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1.
Nanoscale ; 13(44): 18773-18779, 2021 Nov 18.
Artigo em Inglês | MEDLINE | ID: mdl-34747962

RESUMO

Production of ethylene glycol from coal is a particularly interesting route as it is an economic alternative to the petrochemical-based route. In this process, effectively generating dimethyl oxalate (DMO) is a crucial step by CO oxidative coupling reaction under Pd-based catalysts. However, the aggregation of Pd species over the support is still an issue that relates to the deterioration of catalytic activity and stability. To this end, enhancing the metal-support interaction is urgently required. In this work, hierarchical Nb2O5 (H-Nb2O5) microspheres with abundant oxygen defects were synthesized to anchor the Pd species thus promoting the electron transfer between Pd species and Nb species associated with the generation of interfacial Pd-NbOx sites. Besides, the thinned electron density of Pd species resulting from the electron-withdrawing effect of Nb species is beneficial for activating the adsorbed CO molecules, leading to superior catalytic activity. The Pd/H-Nb2O5 catalyst exhibited 63.1% of CO conversion (theoretical maximum conversion: 64.3%) and 92.9% of DMO selectivity, with a DMO weight time yield of 1297.9 g kgcat.-1 h-1, and remained robust even after 50 h of time on stream evaluation. Current work provides a deep insight into the CO activation mechanism and helps improve the catalytic stability by boosting interfacial electron interaction via oxygen defects induction, and also sheds light on the design and synthesis of high-performance catalysts in other heterogeneous catalysis fields.

2.
J Am Chem Soc ; 143(25): 9595-9600, 2021 Jun 30.
Artigo em Inglês | MEDLINE | ID: mdl-34128669

RESUMO

Ligands in ligand-protected metal clusters play a crucial role, not only because of their interaction with the metal core, but also because of the functionality they provide to the cluster. Here, we report the utilization of secondary phosphine oxide (SPO), as a new family of functional ligands, for the preparation of an undecagold cluster Au11-SPO. Different from the commonly used phosphine ligand (i.e., triphenylphosphine, TPP), the SPOs in Au11-SPO work as electron-withdrawing anionic ligands. While coordinating to gold via the phosphorus atom, the SPO ligand keeps its O atom available to act as a nucleophile. Upon photoexcitation, the clusters are found to inject holes into p-type semiconductors (here, bismuth oxide is used as a model), sensitizing the p-type semiconductor in a different way compared to the photosensitization of a n-type semiconductor. Furthermore, the Au11-SPO/Bi2O3 photocathode exhibits a much higher activity toward the hydrogenation of benzaldehyde than a TPP-protected Au11-sensitized Bi2O3 photocathode. Control experiments and density functional theory studies point to the crucial role of the cooperation between gold and the SPO ligands on the selectivity toward the hydrogenation of the C═O group in benzaldehyde.

3.
ACS Appl Mater Interfaces ; 13(21): 24856-24864, 2021 Jun 02.
Artigo em Inglês | MEDLINE | ID: mdl-34009944

RESUMO

Strong metal-support interaction is crucial to the stability of catalysts in heterogeneous catalysis. However, reports on boosting interfacial electron transfer between metal and support via defect induction for enhanced metal-support interaction are limited. In this work, ultrathin reducible ZnTi-layered double hydroxide (LDH) nanosheets with rich oxygen defects were synthesized to stabilize Pd clusters, and the rich oxygen defects promoted Pd cluster bonding with Zn and Ti atoms in supports, thereby forming a metal-metal bond. Electron spin resonance (ESR), X-ray absorption fine spectra (XAFS), and density functional theory (DFT) calculations demonstrate remarkable interfacial electron transfer (0.62 e). The Pd/ZnTi-LDH catalyst shows superior catalytic stability for CO direct esterification to dimethyl oxalate. By contrast, the nonreducible Pd/ZnAl-LDH catalyst with a few oxygen defects shows minimal interfacial electron transfer (0.08 e), which leads to relatively poor catalytic stability. This work provides a deep insight into promoting the stability of catalysts by boosting interfacial electron transfer via defect induction.

