钯单原子负载氮掺杂碳催化剂的制备及其室温催化甲醛水溶液制氢性能

刘小刚; 陈文婕; 张欣; 晏格格; 季汉初; 王阳; 李艳艳; 兰玉典; 郭亚轩

doi:10.3969/j.issn.1003-0972.2023.01.017

钯单原子负载氮掺杂碳催化剂的制备及其室温催化甲醛水溶液制氢性能

Palladium Single-atom Catalyst Supported on Nitrogen-doped Carbon for Catalytic Hydrogen Production from Aqueous Formaldehyde at Room Temperature

摘要

摘要: 以高温热解金属有机框架生成的氮掺杂碳材料（CN）为载体，钯单原子（Pd₁）为活性组分，制备负载Pd₁的催化剂（Pd₁/CN）。使用X-射线粉末衍射（XRD）、扫描电子显微镜（SEM）、透射电子显微镜（TEM）和拉曼光谱（Raman）对Pd₁/CN催化剂进行了结构和形貌表征，并评价了其在室温条件下催化甲醛产氢性能。结果表明：Pd₁/CN催化剂的制氢性能明显优于常规Pd纳米颗粒（NPs）和负载Pd纳米颗粒的Pd/CN。分析反应条件对产氢性能的影响发现，在1 mol/L NaOH和0.6 mol/L HCHO浓度下，Pd₁/CN催化剂30 min内的产氢量最高，可达54.5 mL，并表现出优异的循环稳定性。

Abstract: Single-atom palladium (Pd₁)-supported on nitrogen-doped carbon material (CN) catalyst (Pd₁/CN) is prepared through high-temperature pyrolysis of metal-organic framework as precusor and Pd₁ as the active sites. The structure and morphology of Pd₁/CN catalysts are characterized by X-ray powder diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and Raman spectroscopy(Raman), and their catalytic hydrogen production behavior is evaluated at room temperature. The results show that the hydrogen production performance of Pd₁/CN catalyst is significantly higher than that of conventional Pd nanoparticles (NPs) and Pd/CN supported Pd nanoparticles. The effects of reaction conditions on the hydrogen production are explored, which show that under the optimal concentration of NaOH (1 mol/L) and HCHO (0.6 mol/L), superior hydrogen production of 54.5 mL within 30 min and excellent cycle stability could be achieved.

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