The Experts below are selected from a list of 174 Experts worldwide ranked by ideXlab platform
Hongcai Zhou - One of the best experts on this subject based on the ideXlab platform.
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Systematic Engineering of single substitution in zirconium metal organic frameworks toward high performance catalysis
Journal of the American Chemical Society, 2017Co-Authors: Ning Huang, Shuai Yuan, Xinyu Yang, Jiandong Pang, Junsheng Qin, Yingmu Zhang, Qi Wang, Donglin Jiang, Hannah F Drake, Hongcai ZhouAbstract:Zirconium-based metal–organic frameworks (Zr-MOFs) exhibit great structural tunability and outstanding chemical stability, rendering them promising candidates for a wide range of practical applications. In this work, we synthesized a series of isostructural PCN-224 analogues functionalized by ethyl, bromo, chloro, and fluoro groups on the porphyrin unit, which allowed us to explicitly study the effects of electron-donating and electron-withdrawing substituents on catalytic performance in MOFs. Owing to the different electronic properties of ethyl, bromo, chloro, and fluoro substitutes, the molecular-level control over the chemical environment surrounding a catalytic center could be readily achieved in our MOFs. To investigate the effects of these substitutes on catalytic activity and selectivity, the oxidation of 3-methylpentane to corresponding alcohols and ketones was utilized as a model reaction. Within these five analogues of PCN-224, an extremely high turnover number of 7680 and turnover frequency of...
Matthew B. Francis - One of the best experts on this subject based on the ideXlab platform.
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Systematic Engineering of a protein nanocage for high yield site specific modification
Journal of the American Chemical Society, 2019Co-Authors: Daniel D Brauer, Emily C. Hartman, Daniel L. V. Bader, Zoe N. Merz, Matthew B. Francis, Danielle TullmanercekAbstract:Site-specific protein modification is a widely used strategy to attach drugs, imaging agents, or other useful small molecules to protein carriers. N-terminal modification is particularly useful as a high-yielding, site-selective modification strategy that can be compatible with a wide array of proteins. However, this modification strategy is incompatible with proteins with buried or sterically hindered N termini, such as virus-like particles (VLPs) composed of the well-studied MS2 bacteriophage coat protein. To assess VLPs with improved compatibility with these techniques, we generated a targeted library based on the MS2-derived protein cage with N-terminal proline residues followed by three variable positions. We subjected the library to assembly, heat, and chemical selections, and we identified variants that were modified in high yield with no reduction in thermostability. Positive charge adjacent to the native N terminus is surprisingly beneficial for successful extension, and over 50% of the highest performing variants contained positive charge at this position. Taken together, these studies described nonintuitive design rules governing N-terminal extensions and identified successful extensions with high modification potential.
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Systematic Engineering of a Protein Nanocage for High-Yield, Site-Specific Modification
2019Co-Authors: Daniel D. Brauer, Emily C. Hartman, Daniel L. V. Bader, Zoe N. Merz, Danielle Tullman-ercek, Matthew B. FrancisAbstract:Site-specific protein modification is a widely used strategy to attach drugs, imaging agents, or other useful small molecules to protein carriers. N-terminal modification is particularly useful as a high-yielding, site-selective modification strategy that can be compatible with a wide array of proteins. However, this modification strategy is incompatible with proteins with buried or sterically hindered N termini, such as virus-like particles (VLPs) composed of the well-studied MS2 bacteriophage coat protein. To assess VLPs with improved compatibility with these techniques, we generated a targeted library based on the MS2-derived protein cage with N-terminal proline residues followed by three variable positions. We subjected the library to assembly, heat, and chemical selections, and we identified variants that were modified in high yield with no reduction in thermostability. Positive charge adjacent to the native N terminus is surprisingly beneficial for successful extension, and over 50% of the highest performing variants contained positive charge at this position. Taken together, these studies described nonintuitive design rules governing N-terminal extensions and identified successful extensions with high modification potential
Ning Huang - One of the best experts on this subject based on the ideXlab platform.
