Three molecular photosensitizers (PSs) with carboxylic acid anchors for attachment to platinized titanium dioxide nanoparticles were studied for light‐driven hydrogen production from a fully aqueous medium with ascorbic acid (AA) as the sacrificial electron donor. Two zinc(II) porphyrin (ZnP)‐based PSs were used to examine the effect of panchromatic sensitization on the photocatalytic H₂ generation. A dyad molecular design was used to construct a difluoro boron‐dipyrromethene (bodipy)‐conjugated ZnP PS (ZnP‐dyad), whereas the other one featured an electron‐donating diarylamino moiety (YD2‐o‐C8). To probe the use of the ZnP scaffold in this particular energy conversion process, an organic PS without the ZnP moiety (Bodipy‐dye) was also synthesized for comparison. Ultrafast transient absorption spectroscopy was adopted to map out the energy transfer processes occurring in the dyad and to establish the bodipy‐based antenna effect. In particular, the systems with YD2‐o‐C8 and ZnP‐dyad achieved a remarkable initial activity for the production of H₂ with an initial turnover frequency (TOF_i) higher than 300 h⁻¹ under white light irradiation. The use of ZnP PSs in dye‐sensitized photocatalysis for the H₂ evolution reaction in this study indicated the importance of the panchromatic sensitization capability for the development of light absorbing PSs.

中文翻译：

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ZnII卟啉基光敏剂的全色敏化，用于光驱动制氢

研究了三种具有羧酸锚的分子光敏剂（PSs）与铂化的二氧化钛纳米颗粒的附着力，该光敏剂是从全水介质中以抗坏血酸（AA）作为牺牲电子供体的光驱动制氢。两种基于卟啉锌（II）的锌（II）用于检查全色敏化对光催化H ₂生成的影响。使用二元体分子设计来构建二氟硼二吡咯亚甲基（bodipy）共轭的ZnP PS（ZnP-dyad），而另一种分子具有供电子的二芳基氨基部分（YD2- o‐C8）。为了探索在特定的能量转换过程中使用ZnP支架的方法，还合成了不含ZnP部分的有机PS（Bodipy-dye）用于比较。采用超快速瞬态吸收光谱法来确定在二倍体中发生的能量转移过程，并建立基于身体的天线效应。特别是，在白光照射下，具有YD2 - o -C8和ZnP-dyad的系统在产生H _2方面具有显着的初始活性，其初始转换频率（TOF _i）高于300 h ^-1。ZnP PS在H _2的染料敏化光催化中的用途 这项研究中的进化反应表明，全色敏化能力对于光吸收PS的发展很重要。