4.
J Am Chem Soc ; 143(12): 4639-4645, 2021 Mar 31.
Artigo em Inglês | MEDLINE | ID: mdl-33656891

RESUMO

Developing efficient bifunctional electrocatalysts for overall water splitting in acidic conditions is the essential step for proton exchange membrane water electrolyzers (PEMWEs). We first report the synthesis of core-shell structure nanoparticles (NPs) with an Au core and an AuIr2 alloy shell (Au@AuIr2). Au@AuIr2 displayed 4.6 (5.6) times higher intrinsic (mass) activity toward the oxygen evolution reaction (OER) than a commercial Ir catalyst. Furthermore, it showed hydrogen evolution reaction (HER) catalytic properties comparable to those of commercial Pt/C. Significantly, when Au@AuIr2 was used as both the anode and cathode catalyst, the overall water splitting cell achieved 10 mA/cm2 with a low cell voltage of 1.55 V and maintained this activity for more than 40 h, which greatly outperformed the commercial couples (Ir/C||Pt/C, 1.63 V, activity decreased within minutes) and is among the most efficient bifunctional catalysts reported. Theoretical calculations coupled with X-ray-based structural analyses suggest that partially oxidized surfaces originating from the electronic interaction between Au and Ir provide a balance for different intermediates binding and realize significantly enhanced OER performance.

5.
Angew Chem Int Ed Engl ; 60(8): 4125-4132, 2021 Feb 19.
Artigo em Inglês | MEDLINE | ID: mdl-33200851

RESUMO

The valorization of carbon dioxide (CO2 ) to fine chemicals is one of the most promising approaches for CO2 capture and utilization. Herein we demonstrated a series of porous organometallic polymers could be employed as highly efficient and recyclable catalysts for this purpose. Synergetic effects of specific surface area, iridium content, and CO2 adsorption capability are crucial to achieve excellent selectivity and yields towards N-formylation of diverse amines with CO2 and H2 under mild reaction conditions even at 20 ppm catalyst loading. Density functional theory calculations revealed not only a redox-neutral catalytic pathway but also a new plausible mechanism with the incorporation of the key intermediate formic acid via a proton-relay process. Remarkably, a record turnover number (TON=1.58×106 ) was achieved in the synthesis of N,N-dimethylformamide (DMF), and the solid catalysts can be reused up to 12 runs, highlighting their practical potential in industry.

6.
J Phys Chem A ; 124(35): 7071-7079, 2020 Sep 03.
Artigo em Inglês | MEDLINE | ID: mdl-32786973

RESUMO

Metalla-aromatics have attracted considerable attention due to their fascinating structural and reactive properties as well as their potential as prospective functional materials. Metallabenzenes and their fused-ring counterparts are significant members of metalla-aromatics, while their crystal structures often display seemly counterintuitive nonplanar geometry. The geometric bending of metallabenzenes has been attributed to the unfavorable antibonding interactions in the σ-space orbitals rather than the general opinion regarding the π-space orbitals of an aromatic compound. However, the origin of the geometric bending in fused-ring metallabenzenes remains elusive. In this work, we elucidated that such a "σ-control mechanism" still holds for fused-ring metallabenzenes by performing systematic calculations for a plethora of metallabenzenes and fused-ring metallabenzenes. Furthermore, we found that a more bent geometry can be achieved for fused-ring metallabenzenes than their corresponding metallabenzenes by fusing the aromatic rings at the ortho-position of a metal center to induce extra repulsion. The more significant bending in fused-ring metallabenzenes also favors the aromaticity enhancement. These findings not only provide mechanistic insight into the unexpected geometric distortion in both metallabenzenes and fused-ring metallabenzenes but also pave the way to design and develop bent metalla-aromatics with enhanced metalla-aromaticity, which hold great potential as aromatic functional materials.

