Theoretical-level insights on the molecular structures and LiCl dopant of carbon nitride single crystals for solar-driven overall water splitting

Li，Bingwen1; Tan，Yueyang3; Wang，Wanting2; Sun，Zongzhao2; Wang，Xinfang1; Huang，Limin3

2025-03-01

10.1016/j.seppur.2024.129640

Separation and Purification Technology   影响因子和分区

1383-5866

1873-3794

Addressing energy and environmental challenges requires sustainable technologies like photocatalytic overall water splitting (OWS) using graphitic carbon nitride (GCN). This study investigates the molecular structures and LiCl doping effects in GCN variants-poly(triazine imide) intercalated with LiCl (PTI/LiCl), and heptazine-based crystalline GCN (HCCN)-to understand their suitability for OWS. Experimental results show that PTI/LiCl exhibits superior OWS activity, producing 802.3 μmol h g of H₂ and 395.6 μmol h g of O₂, due to its active planes and favorable electron transfer. In contrast, HCCN shows high H₂ production but no O₂ release. Density functional theory calculations reveal that triazine structures are more favorable for oxygen evolution reaction (OER) while heptazine structures excel in hydrogen evolution reaction (HER). LiCl doping can enhance OWS performance by improving electronic conductivity and reducing reaction activation energy. The results encourage the combination of triazine and heptazine structures with LiCl doping to optimize OWS, offering a theoretical basis for designing efficient GCN-based photocatalysts.

Carbon nitride Heptazine structure LiCl doping Photocatalytic overall water splitting Triazine structure

英语

其他

2-s2.0-85203645298

Scopus

1.Shandong Key Laboratory of Biophysics,Institute of Biophysics,College of Chemistry and Chemical Engineering,Dezhou University,Dezhou,253023,China
2.College of Chemistry and Chemical Engineering,Linyi University,Linyi,276000,China
3.Department of Chemistry,Southern University of Science and Technology,Shenzhen,518055,China

Li，Bingwen,Tan，Yueyang,Wang，Wanting,et al. Theoretical-level insights on the molecular structures and LiCl dopant of carbon nitride single crystals for solar-driven overall water splitting[J]. Separation and Purification Technology,2025,355.

Li，Bingwen,Tan，Yueyang,Wang，Wanting,Sun，Zongzhao,Wang，Xinfang,&Huang，Limin.(2025).Theoretical-level insights on the molecular structures and LiCl dopant of carbon nitride single crystals for solar-driven overall water splitting.Separation and Purification Technology,355.

Li，Bingwen,et al."Theoretical-level insights on the molecular structures and LiCl dopant of carbon nitride single crystals for solar-driven overall water splitting".Separation and Purification Technology 355(2025).