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You searched for: Journal Journal of the American Chemical Society Remove constraint Journal: Journal of the American Chemical Society Publication Year 2018 Remove constraint Publication Year: 2018 Source 2018 v.140 no.30 Remove constraint Source: 2018 v.140 no.30 Text Availability Citation in PubAg Remove constraint Text Availability: Citation in PubAg
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1. Energy Landscape in Supramolecular Coassembly of Platinum(II) Complexes and Polymers: Morphological Diversity, Transformation, and Dilution Stability of Nanostructures

Author:
Zhang, Kaka; Yeung, Margaret Ching-Lam; Leung, Sammual Yu-Lut; Yam, Vivian Wing-Wah
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9594-9605
ISSN:
1520-5126
Subject:
ambient temperature; annealing; composite polymers; kinetics; nanofibers; platinum; sonication; thermodynamics
Abstract:
... Establishment of energy landscape has emerged as an efficient pathway for improved understanding and manipulation of both thermodynamic and kinetic behaviors of complicated supramolecular systems. Herein, we report the establishment of energy landscapes of supramolecular coassembly of platinum(II) complexes and polymers, as well as the fabrication of nanostructures with enhanced complexity and int ...
DOI:
10.1021/jacs.8b04779

2. The Difluoromethyl Group as a Masked Nucleophile: A Lewis Acid/Base Approach

Author:
Geri, Jacob B.; Wade Wolfe, Michael M.; Szymczak, Nathaniel K.
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9404-9408
ISSN:
1520-5126
Subject:
Lewis acids; Lewis bases; ambient temperature; aromatic hydrocarbons; drugs; lipophilicity; moieties; pharmacokinetics
Abstract:
... The difluoromethyl group (R–CF₂H) imparts desirable pharmacokinetic properties to drug molecules and is commonly targeted as a terminal functional group that is not amenable to further modification. Deprotonation of widely available Ar–CF₂H starting materials to expose nucleophilic Ar–CF₂– synthons represents an unexplored, yet promising route to construct benzylic Ar–CF₂–R linkages. Here we show ...
DOI:
10.1021/jacs.8b06093

3. Stereodivergent Rhodium(III)-Catalyzed cis-Cyclopropanation Enabled by Multivariate Optimization

Author:
Piou, Tiffany; Romanov-Michailidis, Fedor; Ashley, Melissa A.; Romanova-Michaelides, Maria; Rovis, Tomislav
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9587-9593
ISSN:
1520-5126
Subject:
alkenes; catalytic activity; diastereoselectivity; energy; ligands; rhodium; statistical models; stereochemistry
Abstract:
... The design of stereodivergent transformations is of great interest to the synthetic community as it allows funneling of a given reaction pathway toward one stereochemical outcome or another by only minor adjustments of the reaction setup. Herein, we present a physical organic approach to invert the sense of induction in diastereoselective cyclopropanation of alkenes with N-enoxyphthalimides throug ...
DOI:
10.1021/jacs.8b04243

4. Antifreeze Glycoproteins Bind Irreversibly to Ice

Author:
Meister, Konrad; DeVries, Arthur L.; Bakker, Huib J.; Drori, Ran
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9365-9368
ISSN:
1520-5126
Subject:
adsorption; antifreeze proteins; borates; crystals; fluorescence microscopy; growth retardation; ice
Abstract:
... Antifreeze proteins (AFPs) and antifreeze glycoproteins (AFGPs) inhibit ice growth via an adsorption-inhibition mechanism that assumes irreversible binding of AF(G)Ps to embryonic ice crystals and the inhibition of further growth. The irreversible binding of antifreeze glycoproteins (AFGPs) to ice has been questioned and remains poorly understood. Here, we used microfluidics and fluorescence micro ...
DOI:
10.1021/jacs.8b04966

5. Conformationally Regulated Peptide Bond Cleavage in Bradykinin

Author:
Fuller, Daniel R.; Conant, Christopher R.; El-Baba, Tarick J.; Brown, Christopher J.; Woodall, Daniel W.; Russell, David H.; Clemmer, David E.
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9357-9360
ISSN:
1520-5126
Subject:
biological resistance; bradykinin; cleavage (chemistry); humans; isomerization; mass spectrometry; temperature
Abstract:
... Ion mobility and mass spectrometry techniques are used to investigate the stabilities of different conformations of bradykinin (BK, Arg¹-Pro²-Pro³-Gly⁴-Phe⁵-Ser⁶-Pro⁷-Phe⁸-Arg⁹). At elevated solution temperatures, we observe a slow protonation reaction, i.e., [BK+2H]²⁺+H⁺ → [BK+3H]³⁺, that is regulated by trans → cis isomerization of Arg¹-Pro², resulting in the Arg¹-cis-Pro²-cis-Pro³-Gly⁴-Phe⁵-Ser ...
DOI:
10.1021/jacs.8b04751

6. Rational Design and Facile Synthesis of a Highly Tunable Quinoline-Based Fluorescent Small-Molecule Scaffold for Live Cell Imaging

Author:
Jun, Joomyung V.; Petersson, E. James; Chenoweth, David M.
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9486-9493
ISSN:
1520-5126
Subject:
catalytic activity; cross-coupling reactions; fluorescence; fluorescent dyes; image analysis; pH; palladium; regioselectivity; screening
Abstract:
... Small-molecule fluorescent probes are powerful tools for chemical biology; however, despite the large number of probes available, there is still a need for a simple fluorogenic scaffold, which allows for the rational design of molecules with predictable photophysical properties and is amenable to concise synthesis for high-throughput screening. Here, we introduce a highly modular quinoline-based p ...
DOI:
10.1021/jacs.8b03738