7.
Nanoscale ; 12(27): 14825-14830, 2020 Jul 16.
Artigo em Inglês | MEDLINE | ID: mdl-32672320

RESUMO

Pd-Based heterogeneous catalysts have been demonstrated to be efficient in numerous heterogeneous reactions. However, the effect of the support resulting in covalent metal-support interaction (CMSI) has not been researched sufficiently. In this work, a Lewis base is modulated over MgAl-LDH to investigate the support effects and it is further loaded with Pd clusters to research the metal-support interactions. MgAl-LDH with ultra-low Pd loading (0.0779%) shows CO conversion (55.0%) and dimethyl oxalate (DMO) selectivity (93.7%) for CO oxidative coupling to DMO, which was gradually deactivated after evaluation for 20 h. To promote the stability of Pd/MgAl-LDH, Zn2+ ions were introduced into the MgAl-LDH support to strengthen the CMSI by forming Pd-Zn bonds, which further increased the adsorption energy of the Pd clusters on ZnMgAl-LDH, and this was verified by X-ray absorption fine structure (XAFS) measurements and density functional theory (DFT) calculations. The stability of the Pd/ZnMgAl-LDH catalyst could be maintained for at least 100 h. This work highlights that covalent metal-support interactions can be strengthened by forming new metal-metal bonds, which could be extended to other systems for the stabilization of noble metals over supports.

8.
Angew Chem Int Ed Engl ; 59(33): 13871-13878, 2020 08 10.
Artigo em Inglês | MEDLINE | ID: mdl-32385924

RESUMO

The global demand for lactic acid (LA) is increasing due to its successful application as monomer for the manufacture of bioplastics. Although N-heterocyclic carbene (NHC) iridium complexes are promising molecular catalysts for LA synthesis, their instabilities have hindered their utilization especially in commercial applications. Here, we report that a porous self-supported NHC-iridium coordination polymer can efficiently prevent the clusterization of corresponding NHC-Ir molecules and can function as a solid molecular recyclable catalyst for dehydrogenation of bio-polyols to form LA with excellent activity (97 %) and selectivity (>99 %). A turnover number of up to 5700 could be achieved in a single batch, due to the synergistic participation of the Ba2+ and hydroxide ions, as well as the blockage of unwanted pathways by adding methanol. Our findings demonstrate a potential route for the industrial production of LA from cheap and abundant bio-polyols, including sorbitol.


Assuntos
Ácido Láctico/química , Polímeros/química , Catálise , Complexos de Coordenação/química , Hidrogenação , Oxirredução
9.
Angew Chem Int Ed Engl ; 59(26): 10421-10425, 2020 06 22.
Artigo em Inglês | MEDLINE | ID: mdl-32187790

RESUMO

An atom-economic approach that has an unprecedented high selectivity for the synthesis of lactic acid (LA) based on a catalytic dehydrogenative cross-coupling by using inexpensive bulk ethylene glycol and methanol is described. This method relies on the synthesis and utilization of a novel iridium catalyst bearing three N-heterocyclic carbenes derived from 1,3-dimethylbenzimidazolium salts, and exhibits outstanding activity in the production of LA [turnover frequency (TOF) up to 3660 h-1 ] owing to an elegant metal-ligand cooperation.

10.
Adv Mater ; 32(8): e1906915, 2020 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-31957117

RESUMO

The efficiency of splitting water into hydrogen and oxygen is highly dependent on the catalyst used. Herein, ultrathin Ni(0)-embedded Ni(OH)2 heterostructured nanosheets, referred to as Ni/Ni(OH)2 nanosheets, with superior water splitting activity are synthesized by a partial reduction strategy. This synthetic strategy confers the heterostructured Ni/Ni(OH)2 nanosheets with abundant Ni(0)-Ni(II) active interfaces for hydrogen evolution reaction (HER) and Ni(II) defects as transitional active sites for oxygen evolution reaction (OER). The obtained Ni/Ni(OH)2 nanosheets exhibit noble metal-like electrocatalytic activities toward overall water splitting in alkaline condition, to offer 10 mA cm-2 in HER and OER, the required overpotentials are only 77 and 270 mV, respectively. Based on such an outstanding activity, a water splitting electrolysis cell using the Ni/Ni(OH)2 nanosheets as the cathode and anode electrocatalysts has been successfully built. When the output voltage of the electrolytic cell is 1.59 V, a current density of 10 mA cm-2 can be obtained. Moreover, the durability of Ni/Ni(OH)2 nanosheets in the alkaline electrolyte is much better than that of noble metals. No obvious performance decay is observed after 20 h of catalysis. This facile strategy paves the way for designing highly active non-precious-metal catalyst to generate both hydrogen and oxygen by electrolyzing water at room temperature.

