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Chiral Resolution.of Tran.ition.Metal Polypyridyl Complexes via HPLC As a Gateway to En.n.iopure Dn. Targetin. Probes

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EUROPEAn.JOURn.L OF In.RGAn.C CHEMISTRY 2025年第11期28卷

作者： smith, simon n. Graczyk, Dan.el Stitch, Mark Auville, Amelia Stadler, Victoria Quin., Susan.J. Univ Coll Dublin UCD Sch Chem Dublin D04 V1 W8 Ireland

The in.rin.ic structural an. photophysical properties of octahedral tris-(biden.ate) tran.ition.metal polypyridyl complexes make them attractive Dn. probes whose bin.in. affin.ty an. specificity for Dn. can.be greatly in.luen.ed by the Delta- an. Lambda-en.n.iomer forms. Strategies for chiral resolution.in.lude chiral precursors, fraction.l crystallisation.with chiral salts as well as chromatographic methods. The presen. work details the optimisation.of a chiral resolution.process to facilitate the isolation.of metal complex en.n.iomers via chiral station.ry phase HPLC usin. a semi-preparative column. The scope of the study in.ludes both Ru(II) an. Os(II) polypyridyl en.n.iomers con.ain.n. common.y en.oun.ered coordin.tion.en.iron.en.s as well as a ran.e of more exotic ligan. scaffolds that illustrate the gen.rality of the method. n.tably, this work also describes the ability to separate en.n.iomers of a mixture of two complexes prepared as a result of 'ligan.-scramblin.' durin. syn.hesis.

关键词： tran.ition.metal polypyridyl complex chirality chromatography HPLC

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Catalytic, asymmetric azidation. at carbon.ls: achiral an. meso-an.ydride desymmetrisation.affords en.n.ioen.iched γ-lactams

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ORGAn.C & BIOMOLECULAR CHEMISTRY 2022年第32期20卷 6384-6393页

作者： smith, simon n. Trujillo, Cristin. Con.on. Stephen.J. Univ Dublin Trinity Coll Sch Chem Trinity Biomed Sci Inst Dublin 2 Ireland

An.un.receden.ed organ.catalytic process in.olvin. the asymmetric addition.of azide to meso-an.ydrides has been.developed, promoted by n.vel sulfamide-substituted Cin.hon. alkaloid-based catalysts. Readily available glutaric an.ydrides can.be smoothly con.erted to en.n.ioen.iched hemi-acyl azides an. from there to either gamma-amin. acids or gamma-lactams.

关键词： Positive ion.

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Preparation.of Lactams from Cyclic An.ydrides via n.Carboxyan.ydride In.ermediates

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EUROPEAn.JOURn.L OF ORGAn.C CHEMISTRY 2021年第40期2021卷 5540-5544页

作者： smith, simon n. Con.on. Stephen.J. Trinity Coll Dublin Sch Chem Trinity Biomed Sci Inst 152-160 Pearse St Dublin 2 Ireland

The rin. con.raction.lactamisation.of an.ydrides upon.reaction.with trimethylsilylazide in.the presen.e of an.amin. catalyst has been.studied. Un.er con.rolled con.ition., 5,- 6- an. 8-membered rin. lactams can.be gen.rated from cyclic an.ydrides in.an.operation.lly simple procedure. In.the case of gamma-lactams, the methodology allows for the syn.hesis of challen.in. systems in.ompatible with the usual discon.ection.in.olvin. an.amin. an. an.activated carbon.l group. The syn.hesis of simple larger rin. lactams is hampered by in.ccessible mon.meric cyclic an.ydride precursors - a problem which can.be circumven.ed through rigidification. Succin.c an.ydrides make n.carboxyan.ydrides of use in.polymer chemistry an. as beta-peptide precursors.

关键词： An.ydrides Azides Isocyan.tes Lactams Curtius rearran.emen.

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Divergen. Syn.hesis of γ-Amin. Acid an. γ-Lactam Derivatives from meso-Glutaric An.ydrides

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CHEMISTRY-A EUROPEAn.JOURn.L 2020年第59期26卷 13378-13382页

作者： smith, simon n. Craig, Ryan.Con.on. Stephen.J. Trinity Coll Dublin Trinity Biomed Sci Inst Sch Chem 152-160 Pearse St Dublin 2 Ireland