7. Total Synthesis of (−)-Nodulisporic Acids D, C, and B: Evolution of a Unified Synthetic Strategy

Author:
Zou, Yike; Li, Xiangqin; Yang, Yun; Berritt, Simon; Melvin, Jason; Gonzales, Stephen; Spafford, Matthew; Smith, Amos B.
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9502-9511
ISSN:
1520-5126
Subject:
alkylation; aromatic compounds; catalytic activity; cross-coupling reactions; cyclization reactions; diastereoselectivity; palladium
Abstract:
... A unified synthetic strategy leading to the total synthesis of (−)-nodulisporic acids D, C, and B is described. Key synthetic transformations include a nickel–chromium-mediated cyclization, an aromatic ring functionalization employing a novel copper-promoted alkylation, a palladium-catalyzed cross-coupling cascade/indole ring construction, and a palladium-mediated regio- and diastereoselective all ...
DOI:
10.1021/jacs.8b04053

8. Branch-Selective and Enantioselective Iridium-Catalyzed Alkene Hydroarylation via Anilide-Directed C–H Oxidative Addition

Author:
Grélaud, Simon; Cooper, Phillippa; Feron, Lyman J.; Bower, John F.
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9351-9356
ISSN:
1520-5126
Subject:
enantioselectivity
Abstract:
... Tertiary benzylic stereocenters are accessed in high enantioselectivity by Ir-catalyzed branch selective addition of anilide ortho-C–H bonds across styrenes and α-olefins. Mechanistic studies indicate that the stereocenter generating step is reversible. ...
DOI:
10.1021/jacs.8b04627

9. Thermodynamic Scale of β-Amino Acid Residue Propensities for an α-Helix-like Conformation

Author:
Fisher, Brian F.; Hong, Seong Ho; Gellman, Samuel H.
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9396-9399
ISSN:
1520-5126
Subject:
amino acids; nitrogen; thermodynamics; thioesters
Abstract:
... A thiol-thioester exchange system has been used to measure the propensities of diverse β-amino acid residues to participate in an α-helix-like conformation. These measurements depend on formation of a parallel coiled-coil tertiary structure when two peptide segments become linked by thioester formation. One peptide segment contains a “guest” site that accommodates diverse β residues and is distal ...
DOI:
10.1021/jacs.8b05162

10. Two-Dimensional Hierarchical Semiconductor with Addressable Surfaces

Author:
Choi, Bonnie; Lee, Kihong; Voevodin, Anastasia; Wang, Jue; Steigerwald, Michael L.; Batail, Patrick; Zhu, Xiaoyang; Roy, Xavier
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9369-9373
ISSN:
1520-5126
Subject:
chemical bonding; ligands; physicochemical properties; semiconductors
Abstract:
... Surfaces play a key role in determining material properties, and their importance is further magnified in the two-dimensional (2D) limit. Though monolayers are entirely composed of surfaces, there is no chemical approach to covalently address them without breaking intralayer bond. Here, we describe a 2D semiconductor that offers two unique features among 2D materials: structural hierarchy within t ...
DOI:
10.1021/jacs.8b05010

11. Selection between Diastereomeric Kinetic vs Thermodynamic Carbonyl Binding Modes Enables Enantioselective Iridium-Catalyzed anti-(α-Aryl)allylation of Aqueous Fluoral Hydrate and Difluoroacetaldehyde Ethyl Hemiacetal

Author:
Cabrera, James M.; Tauber, Johannes; Zhang, Wandi; Xiang, Ming; Krische, Michael J.
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9392-9395
ISSN:
1520-5126
Subject:
Lewis acids; acetates; aldehydes; allylation; binding sites; enantioselectivity; thermodynamics
Abstract:
... Enantioselectivity increases with increasing carbonyl electrophilicity in 2-propanol-mediated reductive couplings of aldehydes with branched aryl-substituted allylic acetates to form products of carbonyl anti-(α-aryl)allylation. This unusual phenomenon is caused by aldehyde coordination to diastereomeric kinetic vs thermodynamic carbonyl binding sites that deliver enantiomeric products. Exploiting ...
DOI:
10.1021/jacs.8b05725

12. Cu-Catalyzed Enantioselective Ring Opening of Cyclic Diaryliodoniums toward the Synthesis of Chiral Diarylmethanes

Author:
Li, Bin; Chao, Zengyin; Li, Chunyu; Gu, Zhenhua
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9400-9403
ISSN:
1520-5126
Subject:
carboxylic acids; catalysts; chemical bonding; crystal structure; enantioselectivity; models; salts; stereochemistry
Abstract:
... A Cu-catalyzed enantioselective desymmetrizing ring-opening reaction of six-membered cyclic diaryliodonium salts with carboxylic acids or thioacids is reported for the facile access to chiral diarylmethanes. A Cu/[cyclopropyl bis(oxazoline)] catalyst well discriminates two C–I bonds of prochiral cyclic diaryliodonium salts. A stereochemical model was proposed to rationalize the stereochemical outc ...
DOI:
10.1021/jacs.8b05743

13. Mechanism of Selective Enzyme Inhibition through Uncompetitive Regulation of an Allosteric Agonist

Author:
Boulton, Stephen; Selvaratnam, Rajeevan; Blondeau, Jean-Paul; Lezoualc’h, Frank; Melacini, Giuseppe
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9624-9637
ISSN:
1520-5126
Subject:
active sites; agonists; amino acids; binding sites; cyclic AMP; enzyme inhibition; enzyme substrates; mechanism of action; mutation; nuclear magnetic resonance spectroscopy; solubility; topology
Abstract:
... Classical uncompetitive inhibitors are potent pharmacological modulators of enzyme function. Since they selectively target enzyme–substrate complexes (E:S), their inhibitory potency is amplified by increasing substrate concentrations. Recently, an unconventional uncompetitive inhibitor, called CE3F4R, was discovered for the exchange protein activated by cAMP isoform 1 (EPAC1). Unlike conventional ...
DOI:
10.1021/jacs.8b05044

