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Photoremovable Protecting Groups in Chemistry and. Reaction Mechanisms and Efficacy. Introduction. Photoremovable (sometimes called photoreleasable, photocleavable. PPGs) provide spatial and. Ca. 2+ ions, oxidants, insecticides, pheromones, fragrances, etc. The latter authors. PPG. Two general perspectives. PPGs in synthesis,8 biochemistry and. The present review covers recent developments. PPGs, which are used to release organic molecules. Photoactivation. of small inorganic species and ions, such as NO,1. CO,1. 6 Ca. 2+,9h,1. Zn. 2+,1. 8 Cd. 2+,1. Cu+,2. 0 is not covered. Simplified basic structures of the photoremovable. Table 1 (the leaving groups are shown in red). Photoremovable Protecting Groups. The criteria for the design of a good PPG. The Thiol-Michael Addition Click Reaction: A Powerful and Widely Used Tool in Materials Chemistry. Capture Technology. Advanced algorithms for better mobile photography and videography Face Detection, Tracking & Recognition. Accurately captures, personalizes. The quantum yield . An important measure for the efficacy. PPG is the product of the quantum yield and the molar decadic. Hence. the PPGs must be pure, exhibit low intrinsic activity, and be stable. The PPGs should be soluble in the. The photochemical byproducts accompanying. Moreover, they must be biocompatible, i. To study the kinetics of rapid responses. PPG must be excited by a short light pulse and the appearance rate constant kapp of the desired. Commonly, there are several reaction steps involving. Therefore, detailed knowledge of the reaction. The decay of their primary quinonoid intermediates. Moreover, photolysis. Quite a. number of alternative PPGs have been developed that do not suffer. The appearance rate constant kapp of. Release rate constants, kr =. Note that the release rate constant kr may be higher or lower than the more relevant. Case (a): kr < kapp if . A trivial example. Scheme 1. Case (b): kr > kapp if the. Simple Case Where the Release Rate Constant of the. Leaving Group) X, kr, Is Smaller than. Its Appearance Rate Constant, kapp. The speed of release is an ambivalent expression. PPG, . The absorption spectra of a number of chromophores frequently. PPGs are shown in Figure . Arylcarbonylmethyl Groups. Aromatic ketones. The lowest energy transition of simple carbonyl. Hydrogen bonding of protic solvents to the carbonyl oxygen stabilizes. Both electron- donating. The lowest . Examples of the absorption spectra. PPG aryl ketones are provided in Figure . Scheme 2 shows. the most important photoreactions that lead to the liberation of a. X) and are discussed in the following paragraphs. Ketones. with n. The singlet or triplet n. The reaction intermediates hereby formed. X– from the . Entry 5 shows the p- hydroxyphenacyl. Favorskii rearrangement to release. X–. Finally, the benzoin derivative in entry 6 releases. X– to form 2- phenylbenzofuran. Photochemistry of. Aromatic Ketones that Release a Leaving Group (X)2. Phenacyl and Other Related Arylcarbonylmethyl. Groups. Using phenacyl compounds as PPGs has been a subject. Homolytic scission of. C–O bond, which would result in the formation of. Instead, a. mechanism that involves hydrogen abstraction from a hydrogen- atom. Scheme 2) has been established by laser. Excited phenacyl. Singh and co- workers. This PPG strategy will be discussed in section 8. When a relatively stable radical can. This has been demonstrated in the reactions of phenacyl. An alternative mechanism, formation of the phenacylium. C–N bond, has been proposed. Recently Kl. Liberation of R. Depending on the presence or absence of H- atom. For example. 2- methylacetophenone (3) undergoes intramolecular 1,5- hydrogen. E) that yields two isomeric, (E)- and (Z)- , photoenols, whereas fast. Z)- isomer (Scheme 4). This scheme may serve as a blueprint. The (Z)- isomer, having a lifetime similar to that of the triplet. Its lifetime is. solvent- dependent because hydrogen bonding of the hydroxyl group to. In contrast, reketonization of the (E)- dienols requires intermolecular proton transfer that. The resulting long lifetime of the (E)- isomers in dry solvents allows for thermal conrotatory. In general, the indanone. Photochemistry of. Alkylphenacyl Compounds. This reaction, reported for the first time on. Bergmark,5. 