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Systematic Engineering of single substitution in zirconium metal organic frameworks toward high performance catalysis
Journal of the American Chemical Society, 2017Co-Authors: Ning Huang, Shuai Yuan, Xinyu Yang, Jiandong Pang, Junsheng Qin, Yingmu Zhang, Qi Wang, Donglin Jiang, Hannah F Drake, Hongcai ZhouAbstract:Zirconium-based metal–organic frameworks (Zr-MOFs) exhibit great structural tunability and outstanding chemical stability, rendering them promising candidates for a wide range of practical applications. In this work, we synthesized a series of isostructural PCN-224 analogues functionalized by ethyl, bromo, chloro, and fluoro groups on the porphyrin unit, which allowed us to explicitly study the effects of electron-donating and electron-withdrawing substituents on catalytic performance in MOFs. Owing to the different electronic properties of ethyl, bromo, chloro, and fluoro substitutes, the molecular-level control over the chemical environment surrounding a catalytic center could be readily achieved in our MOFs. To investigate the effects of these substitutes on catalytic activity and selectivity, the oxidation of 3-methylpentane to corresponding alcohols and ketones was utilized as a model reaction. Within these five analogues of PCN-224, an extremely high turnover number of 7680 and turnover frequency of...
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Systematic Engineering of Single Substitution in Zirconium Metal–Organic Frameworks toward High-Performance Catalysis
2017Co-Authors: Ning Huang, Shuai Yuan, Hannah Drake, Xinyu Yang, Jiandong Pang, Junsheng Qin, Yingmu Zhang, Qi Wang, Donglin JiangAbstract:Zirconium-based metal–organic frameworks (Zr-MOFs) exhibit great structural tunability and outstanding chemical stability, rendering them promising candidates for a wide range of practical applications. In this work, we synthesized a series of isostructural PCN-224 analogues functionalized by ethyl, bromo, chloro, and fluoro groups on the porphyrin unit, which allowed us to explicitly study the effects of electron-donating and electron-withdrawing substituents on catalytic performance in MOFs. Owing to the different electronic properties of ethyl, bromo, chloro, and fluoro substitutes, the molecular-level control over the chemical environment surrounding a catalytic center could be readily achieved in our MOFs. To investigate the effects of these substitutes on catalytic activity and selectivity, the oxidation of 3-methylpentane to corresponding alcohols and ketones was utilized as a model reaction. Within these five analogues of PCN-224, an extremely high turnover number of 7680 and turnover frequency of 10 240 h–1 was achieved by simply altering the substitutes on porphyrin rings. Moreover, a remarkable 99% selectivity of the tertiary alcohol over the five other possible by-products are realized. We demonstrate that this strategy can be used to efficiently screen a suitable peripheral environment around catalytic cores in MOFs for catalysis
Donglin Jiang - One of the best experts on this subject based on the ideXlab platform.
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Systematic Engineering of single substitution in zirconium metal organic frameworks toward high performance catalysis
Journal of the American Chemical Society, 2017Co-Authors: Ning Huang, Shuai Yuan, Xinyu Yang, Jiandong Pang, Junsheng Qin, Yingmu Zhang, Qi Wang, Donglin Jiang, Hannah F Drake, Hongcai ZhouAbstract:Zirconium-based metal–organic frameworks (Zr-MOFs) exhibit great structural tunability and outstanding chemical stability, rendering them promising candidates for a wide range of practical applications. In this work, we synthesized a series of isostructural PCN-224 analogues functionalized by ethyl, bromo, chloro, and fluoro groups on the porphyrin unit, which allowed us to explicitly study the effects of electron-donating and electron-withdrawing substituents on catalytic performance in MOFs. Owing to the different electronic properties of ethyl, bromo, chloro, and fluoro substitutes, the molecular-level control over the chemical environment surrounding a catalytic center could be readily achieved in our MOFs. To investigate the effects of these substitutes on catalytic activity and selectivity, the oxidation of 3-methylpentane to corresponding alcohols and ketones was utilized as a model reaction. Within these five analogues of PCN-224, an extremely high turnover number of 7680 and turnover frequency of...