14. Site-Specific Protein Labeling with N-Hydroxysuccinimide-Esters and the Analysis of Ubiquitin Ligase Mechanisms

Author:
Dempsey, Daniel R.; Jiang, Hanjie; Kalin, Jay H.; Chen, Zan; Cole, Philip A.
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9374-9378
ISSN:
1520-5126
Subject:
chemoselectivity; protein structure; proteins; stoichiometry; thioesters; ubiquitin-protein ligase
Abstract:
... N-Hydroxysuccinimide (NHS)-esters are widely used to label proteins nonselectively on free amino groups. Such broad labeling can be disadvantageous because it can interfere with protein structure or function and because stoichiometry is poorly controlled. Here we describe a simple method to transform NHS-esters into site-specific protein labeling on N-terminal Cys residues. MESNA addition converts ...
DOI:
10.1021/jacs.8b05098

15. Comparison of Two Phosphinidenes Binding to Silicon(IV)dichloride as well as to Silylene

Author:
Kundu, Subrata; Sinhababu, Soumen; Siddiqui, Mujahuddin M.; Luebben, Anna V.; Dittrich, Birger; Yang, Tao; Frenking, Gernot; Roesky, Herbert W.
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9409-9412
ISSN:
1520-5126
Subject:
ambient temperature; carbenes; chlorine; silicon
Abstract:
... The cyclic alkyl(amino) carbene (cAAC) anchored silylene with two phosphinidenes was isolated as (cAAC)Si{P(cAAC)}₂ (3) at room temperature, which was synthesized from the reduction of (Cl₂)Si{P(cAAC)}₂ (2) using 2 equiv of KC₈. Compound 2 resulted from the reaction of 2 equiv of (cAAC)PK (1) with 1 equiv of SiCl₄. Compounds 2 and 3 are the first examples where two terminal phosphinidenes are bind ...
DOI:
10.1021/jacs.8b06230

16. Electrochemical CO Reduction Builds Solvent Water into Oxygenate Products

Author:
Lum, Yanwei; Cheng, Tao; Goddard, William A.; Ager, Joel W.
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9337-9340
ISSN:
1520-5126
Subject:
density functional theory; electrochemistry; electrolytes; ethanol; ethylene; oxygen; solvents; stable isotopes
Abstract:
... Numerous studies have examined the electrochemical reduction of CO (COR) to oxygenates (e.g., ethanol). None have considered the possibility that oxygen in the product might arise from water rather than from CO. To test this assumption, C¹⁶O reduction was performed in H₂¹⁸O electrolyte. Surprisingly, we found that 60–70% of the ethanol contained ¹⁸O, which must have originated from the solvent. We ...
DOI:
10.1021/jacs.8b03986

17. Highly Ordered and Field-Free 3D DNA Nanostructure: The Next Generation of DNA Nanomachine for Rapid Single-Step Sensing

Author:
Zhang, Pu; Jiang, Jie; Yuan, Ruo; Zhuo, Ying; Chai, Yaqin
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9361-9364
ISSN:
1520-5126
Subject:
DNA; biomarkers; equipment; hybridization; irradiation; locomotion; microRNA; nanomaterials; photoisomerization; wavelengths
Abstract:
... Herein, by directly using Watson–Crick base pairing, a highly ordered and field-free three-dimensional (3D) DNA nanostructure is self-assembled by azobenzene (azo)-functionalized DNA nippers in a few minutes, which was applied as a 3D DNA nanomachine with an improved movement efficiency compared to traditional Au-based 3D nanomachines due to the organized and high local concentration of nippers on ...
DOI:
10.1021/jacs.8b04648

18. Sulfide Protects [FeFe] Hydrogenases From O₂

Author:
Rodríguez-Maciá, Patricia; Reijerse, Edward J.; van Gastel, Maurice; DeBeer, Serena; Lubitz, Wolfgang; Rüdiger, Olaf; Birrell, James A.
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9346-9350
ISSN:
1520-5126
Subject:
Chlamydomonas reinhardtii; Desulfovibrio desulfuricans; air; hydrogen; iron; oxidation; oxygen; sulfides
Abstract:
... [FeFe] hydrogenases catalyze proton reduction and hydrogen oxidation with high rates and efficiency under physiological conditions, but are highly oxygen sensitive. The [FeFe] hydrogenase from Desulfovibrio desulfuricans (DdHydAB) can be purified under air in an oxygen stable inactive state Hₒₓᵃⁱʳ. The formation of the Hₒₓᵃⁱʳ state in vitro allows the handling of hydrogenases in air, making their ...
DOI:
10.1021/jacs.8b04339

19. Operando Evolution of the Structure and Oxidation State of Size-Controlled Zn Nanoparticles during CO₂ Electroreduction

Author:
Jeon, Hyo Sang; Sinev, Ilya; Scholten, Fabian; Divins, Nuria J.; Zegkinoglou, Ioannis; Pielsticker, Lukas; Cuenya, Beatriz Roldan
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9383-9386
ISSN:
1520-5126
Subject:
carbon dioxide; catalysts; electrochemistry; hydrogen production; nanoparticles; oxidation; spectroscopy; zinc
Abstract:
... We explored the size-dependent activity and selectivity of Zn nanoparticles (NPs) for the electrochemical CO₂ reduction reaction (CO₂RR). Zn NPs ranging from 3 to 5 nm showed high activity and selectivity (∼70%) for CO production, whereas those above 5 nm exhibited bulk-like catalytic properties. In addition, a drastic increase in hydrogen production was observed for the Zn NPs below 3 nm, which i ...
DOI:
10.1021/jacs.8b05258

20. Scalable Synthesis of Cyclocitrinol

Author:
Wang, Yu; Ju, Wei; Tian, Hailong; Tian, Weisheng; Gui, Jinghan
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9413-9416
ISSN:
1520-5126
Subject:
biomimetics; biosynthesis; pregnenolone
Abstract:
... A 10-step synthesis of the C25 steroid natural product cyclocitrinol from inexpensive, commercially available pregnenolone is reported. This synthesis features a biomimetic cascade rearrangement to efficiently construct the challenging bicyclo[4.4.1] A/B ring system, which enabled a gram-scale synthesis of the bicyclo[4.4.1] enone intermediate 18 in only nine steps. This work also provides experim ...
DOI:
10.1021/jacs.8b06444

