TY - JOUR
T1 - Pseudomorphic Transformation of Interpenetrated Prussian Blue Analogs into Defective Nickel Iron Selenides for Enhanced Electrochemical and Photo-Electrochemical Water Splitting
AU - Yilmaz, Gamze
AU - Tan, Chuan Fu
AU - Lim, Yee Fun
AU - Ho, Ghim Wei
N1 - Funding Information:
This work was supported by Ministry of Education (MOE), Singapore under R-263-000-C85-112, and R-263-000-D08-114 grants.
Publisher Copyright:
© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
Copyright:
Copyright 2019 Elsevier B.V., All rights reserved.
PY - 2019/1/3
Y1 - 2019/1/3
N2 - A significant methodology gap remains in the construction of advanced electrocatalysts, which has collaborative defective functionalities and structural coherence that maximizes electrochemical redox activity, electrical conductivity, and mass transport characteristics. Here, a coordinative self-templated pseudomorphic transformation of an interpenetrated metal organic compound network is conceptualized into a defect-rich porous framework that delivers highly reactive and durable photo(electro)chemical energy conversion functionalities. The coordinative-template approach enables previously inaccessible synthesis routes to rationally accomplish an interconnected porous conductive network at the microscopic level, while exposing copious unsaturated reactive sites at the atomic level without electronic or structural integrity trade-offs. Consequently, porous framework, interconnected motifs, and engineered defects endow remarkable electrocatalytic hydrogen evolution reaction and oxygen evolution reaction activity due to intrinsically improved turnover frequency, electrochemical surface area, and charge transfer. Moreover, when the hybrid is coupled with a silicon photocathode for solar-driven water splitting, it enables photon assisted redox reactions, improved charge separation, and enhanced carrier transport via the built-in heterojunction and additive co-catalyst functionality, leading to a promising photo(electro)chemical hydrogen generation performance. This work signifies a viable and generic approach to prepare other functional interconnected metal organic coordinated compounds, which can be exploited for diverse energy storage, conversion, or environmental applications.
AB - A significant methodology gap remains in the construction of advanced electrocatalysts, which has collaborative defective functionalities and structural coherence that maximizes electrochemical redox activity, electrical conductivity, and mass transport characteristics. Here, a coordinative self-templated pseudomorphic transformation of an interpenetrated metal organic compound network is conceptualized into a defect-rich porous framework that delivers highly reactive and durable photo(electro)chemical energy conversion functionalities. The coordinative-template approach enables previously inaccessible synthesis routes to rationally accomplish an interconnected porous conductive network at the microscopic level, while exposing copious unsaturated reactive sites at the atomic level without electronic or structural integrity trade-offs. Consequently, porous framework, interconnected motifs, and engineered defects endow remarkable electrocatalytic hydrogen evolution reaction and oxygen evolution reaction activity due to intrinsically improved turnover frequency, electrochemical surface area, and charge transfer. Moreover, when the hybrid is coupled with a silicon photocathode for solar-driven water splitting, it enables photon assisted redox reactions, improved charge separation, and enhanced carrier transport via the built-in heterojunction and additive co-catalyst functionality, leading to a promising photo(electro)chemical hydrogen generation performance. This work signifies a viable and generic approach to prepare other functional interconnected metal organic coordinated compounds, which can be exploited for diverse energy storage, conversion, or environmental applications.
KW - electrochemical and PEC water splitting
KW - metal-organic
KW - MOF
KW - PBA
UR - http://www.scopus.com/inward/record.url?scp=85056154122&partnerID=8YFLogxK
U2 - 10.1002/aenm.201802983
DO - 10.1002/aenm.201802983
M3 - Article
AN - SCOPUS:85056154122
VL - 9
JO - Advanced Energy Materials
JF - Advanced Energy Materials
SN - 1614-6840
IS - 1
M1 - 1802983
ER -