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| 1 | Challenges and Prospects of Molecular Spintronics显示文摘Molecular spintronics,as an emerging field that makes full use of the advantage of ultralong room-temperature spin lifetime and abundant electrical-optical-magnetic properties of molecular semiconductors,has gained wide attention for its great potential for further commercial applications.Despite the significant progress that has been made,there remain several huge challenges that limit the future development of this field.This Perspective provides discussions on the spin transport mechanisms and performances of molecular semiconductors,spinterface effect,and related spin injection in spintronic devices,and current spin-charge interactive functionalities,along with the summarization of the main obstacles of these aspects.Furthermore,we particularly propose targeted solutions,aiming to enhance the spin injection and transport efficiency by molecular design and interface engineering and explore diverse spinrelated functionalities.Through this Perspective,we hope it will help the spintronic community identify the research trends and accelerate the development of molecular spintronics. | Xianrong Gu Lidan Guo Yang Qin Tingting Yang Ke Meng Shunhua Hu Xiangnan Sun | 2024 | Precision Chemistry2024，2，1： | 0 |
| 2 | α,β-Dehydroamino Acid Synthesis through Proline-Catalyzed Aldol Condensation with a Glycine Schiff Base显示文摘A general protocol for the synthesis ofα,β-dehydroamino acids and their peptides was developed.Proline efficiently catalyzed an aldol condensation reaction of a glycine Schiff base with a variety of aldehydes.The hydroxy group on the benzophenone imine was crucial for high Z/E selectivity and further transimination for protecting group-freeα,β-dehydroamino esters.Peptide elongation of both the C-and N-terminals highlighted the usefulness of our present protocol. | Jun Sawamura Daikan Ieiri Ryo Yazaki Takashi Ohshima | 2024 | Precision Chemistry2024，2，1： | 0 |
| 3 | Versatile Organogels of Aluminum Oxide Subnanosheets for Locking Solvents and Adhesion显示文摘Herein,we present a facile strategy to prepare versatile aluminum oxide subnanometer nanosheets with oleic acid and stearic acid ligands(OA-Al SNSs and SA-Al SNSs,respectively).The size effect endows subnanosheets with abundant acting sites,remarkable intermolecular interactions,and unique polymer-like properties,including flexibility,viscoelasticity,and sol-gel transitions,which is quite different from traditional inorganic materials.Consequently,subnanosheets could form freestanding organogels and OA-Al SNSs exhibit satisfying semisolidification of various solvents,making it an intriguing candidate for the safe storage and transportation of solvents.Furthermore,SA-Al SNSs exhibit excellent adhesive properties of high strength on diverse substrates,and it is easy to erase it without any damage,demonstrating the promising prospects in practical applications. | Wanyue Ouyang Xun Wang | 2024 | Precision Chemistry2024，2，1： | 0 |
| 4 | Synthesis,Structures,and Chiroptical Properties of NBN-Doped Helicenes with Boron Atoms in the Inner Rims显示文摘The precise synthesis of helicenes with topologically defined length and specific heteroatomic perturbation in the screw-like conjugated skeletons plays an emerging role in the manipulation of chiral materials.Facile,selective,and programmable routes to helicenes or heterohelicenes are highly desirable yet challenging for structure-chiroptical property relationship studies.Herein,we report the synthesis and characterization of NBN-doped helicenes with boron atoms in the inner rims,enabled by the highly regioselective one-pot borylation of rationally designed precursors with,namely,fold-in or pan-out manner.The incorporation of nonbonded boron and nitrogen atoms resulted in narrow-band emission and improved optical properties for the single-stranded carbon helix.In addition,numbers and arrangement modes of fused six-membered rings have distinct effects on configurational stability and chiroptical properties,revealing that BN-[6]H with strong circular dichroism is a promising candidate for chiral sensors.The combination of experimental and theoretical studies on these helical structures might provide insights into the design of helically chiral small-molecule-based sensors or emitters. | Weiwen Zhuang Yujian Liu Ziqi Deng Yu Guo Philip C.Y.Chow David Lee Phillips Wei Jiang Zhaohui Wang Junzhi Liu | 2024 | Precision Chemistry2024，2，1： | 0 |