21. Investigating the Formation of Giant {Pd₇₂}ᴾʳᵒᵖ and {Pd₈₄}ᴳˡʸ Macrocycles Using NMR, HPLC, and Mass Spectrometry

Author:
Christie, Lorna G.; Asche, Silke; Mathieson, Jennifer S.; Vilà-Nadal, Laia; Cronin, Leroy
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9379-9382
ISSN:
1520-5126
Subject:
chemistry; high performance liquid chromatography; ligands; mass spectrometry; nuclear magnetic resonance spectroscopy; propionic acid; wheels
Abstract:
... The formation of giant polyoxometalate (POM) species is relatively underexplored, as their self-assembly process is complex due to the rapid kinetics. Polyoxopalladates (POPds) are a class of POMs based on Pd, the largest of which is the {Pd₈₄}ᴬᶜ wheel, and its slower kinetics mean the system is more amenable to systematic study. Here, we show that it is possible to follow the assembly of two type ...
DOI:
10.1021/jacs.8b05059

22. Gold with +4 and +6 Oxidation States in AuF₄ and AuF₆

Author:
Lin, Jianyan; Zhang, Shoutao; Guan, Wei; Yang, Guochun; Ma, Yanming
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9545-9550
ISSN:
1520-5126
Subject:
chemical composition; copper; fluorides; fluorine; gold; oxidation; physical phases; silver
Abstract:
... An important goal in chemistry is to prepare compounds with unusual oxidation states showing exciting properties. For gold (Au), the relativistic expansion of its 5d orbitals makes it form high oxidation state compounds. Thus far, the highest oxidation state of Au known is +5. Here, we propose high pressure as a controllable method for preparing +4 and +6 oxidation states in Au via its reaction wi ...
DOI:
10.1021/jacs.8b04563

23. Laser-Induced Bipolar Electrochemistry—On-Demand Formation of Bipolar Electrodes in a Solid Polymer Light-Emitting Electrochemical Cell

Author:
AlTal, Faleh; Gao, Jun
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9737-9742
ISSN:
1520-5126
Subject:
batteries; catalytic activity; electrochemistry; electrodes; electrolytes; fuel cells; photons; photosensitizing agents; polymers; redox reactions; solar cells; synthesis
Abstract:
... Bipolar electrochemistry (BPEC) is a versatile and powerful technique that has found applications in sensing, chemical synthesis, catalysis, fuel cells, and batteries, among others. In BPEC, the reactions of interest occur at a wireless, bipolar electrode (BPE). BPEC is most commonly carried out in an electrochemical cell that contains an electrolyte solution, in which a metallic BPE is immersed a ...
DOI:
10.1021/jacs.8b06052

24. Chiral Aldehyde Catalysis for the Catalytic Asymmetric Activation of Glycine Esters

Author:
Wen, Wei; Chen, Lei; Luo, Ming-Jing; Zhang, Yan; Chen, Ying-Chun; Ouyang, Qin; Guo, Qi-Xiang
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9774-9780
ISSN:
1520-5126
Subject:
aldehydes; alkylation; amino acids; catalysts; catalytic activity; density functional theory; esters; imines
Abstract:
... Chiral aldehyde catalysis is uniquely suitable for the direct asymmetric α-functionalization of N-unprotected amino acids, because aldehydes can reversibly form imines. However, there have been few successful reports of these transformations. In fact, only chiral aldehyde catalyzed aldol reactions of amino acids and alkylation of 2-amino malonates have been reported with good chiral induction. Her ...
DOI:
10.1021/jacs.8b06676

25. Electron Transfer Reactions: KOtBu (but not NaOtBu) Photoreduces Benzophenone under Activation by Visible Light

Author:
Nocera, Giuseppe; Young, Allan; Palumbo, Fabrizio; Emery, Katie J.; Coulthard, Graeme; McGuire, Thomas; Tuttle, Tell; Murphy, John A.
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9751-9757
ISSN:
1520-5126
Subject:
acetone; ambient temperature; benzene; benzophenones; color; electron transfer; ethylation; free radicals; irradiation; oxidation; oxygen; potassium; solar radiation; spectral analysis; wavelengths; winter
Abstract:
... Long-standing controversial reports of electron transfer from KOtBu to benzophenone have been investigated and resolved. The mismatch in the oxidation potential of KOtBu (+0.10 V vs SCE in DMF) and the first reduction potential of benzophenone (of many values cited in the literature, the least negative value is −1.31 V vs SCE in DMF), preclude direct electron transfer. Experimental and computation ...
DOI:
10.1021/jacs.8b06089

26. Enzymatic Assemblies Disrupt the Membrane and Target Endoplasmic Reticulum for Selective Cancer Cell Death

Author:
Feng, Zhaoqianqi; Wang, Huaimin; Wang, Shiyu; Zhang, Qiang; Zhang, Xixiang; Rodal, Avital A.; Xu, Bing
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9566-9573
ISSN:
1520-5126
Subject:
Western blotting; amino acids; antineoplastic agents; calcium; caspases; cell death; cell membranes; endoplasmic reticulum; enzyme-linked immunosorbent assay; fluorescence; image analysis; lactate dehydrogenase; light scattering; lipids; micelles; neoplasm cells; neoplasms; peptides; proteins; structure-activity relationships; therapeutics; transmission electron microscopy
Abstract:
... The endoplasmic reticulum (ER) is responsible for the synthesis and folding of a large number of proteins, as well as intracellular calcium regulation, lipid synthesis, and lipid transfer to other organelles, and is emerging as a target for cancer therapy. However, strategies for selectively targeting the ER of cancer cells are limited. Here we show that enzymatically generated crescent-shaped sup ...
DOI:
10.1021/jacs.8b04641