6 was shown by. Kl. Studies by laser flash. E, and two longer- lived, ground- state photoenols assigned to the corresponding. Z)- and (E)- photoenols. For example, the (E)- photoenol. Z)- photoenol (. The mechanism. DMP benzoate (8) photolysis, determined by laser flash. LFP) in degassed methanol, is displayed in Scheme 6. Three intermediates. In this case. only the longer- lived (E)- photoenol. Wang. and co- workers used the DMP photoremovable group in polymer- supported. Park and Lee showed that. On the other hand, the photochemistry. In such cases. releasing the leaving group is not of primary interest; it is designed. Wessig and co- workers used this concept to prepare. B or C (e. g., 1. Scheme 8), in which the key step is the photoenolization reaction of 1. Kl. The authors demonstrated that the photoenols produced by. The same research group also reported that irradiation of. An electronic excited- state. The excited- state character of the parent compound was. In addition. competition of a triplet- state photoenolization reaction with a photo- Favorskii. Photochemistry. of 2- (Alkoxymethyl)- 5- methyl- . The leaving group was reported to be released. Interestingly. irradiation of 2- acetylphenyl- or 2- benzoylphenylacetic acid results. CO2. 7. 7Photochemistry of 1- . Gudmundsdottir and. Z)- and (E)- photoenols are produced by irradiation. Scheme 1. 3). 8d,8. An alcohol, such as geraniol (in up to 9. Methylbenzoyl)benzoate esters are not. In. addition, the 4- oxo- 4- o- tolylbutanoate 2. Scheme 1. 4). 8. 1Photochemistry of 2- (2- Isopropylbenzoyl)benzoate Esters. The purported intermediate. Scheme 1. 5 is reminiscent. Favorskii rearrangement; 8. Favorskii rearrangement. UV–vis. absorption spectra of p- hydroxyphenacyl. X = OPO(OEt)2; p. HP. DEP; dashed, red) and p- hydroxyphenylacetic acid. R = H; black) in H2. O/Me. CN (1: 1). 8. Hydroxyacetophenone (p. HA, 2. 4, X. = H) serves as a model for the p. HP chromophore. In some instances. Nucleophilic Substitution Routes for p. HP (2. 4) Functional. Group Protection. More complex syntheses are required for more reactive. HP ATP (2. 4, X = ATP),8. HP GTP,9. 1 and 1. O- labeled isotopomers of p. HP. GTP. 9. 1,9. 2p- Hydroxyphenacyl monophosphates. HP Br (2. 4, X = Br) or through esterification of 2,4. These protected nucleosides have found several. An advantage of this. O- labeled. isotopomers of GTP9. Fourier transform. TR- FTIR) studies. Of the leaving groups thus far explored. Advantages of the diazoketone approach. The yields are. generally good, and the only byproduct is N2. Furthermore. protection of the phenolic OH group or other, less acidic functional. When the phenolic. OH does require protection, the acetate ester is either retained or. Strategies for . A recent, detailed. HA and the ensuing proton transfer reactions in aqueous solution. Scheme 1. 8): Following fast and. ISC of excited p. HA, . The latter is formed. HA–*. The equilibrium 3p. Q* . The formation of 3p. Q* from 3p. HA*. is accelerated by strong acids (via the protonated species 3. Hp. HA+*) and is suppressed by buffer bases, which form 3p. HA–* upon encounter with 3p. HA*. Adapted with Permission from Ref (8. Copyright 2. 01. 2 American. Chemical.. It has been suggested. HP PPGs, especially those carrying poor leaving. HP triplet anion and the. Furthermore, earlier studies. HP phosphate and carboxylate esters had documented the importance. ET = 7. 1. 2 kcal mol–1). Subsequent work by Wan and Corrie,9. Phillips. 85a,8. 5b,9. 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Maybe there's been infidelity or some other trust broken or whatever it might be. There's a cooling of the relationship. The one that catches my attention is when people say, . What I like to say is, . It takes effort. It doesn't just happen. It's not, you know, just coming out of the ground and you're loving each other endlessly. It takes effort. And it such a tragedy in our culture today that we have removed God from His plan for marriage. I mean, He's the one that designed it. I often smile because man, He's got a knack for pulling opposite people together. I mean, He has wired us that way. Introvert meets extrovert. It's what God placed there. And rightfully, the question is, why did He do that? I think the answer is so you could become more like Him, because it's gonna require selflessness to be successful in that marriage. And He's smilin' goin', . This quick reminder that here at Focus on the Family, we have resources and tools. We have counselors and we have our Hope Restored marriage intensive. We have a lot to offer couples who either need some minor tune- up with regard to the relationship or major overhaul, because those differences are becoming more and more profound. And so, let me encourage you to call us. Our number is 8. 