| 5 | A Trade-off between Solvation and Collision Activation in Steering Competing E2 and S_(N)2 Dynamics显示文摘The prototypical E2 elimination and SN2 sub-stitution reactions between microsolvated fluoride and ethyl bromide show unexpected dynamic behaviors in mechanistic evolution driven by solvation and collision activation.Considering the steric effects,the gas-phase selectivity favors an E2 pathway barely dependent on collision energies.Remarkably,base solvation steers the reaction in an effective way toward substitution at a near-thermal energy,whereas the governing high-energy events retain elimination.Chemical dynamics simulations reproduce exper-imental findings and uncover a crucial solute-solvent coupling in determining such competing processes.Interestingly,collision activation can tune the underlying atomistic dynamics essentially in the reactant entrance channel and cause a mechanism shift.These features for the ubiquitous competing E2/SN2 dynamics remain quite unknown,providing unique insight into reaction selectivity for complex chemical networks. | Hongyi Wang Xu Liu Siwei Zhao Gang Fu Wenqing Zhen Li Yang Jiaxu Zhang | 2024 | Precision Chemistry2024，2，1： | 0 |
| 6 | Challenges in Photocatalytic Carbon Dioxide Reduction显示文摘An energy crisis and significant anthropogenic CO_(2)emissions as a result of rising fossil fuel consumption have caused a rapid increase in global temperature.One of the best solutions to these two issues is thought to be the photocatalytic reduction of CO_(2)into value-added carbon-containing products.In this aspect,the main challenges mainly include the photocatalytic mechanism,reaction activity,and product selectivity,especially in ambiguous reaction pathways and product selectivity,an unclear charge transfer mechanism,and an overestimate of product yield.Therefore,in this perspective,we attempt to exhibit the discussion and in-depth analysis of the possible reaction pathways and product selectivity,the specific charge transfer mechanism,and the origin of carbon-containing products in phtocatalytic CO_(2)reduction.Besides,the fundamentals for photocatalytic CO_(2)reduction are also illustrated.Finally,the state-of-the-art challenges and perspectives in CO_(2)photoreduction are highlighted and discussed in detail.This perspective is expected to evoke more research attention for the photocatalytic reduction of CO_(2)into value-added products. | Guangfu Liao Guixiang Ding Bin Yang Chunxue Li | 2024 | Precision Chemistry2024，2，2： | 0 |
| 7 | An Automated,Highly Selective Reaction Monitoring Instrument Using Molecular Rotational Resonance Spectroscopy显示文摘Online monitoring of chemical reactions by using analytical chemistry tools is a powerful way to maximize control over these processes.In this paper,we demonstrate the use of molecular rotational resonance,an emerging and extraordinarily selective spectroscopic technique,to perform automated reaction monitoring measurements.An interface using a six-port valve with a calibrated sample loop,coupled to a temperature controlled inlet for analyte volatilization,was developed and tested.Two reactions were chosen for initial characterization:an amine-aldehyde condensation reaction to form an imine product and an isotopic exchange reaction of aβ-ketoester with keto-enol tautomerization.The spectrometer was able to provide kinetic information about the reaction and determine reaction completion.In the future,this system can be extended to detect and quantify impurities and characterize reaction selectivity,in addition to the reaction progress. | Ann Adele Byars Khushi R.Kompally Emily Mechnick Reilly E.Sonstrom Alexander Mikhonin Justin L.Neill Ruth Boetzel James MacGregor Courtney Talicska Jian Li Yizhou Liu | 2024 | Precision Chemistry2024，2，2： | 0 |
