Liu Qinzhe, Huang Yuyan, Ye Yu-Xin
Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, LIFM-Lehn Institute of Functional Materials, School of Chemistry, IGCME-Institute of Green Chemistry and Molecular Engineering, Sun Yat-sen University, Guangzhou 510275, China.
School of Chemical Engineering and Technology, IGCME, Sun Yat-sen University, Zhuhai 519082, China.
Materials (Basel). 2024 Jun 3;17(11):2709. doi: 10.3390/ma17112709.
The visible-light-driven photocatalytic production of hydrogen peroxide (HO) is currently an emerging approach for transforming solar energy into chemical energy. In general, the photocatalytic process for producing HO includes two pathways: the water oxidation reaction (WOR) and the oxygen reduction reaction (ORR). However, the utilization efficiency of ORR surpasses that of WOR, leading to a discrepancy with the low oxygen levels in natural water and thereby impeding their practical application. Herein, we report a novel donor-bridge-acceptor (D-B-A) organic polymer conjugated by the Sonogashira-Hagihara coupling reaction with tetraphenylethene (TPE) units as the electron donors, acetylene (A) as the connectors and pyrene (P) moieties as the electron acceptors. Notably, the resulting TPE-A-P exhibits a remarkable solar-to-chemical conversion of 1.65% and a high BET-specific surface area (1132 m·g). Furthermore, even under anaerobic conditions, it demonstrates an impressive HO photosynthetic efficiency of 1770 μmol g h, exceeding the vast majority of previously reported photosynthetic systems of HO. The outstanding performance is attributed to the effective separation of electrons and holes, along with the presence of sufficient reaction sites facilitated by the incorporation of alkynyl electronic bridges. This protocol presents a successful method for generating HO via a water oxidation reaction, signifying a significant advancement towards practical applications in the natural environment.
可见光驱动的光催化过氧化氢（HO）生产目前是一种将太阳能转化为化学能的新兴方法。一般来说，生产HO的光催化过程包括两条途径：水氧化反应（WOR）和氧还原反应（ORR）。然而，ORR的利用效率超过了WOR，导致与天然水中的低氧水平存在差异，从而阻碍了它们的实际应用。在此，我们报道了一种新型的供体-桥-受体（D-B-A）有机聚合物，它通过Sonogashira-Hagihara偶联反应共轭而成，以四苯乙烯（TPE）单元作为电子供体，乙炔（A）作为连接体，芘（P）部分作为电子受体。值得注意的是，所得的TPE-A-P表现出1.65%的显著太阳能到化学能的转化率和高的BET比表面积（1132 m·g）。此外，即使在厌氧条件下，它也表现出令人印象深刻的HO光合效率，为1770 μmol g h，超过了绝大多数先前报道的HO光合系统。这种优异的性能归因于电子和空穴的有效分离，以及通过引入炔基电子桥促进了足够反应位点的存在。该方案提出了一种通过水氧化反应生成HO的成功方法，标志着在自然环境中的实际应用取得了重大进展。