00- A- FAMILY or stop by www. Body: Jim: If you didn't hear the conversation last time with Mark and Jill Savage, I recommend you get the download or CD. Get the app on your Smartphone, whatever you need to do. It was terrific. I mean, it talked about the way we think as human beings, the vulnerability of us. You will appreciate what we have done there in order to set up today. And today we're gonna talk about deeper pain and those things that were causing difficulties in the Savage's marriage. To give a little bit of background, they were in public ministry. Jill was the founder and CEO of Hearts at Home. Mark was a pastor for 2. They would write and speak on family issues, helping save the marriages of others and at the same time, their marriage was crumbling. Let me welcome both of you back to the broadcast. What an introduction, right? Your marriage (Laughter) was crumbling. But you know what's so good about it and we're gonna get there, here you are today. Mr. Mark Savage, Mrs. Jill Savage: Uh- hm. Jim: You're at the table. Mark: Absolutely. Jim: You're together. Jill: That's right. Jim: You're still married. Mark: Yeah. Jill: That's right. Jim: And I just give you so many accolades for fighting through that and doing what the Lord would want done, even in difficult circumstances. Mark, we left off last time where you were just beginning to share 2. You left the pastorate. You're depressed really. I mean, that's what it sounded like to me. You were in a mid- life crisis. Jill, years before had, had this heart flutter for a coworker. She came to you and said, . Let's fix this. We gotta get it take care of. Jill left her job, got out of that situation, but now years later, you're the man. As Nathan said to David. You're the one. Mark: Yes. Jim: Describe briefly what took place and then we'll go to the healing portion. Mark: What took place was my disillusionment and mistrust of God was at the core of all of this. And it played out in experiencing or believing out of my own brokenness, that my marriage was just too hard. Life was too hard. It wasn't worth it. I to start over. I needed something new. I took the steps to pursue something new. I found a new relationship. I left Jill and my kids and (Emotional) I'm sorry. I left Jill and my kids, believing that, that new relationship was gonna be the cure- all. But the problem was, I took somebody with me and that was me. In pursuing this new relationship, what I am so grateful for is, that God just kept pursuing me. 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But there was a turning point for me where I moved it in my head and my heart from being about me to recognizing the confusion that he was in. And I think honestly, that's what allowed me to stay in the game for a while because I began, instead of seeing . It's coming from within. Jill: Scary, uh- hm. Jim: Some people have said, . I was angry. 1 thing you do is pour your heart out to God. I mean, you lay it out there and you express your anger to Him. I mean, Many times . So, I think part of it is, you know, being honest with God. And that doesn't mean . It's really messy. Jim: And don't pretend in that process. Don't feel one way about your spouse and then turn to God and act a different way. Jill: Um- um, no. Jim: Bring that over. Talk to the Father about that. Jill: You don't have to get cleaned up before you talk to Him. You just lay it out there. He knows. Jim: Yeah, He wants your heart. Jill: And not only that, but Christ was betrayed. I mean, you talk about somebody understanding betrayal. Your God gets it. Jim: Hm. Jill: And so, just even remembering that, it's not lost. The pain of that is not lost on Him. Jim: Jill, you meet with many women who have been wounded in this way and I can imagine you get the whole spectrum of response. How do you think through, without giving a free pass—Jill: Uh- hm. Jim: - -to your spouse to say, that's okay, so that it might happen again without any consequence, that's not healthy. Jill: Right. Jim: But how do you balance all that? Just speak to the spectrum of voices of women that you've heard from, from hardcore: ? What can You do through me? And he stopped going to counseling. I continued to go and my counselor was helpful in me trying to figure out the balance between grace- filled love and boundary- filled love. And there had to be both. So, for instance, when he left, one of the things I did is, I changed the locks on the house. 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