| 8 | Synthesis of Ultra-High-Molecular-Weight Polyethylene by Transition-Metal-Catalyzed Precipitation Polymerization显示文摘Ultra-high-molecular-weight polyethylene(UHMWPE)plays an important role in many important fields as engineering plastics.In this contribution,a precipitation polymerization strategy is developed by combination of highly active phosphino-phenolate nickel catalysts with polymer-insoluble solvent(heptane)to access UHMWPE(Mn up to 8.3×10^(6)g mol^(-1))with good product morphology,free-flowing characteristics,and great mechanical properties.Compared with the academically commonly used aromatic solvent(toluene),the utilization of heptane offers simultaneous enhancement in important parameters including activity,polymer molecular weight,and catalyst thermal stability.This system can also generate polar functionalized UHMWPE with molecular weight of up to 1.6×10^(6)g mol^(-1)in the copolymerization of ethylene with polar comonomers.More importantly,this precipitation polymerization strategy is generally applicable to several representative transition metal catalyst systems,leading to UHMWPE synthesis with good product morphology control. | Wenbing Wang Quan Wang Chen Zou Changle Chen | 2024 | Precision Chemistry2024，2，2： | 0 |
| 9 | Computational Screening of Pt1@Ti_(3)C_(2)T_(2)(T=O,S)MXene Catalysts for Water-Gas Shift Reaction显示文摘Single-atom catalysts(SACs)provide an oppor-tunity to elucidate the catalytic mechanism of complex reactions in heterogeneous catalysis.The low-temperature water-gas shift(WGS)reaction is an important industrial technology to obtain high purity hydrogen.Herein,we study the catalytic activity of Pt1@Ti_(3)C_(2)T_(2)(T=O,S)SACs,where one subsurface Ti atom with three T vacancies in the functionalized Ti_(3)C_(2)T_(2)(T=O,S)MXene is substituted by one Pt atom,for the low-temperature show that Pt1@Ti_(3)C_(2)T_(2)provides an excellent platform for the WGS reaction by its bowl-shaped vacancy derived from the Pt1 single atom and three T defects surrounding it.Especially,Pt1@Ti_(3)C_(2)S_(2)SAC has higher catalytic performance for the WGS reaction,due to the weaker electronegativity of the S atom than the O atom,which significantly reduces the energy barrier of H*migration in the WGS reaction,which is often the rate-determining step.In the most favorable redox mechanism of the WGS reaction on Pt1@Ti_(3)C_(2)S_(2),the rate-determining step is the dissociation of OH*into O*and H*with the energy barrier as low as 1.12 eV.These results demonstrate that Pt1@Ti_(3)C_(2)S_(2)is promising in the application of MXenes for low-temperature WGS reactions. | Yang Meng Haiyan Wang Jin-Xia Liang Chun Zhu Jun Li | 2024 | Precision Chemistry2024，2，2： | 0 |
| 10 | On-Surface Synthesis of Anthracene-Fused Zigzag Graphene Nanoribbons from 2,7-Dibromo-9,9′-bianthryl Reveals Unexpected Ring Rearrangements显示文摘On-surface synthesis has emerged as a powerful strategy to fabricate unprecedented forms of atomically precise graphene nanoribbons(GNRs).However,the on-surface synthesis of zigzag GNRs(ZGNR)has met with only limited success.Herein,we report the synthesis and on-surface reactions of 2,7-dibromo-9,9′-bianthryl as the precursor towardπ-extended ZGNRs.Characterization by scanning tunneling microscopy and high-resolution noncontact atomic force microscopy clearly demonstrated the formation of anthracene-fused ZGNRs.Unique skeletal rearrangements were also observed,which could be explained by intramolecular Diels-Alder cycloaddition.Theoretical calculations of the electronic properties of the anthracene-fused ZGNRs revealed spin-polarized edge-states and a narrow bandgap of 0.20 eV. | Xiushang Xu Amogh Kinikar Marco Di Giovannantonio Carlo A.Pignedoli Pascal Ruffieux Klaus Müllen Roman Fasel Akimitsu Narita | 2024 | Precision Chemistry2024，2，2： | 0 |
| 11 | γ-Butyrolactone Synthesis from Allylic Alcohols Using the CO_(2)Radical Anion显示文摘γ-Butyrolactone structures are commonly found in various natural products and serve as crucial building blocks in organic synthesis.Consequently,the development of methods for synthesizingγ-butyrolactones has garnered significant interest within the organic synthesis community.In this study,we present a direct and highly efficient approach for the synthesis ofγ-butyrolactones from allylic alcohols.Notably,this study represents the first instance ofγ-butyrolactone synthesis initiated by radical hydrocarboxylation using CO_(2)^(•–),generated from metal formates,followed by cyclization.This two-step process is achieved through the synergistic interaction