Choi, Hyuck Gu Lee, Ui Young Lee, Ju Hyeok Choi, Hyung Wook Yoo, Jung Hyeon Kim, Jiwon Kim, Hyun You Kang, Bong Kyun Yoon, Dae Ho 2025-03-22T15:00:06Z 2025-03-22T15:00:06Z 2025-03-19 2025-05 0169-4332 https://pubs.kist.re.kr/handle/201004/152028 Hydrogen is eco-friendly with a high energy density, leading to a growing-demand for developing efficient and cost-effective catalysts. For efficient hydrogen evolution reaction (HER), nanoarchitectonics strategy by constructing heterostructure can provide numerous catalytic active sites with enhanced intrinsic activity. This study aimed to achieve enhanced kinetics of HER by in-situ nanoarchitectonics of Ni3FeN/Ni3Fe heterostructure. Vacancy-engineered NiFe PBA, the precursor, was synthesized using a facile hydrothermal method via hydrogen peroxide concentration control without complicated or multiple processes. An in-situ Ni3FeN/Ni3Fe heterostructure was generated through ammonolysis of vacancy-engineered NiFe PBA. Theoretical interpretation by density functional theory (DFT) calculations confirmed that electron transfer from Ni3Fe to Ni3FeN 0.51 e leads to an H adsorption energy down shift (0.36 eV to 0.20 eV), which facilitates catalytic HER. Off-line catalytic alkaline HER performance also showed enhanced kinetic activity with an overpotential of 135 mV at a current density of 10 mA cm- 2. Furthermore, the stability at 200 mA cm- 2 for 100 h showed only 6.61 % decrease in performance, which demonstrated the durability of the Ni3FeN/Ni3Fe heterostructure. This study provides a reasonable design of the enhanced electronic structure and H adsorption energy down-shift from in-situ nanoarchitectonics of Ni3FeN/Ni3Fe heterostructure for enhanced HER performance. English Elsevier BV In-situ nanoarchitectonics of Ni3FeN/Ni3Fe heterostructure via facile synthesis of vacancy-rich NiFe PBA for enhanced hydrogen evolution reaction Article 10.1016/j.apsusc.2025.162652 1 Applied Surface Science, v.691 Applied Surface Science 691 N scie scopus 001428058500001 2-s2.0-85217755699 Chemistry, Physical Materials Science, Coatings & Films Physics, Applied Physics, Condensed Matter Chemistry Materials Science Physics Article PRUSSIAN BLUE EFFICIENT ENERGY ELECTROCATALYSTS ELECTROLYSIS NANOSHEETS ION Prussian blue analogues Transition metal nitrides Hydrogen evolution reaction Electrocatalysts Heterostructure In-situ construction