoelectrocatalysis revealed that the ruthenium bipyridyl chromophore and Pd catalytic centre () were photochemically stable, highlighting the benefits of the approach towards robust, hybrid solar-to-fuel devices.
描述了一种提高用于从水中析氢的染料敏化光阴极法拉第效率的新方法，该方法使用在周边配体上带有酯基的集成光催化剂Ru(decb)(bpt)PdCl(HO) ()和Ru(decb)(2,5 - bpp)PtI(CHCN) ()，(decb = 4,4'-二乙基羧基 - 2,2'-联吡啶，bpp = 2,2':5',2''-三联吡啶，bpt = 3,5 - 双(2 - 吡啶基)-1,2,4 - 三唑)。总体而言，|NiO优于先前报道的光阴极，在 - 0.2 V Ag/AgCl的外加偏压下，经过1小时连续白光照射，产生的光电流密度为30 - 35 μA cm，产生0.41 μmol h cm的H，法拉第效率高达90%。此外，光电催化前后光阴极的表面分析表明，钌联吡啶发色团和Pd催化中心()具有光化学稳定性，突出了该方法对于坚固的混合太阳能到燃料装置的益处。