11.
Angew Chem Int Ed Engl ; 58(32): 10932-10935, 2019 Aug 05.
Artigo em Inglês | MEDLINE | ID: mdl-31165551

RESUMO

Supported single-atom catalysts have been emerging as promising materials in a variety of energy catalysis applications. However, studying the role of metal-support interactions at the molecular level remains a major challenge, primarily due to the lack of precise atomic structures. In this work, by replacing the frequently used TiO2 support with its molecular analogue, titanium-oxo cluster (TOC), we successfully produced a new kind of Ti-O material doped with single silver sites. The as-obtained Ag10 Ti28 cluster, containing four exposed and six embedded Ag sites, is the largest noble-metal-doped Ti-O cluster reported to date. Density functional theory (DFT) calculations show that the Ag10 Ti28 core exhibits properties distinct from those of metallic Ag-based materials. This Ti-O material doped with single Ag sites presents a high ϵd and moderate CO binding capacity comparable to that of metallic Cu-based catalysts, suggesting that it might display different catalytic performance from the common Ag-based catalysts, for example, for CO2 reduction. These results prove that the synergism of active surface metal atoms and the Ti-O cluster support result in unique physical properties, which might open a new direction for single-atom-included catalysts.

12.
J Chem Phys ; 150(4): 044111, 2019 Jan 28.
Artigo em Inglês | MEDLINE | ID: mdl-30709281

RESUMO

Free energy calculations for chemical reactions with a steep energy barrier require well defined reaction coordinates (RCs). However, when multiple parallel channels exist along selected RC, the application of conventional enhanced samplings is difficult to generate correct sampling within limited simulation time and thus cannot give correct prediction about the favorable pathways, the relative stability of multiple products or intermediates. Here, we implement the selective integrated tempering sampling (SITS) method with quantum mechanical and molecular mechanical (QM/MM) potential to investigate the chemical reactions in solution. The combined SITS-QM/MM scheme is used to identify possible reaction paths, intermediate and product states, and the free energy profiles for the different reaction paths. Two double proton transfer reactions were studied to validate the implemented method and simulation protocol, from which the independent and correlated proton transfer processes are identified in two representative systems, respectively. This protocol can be generalized to various kinds of chemical reactions for both academic studies and industry applications, such as in exploration and optimization of potential reactions in DNA encoded compound library and halogen or deuterium substitution of the hit discovery and lead optimization stages of drug design via providing a better understanding of the reaction mechanism along the designed chemical reaction pathways.

13.
Nat Commun ; 9(1): 5002, 2018 11 27.
Artigo em Inglês | MEDLINE | ID: mdl-30479335

RESUMO

Enamine and imine represent two of the most common reaction intermediates in syntheses, and the imine intermediates containing α-hydrogen often exhibit the similar reactivity to enamines due to their rapid tautomerization to enamine tautomers. Herein, we report that the minor structural difference between the enamine and the enamine tautomer derived from imine tautomerization results in the different chemo- and regioselectivity in the reaction of cyclohexanones, amines and TEMPO: the reaction of primary amines furnishes the formal oxygen 1,2-migration product, α-amino-enones, while the reaction of secondary amines under similar conditions generates exclusively arylamines via consecutive dehydrogenation on the cyclohexyl rings. The 18O-labeling experiment for α-amino-enone formation revealed that TEMPO served as oxygen transfer reagent. Experimental and computational studies of reaction mechanisms revealed that the difference in chemo- and regioselectivity could be ascribed to the flexible imine-enamine tautomerization of the imine intermediate containing an α-hydrogen.

14.
J Comput Chem ; 39(27): 2307-2315, 2018 10 15.
Artigo em Inglês | MEDLINE | ID: mdl-30318750

RESUMO

Engineering fluorescent proteins to be the customized in vivo labels for monitoring cellular dynamic events is critical in biochemical and biomedical studies. The design and development of novel red fluorescent proteins is one of the most important fronts in this field due to their potential of imaging the entire organism. A recent fluorescent protein mutant eqFP650-67-HqAla with the 8-hydroxyquinolin-imidazolinone (HQI) chromophore has the plausible bathochromic shift of ~30 nm in its emission spectrum wavelength comparing to the parent fluorescent protein eqFP650. However, molecular mechanism of this significant shift remains somewhat obscure. In this study, we carefully benchmarked our computational methods and performed extensive calculations to investigate various structural components' effect on the chromophore's emission energy and decipher the molecular origin of the spectral shift. The influences of conjugation size, substituent group, substituent site as well as the number of substituents have been examined by elaborately designed chromophore derivatives. Accordingly, we proposed several chromophore mutants with dramatic bathochromic shift of up to ~60 nm in their emission spectra. We further evaluated their structural stability in the protein using molecular dynamics simulations. Present theoretical study connects the structural feature of chromophore derivatives in red fluorescent proteins with their splendid performances in shifting the emission frequency and offer the molecular insight. The computational protocol and successive examination procedure to extract the structural effect utilized herein can also be widely applied to other fluorescent proteins in general. © 2018 Wiley Periodicals, Inc.