of photoredox and hydrogen atom transfer(HAT)catalysis,resulting in the production ofγ-butyrolactones with exceptional efficiency.Additionally,when employingα,α-diaryl allylic alcohol derivatives as substrates,the reaction involves 1,2-aryl migration,which occurs concomitantly with CO_(2)^(•–)addition,leading to the formation of 4,5-substituted lactones in a good yield.The artificial force induced reaction(AFIR)method identified the preferred 1,2-aryl migration pathway along with potential byproduct pathways,in which the targeted 1,2-migration was found to be the most plausible pathway. | Saeesh R.Mangaonkar Hiroki Hayashi Wataru Kanna Suvankar Debbarma Yu Harabuchi Satoshi Maeda Tsuyoshi Mita | 2024 | Precision Chemistry2024，2，3： | 0 |
| 12 | Supported Cu/Ni Bimetallic Cluster Electrocatalysts Boost CO_(2) Reduction显示文摘Supported metal clusters with the integrated advantages of single-atom catalysts and conventional nanoparticles held great promise in the electrocatalytic carbon dioxide reduction(ECO_(2)R)operated at low overpotential and high current density.However,its precise synthesis and the understanding of synergisti-cally catalytic effects remain challenging.Herein,we report a facile method to synthesize the bimetallic Cu and Ni clusters anchored on porous carbon(Cu/Ni-NC)and achieve an enhanced ECO_(2)R.The aberration-corrected high-angle annular dark-field scanning transmission electron microscopy and synchrotron X-ray absorption spectroscopy were employed to verify the metal dispersion and the coordination of Cu/Ni clusters on NC.As a result of this route,the target Cu/Ni-NC exhibits excellent electrocatalytic performance including a stable 30 h electrolysis at 200 mA cm^(-2) with carbon monoxide Faradaic efficiency of∼95.1%using a membrane electrode assembly electrolysis cell.Combined with the in situ analysis of the surface-enhanced Fourier transform infrared spectroelectrochemistry,we propose that the synergistic effects between Ni and Cu can effectively promote the H_(2)O dissociation,thereby accelerate the hydrogenation of CO_(2)to*COOH and the overall reaction process. | Depeng Wang Jiazhi Wang Zhi Wang Ning Zhang Jianrong Zeng Haixia Zhong Xinbo Zhang | 2024 | Precision Chemistry2024，2，3： | 0 |
| 13 | Glycerol Electrooxidation over Precision-Synthesized Gold Nanocrystals with Different Surface Facets显示文摘Electrochemical glycerol oxidation(EGO)emerges as a promising route to valorize glycerol,an underutilized byproduct from biodiesel production,into value-added chemicals.This study employed three types of gold(Au)nanocrystals with controlled shapes to elucidate the facet-dependent electrocatalytic behavior in EGO.Octahedral,rhombic dodecahedral,and cubic Au nanocrystals with{111},{110},and{100}facets,respectively,were precisely synthesized with uniform size and shape.Rhombic dodecahedra exhibited the lowest onset potential for EGO due to facile AuOH formation,while octahedra showed enhanced electrochemical activity for glycerol oxidation and resistance to poisoning.In-situ FTIR analysis revealed that Au{111}surfaces selectively favored C_(2) products,whereas Au{100}surfaces promoted C_(3) product formation,highlighting the significant effect of facet orientation on EGO performance and informing catalyst design. | Hansen Mou Fang Lu Zechao Zhuang Qiaowan Chang Lihua Zhang Xiaobo Chen Yugang Zhang Jingguang G.Chen | 2024 | Precision Chemistry2024，2，3： | 0 |
| 14 | Thiol Ligand-Modified Au for Highly Efficient Electroreduction of Nitrate to Ammonia显示文摘Electroreduction of nitrate(NO_(3)-)to ammonia(NH_(3))is an environmentally friendly route for NH_(3)production,serving as an appealing alternative to the Haber-Bosch process.Recently,various noble metal-based electrocatalysts have been reported for electroreduction of NO_(3)-.However,the application of pure metal electrocatalysts is still limited by unsatisfactory performance,owing to the weak adsorption of nitrogen-containing intermediates on the surface of pure metal electrocatalysts.In this work,we report thiol ligand-modified Au nanoparticles as the effective electrocatalysts toward electroreduction of NO_(3)-.Specifically,three mercaptobenzoic acid(MBA)isomers,thiosalicylic acid(ortho-MBA),3-mercaptobenzoic acid(meta-MBA),and 4-mercaptobenzoic