Interfacial Ni-Te Bond-Length Engineering Enables Selective Urea Oxidation for Sustainable Hydrogen Production and Nitrogen Recovery #MMPMID41391168
Guo P; Cao S; Chen W; Huang W; Lu X; Zhang Y; Wang Y; Zhang P; Zou R; Liu S; Li X
ACS Nano 2025[Dec]; ? (?): ? PMID41391168show ga
Nickel-based catalysts are top candidates for urea oxidation-assisted H(2) production, enabling green energy and wastewater remediation. However, they suffer from NO(x)(-) formation and degradation due to uncontrolled urea peroxidation during the urea oxidation reaction (UOR). Here, we propose a bond-length engineering strategy for nickel telluride (NiTe) catalysts to modulate the interfacial electronic environment and suppress undesired urea peroxidation. With precise elongation of the Ni-Te bond from 2.49 A to 2.71 A, the NiTe catalyst shows asymmetric charge distribution and its d-band center shifts further away the Fermi level, thereby promoting OH(-) adsorption at the electrode-electrolyte interface. This facilitates Ni(3+)-O layer formation, stabilizing the *H(2)NCNO intermediate and enabling N identical withN coupling while suppressing C-N bond cleavage. The catalyst reached 100 mA cm(-2) at 1.33 V vs RHE with high N(2) selectivity maintained even at 1.75 V vs RHE. A membrane electrode assembly using the optimized NiTe catalyst delivers 1000 mA cm(-2) at 1.55 V with >1250 h of stable operation and high N(2) Faradaic efficiency. Integrated into a photovoltaic-electrocatalysis system, it achieves 11.2 +/- 0.6% STH efficiency and 9.39 mmol cm(-2) h(-1) H(2) output with >80% N(2) selectivity. This work offers a targeted design strategy for selective and durable UOR catalysts in sustainable hydrogen energy conversion systems.
ACS+Nano 2025 ; ? (?): ?
