Cai Guorui, Ding Meili, Wu Qianye, Jiang Hai-Long
Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Soft Matter Chemistry, Collaborative Innovation Center of Suzhou Nano Science and Technology, Department of Chemistry, University of Science and Technology of China, Hefei 230026, China.
Natl Sci Rev. 2020 Jan;7(1):37-45. doi: 10.1093/nsr/nwz147. Epub 2019 Oct 1.
Homogeneous molecular catalysts and heterogeneous catalysts possess complementary strengths, and are of great importance in laboratory/commercial procedures. While various porous hosts, such as polymers, carbons, silica, metal oxides and zeolites, have been used in an attempt to heterogenize homogeneous catalysts, realizing the integration of both functions at the expense of discounting their respective advantages, it remains a significant challenge to truly combine their intrinsic strengths in a single catalyst without compromise. Here, we describe a general template-assisted approach to incorporating soluble molecular catalysts into the hollow porous capsule, which prevents their leaching due to the absence of large intergranular space. In the resultant yolk (soluble)-shell (crystalline) capsules, the soluble yolks can perform their intrinsic activity in a mimetic homogeneous environment, and the crystalline porous shells endow the former with selective permeability, substrate enrichment, size-selective and heterogeneous cascade catalysis, beyond the integration of the respective advantages of homogeneous and heterogeneous catalysts.
均相分子催化剂和多相催化剂具有互补的优势，在实验室/商业流程中非常重要。虽然各种多孔载体，如聚合物、碳、二氧化硅、金属氧化物和沸石，已被用于使均相催化剂多相化，试图以牺牲各自优势为代价实现两种功能的整合，但在不妥协的情况下将它们的内在优势真正结合在单一催化剂中仍然是一项重大挑战。在此，我们描述了一种通用的模板辅助方法，将可溶性分子催化剂纳入中空多孔胶囊中，由于不存在大的晶间空间，可防止其浸出。在所得的蛋黄（可溶性）-壳（晶体）胶囊中，可溶性蛋黄可以在模拟的均相环境中发挥其固有活性，而结晶多孔壳赋予前者选择性渗透性、底物富集、尺寸选择性和多相级联催化作用，超越了均相和多相催化剂各自优势的整合。
