Mustafa Rawezh Muhtasim, Çelik Kazıcı Hilal
Faculty of Engineering, Department of Chemical Engineering, Koya University, 45001 Koysinjaq, Iraq.
Faculty of Science, Department of Chemistry, Van Yüzüncü Yıl University, 65080 Van, Turkey.
ACS Omega. 2025 Jul 23;10(30):32987-32997. doi: 10.1021/acsomega.5c02174. eCollection 2025 Aug 5.
In this study, palladium (Pd), ruthenium (Ru), and cobalt (Co) nanoparticles (NP) supported on activated carbon (AC) (denoted as PdRu/AC@1% Co) were successfully synthesized via the impregnation-reduction method. The structural and surface characteristics of the catalyst were thoroughly analyzed by using X-ray diffraction (XRD), scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDX), and X-ray photoelectron spectroscopy (XPS). The catalytic performance of PdRu/AC@1% Co with different atomic ratios was evaluated for hydrogen generation through the hydrolysis of ammonia borane (NHBH, AB). Compared to monometallic (Pd) and bimetallic (PdRu) systems, the trimetallic PdRu@Co catalyst exhibited significantly enhanced catalytic activity, even at low temperatures. Under optimized conditions (1 mmol of AB, 50 mg of catalyst, 25 °C), the highest turnover frequency (TOF) value of 312.8 (mol )/(mol·min) was achieved. The activation parameters for the hydrolysis reaction were calculated as activation energy ( ) = 19.6 kJ/mol, enthalpy change (Δ ) = 17.12 kJ/mol, and entropy change (Δ ) = -184.85 J/(mol·K). These findings suggest that PdRu/AC@1% Co is a highly efficient and reusable catalyst, making it a promising candidate for practical hydrogen production from AB.
在本研究中,通过浸渍还原法成功合成了负载在活性炭(AC)上的钯(Pd)、钌(Ru)和钴(Co)纳米颗粒(NP)(表示为PdRu/AC@1%Co)。利用X射线衍射(XRD)、扫描电子显微镜(SEM)、能量色散X射线光谱(EDX)和X射线光电子能谱(XPS)对催化剂的结构和表面特性进行了全面分析。评估了不同原子比的PdRu/AC@1%Co通过氨硼烷(NHBH,AB)水解产氢的催化性能。与单金属(Pd)和双金属(PdRu)体系相比,即使在低温下,三金属PdRu@Co催化剂也表现出显著增强的催化活性。在优化条件下(1 mmol AB、50 mg催化剂、25°C),实现了最高周转频率(TOF)值312.8(mol)/(mol·min)。水解反应的活化参数计算为活化能()=19.6 kJ/mol、焓变(Δ)=17.12 kJ/mol和熵变(Δ)=-184.85 J/(mol·K)。这些发现表明,PdRu/AC@1%Co是一种高效且可重复使用的催化剂,使其成为从AB实际制氢的有前途的候选者。