Metal–Organic Framework Materials with Ultrahigh Surface Areas: Is the Sky the Limit?

We have synthesized, characterized, and computationally
simulated/validated
the behavior of two new metal–organic framework (MOF) materials
displaying the highest experimental Brunauer–Emmett–Teller
(BET) surface areas of any porous materials reported to date (∼7000
m2/g). Key to evacuating the initially solvent-filled materials
without pore collapse, and thereby accessing the ultrahigh areas,
is the use of a supercritical CO2 activation technique.
Additionally, we demonstrate computationally that by shifting from
phenyl groups to “space efficient” acetylene moieties
as linker expansion units, the hypothetical maximum surface area for
a MOF material is substantially greater than previously envisioned
(∼14600 m2/g (or greater) versus ∼10500 m2/g).

本研究合成并表征了两种新型金属有机框架（metal–organic framework, MOF）材料，并通过计算模拟与验证手段阐明了其性能表现。这两种材料的实验布鲁诺尔-埃米特-特勒（Brunauer–Emmett–Teller, BET）比表面积达到截至目前已报道多孔材料中的最高值，约为7000 m²/g。为脱除材料初始填充的溶剂且避免孔结构坍塌，从而获得该超高比表面积，本研究采用了超临界二氧化碳（supercritical CO2）活化技术，该技术是实现上述目标的关键。此外，本研究通过计算证明：若将连接基扩展单元从苯基替换为“空间高效”的乙炔基团，金属有机框架材料的理论最大比表面积将远高于此前的预期，可达约14600 m²/g（甚至更高），远超此前预估的约10500 m²/g。