制冷对人类发展至关重要，其研究范围从数字时代的电子产品（如芯片冷却）延伸到生活（建筑物节能）的方方面面。其中，发展绿色的被动制冷策略对于实现碳中和与碳达峰目标意义重大。 近期，基于多孔晶体进行被动制冷的研究引起了广泛关注。这种环保且零能耗的方法在冷却电子设备、太阳能电池板和建筑物方面具有巨大的潜力。然而，多孔晶体通常具有较低的热导率，限制了它的传热效率。并且，在被动制冷应用中，金属-有机框架材料可以通过吸附水进行制冷，但其吸附的水分子进一步降低了其有效热导率。这种限制使得通过改变金属-有机框架材料本征热物性以提高其冷却性能差强人意。

针对这一挑战，香港科技大学

周艳光教授团队

将注意力转向调控多孔晶体与其接触材料之间的界面热传递。通常来讲，利用界面工程， 如加工纳米结构、表面化学修饰和生长自组装单分子层等多种方法能有效增强界面热导。然而，合成或制备具有精确原子控制的界面层是一项艰巨的任务，限制了这些方法的潜在应用。

在这项开创性的研究中，研究人员发展了一种可持续且可控的策略，利用金属-有机框架材料中的水吸附来调控接触材料与典型多孔晶体之间的界面热传递。该工作以题为“Direct observation of tunable thermal conductance at solid/porous crystalline solid interfaces induced by water adsorbates”发表在《Nature communications》上。

如图一所示，该团队选取了一种典型的金属有机框架物（HKUST-1）（图1a）作为研究对象， 其良好的结晶性 (图1b)有助于利用频域热反射方法（FDTR）进行热输运的研究。他们在HKUST-1晶体表面溅射上一层平整的金层用以构建多孔晶体材料和固体界面，同时Au还可以用作FDTR测试中的热反射层。切片样品的透射电子显微镜 （TEM）照片显示出样品具有清晰且均匀的界面（图1c）。当HKUST-1晶体浸没在水中一段时间后，水分子会与晶体结构结合，导致拉曼信号的229 cm

-1 峰位发生红移，因此可以用来确定晶体吸水到饱和的时间（图1d）。

图1：多孔晶体/固体界面样品的表征。（a） HKUST-1晶体的扫描电镜照片；（b）HKUST-1晶体的x射线衍射谱；（c）Au/HKUST-1界面的透射电子显微镜照片；（d）不同吸水时间下的HKUST-1晶体的拉曼散射谱。

设想，当样品完全干燥时，多孔晶体HKSUT-1的孔隙中和Au/HKUST-1界面没有水分子占据。对于HKUST-1晶体来讲，由于没有水和框架的声子散射，其热导率会高于充满水的状态。而界面的热输运可以分解成两部分，Au到晶体框架和Au到水分子，这种双通道机制会增加界面热导（ITC）并且可以通过频域热反射测试直观地反映出来（图2）。

图2：不同吸水状态下的Au/HKUST-1样品的FDTR测试曲线。

他们测量了完全干燥的和在水中浸没40分钟后的样品热导率和ITC变化。当吸满水后，热导率从0.742 W/mK降低到0.416 W/mK，这是由于框架中的水分子增加了声子散射通道。十分有趣的是，界面热导从5.17 MW/m

2K 大幅增加到7倍大小 （31.45 MW/m

2K）（图3a），这跟框架中热导率变化趋势截然相反。通过分子动力学模拟（MD）进一步地进行了探究。结果发现，随着水分子逐渐充满整个框架，部分水分子会由于Au与其之间的范德华力被吸附到界面区域，并逐渐形成类水膜 （图3b）。MD结果显示，ITC可以从干燥状态的4.2 MW/m

2K 提高到 35 MW/m

2K，这与实验测试结果十分吻合。有趣的是，测试了数十个样品在不同状态下的结果变化统计发现，干燥样品的ITC十分接近，而吸满水样品的ITC跨越了较大范围。并且，吸满水样品的最低ITC值和干燥样品的平均值很接近。这是否是由于在不同样品中，Au膜对水分子的吸引力不一样，导致界面水分子的密度有差异造成的呢？于是，计算了水分子与Au具有不同强度相互作用体系的界面热导。随着相互作用的强度提升，水饱和状态的体系界面热导也大幅提升。这表明可以通过控制Au与水分子的相互作用强度大小，从而调节界面吸附的水密度，以此来控制在吸附饱和水状态的界面热导。同样地在UiO-66和MOF-505体系中也观察到了类似的现象。

图3：Au/HKUST-1界面热导的实验和分子动力学结果。（a）Au/HKUST-1界面热导在不同吸水浓度下的实验和分子动力学结果；（b）不同吸水浓度下，水分子在体系内部的分布情况。

为了进一步的揭示界面吸附的水分子增强热输运的物理过程和机理，通过自主开发的声子频域直接分解方法分析发现，水的存在激发了高频声子振动模式（> 4THz）的热输运，而这些声子贡献对于无水的Au/HKUST-1可以忽略不计（图4a 和b）。这种高频声子的贡献得益于水分子对于体系的声子态密度的桥梁作用。对于干燥体系而言，Au和HKUST-1的声子态密度在整个频率范围内只发生部分重叠。而Au和水的声子态密度却大范围重叠，特别是在低频区，这促使含水的HKUST-1框架与Au的声子态密度重叠范围增加，从而增强两者间的热输运（图4c）。此外，将ITC的贡献分解到Au/HKUST-1和Au/水热输运通道发现，Au/HKUST-1通道的贡献随着吸水量的增加有轻微上升，而Au/水通道的贡献大幅上升。这表明，界面水的存在增加了额外的热输运通道，从而提高了界面热导(图4d)。

图4：界面热输运的分子动力学结果。（a-b）不同Au与水相互作用强度下的声子透射系数频谱分析；（c）吸满水状态下Au，水和HKUST-1框架的声子态密度分布；（d）通过Au/水和Au/HKUST-1双通道的热输运贡献分解。

这项研究创新地提出利用界面吸附水的桥梁和双通道作用增强界面热输运，不仅为多孔晶体和其他固体材料的界面热传递提供了新的见解，而且对优化基于多孔晶体的冷却应用的性能具有重要意义。这对利用分子吸附操纵界面热传递，并设计更高效的冷却技术奠定了基础。

招聘信息

来源：高分子科学前沿

声明：仅代表个人观点，水平有限，如有不科学之处，请在下方留言指正！

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