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Sreehari Surendran Rajasree Jierui Yu Dr. H. Christopher Fry Ryther Anderson Dr. Wenqian Xu Riya Krishnan Jiaxin Duan Dr. Subhadip Goswami Prof. Dr. Diego A. Gómez-Gualdrón Prof. Dr. Pravas Deria 《Angewandte Chemie (International ed. in English)》2023,62(38):e202305323
High quantum yield triplets, populated by initially prepared excited singlets, are desired for various energy conversion schemes in solid working compositions like porous MOFs. However, a large disparity in the distribution of the excitonic center of mass, singlet-triplet intersystem crossing (ISC) in such assemblies is inhibited, so much so that a carboxy-coordinated zirconium heavy metal ion cannot effectively facilitate the ISC through spin-orbit coupling. Circumventing this sluggish ISC, singlet fission (SF) is explored as a viable route to generating triplets in solution-stable MOFs. Efficient SF is achieved through a high degree of interchromophoric coupling that facilitates electron super-exchange to generate triplet pairs. Here we show that a predesigned chromophoric linker with extremely poor ISC efficiency (kISC) but form triplets in MOF in contrast to the frameworks that are built from linkers with sizable kISC but . This work opens a new photophysical and photochemical avenue in MOF chemistry and utility in energy conversion schemes. 相似文献
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Xinlin Li Sreehari Surendran Rajasree Dr. Venkatesh Gude Karan Maindan Prof. Dr. Pravas Deria 《Angewandte Chemie (International ed. in English)》2023,62(22):e202219046
Traditional MOF e-CRR, constructed from catalytic linkers, manifest a kinetic bottleneck during their multi-electron activation. Decoupling catalysis and charge transport can address such issues. Here, we build two MOF/e-CRR systems, CoPc@NU-1000 and TPP(Co)@NU-1000, by installing cobalt metalated phthalocyanine and tetraphenylporphyrin electrocatalysts within the redox active NU-1000 MOF. For CoPc@NU-1000, the e-CRR responsive CoI/0 potential is close to that of NU-1000 reduction compared to the TPP(Co)@NU-1000. Efficient charge delivery, defined by a higher diffusion (Dhop=4.1×10−12 cm2 s−1) and low charge-transport resistance ( =59.5 Ω) in CoPC@NU-1000 led FECO=80 %. In contrast, TPP(Co)@NU-1000 fared a poor FECO=24 % (Dhop=1.4×10−12 cm2 s−1 and =91.4 Ω). For such a decoupling strategy, careful choice of the host framework is critical in pairing up with the underlying electrochemical properties of the catalysts to facilitate the charge delivery for its activation. 相似文献