响应性纳米反应器中的催化双分子反应
Catalyzed bimolecular reactions in responsive nanoreactors
摘要：
我们描述了一个一般的理论，表面催化的双分子反应在响应nanoreactors，催化活性的纳米粒子由一个刺激响应的“门控”壳，其渗透性控制的过程中的活动。我们解决了该系统中遇到的两个原型场景：第一个，其中两种物质从本体溶液扩散在催化剂表面反应;第二个，其中只有一种反应物从本体扩散，而另一种反应物在纳米颗粒表面产生，例如，通过光转换。我们发现，在这两种情况下的总催化率具有相同的数学结构，一旦扩散率被适当地重新定义。此外，不同反应物的扩散通量强烈耦合，提供比单分子反应更丰富的行为。我们还表明，在形成鲜明对比的本体反应，识别的限制反应物是不是简单地由相对体积浓度，但控制的纳米反应器壳的渗透性。最后，我们描述了我们的理论的应用，通过分析实验数据之间的反应hexacyanoferrate（III）和硼氢化物离子在响应水凝胶为基础的核壳纳米反应器。
英文摘要：
We describe a general theory for surface-catalyzed bimolecular reactions in responsive nanoreactors, catalytically active nanoparticles coated by a stimuli-responsive 'gating' shell, whose permeability controls the activity of the process. We address two archetypal scenarios encountered in this system: The first, where two species diffusing from a bulk solution react at the catalyst's surface; the second where only one of the reactants diffuses from the bulk while the other one is produced at the nanoparticle surface, e.g., by light conversion. We find that in both scenarios the total catalytic rate has the same mathematical structure, once diffusion rates are properly redefined. Moreover, the diffusional fluxes of the different reactants are strongly coupled, providing a richer behavior than that arising in unimolecular reactions. We also show that in stark contrast to bulk reactions, the identification of a limiting reactant is not simply determined by the relative bulk concentrations but controlled by the nanoreactor shell permeability. Finally, we describe an application of our theory by analyzing experimental data on the reaction between hexacyanoferrate (III) and borohydride ions in responsive hydrogel-based core-shell nanoreactors.
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