acid(para-MBA),were employed to modify the surface of the Au nanocatalyst.During the NO_(3)-electroreduction,para-MBA modified Au(denoted as para-Au/C)displayed the highest catalytic activity among these Au-based catalysts.At-1.0 V versus reversible hydrogen electrode(vs RHE),para-Au/C exhibited a partial current density for NH_(3)of 472.2 mA cm^(-2),which was 1.7 times that of the pristine Au catalyst.Meanwhile,the Faradaic efficiency(FE)for NH_(3)reached 98.7%at-1.0 V vs RHE for para-Au/C.The modification of para-MBA significantly improved the intrinsic activity of the Au/C catalyst,thus accelerating the kinetics of NO_(3)-reduction and giving rise to a high NH_(3)yield rate of para-Au/C. | Yuheng Wu Xiangdong Kong Yechao Su Jiankang Zhao Yiling Ma Tongzheng Ji Di Wu Junyang Meng Yan Liu Zhigang Geng Jie Zeng | 2024 | Precision Chemistry2024，2，3： | 0 |
| 15 | Synergy of Prediction Rule and Total Synthesis in Solving the Stereochemical Puzzle of Valactamides显示文摘Natural products with diverse functional groups and stereo-genic centers have inspired therapeutics and underpin the modern drug discovery process.Their three-dimensional molecular structures need to be unambiguously determined in order to be realized as clinical candidates or to achieve further activity-guided structural optimization.Although recent advances in spectroscopic methods have made it possible for researchers to determine the structures of microgram samples of complex natural products,there is no universally accepted method for determining the relative and absolute configuration of a naturally occurring compound.We report the determination of the full stereostructure of valactamide A,an eight-stereogenic-center-containing fungal metabolite by the synergy of prediction rule-guided analysis and chemical synthesis.The expedient total synthesis resulted in unambiguous verification of the predicted stereochemistry for valactamide A. | Tao Zhang Jiaxuan Feng Hideaki Oikawa Yian Guo Tao Ye | 2024 | Precision Chemistry2024，2，3： | 0 |
| 16 | Atomically Precise Imprinting π-Magnetism in Nanographenes via Probe Chemistry显示文摘The precise generation and harnessing of carbon magnetism at the single-molecule level have been captivating areas of research in chemistry and nanotechnology.However,the realization of magnetic nanographenes,also known as single-moleculeπ-magnets,through solution-based synthesis has proven challenging because of their high reactivity and insolubility tendency.Recent advancements in on-surface chemistry and scanning probe techniques have significantly propelled the fabrication of carbon-based magnetic nanostructures to offer a rich platform to probe quantumπ-magnetism at the single-molecule level.Atomic manipulation,also referred to as probe chemistry,stands as an exciting and essential approach in the toolbox of on-surface chemistry.This approach enables site-selective chemical reactions,thereby allowing for the atomically precise imprinting and tailoringπ-magnetism in a variety of nanographenes.This review highlights the recent achievements in the precise synthesis of single-moleculeπ-magnets using atomic manipulation.Furthermore,we also provide an outlook on the future of probe chemistry in the fabrication of this intriguing class of magnetic nanographenes,featuring designer quantum magnetism. | Jie Su Pin Lyu Jiong Lu | 2023 | Precision Chemistry2023，1，10： | 0 |
| 17 | Copper-Catalyzed Enantioconvergent Radical C(sp^(3))−N Cross- Coupling to Access Chiral α-Amino-β-lactams显示文摘A copper-catalyzed enantioconvergent radical C-(sp^(3))-N cross-coupling of racemic tertiaryα-bromo-β-lactams with aromatic amines is developed under mild thermal reaction conditions.The use of a sterically demanded oxazoline-derived sulfonamide N,N,N-ligand is crucial for the reaction initiation and effective enantio-discrimination of the azetidinone-derived cyclic alkyl radicals.The strategy provides an attractive approach to access chiralα-amino-β-lactams,an important structural motif in many biologically active molecules.Preliminary mechanistic studies support the formation of azetidinone-derived alkyl radicals from the L*Cu(I)-amido complex andα-bromo-β-lactams. | Jing-Jing Zheng Wei-Long Liu Qiang-Shuai Gu Zhong-Liang Li Ji-Jun Chen Xin-Yuan Liu | 2023 | Precision Chemistry2023，1，10： | 0 |
