Dipartimento di Chimica e Farmacia, Università di Sassari, Via Vienna 2, Sassari 07100, Italy.
Phys Chem Chem Phys. 2013 Nov 14;15(42):18664-70. doi: 10.1039/c3cp53302f.
The hydrolysis of borohydride salts represents one of the most promising processes for the generation of high purity molecular hydrogen under mild conditions. In this work we show that the sodium borohydride hydrolysis exhibits a fingerprinting periodic oscillatory transient in the hydrogen flow over a wide range of experimental conditions. We disproved the possibility that flow oscillations are driven by supersaturation phenomena of gaseous bubbles in the reactive mixture or by a nonlinear thermal feedback according to a thermokinetic model. Our experimental results indicate that the NaBH4 hydrolysis is a spontaneous inorganic oscillator, in which the hydrogen flow oscillations are coupled to an "oscillophor" in the reactive solution. The discovery of this original oscillator paves the way for a new class of chemical oscillators, with fundamental implications not only for testing the general theory on oscillations, but also with a view to chemical control of borohydride systems used as a source of hydrogen based green fuel.
硼氢化物盐的水解反应是在温和条件下生成高纯度氢气最有前途的方法之一。在这项工作中，我们表明，在广泛的实验条件下，硼氢化钠水解反应在氢气流量中表现出指纹状的周期性振荡瞬变。我们根据热动力学模型否定了流动振荡是由反应混合物中气态气泡的过饱和度或非线性热反馈驱动的可能性。我们的实验结果表明，硼氢化钠水解反应是一种自发的无机振荡器，其中氢气流量的振荡与反应溶液中的“振荡子”耦合。这种新型振荡器的发现为一类新的化学振荡器铺平了道路，这不仅对测试关于振荡的一般理论具有重要意义，而且还有望对作为绿色燃料氢源的硼氢化物系统进行化学控制。