27. Type-II Multiferroic Hf₂VC₂F₂ MXene Monolayer with High Transition Temperature

Author:
Zhang, Jun-Jie; Lin, Lingfang; Zhang, Yang; Wu, Menghao; Yakobson, Boris I.; Dong, Shuai
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9768-9773
ISSN:
1520-5126
Subject:
ambient temperature; magnetism
Abstract:
... Achieving multiferroic two-dimensional (2D) materials should enable numerous functionalities in nanoscale devices. Until now, however, predicted 2D multiferroics are very few and with coexisting yet only loosely coupled (type-I) ferroelectricity and magnetism. Here, a type-II multiferroic MXene Hf₂VC₂F₂ monolayer is identified, where ferroelectricity originates directly from its magnetism. The non ...
DOI:
10.1021/jacs.8b06475

28. Conjugate Addition of Perfluoroarenes to α,β-Unsaturated Carbonyls Enabled by an Alkoxide-Hydrosilane System: Implication of a Radical Pathway

Author:
Xie, Weilong; Park, Sung-Woo; Jung, Hoimin; Kim, Dongwook; Baik, Mu-Hyun; Chang, Sukbok
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9659-9668
ISSN:
1520-5126
Subject:
ambient temperature; aromatic hydrocarbons; catalytic activity; chemical bonding; nuclear magnetic resonance spectroscopy; silicates
Abstract:
... Conjugate addition of organometallic reagents to α,β-unsaturated carbonyls is a key strategy for the construction of carbon–carbon bond in organic synthesis. Although direct C–H addition to unsaturated bonds via transition metal catalysis is explored in recent years, electron-deficient arenes that do not bear directing groups continue to be challenging. Herein we disclose the first example of a co ...
DOI:
10.1021/jacs.8b05744

29. Hetero-oligomeric Amyloid Assembly and Mechanism: Prion Fragment PrP(106–126) Catalyzes the Islet Amyloid Polypeptide β-Hairpin

Author:
Ilitchev, Alexandre I.; Giammona, Maxwell J.; Olivas, Carina; Claud, Sarah L.; Lazar Cantrell, Kristi L.; Wu, Chun; Buratto, Steven K.; Bowers, Michael T.
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9685-9695
ISSN:
1520-5126
Subject:
amino acid sequences; amyloid; atomic force microscopy; catalytic activity; circular dichroism spectroscopy; humans; ligands; mass spectrometry; mechanistic models; molecular models; polypeptides; prions; proline; sequence homology
Abstract:
... Protein aggregation is typically attributed to the association of homologous amino acid sequences between monomers of the same protein. Coaggregation of heterogeneous peptide species can occur, however, and is implicated in the proliferation of seemingly unrelated protein diseases in the body. The prion protein fragment (PrP₁₀₆–₁₂₆) and human islet amyloid polypeptide (hIAPP) serve as an interesti ...
DOI:
10.1021/jacs.8b05925

30. Hydrazide Mimics for Protein Lysine Acylation To Assess Nucleosome Dynamics and Deubiquitinase Action

Author:
Bhat, Shridhar; Hwang, Yousang; Gibson, Matthew D.; Morgan, Michael T.; Taverna, Sean D.; Zhao, Yingming; Wolberger, Cynthia; Poirier, Michael G.; Cole, Philip A.
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9478-9485
ISSN:
1520-5126
Subject:
acylation; antibodies; cysteine; histones; hydrazides; lysine; nucleosomes; post-translational modification; ubiquitinyl hydrolase 1
Abstract:
... A range of acyl-lysine (acyl-Lys) modifications on histones and other proteins have been mapped over the past decade but for most, their functional and structural significance remains poorly characterized. One limitation in the study of acyl-Lys containing proteins is the challenge of producing them or their mimics in site-specifically modified forms. We describe a cysteine alkylation-based method ...
DOI:
10.1021/jacs.8b03572

31. Metal–Organic Frameworks as Efficient Oral Detoxifying Agents

Author:
Rojas, Sara; Baati, Tarek; Njim, Leila; Manchego, Lisbeth; Neffati, Fadoua; Abdeljelil, Nissem; Saguem, Saad; Serre, Christian; Najjar, Mohamed Fadhel; Zakhama, Abdelfateh; Horcajada, Patricia
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9581-9586
ISSN:
1520-5126
Subject:
adsorbents; coordination polymers; decontamination; drugs; gastrointestinal system; histology; intestinal absorption; oral administration; overdose; poisoning; toxicity
Abstract:
... Poisoning and accidental oral intoxication are major health problems worldwide. Considering the insufficient efficacy of the currently available detoxification treatments, a pioneering oral detoxifying adsorbent agent based on a single biocompatible metal–organic framework (MOF) is here proposed for the efficient decontamination of drugs commonly implicated in accidental or voluntary poisoning. Fu ...
DOI:
10.1021/jacs.8b04435

32. Oxidation States, Stability, and Reactivity of Organoferrate Complexes

Author:
Parchomyk, Tobias; Demeshko, Serhiy; Meyer, Franc; Koszinowski, Konrad
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9709-9720
ISSN:
1520-5126
Subject:
Grignard reagents; aromatic hydrocarbons; cross-coupling reactions; electrical conductivity; electrospray ionization mass spectrometry; ferric chloride; ferrous chloride; free radicals; gases; iron; moieties; oxidation; phosphine; tetrahydrofuran
Abstract:
... We have applied a combination of electrospray-ionization mass spectrometry, electrical conductivity measurements, and Mössbauer spectroscopy to identify and characterize the organoferrate species RₙFeₘ– formed upon the transmetalation of iron precursors (Fe(acac)₃, FeCl₃, FeCl₂, Fe(OAc)₂) with Grignard reagents RMgX (R = Me, Et, Bu, Hex, Oct, Dec, Me₃SiCH₂, Bn, Ph, Mes, 3,5-(CF₃)₂-C₆H₃; X = Cl, B ...
DOI:
10.1021/jacs.8b06001