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Systematic Engineering of Single Substitution in Zirconium Metal–Organic Frameworks toward High-Performance Catalysis
2017Co-Authors: Ning Huang, Shuai Yuan, Hannah Drake, Xinyu Yang, Jiandong Pang, Junsheng Qin, Yingmu Zhang, Qi Wang, Donglin JiangAbstract:Zirconium-based metal–organic frameworks (Zr-MOFs) exhibit great structural tunability and outstanding chemical stability, rendering them promising candidates for a wide range of practical applications. In this work, we synthesized a series of isostructural PCN-224 analogues functionalized by ethyl, bromo, chloro, and fluoro groups on the porphyrin unit, which allowed us to explicitly study the effects of electron-donating and electron-withdrawing substituents on catalytic performance in MOFs. Owing to the different electronic properties of ethyl, bromo, chloro, and fluoro substitutes, the molecular-level control over the chemical environment surrounding a catalytic center could be readily achieved in our MOFs. To investigate the effects of these substitutes on catalytic activity and selectivity, the oxidation of 3-methylpentane to corresponding alcohols and ketones was utilized as a model reaction. Within these five analogues of PCN-224, an extremely high turnover number of 7680 and turnover frequency of 10 240 h–1 was achieved by simply altering the substitutes on porphyrin rings. Moreover, a remarkable 99% selectivity of the tertiary alcohol over the five other possible by-products are realized. We demonstrate that this strategy can be used to efficiently screen a suitable peripheral environment around catalytic cores in MOFs for catalysis
Qi Wang - One of the best experts on this subject based on the ideXlab platform.
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Systematic Engineering of single substitution in zirconium metal organic frameworks toward high performance catalysis
Journal of the American Chemical Society, 2017Co-Authors: Ning Huang, Shuai Yuan, Xinyu Yang, Jiandong Pang, Junsheng Qin, Yingmu Zhang, Qi Wang, Donglin Jiang, Hannah F Drake, Hongcai ZhouAbstract:Zirconium-based metal–organic frameworks (Zr-MOFs) exhibit great structural tunability and outstanding chemical stability, rendering them promising candidates for a wide range of practical applications. In this work, we synthesized a series of isostructural PCN-224 analogues functionalized by ethyl, bromo, chloro, and fluoro groups on the porphyrin unit, which allowed us to explicitly study the effects of electron-donating and electron-withdrawing substituents on catalytic performance in MOFs. Owing to the different electronic properties of ethyl, bromo, chloro, and fluoro substitutes, the molecular-level control over the chemical environment surrounding a catalytic center could be readily achieved in our MOFs. To investigate the effects of these substitutes on catalytic activity and selectivity, the oxidation of 3-methylpentane to corresponding alcohols and ketones was utilized as a model reaction. Within these five analogues of PCN-224, an extremely high turnover number of 7680 and turnover frequency of...
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Systematic Engineering of Single Substitution in Zirconium Metal–Organic Frameworks toward High-Performance Catalysis
2017Co-Authors: Ning Huang, Shuai Yuan, Hannah Drake, Xinyu Yang, Jiandong Pang, Junsheng Qin, Yingmu Zhang, Qi Wang, Donglin JiangAbstract:Zirconium-based metal–organic frameworks (Zr-MOFs) exhibit great structural tunability and outstanding chemical stability, rendering them promising candidates for a wide range of practical applications. In this work, we synthesized a series of isostructural PCN-224 analogues functionalized by ethyl, bromo, chloro, and fluoro groups on the porphyrin unit, which allowed us to explicitly study the effects of electron-donating and electron-withdrawing substituents on catalytic performance in MOFs. Owing to the different electronic properties of ethyl, bromo, chloro, and fluoro substitutes, the molecular-level control over the chemical environment surrounding a catalytic center could be readily achieved in our MOFs. To investigate the effects of these substitutes on catalytic activity and selectivity, the oxidation of 3-methylpentane to corresponding alcohols and ketones was utilized as a model reaction. Within these five analogues of PCN-224, an extremely high turnover number of 7680 and turnover frequency of 10 240 h–1 was achieved by simply altering the substitutes on porphyrin rings. Moreover, a remarkable 99% selectivity of the tertiary alcohol over the five other possible by-products are realized. We demonstrate that this strategy can be used to efficiently screen a suitable peripheral environment around catalytic cores in MOFs for catalysis
