氢气传输对钠硼氢化物还原4-硝基苯酚的动力学区域的影响
Effects of Hydrogen Transport on the Kinetic Regimes of 4-Nitrophenol Reduction by Sodium Borohydride
AI总结：
研究揭示氢气传输对钠硼氢化物还原4-硝基苯酚动力学的影响，提出模型解释不同传输模式下的反应行为。
摘要：
4-硝基苯酚（4-NiP）用钠硼氢化物还原被广泛用于异质催化剂的基准测试，但其动力学通常被简化为伪一级动力学。实际上，硼氢化物水解和溶解氢的氢化过程是同时进行的，使氢气传输成为决定表观活性的关键因素。重新审视具有不同孔结构的Pt-SiO2超颗粒数据，我们发现不同的氢气传输模式导致了不同的动力学行为：扩散传输维持伪一级动力学，而气泡介导的逃逸导致氢气损失和不完全转化。我们提出了一种动力学模型，能够捕捉这种转变并使实验数据得到一致的解释。更广泛地说，我们的分析表明，在4-NiP基准测试中表观活性的差异可能是由于氢气传输而非催化剂本身的性质，强调在比较催化剂性能时需要考虑传输效应。
英文摘要：
The reduction of 4-nitrophenol (4-NiP) with sodium borohydride is widely used to benchmark heterogeneous catalysts, yet its kinetics are commonly oversimplified as pseudo-first-order. In reality, borohydride hydrolysis and hydrogenation by dissolved hydrogen proceed concurrently, making hydrogen transport a decisive factor in shaping apparent activity. Re-examining data on Pt-SiO2 supraparticles with different pore structures, we attribute contrasting kinetic behavior to distinct regimes of hydrogen transport: diffusive transport sustains pseudo-first-order kinetics, while bubble-mediated escape causes hydrogen loss and incomplete conversion. We propose a kinetic model that captures this transition and enables consistent interpretation of experimental data. More broadly, our analysis shows that apparent differences in activity during 4-NiP benchmarking can arise from hydrogen transport rather than intrinsic properties of the catalyst, underscoring the need to account for transport effects when comparing catalyst performance.
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