| 18 | Tetravalent Terbium Chelates: Stability Enhancement and Property Tuning显示文摘Coordination chemistry of rare-earth elements has been dominated by the+3 oxidation state.Complexes with higher-valence lanthanide ions are synthetically challenging but are of fundamental research interest and significance as advanced molecular materials.Herein,four tetravalent terbium complexes(2-5)of the common formula[Tb(OSiPh3)4L](L=ethylene glycol dimethyl ether(DME),2,2’-bipyridine(bpy),2,2’-bipyrimidine(bpym),and 1,10-phenanthroline(phen))are reported.Crystallographic analyses reveal in each of these complexes a hexacoordinate Tb(IV)ion situated in a distorted octahedral coordination environment formed by four triphenylsi-loxido ligands and a bidentate chelating ligand.The use of chelating ligands enhances the stability of the resulting complexes over their THF solvate precursor.More significantly,the aromatic N-chelating ligands have been found to tune effectively the electronic structures of the complexes,as evidenced by the sizable potential shifts observed for the quasi-reversible redox Tb(IV/III)process and by the changes in their absorption spectra.The experimental findings are augmented with quantum theoretical calculations in which the ligandπ-donation to the 5d orbitals of the Tb(IV)center is found to be primarily responsible for stability enhancement and the corresponding changes of physical properties observed.Magnetic measurements and results from electron paramagnetic resonance studies produced small absolute values of zero-field splittings of these complexes,ranging from 0.1071(22)to 1.1484(112)cm-1 and comparable to the values reported for analogous Tb(IV)complexes. | Tianjiao Xue You-Song Ding Xue-Lian Jiang Lizhi Tao Jun Li Zhiping Zheng | 2023 | Precision Chemistry2023，1，10： | 0 |
| 19 | Precision of Radiation Chemistry Networks: Playing Jenga with Kinetic Models for Liquid-Phase Electron Microscopy显示文摘Liquid-phase transmission electron microscopy(LP-TEM)is a powerful tool to gain unique insights into dynamics at the nanoscale.The electron probe,however,can induce significant beam effects that often alter observed phenomena such as radiolysis of the aqueous phase.The magnitude of beam-induced radiolysis can be assessed by means of radiation chemistry simulations potentially enabling quantitative application of LP-TEM.Unfortunately,the computational cost of these simulations scales with the amount of reactants regarded.To minimize the computational cost,while maintaining accurate predictions,we optimize the parameter space for the solution chemistry of aqueous systems in general and for diluted HAuCl4 solutions in particular.Our results indicate that sparsened kinetic models can accurately describe steady-state formation during LP-TEM and provide a handy prerequisite for efficient multidimensional modeling.We emphasize that the demonstrated workflow can be easily generalized to any kinetic model involving multiple reaction pathways. | Birk Fritsch Paolo Malgaretti Jens Harting Karl J.J.Mayrhofer Andreas Hutzler | 2023 | Precision Chemistry2023，1，10： | 0 |
| 20 | Simultaneous Dehalogenation and Hydrogenation in Sonogashira Coupling显示文摘We herein report a simultaneous dehalogenation and hydrogenation(DHH)reaction in Sonogashira coupling involving hexahalogenobenzene C6X6(X=I,Br),in which a halogen on the aryl polyhalide substrate was substituted by a hydrogen atom.First,a steric bulky terminal alkyne 5 was designed and synthesized to study the influence of the reaction conditions(e.g.,catalyst,solvent,temperature)and the halogens on the substrates C6X6 on the DHH reaction.Moreover,based on the optimized conditions,a terminal alkyne 6 with less steric hindrance was further synthesized to investigate the influence of alkyne on the DHH reaction.As a result,two aromatic polyynes 7 and 8 were were further studied and compared.The influence produced by the alkynes and aryl polyhalides substrate provide insights into Sonogashira coupling involving terminal alkyne with huge steric hindrance and polyhalogenated aromatic hydrocarbons. | Huafeng Chen Lei Zhai Yulan Zuo Xi Qin Jinling Zhang Kui Tian Peng Xu | 2023 | Precision Chemistry2023，1，10： | 0 |
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