33. Photosensitized Membrane Permeabilization Requires Contact-Dependent Reactions between Photosensitizer and Lipids

Author:
Bacellar, Isabel O. L.; Oliveira, Maria Cecilia; Dantas, Lucas S.; Costa, Elierge B.; Junqueira, Helena C.; Martins, Waleska K.; Durantini, Andrés M.; Cosa, Gonzalo; Di Mascio, Paolo; Wainwright, Mark; Miotto, Ronei; Cordeiro, Rodrigo M.; Miyamoto, Sayuri; Baptista, Mauricio S.
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9606-9615
ISSN:
1520-5126
Subject:
Gibbs free energy; alcohols; aldehydes; chemical bonding; direct contact; hydroperoxides; ketones; lipid bilayers; lipid peroxidation; membrane permeability; methylene blue; phospholipids; photooxidation; photosensitizing agents; singlet oxygen
Abstract:
... Although the general mechanisms of lipid oxidation are known, the chemical steps through which photosensitizers and light permeabilize lipid membranes are still poorly understood. Herein we characterized the products of lipid photooxidation and their effects on lipid bilayers, also giving insight into their formation pathways. Our experimental system was designed to allow two phenothiazinium-based ...
DOI:
10.1021/jacs.8b05014

34. Ag(I)–C–H Activation Enables Near-Room-Temperature Direct α-Arylation of Benzo[b]thiophenes

Author:
Colletto, Chiara; Panigrahi, Adyasha; Fernández-Casado, Jaime; Larrosa, Igor
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9638-9643
ISSN:
1520-5126
Subject:
carbon-hydrogen bond activation; chloroform; palladium; regioselectivity; silver; thiophene
Abstract:
... The first example of near-room-temperature α-arylation of benzo[b]thiophenes is reported. The discovery rests on the observation of a switch in α-/β-regioselectivity at different loadings of Pd₂(dba)₃·CHCl₃ in the coupling between benzo[b]thiophene and 4-iodotoluene. We show that this unprecedented regioselectivity switch is driven by a Ag(I)-mediated C–H activation at the α-C–H position, which be ...
DOI:
10.1021/jacs.8b05361

35. Bioinformatic Expansion and Discovery of Thiopeptide Antibiotics

Author:
Schwalen, Christopher J.; Hudson, Graham A.; Kille, Bryce; Mitchell, Douglas A.
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9494-9501
ISSN:
1520-5126
Subject:
Gram-positive bacteria; antibacterial properties; antibiotics; bioinformatics; biosynthesis; data collection; drug resistance; genomics; heterologous gene expression; livestock; moieties; multigene family; pathogens; piperidines; proteins; sequence analysis
Abstract:
... Thiopeptides are members of the ribosomally synthesized and post-translationally modified peptide family of natural products. Most characterized thiopeptides display nanomolar potency toward Gram-positive bacteria by blocking protein translation with several being produced at the industrial scale for veterinary and livestock applications. Employing our custom bioinformatics program, RODEO, we expa ...
DOI:
10.1021/jacs.8b03896

36. Cyanine-Mediated DNA Nanofiber Growth with Controlled Dimensionality

Author:
Bousmail, Danny; Chidchob, Pongphak; Sleiman, Hanadi F.
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9518-9530
ISSN:
1520-5126
Subject:
DNA; drugs; nanofibers; nanogold; nanomedicine; optical properties; surfactants
Abstract:
... Supramolecular one-dimensional (1D) architectures are of high interest in drug delivery and templation of complex linear arrays due to their high aspect ratio and rigidity. A particular desire is the access of 1D nanostructures with high functionality and biorelevance, which opens the door to their applications in materials science and nanomedicine. Here we report the discovery that the site-speci ...
DOI:
10.1021/jacs.8b04157

37. Electronic Structure Contributions of Non-Heme Oxo-Iron(V) Complexes to the Reactivity

Author:
Mondal, Bhaskar; Neese, Frank; Bill, Eckhard; Ye, Shengfa
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9531-9544
ISSN:
1520-5126
Subject:
anisotropy; chemical bonding; cleavage (chemistry); ferrimagnetic materials; iron; ligands; moieties; oxidation; spectral analysis; spectroscopy; stereoselectivity; stereospecificity
Abstract:
... Oxo-iron(V) species have been implicated in the catalytic cycle of the Rieske dioxygenase. Their synthetic analog, [Feⱽ(O)(OC(O)CH₃)(PyNMe₃)]²⁺ (1, PyNMe₃ = 3,6,9,15-tetraazabicyclo[9.3.1]pentadeca-1(15),11,13-triene-3,6,9-trimethyl), derived from the O–O bond cleavage of its acetylperoxo iron(III) precursor, has been shown experimentally to perform regio- and stereoselective C–H and C═C bond func ...
DOI:
10.1021/jacs.8b04275

38. Eu²⁺ Site Preferences in the Mixed Cation K₂BaCa(PO₄)₂ and Thermally Stable Luminescence

Author:
Qiao, Jianwei; Ning, Lixin; Molokeev, Maxim S.; Chuang, Yu-Chun; Liu, Quanlin; Xia, Zhiguo
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9730-9736
ISSN:
1520-5126
Subject:
barium; calcium; cations; electrons; europium; ionization; phosphates; photoluminescence; potassium; quantitative analysis; thermal stability
Abstract:
... Site preferences of dopant Eu²⁺ on the locations of K⁺, Ba²⁺, and Ca²⁺ in the mixed cation phosphate K₂BaCa(PO₄)₂ (KBCP) are quantitatively analyzed via a combined experimental and theoretical method to develop a blue-emitting phosphor with thermally stable luminescence. Eu²⁺ ions are located at K2 (M2) and K3 (M3) sites of KBCP, with the latter occupation relatively more stable than the former, c ...
DOI:
10.1021/jacs.8b06021

