Heterostructure Interface Engineering in CoP/FeP/CeO x with a Tailored d-Band Center for Promising Overall Water Splitting Electrocatalysis.

Autor: Song XZ; State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China., Zhang T; State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China., Zhao YH; State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China., Ni JC; State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China., Pan Y; Institute of Functional Textiles and Advanced Materials, College of Textiles and Clothing, State Key Laboratory of Bio-Fibers and Eco-Textiles, Qingdao University, Qingdao 266071, China., Tan Z; State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China., Wang XF; Key Laboratory of Materials Modification by Laser, Ion and Electron Beams, Ministry of Education, School of Physics, Dalian University of Technology, Dalian 116024, China.
Jazyk: angličtina
Zdroj: Inorganic chemistry [Inorg Chem] 2023 May 29; Vol. 62 (21), pp. 8347-8356. Date of Electronic Publication: 2023 May 18.
DOI: 10.1021/acs.inorgchem.3c00876
Abstrakt: Accomplishing a green hydrogen economy in reality through water spitting ultimately relies upon earth-abundant efficient electrocatalysts that can simultaneously accelerate the oxygen and hydrogen evolution reactions (OER and HER). The perspective of electronic structure modulation via interface engineering is of great significance to optimize electrocatalytic output but remains a tremendous challenge. Herein, an efficient tactic has been explored to prepare nanosheet-assembly tumbleweed-like CoFeCe-containing precursors with time-/energy-saving and easy-operating features. Subsequently, the final metal phosphide materials containing multiple interfaces, denoted CoP/FeP/CeO x , have been synthesized via the phosphorization process. Through the optimization of the Co/Fe ratio and the content of the rare-earth Ce element, the electrocatalytic activity has been regulated. As a result, bifunctional Co3Fe/Ce0.025 reaches the top of the volcano for both OER and HER simultaneously, with the smallest overpotentials of 285 mV (OER) and 178 mV (HER) at 10 mA cm -2 current density in an alkaline environment. Multicomponent heterostructure interface engineering would lead to more exposed active sites, feasible charge transport, and strong interfacial electronic interaction. More importantly, the appropriate Co/Fe ratio and Ce content can synergistically tailor the d-band center with a downshift to enhance the per-site intrinsic activity. This work would provide valuable insights to regulate the electronic structure of superior electrocatalysts toward water splitting by constructing rare-earth compounds containing multiple heterointerfaces.
Databáze: MEDLINE