Fang Zhengsong, Li Yuan, Li Jing, Shu Chenhao, Zhong Linfeng, Lu Shaolin, Mo Chunshao, Yang Meijia, Yu Dingshan
Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education, School of Chemistry, Sun Yat-Sen University, Guangzhou, 510275, China.
Angew Chem Int Ed Engl. 2021 Aug 2;60(32):17615-17621. doi: 10.1002/anie.202104790. Epub 2021 Jun 30.
We report facile synthesis of low-band-gap mesoporous C N particles and their use as responsive bifunctional oxygen catalysts for visible-light-sensitive (VLS) rechargeable Zn-air battery (RZAB) and polymer-air battery (RPAB). Compared to widely studied g-C N , C N shows a smaller band gap of 1.99 eV, with a larger photocurrent response, and it can function as visible-light-harvesting antenna and bifunctional oxygen reduction/evolution (ORR/OER) catalysts, enabling effective photocoupling to tune oxygen catalysis. The C N-enabled VLS-RZAB displays a low charge voltage of 1.35 V under visible light, which is below the theoretical RZAB voltage of 1.65 V, corresponding to a high energy efficiency of 97.78 %. Pairing a C N cathode with a polymer anode also endows an VLS-RPAB with light-boosted charge performance. It is revealed that the ORR and OER active sites in C N are separate carbon sites near pyrazine-nitrogen atoms and photogenerated energetic holes can activate OER for improved reaction kinetics.