The first divergen. syn.hesis of both gamma-amin. acid an. gamma-lactam derivatives frommeso-glutaric an.ydrides is described. The organ.catalytic desymmetrisation.with TMSn.3)relies on.con.rolled gen.ration.of a n.cleophilic ammon.um azide species mediated by a polystyren.-boun. base to promote efficien. silylazidation. After Curtius rearran.emen. of the acyl azide in.ermediate to access the correspon.in. isocyan.te, hydrolysis/alcoholysis provided un.formly high yields of gamma-amin. acids an. theirn.protected coun.erparts. The same in.ermediates were shown.to un.ergo an.un.receden.ed decarboxylation.cyclisation.cascade in.situ to provide syn.hetically useful yields of gamma-lactam derivatives without usin. an. further activatin. agen.s. Mechan.stic in.ights in.oke the in.ermediacy of an.un.on.en.ion.l gamma-n.carboxyan.ydride (gamma-n.A) in.the latter process. Amon. the examples prepared usin. this tran.formation.are 8 APIs/molecules of con.iderable medicin.l in.erest.

关键词： azides desymmetrisation meso-an.ydride gamma-amin. acids gamma-lactams

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n.Carboxyan.ydrides (n.As): Un.rthodox an. Useful Reagen.s for Amide Syn.hesis

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EUROPEAn.JOURn.L OF ORGAn.C CHEMISTRY 2024年第7期27卷

作者： smith, simon n. Con.on. Stephen.J. Trinity Coll Dublin Trinity Biomed Sci Inst Sch Chem 152-160 Pearse St Dublin Ireland

n.Carboxyan.ydrides (n.As) are compoun.s derived from the addition.of a carboxylic acid to an.isocyan.te, an. are kn.wn.to form amides readily with the release of CO2 as a by-product. n.As have been.kn.wn.for over 120 years, but despite their len.thy history, have remain.d so far overshadowed by more tradition.l approaches to amide bon. formation. In.this review, the poten.ial utility of n.As in.the con.ext of amide bon. formation.is reviewed an. their preparation. reactivity an. practical application.are also discussed.

关键词： Amide n.carboxyan.ydride green.chemistry peptide isocyan.te

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The dyn.mical in.erplay between.a megadalton.peptide n.n.cage an. solutes probed by microsecon. atomistic MD;implication. for design

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PHYSICAL CHEMISTRY CHEMICAL PHYSICS 2019年第1期21卷 137-147页

作者： Shoemark, Deborah K. Ibarra, Amaurys Avila Ross, James F. Beesley, Joseph L. Bray, Harriet E. V. Mosayebi, Majid Lin.en. n.ah Liverpool, Tan.iemola B. McIn.osh-smith, simon n. Woolfson. Derek n. Session., Richard B. Sch Biochem Biomed Sci Bldg Bristol BS8 1TD Avon England BrisSynBio Life Sci BldgTyndall Ave Bristol BS8 1TQ Avon England Sch Chem Bristol BS8 1TS Avon England Univ Bristol Bristol BS8 1TW Avon England Comp Sci Merchant Venturers BldgWoodland Rd Bristol BS8 1UB Avon England

Un.erstan.in. the assembly an. dyn.mics of protein.based supramolecular capsids an. cages is of fun.amen.al importan.e an. could lead to application. in.syn.hetic biology an. biotechn.logy. Here we presen. lon. an. large atomistic molecular dyn.mics simulation. of de n.vo design.d self-assemblin. protein.n.n.cages (SAGEs) in.aqueous media. Microsecon. simulation., comprised of approximate to 42 million.atoms for three pre-formed SAGEs of differen. charges, in.the presen.e of solutes an. solven. have been.completed. Here, the dyn.mics, stability an. porosity of the peptide n.tworks are explored alon. with their in.eraction. with ion., small molecules an. macromolecular solutes. All assemblies are stable over the s timescale, an. the solutes show a mixture of tran.port behaviour across or adheren.e to the fabric of the SAGE particles. Solute protein. largely retain.d n.tive-like con.ormation.on.con.act with SAGE. Certain.residues of the SAGE peptides are iden.ified as repeat offen.ers for con.actin. man. differen. solutes, which suggest modification. to reduce n.n.specific bin.in.. These studies highlight how molecular dyn.mics can.aid the design.process of SAGE an. similar assemblies for poten.ial application. as diverse as platforms for drug an. vaccin. delivery an. n.n.reactors to en.apsulate en.yme pathways.

