Volume 20, Issue 31 2311505
Research Article

A Coordination-Derived Cerium-Based Amorphous–Crystalline Heterostructure with High Electrocatalytic Oxygen Evolution Activity

Haiyan An

Haiyan An

Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, 730000 P. R. China

Search for more papers by this author
Xijiao Mu

Xijiao Mu

Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, 730000 P. R. China

Search for more papers by this author
Guoying Tan

Guoying Tan

Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, 730000 P. R. China

Search for more papers by this author
Pingru Su

Pingru Su

Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, 730000 P. R. China

Search for more papers by this author
Liangliang Liu

Liangliang Liu

Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, 730000 P. R. China

Search for more papers by this author
Nan Song

Nan Song

Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, 730000 P. R. China

Search for more papers by this author
Shiqiang Bai

Shiqiang Bai

Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, 730000 P. R. China

Search for more papers by this author
Chun-Hua Yan

Chun-Hua Yan

Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, 730000 P. R. China

Search for more papers by this author
Yu Tang

Corresponding Author

Yu Tang

Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, 730000 P. R. China

State Key Laboratory of Baiyunobo Rare Earth Resource Researches and Comprehensive Utilization, Baotou Research Institute of Rare Earths, Baotou, 014030 P. R. China

E-mail: [email protected]

Search for more papers by this author
First published: 03 March 2024
Citations: 13

Abstract

The rational design of heterogeneous catalysts is crucial for achieving optimal physicochemical properties and high electrochemical activity. However, the development of new amorphous–crystalline heterostructures is significantly more challenging than that of the existing crystalline–crystalline heterostructures. To overcome these issues, a coordination-assisted strategy that can help fabricate an amorphous NiO/crystalline NiCeOx (a-NiO/c-NiCeOx) heterostructure is reported herein. The coordination geometry of the organic ligands plays a pivotal role in permitting the formation of coordination polymers with high Ni contents. This consequently provides an opportunity for enabling the supersaturation of Ni in the NiCeOx structure during annealing, leading to the endogenous spillover of Ni from the depths of NiCeOx to its surface. The resulting heterostructure, featuring strongly coupled amorphous NiO and crystalline NiCeOx, exhibits harmonious interactions in addition to low overpotentials and high catalytic stability in the oxygen evolution reaction (OER). Theoretical calculations prove that the amorphous–crystalline interfaces facilitate charge transfer, which plays a critical role in regulating the local electron density of the Ni sites, thereby promoting the adsorption of oxygen-based intermediates on the Ni sites and lowering the dissociation-related energy barriers. Overall, this study underscores the potential of coordinating different metal ions at the molecular level to advance amorphous–crystalline heterostructure design.

Conflict of Interest

The authors declare no conflict of interest.

Data Availability Statement

Research data are not shared.

The full text of this article hosted at iucr.org is unavailable due to technical difficulties.