Bai Yang, Li Chao, Liu Lunjie, Yamaguchi Yuichi, Bahri Mounib, Yang Haofan, Gardner Adrian, Zwijnenburg Martijn A, Browning Nigel D, Cowan Alexander J, Kudo Akihiko, Cooper Andrew I, Sprick Reiner Sebastian
Materials Innovation Factory & Department of Chemistry, University of Liverpool, Liverpool, L7 3NY, UK.
Institute of Materials Research and Engineering, Agency for Science Technology and Research, Singapore, 138634, Singapore.
Angew Chem Int Ed Engl. 2022 Jun 27;61(26):e202201299. doi: 10.1002/anie.202201299. Epub 2022 Apr 26.
Polymer photocatalysts have received growing attention in recent years for photocatalytic hydrogen production from water. Most studies report hydrogen production with sacrificial electron donors, which is unsuitable for large-scale hydrogen energy production. Here we show that the palladium/iridium oxide-loaded homopolymer of dibenzo[b,d]thiophene sulfone (P10) facilitates overall water splitting to produce stoichiometric amounts of H and O for an extended period (>60 hours) after the system stabilized. These results demonstrate that conjugated polymers can act as single component photocatalytic systems for overall water splitting when loaded with suitable co-catalysts, albeit currently with low activities. Transient spectroscopy shows that the IrO co-catalyst plays an important role in the generation of the charge separated state required for water splitting, with evidence for fast hole transfer to the co-catalyst.
近年来,聚合物光催化剂在光催化水制氢方面受到越来越多的关注。大多数研究报道的是使用牺牲电子供体进行产氢,这不适用于大规模氢能生产。在此,我们展示了负载钯/氧化铱的二苯并[b,d]噻吩砜均聚物(P10)在系统稳定后能够促进全水分解,长时间(>60小时)产生化学计量的氢气和氧气。这些结果表明,当负载合适的助催化剂时,共轭聚合物可以作为全水分解的单组分光催化体系,尽管目前活性较低。瞬态光谱表明,IrO助催化剂在产生水分解所需的电荷分离态中起重要作用,有证据表明空穴快速转移到助催化剂上。