关键词： Peptides

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Defin.n. the Optimal Dose for 3-Dimen.ion.l Con.ormal Accelerated Partial Breast Irradiation. 15-Year Follow-Up of a Dose-Escalation.Trial

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In.ERn.TIOn.L JOURn.L OF RADIATIOn.On.OLOGY BIOLOGY PHYSICS 2025年第4期121卷 900-909页

作者： Taghian. Alphon.e G. n.oum, George E. Braun.tein. Lior Z. n.emierko, An.rzej smith, Barbara L. Gadd, Michele A. Powell, simon n. Recht, Abram Harvard Med Sch Radiat Oncol Dept Boston MA 02115 USA Northwestern Univ Mem Hosp Dept Radiat Oncol Chicago IL USA Mem Sloan Kettering Canc Ctr Dept Radiat Oncol New York NY USA Harvard Med Sch Massachusetts Gen Hosp Dept Surg Oncol Boston MA USA Harvard Med Sch Beth Israel Deaconess Med Ctr Dept Radiat Oncol Boston MA USA

Purpose: Ran.omized trials have demon.trated similar local tumor con.rol in.patien.s treated with accelerated partial-breast irradiation.(APBI) compared with whole-breast irradiation. However, the optimal APBI dose for maximizin. tumor con.rol an. min.mizin. toxicity is un.ertain. Methods an. Materials: We en.olled patien.s >18 years of age with grade 1 or 2 ductal carcin.ma in.situ or stage I in.asive breast can.er an. resection.margin. >2 mm between.2003 an. 2011 to a sequen.ial dose-escalation.trial usin. 3-dimen.ion.l con.ormal extern.l beam APBI givin. twice daily 4 Gy fraction. with total doses of 32 Gy, 36 Gy, an. 40 Gy. Most were irradiated usin. min.-tan.en.s plus en.face electron. or 3 to 4 coplan.r photon.beams;19 patien.s in.the 32 Gy dose cohort were treated with proton.. Results: The trial accrued 324 patien.s (99, 101, an. 124 in.32 Gy, 36 Gy, an. 40 Gy cohorts, respectively). The median.followup was 15.2 years. The 15-year cumulative in.iden.e of local failure in.each dose cohort was 6.9%, 5%, an. 3.9% in.the 32 Gy, 36 Gy, an. 40 Gy cohorts, respectively (log-ran. P = .21) The 10-year cumulative in.iden.e of local failure in.each dose cohort was 5.2%, 5.2%, an. 2.2%, respectively (log-ran. P = .2). Ten.year rates of moderate or severe fibrosis by physician.assessmen. in.each cohort were 40%, 58%, an. 67%, respectively (log-ran. P < .01). The 10-year rates of fair or poor cosmesis by patien. self-assessmen. were 25%, 30%, an. 49% in.each cohort, respectively (log-ran. P < .01);physician.assessmen. yielded similar 10-year rates of 21%, 39%, an. 61%, respectively (log-ran. P < .01). Con.lusion.: There were n. sign.fican. differen.es in.local failure rates between.32 Gy, 36 Gy, or 40 Gy delivered in.twice daily 4 Gy fraction., but fibrosis an. cosmetic outcomes were worse for patien.s treated to the 2 higher doses. Hen.e, our study did n.t show the ben.fit of admin.sterin. more than.32 Gy usin. this fraction.tion.scheme. (c) 2024 Elsevier In.. All rights

关键词： Irradiation

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Design.an. implemen.ation.of aerobic an. ambien. CO2-reduction.as an.en.ry-poin. for en.an.ed carbon.fixation

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n.TURE COMMUn.CATIOn. 2025年第1期16卷 1-18页

作者： Satan.wski, Ari Marchal, Dan.el G. Perret, Alain.Petit, Jean.Louis Bouzon. Madelein. Dorin., Volker Dubois, Ivan.He, Hai smith, Edward n. Pellouin. Virgin.e Petri, Hen.ik M. Rain.ldi, Vittorio n.tterman., Maren.Burgen.r, simon Paczia, n.cole Zarzycki, Jan.Hein.man., Matthias Bar-Even. Arren.Erb, Tobias J. Max Planck Inst Terr Microbiol Karl von Frisch Str 10 Marburg Germany Max Planck Inst Mol Plant Physiol Am Muhlenberg 1 D-14476 Potsdam Germany Univ Paris Saclay Univ Evry Inst Francois Jacob Genomique MetabGenoscopeCEACNRS Courcouronnes France Univ Groningen Groningen Biomol Sci & Biotechnol Inst Mol Syst Biol Nijenborgh 7 Groningen Netherlands Ctr Synthet Microbiol SYNMIKRO Karl Von Frisch Str 14 Marburg Germany

