材料科学
光电流
分解水
催化作用
化学工程
氧化物
石墨氮化碳
可逆氢电极
电化学
法拉第效率
氮化碳
量子产额
氮化物
电解质
石墨烯
光催化
电子转移
光化学
电极
碳纤维
析氧
纳米技术
图层(电子)
工作电极
化学
物理化学
复合数
光电子学
复合材料
荧光
冶金
工程类
量子力学
生物化学
物理
作者
Neeta Karjule,Chanderpratap Singh,Jesús Barrio,Jonathan Tzadikov,Itamar Liberman,Michael Volokh,Emilio Palomares,Idan Hod,Menny Shalom
标识
DOI:10.1002/adfm.202101724
摘要
Abstract Carbon nitrides (CN) have emerged as promising photoanode materials for water‐splitting photoelectrochemical cells (PECs). However, their poor charge separation and transfer properties, together with slow water‐oxidation kinetics, have resulted in low PEC activity and instability, which strongly impede their further development. In this work, these limitations are addressed by optimizing the charge separation and transfer process. To this end, a nickel–iron based metal‐organic framework, Ni/Fe‐MIL‐53, is deposited, that acts as an oxygen evolution pre‐catalyst within the CN layer and incorporate reduced graphene oxide as an electron acceptor. Upon electrochemical activation, a uniform distribution of highly active oxygen evolution reaction (OER) catalysts is obtained on the porous CN surface. Detailed mechanistic studies reveal excellent hole extraction properties with high OER catalytic activity (83% faradaic efficiency) and long‐term stability, up to 35 h. These results indicate that the decrease in performance is mainly due to the slow leaching of the catalyst from the CN layer. The CN photoanode exhibits a reproducible photocurrent density of 472 ± 20 µA cm −2 at 1.23 V versus reversible hydrogen electrode (RHE) in 0.1 m KOH, an exceptionally low onset potential of ≈0.034 V versus RHE, and high external quantum yield.
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