Assuntos
Imidazolinas/química , Proteínas Luminescentes/síntese química , Proteínas Luminescentes/genética , Mutação , Oxiquinolina/química , Teoria da Densidade Funcional , Proteínas Luminescentes/química , Conformação Molecular , Simulação de Dinâmica Molecular , Engenharia de Proteínas
15.
Inorg Chem ; 57(15): 9205-9214, 2018 Aug 06.
Artigo em Inglês | MEDLINE | ID: mdl-30024149

RESUMO

Metallabenzenes, the organometallic counterparts of benzene with one of the C atoms being replaced by a metal atom, expand the family of aromatics and further create prospective candidates for novel applications as functional materials. One intriguing feature of these complexes is that their MC5 rings do not always constrict into a planar configuration as in the C6 ring of benzene. Such a deviation has often been attributed to the unfavorable antibonding interactions between an occupied metal d orbital and the π orbitals of the C5 moiety. We herein scrutinize the frontier orbital interactions in both σ and π spaces in a plethora of metallabenzene complexes using extensive density functional theory calculations. Unexpectedly, the nonplanarity in metallabenzenes is found to be hardly related to the π orbitals. It is the antibonding interaction between an occupied metal d orbital and the σ orbitals of the C5 moiety that dominates the observed distortion. Such a σ-control mechanism not only provides an explanation for the commonly observed nonplanarity in metallabenzenes but also points out a novel direction toward the rational design of functional materials with enhanced metalla-aromaticity.

16.
Phys Chem Chem Phys ; 19(3): 2417-2424, 2017 Jan 18.
Artigo em Inglês | MEDLINE | ID: mdl-28058426

RESUMO

In this work, five new palladium(ii) complexes have been designed as the model catalysts for methane to methyl trifluoroacetate conversion. All these compounds are analogues of the well-established (bis-NHC)PdBr2 complex (NHC, N-heterocyclic carbenes), derived by complexing the palladium(ii) metal ion with the derivatives of bis-2-borabicyclo[1.1.0]but-1(3)-ene (bis-2BB) ligands using the sp2 carbons. Our density functional theory calculation results suggest that the (bis-2BB)PdBr2 catalysts outperform the popular (bis-NHC)PdBr2 complex in the desired catalytic process, and further reveal that the charge-shift bonding in the bis-2BB ligands contributes to the improved catalytic performance. These findings may spark new ideas for experimental design of more efficient organometallic catalysts for C-H bond activation and functionalization.

17.
J Chem Phys ; 146(2): 024103, 2017 Jan 14.
Artigo em Inglês | MEDLINE | ID: mdl-28088161

RESUMO

Although energy barriers can be efficiently crossed in the reaction coordinate (RC) guided sampling, this type of method suffers from identification of the correct RCs or requirements of high dimensionality of the defined RCs for a given system. If only the approximate RCs with significant barriers are used in the simulations, hidden energy barriers with small to medium height would exist in other degrees of freedom (DOFs) relevant to the target process and consequently cause the problem of insufficient sampling. To address the sampling in this so-called hidden barrier situation, here we propose an effective approach to combine temperature accelerated molecular dynamics (TAMD), an efficient RC-guided sampling method, with the integrated tempering sampling (ITS), a generalized ensemble sampling method. In this combined ITS-TAMD method, the sampling along the major RCs with high energy barriers is guided by TAMD and the sampling of the rest of the DOFs with lower but not negligible barriers is enhanced by ITS. The performance of ITS-TAMD to three systems in the processes with hidden barriers has been examined. In comparison to the standalone TAMD or ITS approach, the present hybrid method shows three main improvements. (1) Sampling efficiency can be improved at least five times even if in the presence of hidden energy barriers. (2) The canonical distribution can be more accurately recovered, from which the thermodynamic properties along other collective variables can be computed correctly. (3) The robustness of the selection of major RCs suggests that the dimensionality of necessary RCs can be reduced. Our work shows more potential applications of the ITS-TAMD method as the efficient and powerful tool for the investigation of a broad range of interesting cases.