39. Exhaustively Trichlorosilylated C₁ and C₂ Building Blocks: Beyond the Müller–Rochow Direct Process

Author:
Georg, Isabelle; Teichmann, Julian; Bursch, Markus; Tillmann, Jan; Endeward, Burkhard; Bolte, Michael; Lerner, Hans-Wolfram; Grimme, Stefan; Wagner, Matthias
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9696-9708
ISSN:
1520-5126
Subject:
X-ray diffraction; alkynes; ambient temperature; carbon; carbon monoxide; carbon tetrachloride; chemical bonding; chemical structure; chlorides; electron paramagnetic resonance spectroscopy; extrusion; heterolytic cleavage; ions; methylene chloride; nuclear magnetic resonance spectroscopy; oxidation; stable isotopes
Abstract:
... The Cl–-induced heterolysis of the Si–Si bond in Si₂Cl₆ generates an [SiCl₃]⁻ ion as reactive intermediate. When carried out in the presence of CCl₄ or Cl₂C═CCl₂ (CH₂Cl₂ solutions, room temperature or below), the reaction furnishes the monocarbanion [C(SiCl₃)₃]⁻ ([A]⁻; 92%) or the vicinal dianion [(Cl₃Si)₂C–C(SiCl₃)₂]²– ([B]²–; 85%) in excellent yields. Starting from [B]²–, the tetrasilylethane (C ...
DOI:
10.1021/jacs.8b05950

40. Synthesis of Functionalized N-Acetyl Muramic Acids To Probe Bacterial Cell Wall Recycling and Biosynthesis

Author:
DeMeester, Kristen E.; Liang, Hai; Jensen, Matthew R.; Jones, Zachary S.; D’Ambrosio, Elizabeth A.; Scinto, Samuel L.; Zhou, Junhui; Grimes, Catherine L.
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9458-9465
ISSN:
1520-5126
Subject:
bacteria; biosynthesis; cell walls; fluorescent labeling; immunology; muramic acid; peptidoglycans; phosphates; polymers; transferases; uridine diphosphate
Abstract:
... Uridine diphosphate N-acetyl muramic acid (UDP NAM) is a critical intermediate in bacterial peptidoglycan (PG) biosynthesis. As the primary source of muramic acid that shapes the PG backbone, modifications installed at the UDP NAM intermediate can be used to selectively tag and manipulate this polymer via metabolic incorporation. However, synthetic and purification strategies to access large quant ...
DOI:
10.1021/jacs.8b03304

41. Visible-Light-Activated Quinolone Carbon-Monoxide-Releasing Molecule: Prodrug and Albumin-Assisted Delivery Enables Anticancer and Potent Anti-Inflammatory Effects

Author:
Popova, Marina; Soboleva, Tatiana; Ayad, Suliman; Benninghoff, Abby D.; Berreau, Lisa M.
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9721-9729
ISSN:
1520-5126
Subject:
albumins; anti-inflammatory activity; byproducts; carbon monoxide; cytotoxicity; fluorescence microscopy; inhibitory concentration 50; lighting; neoplasm cells; neoplasms; oxidation; quinolones; thiols
Abstract:
... The delivery of controlled amounts of carbon monoxide (CO) to biological targets is of significant current interest. Very few CO-releasing compounds are currently known that can be rigorously controlled in terms of the location and amount of CO released. To address this deficiency, we report herein a new metal-free, visible-light-induced CO-releasing molecule (photoCORM) and its prodrug oxidized f ...
DOI:
10.1021/jacs.8b06011

42. Water Dynamics in Polyacrylamide Hydrogels

Author:
Yan, Chang; Kramer, Patrick L.; Yuan, Rongfeng; Fayer, Michael D.
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9466-9477
ISSN:
1520-5126
Subject:
anions; biocompatible materials; crosslinking; electrophoresis; hydrogels; hydrogen bonding; molecular dynamics; polyacrylamide; solutes
Abstract:
... Polymeric hydrogels have wide applications including electrophoresis, biocompatible materials, water superadsorbents, and contact lenses. The properties of hydrogels involve the poorly characterized molecular dynamics of water and solutes trapped within the three-dimensional cross-linked polymer networks. Here we apply ultrafast two-dimensional infrared (2D IR) vibrational echo and polarization-se ...
DOI:
10.1021/jacs.8b03547

43. Covalent Post-assembly Modification Triggers Multiple Structural Transformations of a Tetrazine-Edged Fe₄L₆ Tetrahedron

Author:
Roberts, Derrick A.; Pilgrim, Ben S.; Sirvinskaite, Giedre; Ronson, Tanya K.; Nitschke, Jonathan R.
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9616-9623
ISSN:
1520-5126
Subject:
aniline; cycloaddition reactions
Abstract:
... Covalent post-assembly modification (PAM) reactions are useful synthetic tools for functionalizing and stabilizing self-assembled metal–organic complexes. Recently, PAM reactions have also been explored as stimuli for triggering supramolecular structural transformations. Herein we demonstrate the use of inverse electron-demand Diels–Alder (IEDDA) PAM reactions to induce supramolecular structural t ...
DOI:
10.1021/jacs.8b05082

44. Epimerization of Tertiary Carbon Centers via Reversible Radical Cleavage of Unactivated C(sp³)–H Bonds

Author:
Wang, Yaxin; Hu, Xiafei; Morales-Rivera, Cristian A.; Li, Guo-Xing; Huang, Xin; He, Gang; Liu, Peng; Chen, Gong
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9678-9684
ISSN:
1520-5126
Subject:
azides; biosynthesis; carbon; carbonyl compounds; chemical bonding; iodine; stereochemistry
Abstract:
... Reversible cleavage of C(sp³)–H bonds can enable racemization or epimerization, offering a valuable tool to edit the stereochemistry of organic compounds. While epimerization reactions operating via cleavage of acidic C(sp³)–H bonds, such as the Cα–H of carbonyl compounds, have been widely used in organic synthesis and enzyme-catalyzed biosynthesis, epimerization of tertiary carbons bearing a nona ...
DOI:
10.1021/jacs.8b05753

