Photocatalytic Overall Water Splitting Under Visible Light Enabled by a Particulate Conjugated Polymer Loaded with Palladium and Iridium.
Photocatalytic Overall Water Splitting Under Visible Light Enabled by a Particulate Conjugated Polymer Loaded with Palladium and Iridium.
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DOI：
10.1002/anie.202201299
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发表时间：
2022-06-27
影响因子：
16.6
通讯作者：
Sprick, Reiner Sebastian
中科院分区：
文献类型：
--
作者：
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
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。大多数研究报道了牺牲电子供体制氢，这不适用于大规模的氢能生产。本研究表明，负载钯/氧化铱的二苯并[b，d]噻吩砜（P10）均聚物在系统稳定后的较长时间内（bbb60小时）促进了整体水分解，产生化学量的H2和O2。这些结果表明，当负载合适的共催化剂时，共轭聚合物可以作为单组分光催化系统进行整体水分解，尽管目前活性较低。瞬态光谱分析表明，IrO2共催化剂在水分解所需的电荷分离状态的产生中起着重要作用，并有证据表明，IrO2共催化剂具有快速空穴转移。负载Pd/IrO2的聚（二苯并[b，d]噻吩砜）在系统稳定后的较长时间内促进了化学计量的整体水分解，尽管目前活性较低。该研究证明了共催化剂对聚合物光催化剂的重要性，并通过瞬态吸收光谱对结果进行了验证。
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 H2 and O2 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 IrO2 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. Poly(dibenzo[b,d]thiophene sulfone) loaded with Pd/IrO2 facilitates stoichiometric overall water splitting for an extended period after the system stabilized, albeit currently with low activities. The study demonstrates the importance of co‐catalysts for polymer photoatalysts and results were rationalized by transient absorption spectroscopy.
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影响因子：
41.2
作者：
Kosco J;Bidwell M;Cha H;Martin T;Howells CT;Sachs M;Anjum DH;Gonzalez Lopez S;Zou L;Wadsworth A;Zhang W;Zhang L;Tellam J;Sougrat R;Laquai F;DeLongchamp DM;Durrant JR;McCulloch I
通讯作者：
McCulloch I
影响因子：
15
作者：
Frame, F. Andrew;Townsend, Troy K.;Osterloh, Frank E.
通讯作者：
Osterloh, Frank E.
影响因子：
8.4
作者：
Pan, Zhiming;Zheng, Yun;Wang, Xinchen
通讯作者：
Wang, Xinchen
影响因子：
3.7
作者：
Lee, Yumin;Kang, Minkyung;Kim, Myung Hwa
通讯作者：
Kim, Myung Hwa
DOI：
10.1021/acs.jpclett.1c03073
发表时间：
2021-11-11
期刊：
The journal of physical chemistry letters
影响因子：
--
作者：
Piercy VL;Saeed KH;Prentice AW;Neri G;Li C;Gardner AM;Bai Y;Sprick RS;Sazanovich IV;Cooper AI;Rosseinsky MJ;Zwijnenburg MA;Cowan AJ
通讯作者：
Cowan AJ