Coordination Chemistry Engineered Polymeric Carbon Nitride Photoanode with Ultralow Onset Potential for Water Splitting. Issue 32 (29th June 2022)

• Record Type: Journal Article
• Authors: Fan, Xiangqian; Wang, Zhiliang; Lin, Tongen; Du, Du; Xiao, Mu; Chen, Peng; Monny, Sabiha Akter; Huang, Hengming; Lyu, Miaoqiang; Lu, Mingyuan; Wang, Lianzhou
• Is Part Of: Angewandte Chemie international edition. Volume 61:Issue 32(2022)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2022-06-29
• Subjects: Carbon Nitride -- Coordination Bonds -- Interfacial Engineering -- Photoanode -- Water Splitting; Chemistry -- Periodicals; 540
• DOI: 10.1002/anie.202204407
• Languages: English
• ISSNs: 1433-7851

Abstract

Abstract: Construction of an intimate film/substrate interface is of great importance for a photoelectrode to achieve efficient photoelectrochemical performance. Inspired by coordination chemistry, a polymeric carbon nitride (PCN) film is intimately grown on a Ti‐coated substrate by an in situ thermal condensation process. The as‐prepared PCN photoanode exhibits a record low onset potential ( E onset ) of −0.38 V versus the reversible hydrogen electrode (RHE) and a decent photocurrent density of 242 μA cm −2 at 1.23 VRHE for water splitting. Detailed characterization confirms that the origin of the ultralow onset potential is mainly attributed to the substantially reduced interfacial resistance between the Ti‐coated substrate and the PCN film benefitting from the constructed interfacial sp 2 N→Ti coordination bonds. For the first time, the ultralow onset potential enables the PCN photoanode to drive water splitting without external bias with a stable photocurrent density of ≈9 μA cm −2 up to 1 hour. Abstract : By engineering the film/substrate interface via coordination chemistry, a polymeric carbon nitride (PCN) photoanode featuring intimate contact between the PCN film and the titanium‐coated fluorine‐doped SnO2 (FTO) substrate was derived. Benefitting from the substantially reduced interfacial resistance credited by the strong coordination interaction, a record ultralow onset potential which enables unbiased water splitting is achieved.