Coulombic interactions can be used to assemble charged nanoparticles into higher-order structures, but the process requires oppositely charged partners that are similarly sized. The ability to mediate the assembly of such charged nanoparticles using structurally simple small molecules would greatly facilitate the fabrication of nanostructured materials and harnessing their applications in catalysis, sensing and photonics. Here we show that small molecules with as few as three electric charges can effectively induce attractive interactions between oppositely charged nanoparticles in water. These interactions can guide the assembly of charged nanoparticles into colloidal crystals of a quality previously only thought to result from their co-crystallization with oppositely charged nanoparticles of a similar size. Transient nanoparticle assemblies can be generated using positively charged nanoparticles and multiply charged anions that are enzymatically hydrolysed into mono- and/or dianions. Our findings demonstrate an approach for the facile fabrication, manipulation and further investigation of static and dynamic nanostructured materials in aqueous environments.

库仑相互作用可用于将带电纳米粒子组装成高阶结构，但该过程需要大小相似、带相反电荷的伙伴。使用结构简单的小分子介导此类带电纳米粒子组装的能力将极大地促进纳米结构材料的制造并利用它们在催化、传感和光子学中的应用。在这里，我们表明具有少至三个电荷的小分子可以有效地诱导水中带相反电荷的纳米粒子之间的吸引相互作用。这些相互作用可以引导带电纳米粒子组装成胶体晶体，这种胶体晶体以前只被认为是由它们与具有相似尺寸的带相反电荷的纳米粒子共结晶产生的。可以使用带正电的纳米粒子和酶促水解成单和/或双阴离子的多电荷阴离子来生成瞬态纳米粒子组装体。我们的研究结果展示了一种在水环境中轻松制造、操作和进一步研究静态和动态纳米结构材料的方法。