催化作用
电流密度
扩散
电化学
合金
材料科学
碳纤维
氢
摩尔质量
兴奋剂
分析化学(期刊)
传质
化学工程
化学
无机化学
冶金
电极
物理化学
复合材料
热力学
光电子学
有机化学
物理
工程类
量子力学
复合数
色谱法
聚合物
作者
Lei Ding,Xiaoyu Qian,Anqi Li,Yupei Zhao,Zhichun Li,Xiaobo He
标识
DOI:10.1016/j.apsusc.2023.158652
摘要
A series of catalysts, which consist of PdNi alloy cores and N, O co-doped carbon (NOC) shells, are developed by pyrolysis of metal–organic framework (PdNi) for hydrogen production with high current densities. The bulk or surface Pd compositions (Pd/(Pd + Ni) molar ratios) of PdNi alloys can be well controlled by the fed ones. Meanwhile, some structural features that are favorable to HER activity, especially to achieving high HER current densities under low overpotentials, are further adjusted by the Pd compositions, including d-band center (εd) of PdNi alloy affected by surface segregation of Pd, hydrophilicity of NOC shell, and charge transfer and mass diffusion efficiency of an entire catalyst. When the bulk Pd/(Pd + Ni) molar ratio is ∼ 0.21, Pd0.21Ni0.79@NOC has a moderate εd, the highest hydrophilicity, the highest charge transfer and mass diffusion efficiency, and finally the highest electric double-layer capacitance (or electrochemical active surface area). Accordingly, it affords the optimal apparent or specific activity for hydrogen production with high current densities under low overpotentials in 0.5 M H2SO4, including a low apparent η1000 of ∼ 240 mV or specific η2500(BET) of ∼ 240.9 mV, and a high current density of ∼ 1590 mA cm−2 at only ∼ 242 mV.
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