Assuntos
Conceitos Matemáticos , Proteínas/química , Termodinâmica , Dipeptídeos/química , Transferência de Energia , Isomerismo , Simulação de Dinâmica Molecular , Conformação Proteica , Temperatura
18.
Inorg Chem ; 54(4): 1314-24, 2015 Feb 16.
Artigo em Inglês | MEDLINE | ID: mdl-25646570

RESUMO

Because formic acid can be effectively decomposed by catalysis into very pure hydrogen gas, the synthesis of formic acid, especially using CO and H2O as an intermediate of the water gas shift reaction (WGSR), bears important application significance in industrial hydrogen gas production. Here we report a theoretical study on the mechanism of efficient preparation of formic acid using CO and H2O catalyzed by a water-soluble [Ru(3+)]-EDTA complex. To determine the feasibility of using the [Ru(3+)]-EDTA catalyst to produce CO-free hydrogen gas in WGSR, two probable reaction paths have been examined: one synthesizes formic acid, while the other converts the reactants directly into CO2 and H2, the final products of WGSR. Our calculation results provide a detailed mechanistic rationalization for the experimentally observed selective synthesis of HCOOH by the [Ru(3+)]-EDTA catalyst. The results support the applicability of using the [Ru(3+)]-EDTA catalyst to efficiently synthesize formic acid for hydrogen production. Careful analyses of the electronic structure and interactions of different reaction complexes suggest that the selectivity of the reaction processes is achieved through the proper charge/valence state of the metal center of the [Ru(3+)]-EDTA complex. With the catalytic roles of the ruthenium center and the EDTA ligand being carefully understood, the detailed mechanistic information obtained in this study will help to design more efficient catalysts for the preparation of formic acid and further to produce CO-free H2 at ambient temperature.

19.
J Am Chem Soc ; 136(20): 7209-12, 2014 May 21.
Artigo em Inglês | MEDLINE | ID: mdl-24802277

RESUMO

A porous metal-organic framework composite with flexible anion-exchange polymers threaded within the host cavity demonstrates very fast and reversible ion-exchange activity. Polyvinyl benzyl trimethylammonium hydroxide (PVBTAH) caged in ZIF-8 is synthesized in steps of chloro-monomer impregnation, in situ polymerization, amination, and alkaline ion exchange. The synthesized non-cross-linked PVBTAH∼ZIF-8 material exhibits superior ion-exchange kinetics compared to conventional ion-exchange resins.

20.
Org Biomol Chem ; 10(47): 9491-500, 2012 Dec 21.
Artigo em Inglês | MEDLINE | ID: mdl-23132377

RESUMO

Here we present a systematic theoretical investigation on the mechanisms of Grignard reagent formation (GRF) for CH(3)Cl reacting with Mg atom, Mg(2) and a series of Mg clusters (Mg(4)-Mg(20)). Our calculations reveal that the ground state Mg atom is inactive under matrix condition, whereas it is active under metal vapor synthesis (MVS) conditions. On the other hand, the excited state Mg ((3)P) atom, as produced by laser-ablation, can react with CH(3)Cl barrierlessly, and hence is active under matrix condition. We predict that the bimagnesium Grignard reagent, though often proposed, can barely be observed experimentally, due to its high reactivity towards additional CH(3)Cl to produce more stable Grignard reagent dimer, and that the cluster Grignard reagent RMg(4)X possesses a flat Mg(4) unit rather than a tetrahedral geometry. Our calculations further reveal that the radical pathway (T4) is prevalent on Mg, Mg(2) and Mg(n) clusters of small size, while the no-radical pathway (T2), which starts at Mg(4), becomes competitive with T4 as the cluster size increases. A structure-reactivity relationship between barrier heights and ionization potentials of Mg(n) is established. These findings not only resolve controversy in experiment and theory, but also provide insights which can be used in the design of effective synthesis approaches for the preparation of chiral Grignard reagents.

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