Breaking Platinum Nanoparticles to Single‐Atomic Pt‐C4 Co‐catalysts for Enhanced Solar‐to‐Hydrogen Conversion. Issue 5 (26th November 2020)

• Record Type: Journal Article
• Authors: Yan, Junqing; Ji, Yujin; Batmunkh, Munkhbayar; An, Pengfei; Zhang, Jing; Fu, Yang; Jia, Baohua; Li, Youyong; Liu, Shengzhong; Ye, Jinhua; Ma, Tianyi
• Is Part Of: Angewandte Chemie international edition. Volume 60:Issue 5(2021)
• Page Start: 2541
• Page End: 2547
• Publication Date: 2020-11-26
• Subjects: co-catalyst -- H2 generation -- photocatalysis -- single-atom doping -- water splitting; Chemistry -- Periodicals; 540
• DOI: 10.1002/anie.202013206
• Languages: English
• ISSNs: 1433-7851

Abstract

Abstract: Effective transfer and utilization of the photogenerated electrons are a key factor for achieving highly efficient H2 generation by photocatalytic water splitting. Apart from the activity of the co‐catalyst, the interface between the co‐catalyst and semiconductor is of particular importance. Guided by DFT calculations, single‐atom (SA) Pt doped carbon nitride (CN) is successfully synthesized for use as the co‐catalyst to the semiconducting CuS. The catalyst system (Pt1‐CN@CuS) exhibits an enhanced photocatalytic performance for water splitting with a H2 production rate of 25.4 μmol h −1 and an apparent quantum yield (AQY) of 50.3 % under the illumination of LED‐530. Solar‐to‐hydrogen (STH) conversion efficiency is calculated to be 0.5 % under AM 1.5 illumination. This is the very first investigation of SA as the co‐catalyst, which decreases the overpotential of CN during the water splitting and lowers interfacial resistance of the catalyst/co‐catalyst and co‐catalyst/electrolyte. Abstract : The single site of Pt‐C4 in nitrogen‐doped carbon (Pt1‐CN) is reported by a high‐temperature calcination process. It features fast carrier migration with low resistance across the catalyst–solution interface. Benefiting from above merits and the tight contact between CuS semiconductor and Pt1‐CN, the Pt1‐CN@CuS gives a photocatalytic H2 generation rate of 25.4 μmol h −1 with an AQY of 50.3 % under the illumination of LED‐530.