45. Rhodamine 6G-Labeled Pyridyl Aroylhydrazone Fe(II) Complex Exhibiting Synergetic Spin Crossover and Fluorescence

Author:
Yuan, Juan; Wu, Shu-Qi; Liu, Mei-Jiao; Sato, Osamu; Kou, Hui-Zhong
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9426-9433
ISSN:
1520-5126
Subject:
ambient temperature; fluorescence; hydrazones; hysteresis; iron; ligands; magnetism; rhodamines
Abstract:
... Here, we use a pyridinecarbaldehyde rhodamine 6G hydrazone ligand (L) to synthesize an Fe(II) complex 1 for the search of new fluorescent-spin crossover (SCO) materials. Single-crystal structural determinations suggest that the Fe(II) ion is chelated by two ring-opened ligands (L-o) to form a FeN₄O₂ coordination environment, and intermolecular π---π contacts of the xanthene groups connect the adja ...
DOI:
10.1021/jacs.8b00103

46. Concise Synthesis of (−)-Cycloclavine and (−)-5-epi-Cycloclavine via Asymmetric C–C Activation

Author:
Deng, Lin; Chen, Mengqing; Dong, Guangbin
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9652-9658
ISSN:
1520-5126
Subject:
alkenes; alkylation; catalysts; catalytic activity; chemical bonding; diastereoselectivity; enantioselectivity; palladium
Abstract:
... To illustrate the synthetic significance of C–C activation methods, here we describe an efficient strategy for the enantioselective total syntheses of (−)-cycloclavine and (−)-5-epi-cycloclavine, which is enabled by an asymmetric Rh-catalyzed “cut-and-sew” transformation between benzocyclobutenones and olefins. Despite the compact structure of cycloclavine with five-fused rings, the total synthesi ...
DOI:
10.1021/jacs.8b05549

47. Modulating the σ-Accepting Properties of an Antimony Z-type Ligand via Anion Abstraction: Remote-Controlled Reactivity of the Coordinated Platinum Atom

Author:
You, Di; Yang, Haifeng; Sen, Srobona; Gabbaï, François P.
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9644-9651
ISSN:
1520-5126
Subject:
Lewis acids; acetonitrile; antimony; catalytic activity; chemical bonding; cyclization reactions; fluorides; ligands; moieties; platinum
Abstract:
... In search of ligand platforms, which can be used to remotely control the catalytic activity of a transition metal, we have investigated the coordination noninnocence of ambiphilic L₂/Z-type ligands containing a trifluorostiborane unit as a Lewis acid. The known dichlorostiboranyl platinum complex ((o-(Ph₂P)C₆H₄)₂SbCl₂)PtCl (1) reacts with TlF in the presence of acetonitrile (MeCN) and cyclohexyl i ...
DOI:
10.1021/jacs.8b05520

48. Fully Dispersed Rh Ensemble Catalyst To Enhance Low-Temperature Activity

Author:
Jeong, Hojin; Lee, Geonhee; Kim, Beom-Sik; Bae, Junemin; Han, Jeong Woo; Lee, Hyunjoo
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9558-9565
ISSN:
1520-5126
Subject:
adsorption; carbon monoxide; catalysts; hot water treatment; moieties; oxidation; propane; propylene; temperature
Abstract:
... Minimizing the use of precious metal catalysts is important in many applications. Single-atom catalysts (SACs) have received much attention because all of the metal atoms can be used for surface reactions. However, SACs cannot catalyze some important reactions that require ensemble sites. Here, Rh catalysts were prepared by treating 2 wt % Rh/CeO₂ hydrothermally at 750 °C for 25 h. Nearly 100% dis ...
DOI:
10.1021/jacs.8b04613

49. pseudo[1]Catenane-Type Pillar[5]thiacrown Whose Planar Chiral Inversion is Triggered by Metal Cation and Controlled by Anion

Author:
Lee, Eunji; Ju, Huiyeong; Park, In-Hyeok; Jung, Jong Hwa; Ikeda, Mari; Kuwahara, Shunsuke; Habata, Yoichi; Lee, Shim Sung
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9669-9677
ISSN:
1520-5126
Subject:
DNA; anion exchange; anions; aromatic hydrocarbons; circular dichroism spectroscopy; enantiomers; iodides; mercury; metal ions; nanomaterials; nitrates; optical isomerism; perchlorates; proteins; sulfides
Abstract:
... Chiral inversion of single molecules has been a challenging task because chirality information controls structures and functions of various molecules, artificial nanostructures, DNA, and proteins. Herein we present a pseudo[1]catenane-type molecule whose planar chiral inversion is driven by a metal ion under the control of anions for the first time. Considering an in–out equilibrium of a fused thi ...
DOI:
10.1021/jacs.8b05751

50. Rational Design of Mononuclear Iron Porphyrins for Facile and Selective 4e–/4H⁺ O₂ Reduction: Activation of O–O Bond by 2nd Sphere Hydrogen Bonding

Author:
Bhunia, Sarmistha; Rana, Atanu; Roy, Pronay; Martin, Daniel J.; Pegis, Michael L.; Roy, Bijan; Dey, Abhishek
Source:
Journal of the American Chemical Society 2018 v.140 no.30 pp. 9444-9457
ISSN:
1520-5126
Subject:
catalysts; cleavage (chemistry); copper; cytochrome-c oxidase; electrochemistry; electrodes; electron transfer; heme; hydrogen bonding; iron; oxygen
Abstract:
... Facile and selective 4e–/4H⁺ electrochemical reduction of O₂ to H₂O in aqueous medium has been a sought-after goal for several decades. Elegant but synthetically demanding cytochrome c oxidase mimics have demonstrated selective 4e–/4H⁺ electrochemical O₂ reduction to H₂O is possible with rate constants as fast as 10⁵ M–¹ s–¹ under heterogeneous conditions in aqueous media. Over the past few years, ...
DOI:
10.1021/jacs.8b02983