Work

Homogeneous electrocatalytic hydrogen evolution by a N2P2Fe(II) complex: Structural characterization of iron-hydride intermediate

Year: 2024

Type: article

Abstract: Development of efficient earth-abundant molecular catalysts for hydrogen evolution is an area of active research for replacing platinum as the preeminent catalyst in hydrogen evolution reaction. [FeFe] hydrogenases exhibit remarkable hydrogen evolution performance, which indicates that earth-abundant iron is the most attractive candidate for development of molecular catalysts. Inspired by [FeFe] hydrogenase, considerable progress has been made in the functional and structural modeling of mono-/di-nuclear molecular catalysts. However, the characterization of iron-hydride involved in the catalytic pathways have largely remained elusive. Herein, we report an air-stable mononuclear N 2 P 2 Fe(II) complex as a functional model of the distal iron in [FeFe] hydrogenase active site and the full characterization of iron-hydride intermediate. This N 2 P 2 Fe(II) complex is an active electrocatalyst for hydrogen evolution from mildly acidic solutions. Notably, the possible iron-hydride intermediate is synthesized by chemical hydride transfer strategy and structurally characterized, which provide insights into the catalytic pathway of the electrocatalytic hydrogen production. This work thus presents an example of iron-based molecular catalyst for hydrogen generation from mildly acid, and molecular structure of possible hydride intermediate.

Source: Journal of Molecular Structure

DOI: 10.1016/j.molstruc.2024.141021

Authors: Danyang Huang, Bing He, Yipei Zhao, Mengqing Liu, Lianke Wang

Language: English

Topic: Metalloenzymes and iron-sulfur proteins

Subfield: Renewable Energy, Sustainability and the Environment

Field: Energy

Domain: Physical Sciences

Open Access status: hybrid

Estimated APC paid: $3,570

Funders: National Natural Science Foundation of China, Anhui University

Award: 非血红素铁-硫配合物催化氧还原反应的性能和机制研究