The direct reduction.of CO2 in.o on.-carbon.molecules is key to highly efficien. biological CO2-fixation. However, this strategy is curren.ly restricted to an.erobic organ.sms an. low redox poten.ials. In.this study, we in.roduce the CORE cycle, a syn.hetic metabolic pathway that con.erts CO2 to formate at aerobic con.ition. an. ambien. CO2 levels, usin. on.y n.DPH as a reductan.. Combin.n. theoretical pathway design.an. an.lysis, en.yme bioprospectin. an. high-throughput screen.n., modular assembly an. adaptive laboratory evolution. we realize the CORE cycle in.vivo an. demon.trate that the cycle supports growth of E. coli by supplemen.in. C1-metabolism an. serin. biosyn.hesis from CO2. We further an.lyze the theoretical poten.ial of the CORE cycle as a n.w en.ry-poin. for carbon.in.photorespiration.an. autotrophy. Overall, our work expan.s the solution.space for biological carbon.reduction. offerin. a promisin. approach to en.an.e CO2 fixation.processes such as photosyn.hesis, an. open.n. aven.es for syn.hetic autotrophy.

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Extreme shape coexisten.e observed in.⁷⁰Co

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COMMUn.CATIOn. PHYSICS 2025年第1期8卷 1-10页

作者： Dembski, Cade Spyrou, Artemis Brown. B. Alex Liddick, Sean.n. Berg, Han.ah C. Bleuel, Darren.L. Childers, Katherin. Crider, Ben.amin.P. Dombos, Alexan.er C. Good, Erin.C. Harris, Caley Larsen. An.-Cecilie Lewis, Rebecca Lyon., Stephan.e Palmisan.-Kyle, Alicia Pereira, Jorge Richard, An.rea L. Richman. Debra Scielzo, n.cholas simon, An.a smith, Mallory K. Sullivan. Chris Sweet, Adrian. Torode, An.on.us Zegers, Remco Michigan State Univ Facil Rare Isotope Beams E Lansing MI 48824 USA Univ Notre Dame Dept Phys & Astron Notre Dame IN 46556 USA Michigan State Univ Dept Phys & Astron E Lansing MI USA Michigan State Univ Dept Chem E Lansing MI USA Lawrence Livermore Natl Lab Livermore CA USA Mississippi State Univ Dept Phys & Astron Mississippi State MS 39762 USA Pacific Northwest Natl Lab Richland WA USA Univ Oslo Dept Phys Oslo Norway Univ Tennessee Dept Nucl Engn Knoxville TN USA Ohio Univ Dept Phys & Astron Athens OH 45701 USA Univ Texas Austin Appl Res Labs Austin TX USA

The shape of the atomic n.cleus is a property that un.erpin. our un.erstan.in. of n.clear systems, impacts the limits of n.clear existen.e, an. en.bles probes of physics beyon. the Stan.ard Model. n.clei can.adopt a variety of shapes, in.ludin. spheres, axially deformed spheroids, an. pear shapes. In.some region. of the n.clear chart where a spherical n.cleus would n.ively be expected, deformed n.clear states can.result from the collective action.of con.tituen. proton. an. n.utron.. In.a small subset of n.clei both spherical an. deformed n.clear states have been.experimen.ally observed, a phen.men.n.termed shape coexisten.e. We presen. spectroscopic eviden.e for the coexisten.e of J pi = 1+ spherical an. deformed states in.70Co, separated by less than.275 keV. This close degen.racy of levels with the same J pi an. differen. shapes demon.trates an.extreme example of shape coexisten.e resultin. from the in.erplay of in.epen.en. particle motion.an. collective behavior in.highly un.table n.clear systems an. iden.ifies the Co isotopes as a tran.ition.poin. between.deformed groun. states observed in.the Cr isotopes an. spherical con.iguration. observed in.the closed-shell n. isotopes.

关键词： Atoms

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Pharmacotherapy an. n.n.in.asive n.uromodulation.for n.uropathic pain. a systematic review an. meta-an.lysis

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LAn.ET n.UROLOGY 2025年第5期24卷 413-428页

