title: Development of a Dinitrosyl Iron Complex Molecular Catalyst into a Hydrogen Evolution Cathode.
abstract: Despite extensive efforts, the electrocatalytic reduction of water using homogeneous/heterogeneous Fe, Co, Ni, Cu, W, and Mo complexes remains challenging because of issues involving the development of efficient, recyclable, stable, and aqueous-compatible catalysts. In this study, evolution of the de novo designed dinitrosyl iron complex DNIC-PMDTA from a molecular catalyst into a solid-state hydrogen evolution cathode, considering all the parameters to fulfill the electronic and structural requirements of each step of the catalytic cycle, is demonstrated. DNIC-PMDTA reveals electrocatalytic reduction of water at neutral and basic media, whereas its deposit on electrode preserves exceptional longevity, 139 h. This discovery will initiate a systematic study on the assembly of [Fe(NO)2] motif into current collector for mass production of H2, whereas the efficiency remains tailored by its molecular precursor [(L)Fe(NO)2].
authors.affiliation: Department of Chemistry, National Tsing Hua University, No. 101, Section 2, Guangfu Rd., Hsinchu, 30013 (Taiwan). d9623817@oz.nthu.edu.tw.
authors.forename: Tzung-Wen
authors.initials: TW
authors.lastname: Chiou
authors.affiliation: Department of Chemistry, Chung Yuan Christian University, No. 200, Chung Pei Rd. Taoyuan, 32023 (Taiwan). TTLu@cycu.edu.tw.
authors.forename: Tsai-Te
authors.initials: TT
authors.lastname: Lu
authors.affiliation: Department of Chemistry, National Tsing Hua University, No. 101, Section 2, Guangfu Rd., Hsinchu, 30013 (Taiwan).
authors.forename: Ying-Hao
authors.initials: YH
authors.lastname: Wu
authors.affiliation: Department of Chemistry, National Tsing Hua University, No. 101, Section 2, Guangfu Rd., Hsinchu, 30013 (Taiwan).
authors.forename: Yi-Ju
authors.initials: YJ
authors.lastname: Yu
authors.affiliation: Department of Chemistry, National Tsing Hua University, No. 101, Section 2, Guangfu Rd., Hsinchu, 30013 (Taiwan).
authors.forename: Li-Kang
authors.initials: LK
authors.lastname: Chu
authors.affiliation: Department of Chemistry, National Tsing Hua University, No. 101, Section 2, Guangfu Rd., Hsinchu, 30013 (Taiwan). wfliaw@mx.nthu.edu.tw.
authors.forename: Wen-Feng
authors.initials: WF
authors.lastname: Liaw
keywords: electrocatalysis; hydrogen; iron; nitric oxide; water reduction