Years of research have demonstrated that the use of multiple components is essential to the development of a commercial photoelectrode to address specific bottlenecks,such as low charge separation and injection effici...Years of research have demonstrated that the use of multiple components is essential to the development of a commercial photoelectrode to address specific bottlenecks,such as low charge separation and injection efficiency,low carrier diffusion length and lifetime,and poor durability.A facile strategy for the synthesis of multilayered photoanodes from atomic-layer-deposited ultrathin films has enabled a new type of electrode architecture with a total multilayer thickness of 15–17 nm.We illustrate the advantages of this electrode architecture by using nanolayers to address different bottlenecks,thus producing a multilayer photoelectrode with improved interface kinetics and shorter electron transport path,as determined by interface analyses.The photocurrent density was twice that of the bare structure and reached a maximum of 33.3±2.1 mA cm^(−2) at 1.23 VRHE.An integrated overall water-splitting cell consisting of an electrocatalytic NiS cathode and Bi_(2)S_(3)/NiS/NiFeO/TiO_(2) photoanode was used for precious-metal-free seawater splitting at a cell voltage of 1.23 V without degradation.The results and root analyses suggest that the distinctive advantages of the electrode architecture,which are superior to those of bulk bottom-up core–shell and hierarchical architectures,originate from the high density of active sites and nanometer-scale layer thickness,which enhance the suitability for interface-oriented energy conversion processes.展开更多
基金We are grateful to Prof.Hong H.Lee for the valuable and in-depth conversations related to this study.This study was financially supported by the National Research Foundation of Korea(2021R1A2C1012735)Open access funding provided by Shanghai Jiao Tong University
文摘Years of research have demonstrated that the use of multiple components is essential to the development of a commercial photoelectrode to address specific bottlenecks,such as low charge separation and injection efficiency,low carrier diffusion length and lifetime,and poor durability.A facile strategy for the synthesis of multilayered photoanodes from atomic-layer-deposited ultrathin films has enabled a new type of electrode architecture with a total multilayer thickness of 15–17 nm.We illustrate the advantages of this electrode architecture by using nanolayers to address different bottlenecks,thus producing a multilayer photoelectrode with improved interface kinetics and shorter electron transport path,as determined by interface analyses.The photocurrent density was twice that of the bare structure and reached a maximum of 33.3±2.1 mA cm^(−2) at 1.23 VRHE.An integrated overall water-splitting cell consisting of an electrocatalytic NiS cathode and Bi_(2)S_(3)/NiS/NiFeO/TiO_(2) photoanode was used for precious-metal-free seawater splitting at a cell voltage of 1.23 V without degradation.The results and root analyses suggest that the distinctive advantages of the electrode architecture,which are superior to those of bulk bottom-up core–shell and hierarchical architectures,originate from the high density of active sites and nanometer-scale layer thickness,which enhance the suitability for interface-oriented energy conversion processes.