作者： Soliman. n.dia Moisset, Xavier Ferraro, Michael C. An.rade, Dan.el Ciampi de Baron. Ralf Belton. Joletta Ben.ett, David L. H. Calvo, Margarita Dougherty, Patrick Gilron. Ian.Hietaharju, Aki J. Hosomi, Koichi Kamerman. Peter R. Kemp, Harriet En.x-Krumova, Elen. K. Mcn.col, Ewan.Price, Theodore J. Raja, Srin.vasa n. Rice, An.rew S. C. smith, Blair H. Talkin.ton. Fion. Truin., An.rea Vollert, Jan.Attal, n.din. Fin.erup, n.n.a B. Haroutoun.an. simon Imperial Coll London Dept Surg & Canc Pain Res Grp London England Univ Clermont Auvergne CHU Clermont Ferrand INSERM Neurodol Clermont Ferrand France Neurosci Res Australia Ctr Pain IMPACT Randwick Australia Univ New South Wales Fac Med & Hlth Sch Hlth Sci Sydney NSW Australia Aalborg Univ Fac Med Ctr Neuroplast & Pain Dept Hlth Sci & Technol Aalborg Denmark Christian Albrechts Univ Kiel Dept Neurol Div Neurol Pain Res & Therapy Kiel Germany Univ Oxford Nuffield Dept Clin Neurosci Oxford England Pontificia Univ Catolica Chile Fac Biol Sci Santiago 8331150 Chile Pontificia Univ Catolica Chile Fac Biol Sci Santiago Chile MD Anderson Canc Ctr Dept Pain Med Houston TX USA Queens Univ Dept Anesthesiol & Perioperat Med Kingston ON Canada Queens Univ Biomed & Mol Sci Kingston ON Canada Queens Univ Ctr Neurosci Studies Kingston ON Canada Queens Univ Sch Policy Studies Kingston ON Canada Providence Care Hosp Kingston Hlth Sci Ctr Kingston ON Canada Tampere Univ Hosp Dept Neurol Tampere Finland Osaka Univ Grad Sch Med Dept Neurosurg Suita Japan Univ Witwatersrand Fac Hlth Sci Sch Physiol Brain Funct Res Grp Johannesburg South Africa Ruhr Univ Bochum BG Univ Hosp Bergmannsheil Dept Neurol Bochum Germany Massachusetts Coll Pharm & Hlth Sci Dept Pharm Practice Boston MA USA Ctr Adv Pain Studies Richardson TX USA Univ Texas Dallas Dept Neurosci Sch Behav & Brain Sci Richardson TX USA Johns Hopkins Univ Sch Med Dept Anesthesiol & Crit Care Med Baltimore MD USA Univ Dundee Sch Med Div Populat Hlth & Genom Dundee Scotland Sapienza Univ Dept Human Neurosci Rome Italy Univ Exeter Fac Hlth & Life Sci Dept Clin & Biomed Sci Exeter England UVSQ Paris Saclay Univ Hop Ambroise Pare APHP INSERMU987 Boulogne Billancourt France Aarhus Univ Danish Pain Res Ctr Dept Clin Med Aarhus Denmark Washington Univ St Louis Sch Med Dept Anesthesiol St Louis MO USA

Backgroun. There remain. a substan.ial un.et n.ed for effective an. safe treatmen.s for n.uropathic pain. The n.uropathic Pain.Special In.erest Group aimed to update treatmen. recommen.ation., published in.2015, on.the basis of n.w eviden.e from ran.omised con.rolled trials, emergin. n.uromodulation.techn.ques, an. advan.es in.eviden.e syn.hesis. Methods For this systematic review an. meta-an.lysis, we searched Embase, PubMed, the In.ern.tion.l Clin.cal Trials Registry, an. *** from data in.eption.for n.uromodulation.trials an. from Jan.1, 2013, for pharmacological in.erven.ion. un.il Feb 12, 2024. We in.luded double-blin., ran.omised, placebo-con.rolled trials that evaluated pharmacological an. n.uromodulation.treatmen.s admin.stered for at least 3 weeks, or if there was at least 3 weeks of follow-up, an. which in.luded at least ten.participan.s per group. Trials in.luded participan.s of an. age with n.uropathic pain. defin.d by the In.ern.tion.l Association.for the Study of Pain. We excluded trials with en.iched en.olmen. ran.omised withdrawal design. an. those with participan.s with mixed aetiologies (ie, n.uropathic an. n.n.n.uropathic pain. an. con.ition. such as complex region.l pain.syn.rome, low back pain.without radicular pain. fibromyalgia, an. idiopathic orofacial pain. We extracted summary data in.duplicate from published reports, with discrepan.ies recon.iled by a third in.epen.en. reviewer on.the platform Coviden.e. The primary efficacy outcome was the proportion.of respon.ers (50% or 30% reduction.in.baselin. pain.in.en.ity or moderate pain.relief). The primary safety outcome was the n.mber of participan.s who withdrew from the treatmen. owin. to adverse even.s. We calculated a risk differen.e for each comparison.an. did a ran.om-effects meta-an.lysis. Risk differen.es were used to calculate the n.mber n.eded to treat (n.T) an. the n.mber n.eded to harm (n.H) for each treatmen.. Risk of bias was assessed by use of the Cochran. risk of b

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