Citation: Sheng Qian, Jingying Wei, Junhua Wang, Yi Zhang, Huaiguo Xue, Tengfei Jiang, Jingqi Tian. Conjugated N-heterocycles in heterostructured support manipulate d-band center for hydrogen electrocatalysis[J]. Chinese Chemical Letters, ;2026, 37(8): 112106. doi: 10.1016/j.cclet.2025.112106 shu

Conjugated N-heterocycles in heterostructured support manipulate d-band center for hydrogen electrocatalysis

School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou 225002, China

tianjq@yzu.edu.cn

Received Date: 14 August 2025
Revised Date: 29 October 2025
Accepted Date: 11 November 2025
Available Online: 12 November 2025

Figures(5)

The interfacial electronic interaction between the support and catalyst has been demonstrated to play a significant role in regulating the d-band structure of metal centers. Still, it requires dedicated control over the interaction in a reasonable manner. Herein, we developed a heterostructured support by covalently linking carbon nitride quantum dots (CNQDs) on TiO₂, to anchor electroactive CoP clusters (TiO₂–CNQD/CoP) for hydrogen evolution reaction (HER). The interfacial electronic interaction between the heterostructured support (TiO₂–CNQD) and CoP can be controlled by varying the size of CNQDs, owing to the number of conjugated N-heterocycles in CNQDs induces tunable π-electron delocalization. As a result, a volcano-shaped correlation between the shift of the Co d-band center (Δd) and the HER performance was established, suggesting that TiO₂–CNQD/CoP-C2 with a moderate size of CNQD is the optimal HER catalyst. This study highlights the critical role of interfacial interaction in supported catalysts, providing a predictive descriptor focusing on the support design of advanced HER catalysts.
- Heterostructured support,
- d-Band center,
- Descriptor,
- Interfacial electron transfer,
- Electrocatalysis
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